Jurnal Inggris 1

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}

{\shp {\*\shpinst\shpleft816\shptop10142\shpright4306\shpbottom10542\shpfhdr0\
shpbxpage\shpbypage\shpwr3\shpwrk0\shpfblwtxt1\shpz10001\shplid10001
{\sp{\sn shapeType}{\sv 202}}{\sp{\sn fFlipH}{\sv 0}}{\sp{\sn fFlipV}{\sv 0}}{\sp{\
sn fRecolorFillAsPicture}{\sv 0}}{\sp{\sn fUseShapeAnchor}{\sv 0}}{\sp{\sn fLine}{\
sv 0}}{\sp{\sn fFilled}{\sv 0}}{\sp{\sn fLayoutInCell}{\sv 1}}{\sp{\sn
fBehindDocument}{\sv 1}}{\shptxt\pard\plain \qj\sl147 \li0\ri0 \expndtw0\
charscalex104\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1957;
Sun & He�le{\par}}}}\pard\sb0\sl-240{\bkmkstart Pg1}{\bkmkend Pg1}\par\pard\ql \
li7513\sb0\sl-207\slmult0 \par\pard\ql\li7513\sb142\sl-207\slmult0 \up0 \expndtw0\
charscalex100 \ul0\nosupersub\cf1\f2\fs18 J. Mol. Biol. (1996)\ul0\nosupersub\cf2\
f3\fs18 257\ul0\nosupersub\cf1\f2\fs18 , 1052-1069 \par\pard\qj \li956\sb0\sl-400\
slmult0 \par\pard\qj\li956\sb0\sl-400\slmult0 \par\pard\qj\li956\sb0\sl-400\slmult0
\par\pard\qj\li956\ri1604\sb174\sl-400\slmult0 \up0 \expndtw0\charscalex99 \ul0\
nosupersub\cf3\f4\fs36 Solution Structure of a Pyrimidine�Purine�Pyrimidine \up0 \
expndtw0\charscalex98 Triplex Containing the Sequence-specific Intercalating \up0 \
expndtw0\charscalex99 Non-natural Base D\ul0\sub\cf4\f5\fs29 3 \par\pard\qj \li956\
ri2042\sb227\sl-320\slmult0 \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf5\f6\
fs28 Edmond Wang\ul0\super\cf6\f7\fs24\ul0\super\cf6\f7\fs23 1\ul0\nosupersub\cf5\
f6\fs28 , Karl M. Koshlap\ul0\super\cf6\f7\fs24\ul0\super\cf6\f7\fs23 1\ul0\
nosupersub\cf5\f6\fs28 , Paul Gillespie\ul0\super\cf6\f7\fs24\ul0\super\cf6\f7\fs23
2\ul0\nosupersub\cf5\f6\fs28 , Peter B. Dervan\ul0\super\cf6\f7\fs24\ul0\super\cf6\
f7\fs23 2 \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf5\f6\fs28 and Juli Feigon\
ul0\super\cf6\f7\fs24\ul0\super\cf6\f7\fs23 1\ul0\nosupersub\cf5\f6\fs28 *\par\
pard\sect\sectd\sbknone\cols2\colno1\colw3664\colsr160\colno2\colw8276\colsr160\
ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb229\sl-230\slmult0 \up0 \
expndtw0\charscalex100 \ul0\super\cf8\f9\fs17\ul0\super\cf8\f9\fs16 1\ul0\
nosupersub\cf9\f10\fs20 Department of Chemistry\par\pard\ql \li956\sb1\sl-216\
slmult0 \up0 \expndtw0\charscalex101 and Biochemistry and\par\pard\qj \li956\ri381\
sb1\sl-219\slmult0 \up0 \expndtw-1\charscalex100 Molecular Biology Institute \up0 \
expndtw0\charscalex100 University of California\par\pard\ql \li956\sb0\sl-219\
slmult0 \up0 \expndtw0\charscalex101 Los Angeles, CA 90095, USA\par\pard\qj \li956\
ri386\sb120\sl-219\slmult0 \up0 \expndtw0\charscalex101 \ul0\super\cf8\f9\fs17\ul0\
super\cf8\f9\fs16 2\ul0\nosupersub\cf9\f10\fs20 Division of Chemistry and \up0 \
expndtw-2\charscalex100 Chemical Engineering\par\pard\ql \li956\sb0\sl-219\
slmult0 \up0 \expndtw0\charscalex100 California Institute of\par\pard\ql \li956\
sb0\sl-219\slmult0 \up0 \expndtw-5\charscalex100 Technology, Pasadena\par\pard\ql \
li956\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex101 CA 91125, USA\par\pard\ql \
li956\sb0\sl-207\slmult0 \par\pard\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \
li956\sb0\sl-207\slmult0 \par\pard\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \
li956\sb0\sl-207\slmult0 \par\pard\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \
li956\sb63\sl-207\slmult0 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf14\f15\
fs18 *Corresponding author\par\pard\column \ql \li3824\sb0\sl-230\slmult0 \par\
pard\ql \li20\sb229\sl-230\slmult0 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\
cf7\f8\fs20 We have used NMR spectroscopy to study a pyrimidine�purine�pyrimidine\
par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-1\charscalex100 DNA
triplex containing a non-natural base, 1-(2-deoxy-\ul0\nosupersub\cf10\f11\fs20 b\
ul0\nosupersub\cf7\f8\fs20 -\ul0\nosupersub\cf11\f12\fs16 D\ul0\nosupersub\cf7\f8\
fs20 -ribofuranosyl)-\line \up0 \expndtw-1\charscalex100 4-(3-
benzamido)phenylimidazole (D\ul0\sub\cf8\f9\fs16 3\ul0\nosupersub\cf7\f8\fs20 ), in
the third strand. The D\ul0\sub\cf8\f9\fs16 3\ul0\nosupersub\cf7\f8\fs20 base has
\line \up0 \expndtw-2\charscalex100 been previously shown to specifically recognize
T�A and C�G base-pairs\ul0\nosupersub\cf9\f10\fs20 via \line \up0 \expndtw0\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 intercalation on the 3' side (with
respect to the purine strand) of the target \line \up0 \expndtw0\charscalex101 base
pair, instead of forming sequence-specific hydrogen bonds. \up0 \expndtw-2\
charscalex100 \ul0\super\cf8\f9\fs17\ul0\super\cf8\f9\fs16 1\ul0\nosupersub\cf7\f8\
fs20 H\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex101
resonance assignments have been made for the D\ul0\sub\cf8\f9\fs16 3\ul0\
nosupersub\cf7\f8\fs20 base and most of the \line \up0 \expndtw0\charscalex102
non-loop portion of the triplex. The solution structure of the triplex was \line \
up0 \expndtw0\charscalex100 calculated using restrained molecular dynamics and
complete relaxation \line \up0 \expndtw-1\charscalex100 matrix refinement. The
duplex portion of the triplex has an over-all helical \line \up0 \expndtw0\
charscalex100 structure that is more similar to\ul0\nosupersub\cf9\f10\fs20
B\ul0\nosupersub\cf7\f8\fs20 -DNA than to\ul0\nosupersub\cf9\f10\fs20 A\ul0\
nosupersub\cf7\f8\fs20 -DNA. The three \line \up0 \expndtw0\charscalex103
aromatic rings of the D\ul0\sub\cf8\f9\fs16 3\ul0\nosupersub\cf7\f8\fs20 base
stack on the bases of all three strands and \line \up0 \expndtw-3\charscalex100
mimic a triplet. The conformation of the D\ul0\sub\cf8\f9\fs16 3\ul0\nosupersub\
cf7\f8\fs20 base and its sequence specificity \line \up0 \expndtw-1\charscalex100
are discussed.\par\pard\ql \li3944\sb9\sl-207\slmult0 \up0 \expndtw0\
charscalex104 \ul0\nosupersub\cf12\f13\fs18 7\ul0\nosupersub\cf13\f14\fs18 1996
Academic Press Limited\par\pard\qj \li20\ri2258\sb103\sl-219\slmult0 \up0 \
expndtw0\charscalex100 \ul0\nosupersub\cf9\f10\fs20 Keywords:\ul0\nosupersub\cf7\
f8\fs20 DNA; triplex; NMR; 2DNMR; triple helix; triple strand; \up0 \expndtw-4\
charscalex100 intercalator\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\
colsr160\colno2\colw6244\colsr160\ql \li956\sb0\sl-276\slmult0 \par\pard\ql \li956\
sb0\sl-276\slmult0 \par\pard\ql \li956\sb39\sl-276\slmult0 \up0 \expndtw-3\
charscalex100 \ul0\nosupersub\cf15\f16\fs24 Introduction\par\pard\qj \li956\ri149\
sb130\sl-219\slmult0\fi199 \up0 \expndtw-4\charscalex100 \ul0\nosupersub\cf7\f8\
fs20 Canonical nucleic acid triplexes are formed by the \line \up0 \expndtw0\
charscalex100 binding of a single strand in the major groove of a \line \up0 \
expndtw-3\charscalex100 homopurine�homopyrimidine duplex \up0 \expndtw-3\
charscalex100 (Felsenfeld\par\pard\ql \li2996\sb1\sl-219\slmult0 \up0 \expndtw0\
charscalex102 `ne, 1993; Moser & Dervan,\par\pard\ql \li956\sb0\sl-219\slmult0 \up0
\expndtw-1\charscalex100 1987; Wells\ul0\nosupersub\cf9\f10\fs20 et al\ul0\
nosupersub\cf7\f8\fs20 ., \up0 \expndtw-2\charscalex100 1988). Two general
motifs for\par\pard\qj \li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw-1\
charscalex100 triplexes exist, parallel and anti-parallel, which are \line \up0 \
expndtw-1\charscalex100 defined by their third strand orientation relative to \line
\up0 \expndtw-1\charscalex100 the homopurine strand in the Watson-Crick paired \
line \up0 \expndtw-1\charscalex100 target duplex. In parallel triplexes, the third
strand \line \up0 \expndtw0\charscalex106 is homopyrimidine and binds parallel
to the \line \up0 \expndtw0\charscalex100 homopurine strand of the duplex. A
protonated C \line \up0 \expndtw0\charscalex104 in the third strand binds to a G in
the duplex\ul0\nosupersub\cf9\f10\fs20 via \line \up0 \expndtw-2\charscalex100 \
ul0\nosupersub\cf7\f8\fs20 Hoogsteen base-pairing forming a C\ul0\super\cf16\
f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 �G�C triplet.\par\
pard\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \li956\sb0\sl-207\slmult0 \par\pard\
ql \li1135\sb33\sl-207\slmult0 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf13\
f14\fs18 Abbreviations used: D\ul0\nosupersub\cf17\f18\fs10 3\ul0\nosupersub\cf13\
f14\fs18 , 1-(2-deoxy-\ul0\nosupersub\cf12\f13\fs18 b\ul0\nosupersub\cf13\f14\fs18
-\ul0\nosupersub\cf18\f19\fs14 D\ul0\nosupersub\cf13\f14\fs18 -\par\pard\ql \li956\
ri151\sb0\sl-199\slmult0\fi0 \up0 \expndtw-2\charscalex100 ribofuranosyl)-4-(3-
benzamido)phenylimidazole; DTA \up0 \expndtw-4\charscalex100 triplex, d(AGA\ul0\
nosupersub\cf19\f20\fs18 T\ul0\nosupersub\cf13\f14\fs18 AGAACCCCTTCT\ul0\
nosupersub\cf19\f20\fs18 A\ul0\nosupersub\cf13\f14\fs18 TCTTATATCT\ul0\nosupersub\
cf19\f20\fs18 D\ul0\nosupersub\cf17\f18\fs10 3\ul0\nosupersub\cf13\f14\fs18 -\
line \up0 \expndtw-1\charscalex100 TCTT; NOE, nuclear Overhauser enhancement;
NOESY, \up0 \expndtw-2\charscalex100 NOE spectroscopy; P.COSY, purged correlation\
par\pard\qj \li956\ri351\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100
spectroscopy; HOHAHA, Homonuclear-Hartmann-\line \up0 \expndtw0\charscalex100 Hahn;
HOENOE, HOHAHA edited NOESY; HMQC, \up0 \expndtw-1\charscalex100 Heteronuclear
multiple quantum coherence\par\pard\qj \li956\ri351\sb0\sl-199\slmult0 \up0 \
expndtw-1\charscalex100 spectroscopy; RMSD, root-mean-squared deviation; \up0 \
expndtw-1\charscalex100 FPLC, fast protein liquid chromatography; VDW, van \up0 \
expndtw-2\charscalex100 der Waals. \par\pard\qj\pvpg\phpg\posx956\posy15381\
absw2553 \ul0\nosupersub\cf11\f12\fs16 0022-2836/96/151052-18\par\pard\ql \li2795\
sb0\sl-184\slmult0 \par\pard\ql \li2795\sb182\sl-184\slmult0 \up0 \expndtw0\
charscalex105 $18.00/0\par\pard\column \ql \li5856\sb0\sl-230\slmult0 \par\pard\
ql \li5856\sb0\sl-230\slmult0 \par\pard\ql \li20\sb089\sl-230\slmult0 \up0 \
expndtw-2\charscalex100 \ul0\nosupersub\cf7\f8\fs20 Similarly, a T in the third
strand recognizes an A in\par\pard\ql \li20\ri1643\sb0\sl-219\slmult0\tx229 \up0 \
expndtw0\charscalex102 the duplex forming a T�A�T triplet (de los Santos \line \
up0 \expndtw0\charscalex103 \ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\
f8\fs20 ., 1989; Le Doan\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\
fs20
., 1987; Moser & Dervan, \line \up0 \expndtw-1\charscalex100 1987; Rajagopal &
Feigon, 1989a,b). In anti-parallel \line \up0 \expndtw0\charscalex102 triplexes,
the third strand is homopurine or a \line \up0 \expndtw0\charscalex106
mixture of purines and thymines, and binds \line \up0 \expndtw0\charscalex104
anti-parallel to the homopurine strand of the \line \up0 \expndtw-2\
charscalex100 duplex. The G�C and A�T base-pairs are recognized \line \up0 \
expndtw-5\charscalex100 by a G and A (or T), respectively, forming G�G�C and \
line \up0 \expndtw0\charscalex100 A�A�T (or T�A�T) triplets\ul0\nosupersub\cf9\
f10\fs20 via\ul0\nosupersub\cf7\f8\fs20 reverse Hoogsteen \line \up0 \
expndtw0\charscalex100 base-pairing (Beal & Dervan, 1991; Broitman\ul0\nosupersub\
cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., \line \up0 \expndtw0\
charscalex101 1987; Lipsett, 1964; Radhakrishnan\ul0\nosupersub\cf9\f10\fs20 et
al\ul0\nosupersub\cf7\f8\fs20 ., 1991). \line\tab \up0 \expndtw0\charscalex102 The
possibility of targeting genes with high \line \up0 \expndtw0\charscalex101
sequence specificity makes triplexes potentially \line \up0 \expndtw-4\
charscalex100 versatile biochemical tools. Triplexes have been used \line \up0 \
expndtw-4\charscalex100 for gene regulation (Cooney\ul0\nosupersub\cf9\f10\fs20 et
al\ul0\nosupersub\cf7\f8\fs20 ., 1988; Degols\ul0\nosupersub\cf9\f10\fs20 et al\
ul0\nosupersub\cf7\f8\fs20 ., \line \up0 \expndtw-1\charscalex100 1994; Grigoriev\
ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., \up0 \expndtw-1\
charscalex100 1992; Maher, 1992), DNA\par\pard\ql \li20\sb1\sl-217\slmult0 \
up0 \expndtw-3\charscalex100 isolation and detection \up0 \expndtw0\charscalex101
(Ji\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., \up0 \
expndtw-1\charscalex100 1994; Olivas &\par\pard\qj \li20\ri1643\sb1\sl-219\
slmult0 \up0 \expndtw0\charscalex101 Maher, 1994) and DNA modification (Havre\ul0\
nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., \line \up0 \expndtw0\
charscalex101 1993; Luebke & Dervan, 1991). While most DNA-\line \up0 \expndtw-2\
charscalex100 binding proteins are limited to recognition of a few \line \up0 \
expndtw-1\charscalex100 base-pairs of DNA, triplex formation can easily \line
\up0 \expndtw-2\charscalex100 encompass sequences longer than ten base-pairs \
line \up0 \expndtw-2\charscalex100 with a mismatch discrimination comparable to
that \line \up0 \expndtw-3\charscalex100 of duplex formation (Greenberg &
Dervan, 1995; \line \up0 \expndtw0\charscalex100 Mergny\ul0\nosupersub\cf9\f10\
fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1991; Roberts & Crothers, 1991). \
line \up0 \expndtw-3\charscalex100 Triplexes could potentially be designed to
recognize \par\pard\qj\pvpg\phpg\posx8102\posy15381\absw2395 \ul0\nosupersub\cf20\
f21\fs14 7\ul0\nosupersub\cf11\f12\fs16 1996 Academic Press Limited\par\pard\sect\
sectd\fs24\paperw12240\paperh15840{\shp
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4514500145145001451450014514500145145001451450014514500145145007fffd9}}}}}\pard\
sb0\sl-240{\bkmkstart Pg2}{\bkmkend Pg2}\par\pard\li956\sb0\sl-218\slmult0\par\
pard\li956\sb151\sl-218\slmult0\fi0\tx9955 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\
ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1053\par\pard\qj \li5856\sb0\sl-220\
slmult0 \par\pard\qj\li5856\ri1623\sb192\sl-220\slmult0\fi0 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 NMR spectroscopy demonstrated that this
D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 -con-\line \up0 \expndtw0\
charscalex100 taining oligonucleotide forms an intramolecular \line \up0 \
expndtw-4\charscalex100 triplex, with a CCCC and a TATA loop connect-\
line \up0 \expndtw-1\charscalex100 ing the Watson-Crick and the Hoogsteen-
paired \line \up0 \expndtw-1\charscalex100 strands, respectively \up0 \expndtw-1\
charscalex100 (Koshlap\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\
fs20 ., \up0 \expndtw-2\charscalex100 1993) \up0 \expndtw-2\charscalex100 (Fig-\
par\pard\qj \li5856\ri1623\sb0\sl-220\slmult0 \up0 \expndtw0\charscalex101 ure
1(b)). This study also revealed that instead of \line \up0 \expndtw-3\charscalex100
hydrogen-bonding to the Watson-Crick base-pair, \line \up0 \expndtw0\
charscalex101 the D\ul0\sub\cf16\f17\fs18 3 \up0 \expndtw0\charscalex100 \ul0\
nosupersub\cf7\f8\fs20 base intercalates between its target T�A \line \up0 \
expndtw-3\charscalex100 base-pair and the adjacent 3' T�A�T triplet (i.e 3' with \
line \up0 \expndtw-3\charscalex100 respect to the purine strand). Here we present
the \par\pard\ql \li5856\sb0\sl-180\slmult0\tx6016 \up2 \expndtw-2\charscalex100 \
ul0\nosupersub\cf16\f17\fs12 1 \tab \dn4 \expndtw-1\charscalex100 \ul0\nosupersub\
cf7\f8\fs20 H NMR assignments and solution structure of the \par\pard\qj \li5856\
ri1623\sb41\sl-220\slmult0 \up0 \expndtw-3\charscalex100 DTA triplex. The structure
reveals that intercalation \line \up0 \expndtw-4\charscalex100 of the D\ul0\sub\
cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base is readily accommodated and that
the \par\pard\li956\sb1\sl-227\slmult0\fi4900\tx6219 \up0 \expndtw0\charscalex101
D\ul0\sub\cf16\f17\fs18 3\tab \up0 \expndtw0\charscalex101 \ul0\nosupersub\cf7\f8\
fs20 base mimics a triplet. The over-all helical\par\pard\li956\sb1\sl-217\
slmult0\fi4900 \up0 \expndtw0\charscalex101 structure is more similar to\ul0\
nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -DNA than to\ul0\nosupersub\
cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -DNA.\par\pard\li956\sb1\sl-219\slmult0\
fi4900 \up0 \expndtw0\charscalex101 The effect of the D\ul0\sub\cf16\f17\fs18 3\
ul0\nosupersub\cf7\f8\fs20 base intercalation in a triplex\par\pard\sect\sectd\
sbknone\cols2\colno1\colw5696\colsr160\colno2\colw6244\colsr160\ql \li1135\sb49\sl-
207\slmult0 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\cf19\f20\fs18 Figure 1.\
ul0\nosupersub\cf13\f14\fs18 (a) Chemical structure of the D\ul0\nosupersub\cf8\
f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base with the\par\pard\qj \li956\ri149\
sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 atom numbering scheme. The torsion
angles N3A-C4A-\line \up0 \expndtw-2\charscalex100 C1B-C2B (\ul0\nosupersub\cf12\
f13\fs18 u\ul0\nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 ), C2B-C3B-N-
C (\ul0\nosupersub\cf12\f13\fs18 u\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\
cf13\f14\fs18 ) and N-C-C1C-C2C (\ul0\nosupersub\cf12\f13\fs18 u\ul0\nosupersub\
cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 ) \line \up0 \expndtw-1\charscalex100
are indicated. (b) Folding schematic drawing of the DTA \line \up0 \expndtw0\
charscalex102 triplex with the residue numbering scheme used in the \line \up0 \
expndtw-1\charscalex100 text. The Watson-Crick base-pairs are indicated by filled \
line \up0 \expndtw0\charscalex101 circles, the Hoogsteen base-pairs are indicated
by open \line \up0 \expndtw0\charscalex102 circles, and the protonated C Hoogsteen
base-pairs are \line \up0 \expndtw0\charscalex103 indicated with a +.\par\pard\qj \
li956\sb0\sl-219\slmult0 \par\pard\qj \li956\ri149\sb124\sl-219\slmult0 \up0 \
expndtw-2\charscalex100 \ul0\nosupersub\cf7\f8\fs20 a single site in an entire
genome (Strobel & Dervan, \line \up0 \expndtw-3\charscalex100 1991; Strobel\ul0\
nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1991). Unfortunately,
recognition \line \up0 \expndtw-3\charscalex100 by the third strand is limited to
only two of the four \line \up0 \expndtw-1\charscalex100 possible base-pairs. To
some extent a T�A base-pair \line \up0 \expndtw0\charscalex100 can be recognized by
a G (Griffin & Dervan, 1989) \line \up0 \expndtw0\charscalex101 and possibly a C
(Belotserkovskii\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 .,
1990), and \line \up0 \expndtw0\charscalex105 a C�G base-pair can be recognized by
a T (Yoon \line \up0 \expndtw0\charscalex102 \ul0\nosupersub\cf9\f10\fs20 et al\
ul0\nosupersub\cf7\f8\fs20 ., \up0 \expndtw-1\charscalex100 1992), but triplexes
containing these non-\par\pard\qj \li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw-
2\charscalex100 canonical triplets are less stable. Also, since a C and \up0 \
expndtw0\charscalex103 T already recognize a G�C and A�T base-pair, \up0 \
expndtw0\charscalex104 respectively, sequence specificity is lost when \up0 \
expndtw-1\charscalex100 employing such alternative triplets.\par\pard\ql \li1155\
sb0\sl-219\slmult0 \up0 \expndtw-1\charscalex100 The non-natural
deoxyribonucleoside, \up0 \expndtw-3\charscalex100 1-(2-de-\par\pard\qj \li956\
ri149\sb0\sl-219\slmult0\fi0 \up0 \expndtw-2\charscalex100 oxy-\ul0\nosupersub\
cf10\f11\fs20 b\ul0\nosupersub\cf7\f8\fs20 -\ul0\nosupersub\cf11\f12\fs16 D\ul0\
nosupersub\cf7\f8\fs20 -ribofuranosyl)-4-(3-benzamido)phenylimi-\line \up0 \
expndtw-2\charscalex100 dazole (D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\
fs20 ) (Figure 1(a)) was designed to recognize \up0 \expndtw0\charscalex103 a C�G
base-pair by forming specific hydrogen \up0 \expndtw-4\charscalex100 bonds \up0
\expndtw0\charscalex103 (Griffin\ul0\nosupersub\cf9\f10\fs20 et al\ul0\
nosupersub\cf7\f8\fs20 ., \up0 \expndtw-1\charscalex100 1992). However, chemical\
par\pard\qj \li956\ri149\sb1\sl-219\slmult0 \up0 \expndtw-2\charscalex100
footprinting studies found that when the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\
cf7\f8\fs20 base is \line \up0 \expndtw-3\charscalex100 incorporated into a
pyrimidine oligonucleotide it \line \up0 \expndtw-2\charscalex100 recognizes
both T�A and C�G base-pairs (Griffin \line \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1992). Moreover,
recognition was found to be \line \up0 \expndtw0\charscalex105 strongly dependent
on the identity of the \up0 \expndtw-2\charscalex100 3'\par\pard\qj \li956\
ri149\sb0\sl-219\slmult0 \up0 \expndtw-3\charscalex100 neighboring triplet (i.e. 3'
with respect to the purine \line \up0 \expndtw-1\charscalex100 strand) but only
weakly dependent on the identity \line \up0 \expndtw-2\charscalex100 of the 5'
neighboring triplet (Griffin\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\
cf7\f8\fs20 ., \up0 \expndtw-2\charscalex100 1992;\par\pard\qj \li956\ri149\sb1\sl-
219\slmult0 \up0 \expndtw-3\charscalex100 Kiessling\ul0\nosupersub\cf9\f10\fs20
et al\ul0\nosupersub\cf7\f8\fs20 ., 1992). In order to investigate the \
up0 \expndtw0\charscalex108 binding mode of the D\ul0\sub\cf16\f17\fs18 3 \
up0 \expndtw0\charscalex108 \ul0\nosupersub\cf7\f8\fs20 base targeted to a\par\
pard\qj \li956\ri66\sb0\sl-219\slmult0\fi0 \up0 \expndtw-1\charscalex100 Watson-
Crick T�A base-pair, the oligonucleotide \line \up0 \expndtw0\charscalex101
with the sequence d(AGA\ul0\nosupersub\cf26\f27\fs20 T\ul0\nosupersub\cf7\f8\
fs20 AGAACCCCTTC-\line
\up0 \expndtw-3\charscalex100 T\ul0\nosupersub\cf26\f27\fs20 A\ul0\nosupersub\cf7\
f8\fs20 TCTTATATCT\ul0\nosupersub\cf26\f27\fs20 D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 TCTT), (DTA triplex) was syn-\line \up0 \expndtw-1\
charscalex100 thesized (the bases in the two loops are underlined \line \up0 \
expndtw-1\charscalex100 and the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\
fs20 base and the target T�A base-pair are in \line \up0 \expndtw-2\charscalex100
bold). This was designed to be similar to sequences \line \up0 \expndtw0\
charscalex100 that had previously been shown to fold into stable \line \up0 \
expndtw-3\charscalex100 intramolecular triplexes (Macaya\ul0\nosupersub\cf9\f10\
fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1991c, 1992b; \line \up0 \expndtw0\
charscalex103 Sklena�\u345? & Feigon, 1990; Wang\ul0\nosupersub\cf9\f10\fs20 et
al\ul0\nosupersub\cf7\f8\fs20 ., 1992). A pre-\line \up0 \expndtw-1\charscalex100
liminary study using one- and two-dimensional\par\pard\column \ql \li20\sb1\
sl-218\slmult0 \up0 \expndtw-3\charscalex100 structure is discussed, and the
results are compared\par\pard\qj \li20\ri1643\sb1\sl-219\slmult0 \up0 \expndtw-2\
charscalex100 with those from fiber diffraction and NMR-derived \up0 \expndtw-2\
charscalex100 triplex structures.\par\pard\ql \li20\sb212\sl-276\slmult0 \up0 \
expndtw-3\charscalex100 \ul0\nosupersub\cf15\f16\fs24 Results\par\pard\ql \li5856\
sb0\sl-172\slmult0 \par\pard\ql \li20\sb42\sl-172\slmult0\tx191 \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf23\f24\fs12 1\tab \up0 \expndtw0\charscalex100 \
ul0\nosupersub\cf24\f25\fs20 H NOESY spectrum of exchangeable\par\pard\ql \li20\
sb83\sl-219\slmult0 \up0 \expndtw-1\charscalex100 resonances of DTA\par\pard\qj \
li20\ri1560\sb139\sl-219\slmult0\fi199 \up0 \expndtw0\charscalex104 \ul0\
nosupersub\cf7\f8\fs20 The imino region of a NOESY spectrum of the \line \up0 \
expndtw0\charscalex100 DTA triplex in water at 1\ul0\nosupersub\cf25\f26\fs20 \u-
3920?\ul0\nosupersub\cf7\f8\fs20 C is shown in Figure 2. \line \up0 \expndtw0\
charscalex102 This spectrum exhibits features typical of pre-\line \up0 \
expndtw-1\charscalex100 viously characterized intramolecular triplexes, e.g. \
line \up0 \expndtw0\charscalex100 imino proton resonances corresponding to
both \line \up0 \expndtw0\charscalex100 Watson-Crick and Hoogsteen hydrogen-
bonded \line \up0 \expndtw-3\charscalex100 base-pairs are observed (Sklena�\
u345? & Feigon, 1990) \line \up0 \expndtw-2\charscalex100 (Figure \up0 \
expndtw0\charscalex103 2(a)). Crosspeaks from the downfield-\par\pard\qj \li20\
ri1643\sb0\sl-219\slmult0 \up0 \expndtw-1\charscalex100 shifted amino protons,
characteristic of protonated \line \up0 \expndtw0\charscalex100 cytosine bases,
are also observed \up0 \expndtw-2\charscalex100 (Figure \up0 \expndtw-2\
charscalex100 2(b)).\par\pard\qj \li20\ri1643\sb1\sl-219\slmult0 \up0 \expndtw-1\
charscalex100 Assignment of the spectrum followed protocols \line \up0 \
expndtw-2\charscalex100 previously developed in our laboratory (Macaya \line \
up0 \expndtw0\charscalex105 \ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\
f8\fs20 ., \up0 \expndtw-2\charscalex100 1991, \up0 \expndtw0\charscalex100 1992b;
Rajagopal & Feigon, \up0 \expndtw-2\charscalex100 1989a;\par\pard\qj \li20\
ri1560\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex101 Sklena�\u345? & Feigon,
1990) and are given in Table 1. \up0 \expndtw-1\charscalex100 Analysis of the
NOESY spectrum confirms that \up0 \expndtw-4\charscalex100 the DTA
oligonucleotide forms an intramolecular \up0 \expndtw-1\charscalex100 triplex.
In Figure \up0 \expndtw-1\charscalex100 2(a), the Watson-Crick imino-\par\pard\
qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-2\charscalex100 imino sequential
connectivities are indicated above \line \up0 \expndtw-1\charscalex100 the
diagonal and the Hoogsteen imino-imino \line \up0 \expndtw-2\charscalex100
sequential connectivities are indicated below the \line \up0 \expndtw0\
charscalex101 diagonal. There is an unexpected break in the \line \up0 \
expndtw0\charscalex101 sequential connectivities between T4 and T16. No \line \
up0 \expndtw-3\charscalex100 imino-imino crosspeaks are observed to C\ul0\super\
cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 26 due to \
line \up0 \expndtw0\charscalex102 chemical exchange with water during the mixing \
line \up0 \expndtw0\charscalex100 time. However, the C\ul0\super\cf16\f17\
fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 26 \up0 \expndtw0\
charscalex100 imino was readily\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \
up0 \expndtw0\charscalex102 identified by the crosspeaks to its own amino \
line \up0 \expndtw-3\charscalex100 resonances \up0 \expndtw-2\charscalex100 (Figure
\up0 \expndtw0\charscalex100 2(b)). T27 \up0 \expndtw0\charscalex100 and T25 \
up0 \expndtw-2\charscalex100 were\par\pard\qj \li20\ri1560\sb0\sl-219\slmult0\fi0 \
up0 \expndtw0\charscalex102 identified on the basis of some of the intra-triplet \
line \up0 \expndtw-2\charscalex100 NOE crosspeaks characteristic of T�A�T triplets,
e.g. \line \up0 \expndtw-1\charscalex100 both the Watson-Crick and the Hoogsteen T
imino \line \up0 \expndtw-2\charscalex100 protons have crosspeaks to the
central A amino \line \up0 \expndtw0\charscalex100 resonances (Sklena�\u345? &
Feigon, 1990). Of particular \line \up0 \expndtw-2\charscalex100 interest are the
crosspeaks observed between imino \line \up0 \expndtw0\charscalex100 and D\ul0\sub\
cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 protons. As is indicated in Figure
2(b), the \line \up0 \expndtw-4\charscalex100 T16 imino proton of the DTA triplex
has a crosspeak \line \up0 \expndtw-2\charscalex100 to the D\ul0\sub\cf16\f17\
fs18 3\ul0\nosupersub\cf7\f8\fs20 H3/5C resonance. Crosspeaks are also \line
\up0 \expndtw-2\charscalex100 observed between the T29 imino resonance and the \
line \up0 \expndtw-1\charscalex100 D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\
fs20 H5B and H6B protons. \par\pard\sect\sectd\fs24\paperw12240\paperh15840{\shp
{\*\shpinst\shpleft0\shptop0\shpright12240\shpbottom15840\shpwr3\shpfblwtxt0\shpz-
10000\shplid2
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a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a00
28a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0064b
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40051451400514514005145140051451400514514005145140051451400514514005145140051451400
51451400514514005145140051451400514514005145140051451400514514005145140051451400514
51400514514005145140051451400514514005145140051451400514514005145140051451400514514
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05145140051451400514514005145140051451400514514005145140051451400514514005145140051
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51451400514514005145140051451400514514005145140051451400514514005145140051451400514
51400514514005145140051451400514514005145140051451400514514005145140051451400514514
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051451400514514005145140051451400514514
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51400514514005145140051451400514514005145140051451400514514005145140051451400514514
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14514005145140051451400514514005145140051451400514514005145140051451400514514005145
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51451400514514005145140051451400514514005145140051451400514514005145140051451400514
51400514514005145140051451400514514005145140051451400514514005145140051451400514514
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14005145140051451400514514005145140051451400514514005145140051451400514514005145140
05145140051451400514514005145140051451400514514005145140051451400514514005145140051
45140051451400514514005145140051451400514514005145140051451400514514005145140051451
40051451400514514005145140051451400514514005145140051451400514514005145140051451400
51451400514514005145140051451400514514005145140051451400514514005145140051451400514
51400514514005145140051451400514514005145140051451400514514005145140051451400514514
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14005145140051451400514514005145140051451400514514005145140051451400514514005145140
1fffd9}}}}}\pard\sb0\sl-240{\bkmkstart Pg3}{\bkmkend Pg3}\par\pard\li956\sb0\sl-
230\slmult0\par\pard\li956\sb100\sl-230\slmult0\fi0\tx6448 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1054\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\
cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\par\pard\ql \
li5856\sb0\sl-230\slmult0 \par\pard\ql\li5856\sb200\sl-230\slmult0 \up0 \expndtw0\
charscalex100 \ul0\nosupersub\cf24\f25\fs20 Assignments of the \par\pard\ql \
li5856\sb1\sl-217\slmult0 \up0 \expndtw-2\charscalex100 non-exchangeable resonances
\par\pard\ql \li6055\sb213\sl-230\slmult0\tx9113 \up0 \expndtw0\charscalex102 \ul0\
nosupersub\cf7\f8\fs20 Regions of a two-dimensional \tab \up0 \expndtw-1\
charscalex100 \ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 2\ul0\nosupersub\
cf7\f8\fs20 H\ul0\sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 O NOESY \par\
pard\qj \li5856\ri1638\sb0\sl-220\slmult0\fi0 \up0 \expndtw0\charscalex101 spectrum
of the DTA triplex at 25\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\nosupersub\cf7\
f8\fs20 C are shown in \line \up0 \expndtw-3\charscalex100 Figures 3 and 4.
Except for the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base,
assign-\line \up0 \expndtw0\charscalex103 ment of the DTA triplex could largely be
done as \line \up0 \expndtw-2\charscalex100 previously described for
intramolecular triplexes \line \up0 \expndtw0\charscalex100 using NOESY, P.COSY,
HOHAHA and HOENOE \line \up0 \expndtw-3\charscalex100 spectra (Macaya\ul0\
nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1992b).
Assignments were \line \up0 \expndtw-3\charscalex100 obtained for all of the
base, H1', H2',2" and H3' \line \up0 \expndtw-2\charscalex100 resonances in the
triplex, except for the nucleotides \line \up0 \expndtw-1\charscalex100 in the TATA
loop and several of the nucleotides in \line \up0 \expndtw0\charscalex103 the two
triplets at the 5' end (with respect to the \line \up0 \expndtw0\charscalex102
purine strand) of the triplex. The assignments are \line \up0 \expndtw0\
charscalex100 given in Table 1. \par\pard\qj \li5856\ri1623\sb0\sl-219\slmult0\
fi199 \up0 \expndtw-2\charscalex100 The assignments of the D\ul0\sub\cf16\f17\
fs18 3\ul0\nosupersub\cf7\f8\fs20 base protons were \line \up0 \expndtw0\
charscalex100 obtained by analysis of the data from P.COSY, \line \up0 \
expndtw0\charscalex102 NOESY and\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17
1\ul0\nosupersub\cf7\f8\fs20 H-\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 13\
ul0\nosupersub\cf7\f8\fs20 C HMQC NMR experiments. In \line \up0 \expndtw-3\
charscalex100 the P.COSY spectrum (Marion & Bax, 1988; Mueller, \line \up0 \
expndtw0\charscalex100 1987) of the triplex (data not shown), four unusual \line \
up0 \expndtw0\charscalex101 crosspeaks are observed in the H1'-H1' region, \
line \up0 \expndtw0\charscalex105 which are absent in the P.COSY spectra of other \
line \up0 \expndtw0\charscalex100 triplexes. These crosspeaks form two spin systems
\line \up0 \expndtw-1\charscalex100 of three protons each. In the NOESY spectrum,
the \line \up0 \expndtw0\charscalex103 same crosspeaks are observed with
additional \line \up0 \expndtw0\charscalex100 crosspeaks between the outer protons
within each \line \up0 \expndtw-3\charscalex100 spin system (Figure 3). These two
sets of spins must \line \up0 \expndtw0\charscalex101 be attributed to protons of
rings B and C of the D\ul0\sub\cf16\f17\fs18 3 \line \up0 \expndtw-4\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 base. Protons H2A and H5A were identified
by their \line \up0 \expndtw-3\charscalex100 aromatic-aromatic sequential
connectivity to T29H6 \line \up0 \expndtw-2\charscalex100 (Figure 3, peaks a and
b), and confirmed by a weak \line \up0 \expndtw-2\charscalex100 crosspeak between
the two. In the aromatic-methyl \line \up0 \expndtw0\charscalex103 region of the
NOESY, there is a proton that has a \line \up0 \expndtw-1\charscalex100 crosspeak
to only T4Me and was identified as H2B \line \up0 \expndtw0\charscalex100 (Figure
4, peak e). This, as well as other D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\
fs20 proton \line \up0 \expndtw0\charscalex100 resonance assignments, was
supported by a\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17
1\ul0\nosupersub\cf7\f8\fs20 H-\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17
13\ul0\nosupersub\cf7\f8\fs20 C \line \up0 \expndtw-1\charscalex100 HMQC spectrum
(Bax\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1983; data
not shown). \line \up0 \expndtw0\charscalex100 If the relative orientation of rings
A and B of D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 \line \up0 \
expndtw-2\charscalex100 were opposite from what is depicted in Figure 1(a), \line \
up0 \expndtw0\charscalex105 one would also expect to see an NOE crosspeak \line \
up0 \expndtw0\charscalex103 between protons H2B and H5A, which is not \
line \up0 \expndtw0\charscalex102 observed. Likewise, this alternative
orientation \line \up0 \expndtw-3\charscalex100 would cause any NOE crosspeaks
between H5A\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\
colw6244\colsr160\ql \li1135\sb1\sl-170\slmult0 \up0 \expndtw-2\charscalex100 \ul0\
nosupersub\cf19\f20\fs18 Figure \up0 \expndtw-2\charscalex100 2. \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf8\f9\fs11 1 \up0 \expndtw-2\charscalex100 \ul0\
nosupersub\cf13\f14\fs18 H \up0 \expndtw0\charscalex101 2D NOESY spectrum of the
DTA triplex\par\pard\ql \li956\sb6\sl-199\slmult0\tx1221 \up0 \expndtw-2\
charscalex100 in\tab \up0 \expndtw-1\charscalex100 90%H\ul0\nosupersub\cf8\f9\fs11
2\ul0\nosupersub\cf13\f14\fs18 O/10%\ul0\super\cf8\f9\fs16 2\ul0\nosupersub\cf13\
f14\fs18 H\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O at 1\ul0\
nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 C with \up0 \
expndtw0\charscalex101 a mixing time of\par\pard\qj \li956\ri149\sb0\sl-199\
slmult0 \up0 \expndtw-3\charscalex100 100 ms. (a) The imino-imino region. The
Watson-Crick \line \up0 \expndtw-1\charscalex100 imino sequential
connectivities are indicated above \line \up0 \expndtw0\charscalex105 the
diagonal, and the Hoogsteen imino sequential \line \up0 \expndtw0\
charscalex101 connectivities are indicated below the diagonal. The \line \up0
\expndtw-2\charscalex100 missing sequential crosspeak between the T4 and T16
\line \up0 \expndtw0\charscalex104 iminos is indicated by a box and connected by
broken \line \up0 \expndtw-3\charscalex100 lines. \up0 \expndtw0\charscalex101 (b)
The imino-aromatic, amino region. The\par\pard\qj \li956\ri149\sb26\sl-192\
slmult0 \up0 \expndtw-2\charscalex100 crosspeaks from the T16 and T29 iminos
to the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 28 \up0 \
expndtw-3\charscalex100 aromatic protons are indicated. The C\ul0\super\cf8\
f9\fs16 +\ul0\nosupersub\cf13\f14\fs18 26 imino-amino \up0 \expndtw-1\
charscalex100 crosspeaks are also indicated. The NOESY spectrum was \up0 \expndtw0\
charscalex104 acquired with a sweep width of \up0 \expndtw0\charscalex102
12048 Hz in both\par\pard\qj \li956\ri149\sb21\sl-199\slmult0 \up0 \expndtw-2\
charscalex100 dimensions, 2048 and 300 complex points in t\ul0\nosupersub\cf8\
f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 and t\ul0\nosupersub\cf8\f9\fs11 1\ul0\
nosupersub\cf13\f14\fs18 , \line \up0 \expndtw-1\charscalex100 respectively, and
64 scans per t\ul0\nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 block.
In t\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 600 points \
line \up0 \expndtw-2\charscalex100 were apodized using a 60\ul0\nosupersub\cf27\
f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 phase-shifted squared sinebell \
line \up0 \expndtw-1\charscalex100 with a skew factor of 0.8; the baseline
was flattened \line \up0 \expndtw0\charscalex100 with a first-order polynomial.
In t\ul0\nosupersub\cf8\f9\fs11 1 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\
cf13\f14\fs18 300 \up0 \expndtw0\charscalex100 points were\par\pard\qj \li956\
ri149\sb0\sl-199\slmult0\fi0 \up0 \expndtw-2\charscalex100 apodized using a 60\ul0\
nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 phase-shifted
squared sinebell with \line \up0 \expndtw-1\charscalex100 a skew factor of 0.8, and
then zero-filled to 2048 complex \line \up0 \expndtw-2\charscalex100 points.\par\
pard\column \ql \li20\sb1\sl-218\slmult0 \up0 \expndtw0\charscalex103 \ul0\
nosupersub\cf7\f8\fs20 and both H6B and H5B to be either very weak or\par\pard\qj \
li20\ri1643\sb1\sl-219\slmult0 \up0 \expndtw-2\charscalex100 non-existent. Thus,
the lack of any NOE crosspeaks \up0 \expndtw0\charscalex103 other than that of T4Me
to H2B, as well as strong \up0 \expndtw0\charscalex101 crosspeaks between both
the central and outer \up0 \expndtw-3\charscalex100 protons of one of the spin
systems mentioned above \up0 \expndtw-1\charscalex100 and the resonance identified
as either H5A or H2A \up0 \expndtw-2\charscalex100 distinguishes ring B from C, as
well as protons H6B \up0 \expndtw0\charscalex102 from H4B, and H5A from H2A.\par\
pard\qj \li20\ri1643\sb0\sl-219\slmult0\fi199 \up0 \expndtw0\charscalex107 The
remaining three spin system must be \line \up0 \expndtw0\charscalex107
assigned to the C ring. Although the C ring is a \line \up0 \expndtw-2\
charscalex100 five-spin system, resonances for H2C and H6C and \line \up0 \expndtw-
3\charscalex100 for H3C and H5C are degenerate. This is apparently \line \up0 \
expndtw0\charscalex101 due to motional averaging (ring flips). H3/5C was \line \up0
\expndtw0\charscalex100 assigned from the P.COSY spectrum as the central \line \up0
\expndtw0\charscalex101 spin in the three-spin system. H4C and H2/6C are \line \up0
\expndtw0\charscalex103 distinguished on the basis of their NOESY cross-\line \
up0 \expndtw-1\charscalex100 peaks, i.e. crosspeaks between H4C to both A17H8 \line
\up0 \expndtw0\charscalex100 and T16H1', and H2/6C to A17H2 (Figure 3, peaks \
line \up0 \expndtw0\charscalex105 t, m and s). \par\pard\sect\sectd\fs24\
paperw12240\paperh15840\pard\sb0\sl-240{\bkmkstart Pg4}{\bkmkend Pg4}\par\pard\
li956\sb0\sl-218\slmult0\par\pard\li956\sb151\sl-218\slmult0\fi0\tx9955 \up0 \
expndtw-1\charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\
nosupersub\cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\tab \
up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf22\f23\fs20 1055\par\pard\li2091\
sb0\sl-207\slmult0\par\pard\li2091\sb0\sl-207\slmult0\par\pard\li2091\sb6\sl-207\
slmult0\fi0 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf19\f20\fs18 Table 1.\
ul0\nosupersub\cf13\f14\fs18 DTA triplex chemical shifts\par\pard\li2091\sb81\sl-
184\slmult0\fi0\tx3198\tx3966\tx4847\tx5550\tx6630\tx7347\tx8051\tx8781 \up0 \
expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\fs16 Residue\tab \up0 \expndtw-1\
charscalex100 Imino\tab \up0 \expndtw-1\charscalex100 Aminos\tab \up0 \expndtw-1\
charscalex100 H6,H8\tab \up0 \expndtw-1\charscalex100 H2,H5,Me\tab \up0 \expndtw-1\
charscalex100 H1'\tab \up0 \expndtw-1\charscalex100 H2'\tab \up0 \expndtw-1\
charscalex100 H2"\tab \up0 \expndtw-1\charscalex100 H3'\par\pard\li2091\sb85\sl-
184\slmult0\fi0\tx3301\tx3924\tx5776 \up0 \expndtw-1\charscalex100 A1\tab \up0 \
expndtw-1\charscalex100 \u8212?\ul0\nosupersub\cf28\f29\fs10 a\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf11\f12\fs16 6.99,7.73\tab \up0 \expndtw-1\
charscalex100 7.73\par\pard\li2091\sb0\sl-180\slmult0\fi0\tx3227\tx7270 \up0 \
expndtw-1\charscalex100 G2\tab \up0 \expndtw-1\charscalex100 12.69\tab \up0 \
expndtw-1\charscalex100 \u8212?\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\
tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 A3\
tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100
7.63,7.71\tab \up0 \expndtw-1\charscalex100 7.43\tab \up0 \expndtw-1\charscalex100
7.56\tab \up0 \expndtw-1\charscalex100 5.92\tab \up0 \expndtw-1\charscalex100 1.89\
tab \up0 \expndtw-1\charscalex100 2.51\tab \up0 \expndtw-1\charscalex100 4.76\par\
pard\li2091\sb0\sl-179\slmult0\fi0\tx3227\tx4163\tx4940\tx5776\tx6613\tx7310\
tx8047\tx8764 \up0 \expndtw-1\charscalex100 T4\tab \up0 \expndtw-1\charscalex100
13.34\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100
6.32\tab \up0 \expndtw-1\charscalex100 0.34\tab \up0 \expndtw-1\charscalex100 5.61\
tab \up0 \expndtw-1\charscalex100 1.81\tab \up0 \expndtw-1\charscalex100 2.15\tab \
up0 \expndtw-1\charscalex100 4.70\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\
tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 A5\
tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100
7.08,7.47\tab \up0 \expndtw-1\charscalex100 7.67\tab \up0 \expndtw-1\charscalex100
7.14\tab \up0 \expndtw-1\charscalex100 6.05\tab \up0 \expndtw-1\charscalex100 2.59\
tab \up0 \expndtw-1\charscalex100 2.90\tab \up0 \expndtw-1\charscalex100 4.86\par\
pard\li2091\sb1\sl-180\slmult0\fi0\tx3227\tx4940\tx5836\tx6613\tx7310\tx8047\tx8764
\up0 \expndtw-1\charscalex100 G6\tab \up0 \expndtw-1\charscalex100 12.46\tab \up0 \
expndtw-1\charscalex100 7.20\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \
expndtw-1\charscalex100 5.76\tab \up0 \expndtw-1\charscalex100 2.38\tab \up0 \
expndtw-1\charscalex100 2.87\tab \up0 \expndtw-1\charscalex100 4.85\par\pard\
li2091\sb0\sl-179\slmult0\fi0\tx3326\tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\
tx8764 \up0 \expndtw-1\charscalex100 A7\tab \up0 \expndtw-1\charscalex100 \u8212?\
tab \up0 \expndtw-1\charscalex100 7.52,7.71\tab \up0 \expndtw-1\charscalex100 7.37\
tab \up0 \expndtw-1\charscalex100 7.35\tab \up0 \expndtw-1\charscalex100 5.84\tab \
up0 \expndtw-1\charscalex100 2.44,\tab \up0 \expndtw-1\charscalex100 2.72\tab \
up0 \expndtw-1\charscalex100 4.88\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\
tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 A8\
tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100
7.52,7.72\tab \up0 \expndtw-1\charscalex100 7.77\tab \up0 \expndtw-1\charscalex100
7.94\tab \up0 \expndtw-1\charscalex100 6.04\tab \up0 \expndtw-1\charscalex100
2.44,\tab \up0 \expndtw-1\charscalex100 2.57\tab \up0 \expndtw-1\charscalex100
4.77\par\pard\li2091\sb1\sl-180\slmult0\fi0\tx3326\tx4940\tx5776\tx6613\tx7310\
tx8047\tx8764 \up0 \expndtw-1\charscalex100 C9\tab \up0 \expndtw-1\charscalex100 \
u8212?\tab \up0 \expndtw-1\charscalex100 7.41\tab \up0 \expndtw-1\charscalex100
5.50\tab \up0 \expndtw-1\charscalex100 5.75\tab \up0 \expndtw-1\charscalex100
1.97,\tab \up0 \expndtw-1\charscalex100 2.32\tab \up0 \expndtw-1\charscalex100
4.66\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\tx4940\tx5776\tx6613\tx7310\
tx8047\tx8764 \up0 \expndtw-1\charscalex100 C10\tab \up0 \expndtw-1\charscalex100 \
u8212?\tab \up0 \expndtw-1\charscalex100 7.73\tab \up0 \expndtw-1\charscalex100
5.97\tab \up0 \expndtw-1\charscalex100 6.04\tab \up0 \expndtw-1\charscalex100
2.01,\tab \up0 \expndtw-1\charscalex100 2.36\tab \up0 \expndtw-1\charscalex100
4.50\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\tx4940\tx5776\tx6613\tx7310\
tx8047\tx8764 \up0 \expndtw-1\charscalex100 C11\tab \up0 \expndtw-1\charscalex100 \
u8212?\tab \up0 \expndtw-1\charscalex100 7.55\tab \up0 \expndtw-1\charscalex100
5.59\tab \up0 \expndtw-1\charscalex100 5.73\tab \up0 \expndtw-1\charscalex100
1.88,\tab \up0 \expndtw-1\charscalex100 2.34\tab \up0 \expndtw-1\charscalex100
4.66\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\tx4940\tx5776\tx6613\tx7310\
tx8047\tx8764 \up0 \expndtw-1\charscalex100 C12\tab \up0 \expndtw-1\charscalex100 \
u8212?\tab \up0 \expndtw-1\charscalex100 7.94\tab \up0 \expndtw-1\charscalex100
6.12\tab \up0 \expndtw-1\charscalex100 6.21\tab \up0 \expndtw-1\charscalex100
2.41,\tab \up0 \expndtw-1\charscalex100 2.67\tab \up0 \expndtw-1\charscalex100
4.73\par\pard\li2091\sb1\sl-180\slmult0\fi0\tx3227\tx4163\tx4940\tx5776\tx6613\
tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 T13\tab \up0 \expndtw-1\
charscalex100 14.89\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\
charscalex100 7.66\tab \up0 \expndtw-1\charscalex100 1.79\tab \up0 \expndtw-1\
charscalex100 6.09\tab \up0 \expndtw-1\charscalex100 2.26,\tab \up0 \expndtw-1\
charscalex100 2.71\tab \up0 \expndtw-1\charscalex100 4.85\par\pard\li2091\sb0\sl-
179\slmult0\fi0\tx3227\tx4163\tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \
expndtw-1\charscalex100 T14\tab \up0 \expndtw-1\charscalex100 14.09\tab \up0 \
expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100 7.53\tab \up0 \
expndtw-1\charscalex100 1.65\tab \up0 \expndtw-1\charscalex100 6.07\tab \up0 \
expndtw-1\charscalex100 2.28,\tab \up0 \expndtw-1\charscalex100 2.61\tab \up0 \
expndtw-1\charscalex100 4.90\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\tx3924\
tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 C15\tab \
up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100 7.12,8.18\
tab \up0 \expndtw-1\charscalex100 7.55\tab \up0 \expndtw-1\charscalex100 5.53\tab \
up0 \expndtw-1\charscalex100 5.92\tab \up0 \expndtw-1\charscalex100 2.02,\tab \
up0 \expndtw-1\charscalex100 2.45\tab \up0 \expndtw-1\charscalex100 4.74\par\pard\
li2091\sb1\sl-180\slmult0\fi0\tx3227\tx4163\tx4940\tx5776\tx6613\tx7310\tx8047\
tx8764 \up0 \expndtw-1\charscalex100 T16\tab \up0 \expndtw-1\charscalex100 13.12\
tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100 7.37\
tab \up0 \expndtw-1\charscalex100 1.63\tab \up0 \expndtw-1\charscalex100 6.02\tab \
up0 \expndtw-1\charscalex100 2.36,\tab \up0 \expndtw-1\charscalex100 2.51\tab \
up0 \expndtw-1\charscalex100 4.98\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326\
tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 A17\
tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100
6.45,6.99\tab \up0 \expndtw-1\charscalex100 8.30\tab \up0 \expndtw-1\charscalex100
7.55\tab \up0 \expndtw-1\charscalex100 5.99\tab \up0 \expndtw-1\charscalex100
2.65,\tab \up0 \expndtw-1\charscalex100 2.80\tab \up0 \expndtw-1\charscalex100
4.90\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3227\tx4163\tx4940\tx5776\tx6613\
tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 T18\tab \up0 \expndtw-1\
charscalex100 13.73\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\
charscalex100 7.22\tab \up0 \expndtw-1\charscalex100 1.29\tab \up0 \expndtw-1\
charscalex100 5.92\tab \up0 \expndtw-1\charscalex100 2.18,\tab \up0 \expndtw-1\
charscalex100 2.50\tab \up0 \expndtw-1\charscalex100 4.78\par\pard\li2091\sb0\sl-
179\slmult0\fi0\tx3326\tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \
expndtw-1\charscalex100 C19\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \
expndtw-1\charscalex100 6.89,8.17\tab \up0 \expndtw-1\charscalex100 7.49\tab \up0 \
expndtw-1\charscalex100 5.45\tab \up0 \expndtw-1\charscalex100 5.91\tab \up0 \
expndtw-1\charscalex100 2.01,\tab \up0 \expndtw-1\charscalex100 2.46\tab \up0 \
expndtw-1\charscalex100 4.60\par\pard\li2091\sb1\sl-180\slmult0\fi0\tx3227\tx4163\
tx5776 \up0 \expndtw-1\charscalex100 T20\tab \up0 \expndtw-1\charscalex100 14.45\
tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100 1.53\
par\pard\li2091\sb0\sl-179\slmult0\fi0\tx4163\tx5776 \up0 \expndtw-1\charscalex100
T21\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100
1.71\par\pard\li2091\sb0\sl-179\slmult0\fi0\tx3326 \up0 \expndtw-1\charscalex100
A22\tab \up0 \expndtw-1\charscalex100 \u8212?\par\pard\li2091\sb0\sl-179\slmult0\
fi0\tx4163 \up0 \expndtw-1\charscalex100 T23\tab \up0 \expndtw-1\charscalex100 \
u8212?\par\pard\li2091\sb1\sl-180\slmult0\fi0\tx3326 \up0 \expndtw-1\charscalex100
A24\tab \up0 \expndtw-1\charscalex100 \u8212?\par\pard\li2091\sb0\sl-179\slmult0\
fi0\tx3227\tx4163 \up0 \expndtw-1\charscalex100 T25\tab \up0 \expndtw-1\
charscalex100 13.98\tab \up0 \expndtw-1\charscalex100 \u8212?\par\pard\li2091\sb0\
sl-179\slmult0\fi0\tx3227\tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \
expndtw-1\charscalex100 C\ul0\nosupersub\cf17\f18\fs10 +\ul0\nosupersub\cf11\f12\
fs16 26\tab \up0 \expndtw-1\charscalex100 15.56\tab \up0 \expndtw-1\charscalex100
9.17,10.04\tab \up0 \expndtw-1\charscalex100 7.92\tab \up0 \expndtw-1\charscalex100
5.91\tab \up0 \expndtw-1\charscalex100 6.09\tab \up0 \expndtw-1\charscalex100
2.18,\tab \up0 \expndtw-1\charscalex100 2.66\tab \up0 \expndtw-1\charscalex100
4.57\par\pard\li2091\sb1\sl-180\slmult0\fi0\tx3227\tx4163\tx4940\tx5776\tx6613\
tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 T27\tab \up0 \expndtw-1\
charscalex100 12.81\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\
charscalex100 7.65\tab \up0 \expndtw-1\charscalex100 1.74\tab \up0 \expndtw-1\
charscalex100 6.34\tab \up0 \expndtw-1\charscalex100 2.33,\tab \up0 \expndtw-1\
charscalex100 2.53\tab \up0 \expndtw-1\charscalex100 5.04\par\pard\li2091\sb8\sl-
184\slmult0\fi0\tx3326\tx4163\tx4999\tx5836\tx6613\tx7310\tx8047\tx8764 \dn2 \
expndtw-1\charscalex100 D\ul0\nosupersub\cf17\f18\fs10 3\ul0\nosupersub\cf11\f12\
fs16 28\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\
charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-
1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100 6.04\tab \up0 \expndtw-1\
charscalex100 2.55,\tab \up0 \expndtw-1\charscalex100 3.05\tab \up0 \expndtw-1\
charscalex100 4.88\par\pard\li2091\sb1\sl-163\slmult0\fi0\tx3227\tx4163\tx4940\
tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 T29\tab \up0 \
expndtw-1\charscalex100 13.07\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \
expndtw-1\charscalex100 7.31\tab \up0 \expndtw-1\charscalex100 1.64\tab \up0 \
expndtw-1\charscalex100 6.16\tab \up0 \expndtw-1\charscalex100 2.26,\tab \up0 \
expndtw-1\charscalex100 2.59\tab \up0 \expndtw-1\charscalex100 4.92\par\pard\
li2091\sb3\sl-179\slmult0\fi0\tx3227\tx3924\tx4940\tx5776\tx6613\tx7310\tx8047\
tx8764 \up0 \expndtw-1\charscalex100 C\ul0\super\cf17\f18\fs14 +\ul0\nosupersub\
cf11\f12\fs16 30\tab \up0 \expndtw-1\charscalex100 15.37\tab \up0 \expndtw-1\
charscalex100 9.38,9.76\tab \up0 \expndtw-1\charscalex100 7.86\tab \up0 \expndtw-1\
charscalex100 5.71\tab \up0 \expndtw-1\charscalex100 6.12\tab \up0 \expndtw-1\
charscalex100 2.20,\tab \up0 \expndtw-1\charscalex100 2.67\tab \up0 \expndtw-1\
charscalex100 4.73\par\pard\li2091\sb1\sl-180\slmult0\fi0\tx3227\tx4163\tx4940\
tx5776\tx6613\tx7310\tx8047\tx8764 \up0 \expndtw-1\charscalex100 T31\tab \up0 \
expndtw-1\charscalex100 13.34\tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \
expndtw-1\charscalex100 7.70\tab \up0 \expndtw-1\charscalex100 1.70\tab \up0 \
expndtw-1\charscalex100 6.18\tab \up0 \expndtw-1\charscalex100 2.27,\tab \up0 \
expndtw-1\charscalex100 2.69\tab \up0 \expndtw-1\charscalex100 4.87\par\pard\
li2091\sb0\sl-179\slmult0\fi0\tx3227\tx4163\tx4940\tx5776\tx6613\tx7310\tx8047\
tx8764 \up0 \expndtw-1\charscalex100 T32\tab \up0 \expndtw-1\charscalex100 12.51\
tab \up0 \expndtw-1\charscalex100 \u8212?\tab \up0 \expndtw-1\charscalex100 7.53\
tab \up0 \expndtw-1\charscalex100 1.59\tab \up0 \expndtw-1\charscalex100 6.33\tab \
up0 \expndtw-1\charscalex100 2.25,\tab \up0 \expndtw-1\charscalex100 2.30\tab \
up0 \expndtw-1\charscalex100 4.55\par\pard\li2091\sb0\sl-184\slmult0\par\pard\
li2091\sb4\sl-184\slmult0\fi0 \up0 \expndtw0\charscalex100 D\ul0\nosupersub\cf17\
f18\fs10 3\ul0\nosupersub\cf11\f12\fs16 28 aromatic resonances\par\pard\li2091\
sb1\sl-163\slmult0\fi239\tx3739\tx5197 \up0 \expndtw0\charscalex100 H2A = 8.22\
tab \up0 \expndtw0\charscalex100 H2B = 7.17\tab \up0 \expndtw0\charscalex100 H2/6C
= 7.08\par\pard\li2091\sb3\sl-179\slmult0\fi239\tx3739\tx5197 \up0 \expndtw0\
charscalex100 H5A = 7.45\tab \up0 \expndtw0\charscalex100 H4B = 6.22\tab \up0 \
expndtw0\charscalex100 H3/5C = 6.46\par\pard\li2091\sb1\sl-178\slmult0\fi1647\
tx5205 \up0 \expndtw-1\charscalex100 H5B = 6.55\tab \up0 \expndtw-1\charscalex100
H4C = 6.16\par\pard\li2091\sb1\sl-180\slmult0\fi1647 \up0 \expndtw-1\charscalex100
H6B = 6.88\par\pard\li2091\sb86\sl-184\slmult0\fi159\tx7963\tx8181\tx8528
\up0 \expndtw-1\charscalex100 Chemical shifts for the exchangeable and non-
exchangeable resonances are\tab \up0 \expndtw-6\charscalex100 at\tab \up0 \
expndtw-4\charscalex100 1\ul0\nosupersub\cf29\f30\fs16 \u-3920?\ul0\nosupersub\
cf11\f12\fs16 C\tab \up0 \expndtw-1\charscalex100 and 25\ul0\nosupersub\cf29\f30\
fs16 \u-3920?\ul0\nosupersub\cf11\f12\fs16 C,\par\pard\li2091\sb0\sl-179\slmult0\
fi0 \up0 \expndtw0\charscalex100 respectively. Not all resonances in the loops and
in the two 5'-terminal triplets could be assigned due\par\pard\li2091\sb0\sl-179\
slmult0\fi0 \up0 \expndtw-1\charscalex100 to chemical exchange broadening.\par\
pard\li2091\sb0\sl-179\slmult0\fi159 \up0 \expndtw-1\charscalex100 \ul0\super\cf28\
f29\fs14 a\ul0\nosupersub\cf11\f12\fs16 Not applicable.\par\pard\sect\sectd\
sbknone\cols2\colno1\colw5696\colsr160\colno2\colw6244\colsr160\ql \li956\sb0\sl-
230\slmult0 \par\pard\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb126\sl-
230\slmult0 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf24\f25\fs20 Evidence
for D\ul0\sub\cf23\f24\fs18 3\ul0\nosupersub\cf24\f25\fs20 intercalation\par\
pard\qj \li956\ri149\sb218\sl-219\slmult0\fi199 \up0 \expndtw0\charscalex100 \ul0\
nosupersub\cf7\f8\fs20 Numerous NOE crosspeaks are observed be-\line \up0 \
expndtw0\charscalex100 tween protons from all three aromatic rings of \
line \up0 \expndtw-4\charscalex100 the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\
cf7\f8\fs20 base and other nucleotides in the DTA triplex. \line \up0 \expndtw0\
charscalex104 In all cases, the observed NOE crosspeaks are to \line \up0 \
expndtw0\charscalex101 protons of either the T29�A5�T16 \up0 \expndtw0\
charscalex101 triplet or the\par\pard\qj \li956\ri149\sb0\sl-219\slmult0\fi0 \up0
\expndtw0\charscalex100 T4�A17 base-pair. No crosspeaks are seen between \line \up0
\expndtw0\charscalex102 the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20
base protons and those of the T27�A3�T18 \line \up0 \expndtw0\charscalex101
triplet. Figure \up0 \expndtw-2\charscalex100 3 \up0 \expndtw0\charscalex105 shows
the H1', H5 \up0 \expndtw-3\charscalex100 aromatic\par\pard\qj \li956\ri149\sb0\
sl-219\slmult0 \up0 \expndtw-1\charscalex100 region of a\ul0\super\cf16\f17\fs18\
ul0\super\cf16\f17\fs17 2\ul0\nosupersub\cf7\f8\fs20 H\ul0\sub\cf16\f17\fs18 2\
ul0\nosupersub\cf7\f8\fs20 O NOESY spectrum of the DTA \up0 \expndtw-2\
charscalex100 triplex at \up0 \expndtw0\charscalex100 25\ul0\nosupersub\cf25\f26\
fs20 \u-3920?\ul0\nosupersub\cf7\f8\fs20 C. The lettered crosspeaks are be-\
par\pard\qj \li956\ri149\sb0\sl-219\slmult0\fi0 \up0 \expndtw-3\charscalex100 tween
protons of the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 ring
systems and those \up0 \expndtw0\charscalex102 of either the targeted
T4�A17 \up0 \expndtw0\charscalex101 base-pair or the\par\pard\qj \li956\ri149\
sb0\sl-219\slmult0 \up0 \expndtw-2\charscalex100 adjacent T29�A5�T16 triplet.
Specifically, crosspeaks \up0 \expndtw-1\charscalex100 a through c involve the
A ring of D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28, cross-\line
\up0 \expndtw0\charscalex109 peaks d through k involve the B ring, and \up0
\expndtw0\charscalex101 crosspeaks l through u involve the C ring. \
up0 \expndtw0\charscalex100 Crosspeak v is the large T27H3'-T27H6 crosspeak, \up0 \
expndtw0\charscalex104 indicating that the T27 \up0 \expndtw0\charscalex106
sugar has an N-type\par\pard\qj \li956\ri149\sb1\sl-219\slmult0 \up0 \expndtw0\
charscalex100 pucker. In addition, each ring primarily has NOEs \line \up0 \
expndtw0\charscalex103 to a different strand of the triplex. All crosspeaks \line \
up0 \expndtw0\charscalex104 from the A ring are to the third strand base, T29.\par\
pard\column \ql \li5856\sb0\sl-230\slmult0 \par\pard\ql \li5856\sb0\sl-230\
slmult0 \par\pard\ql \li20\sb126\sl-230\slmult0 \up0 \expndtw0\charscalex102 All
crosspeaks from the B ring are to the\par\pard\qj \li20\ri1643\sb0\
sl-219\slmult0 \up0 \expndtw-2\charscalex100 Watson-Crick purine strand (T4 and
A5), except \line \up0 \expndtw0\charscalex102 crosspeak d, which is to T29. All
crosspeaks from \line \up0 \expndtw0\charscalex100 the C ring are to the
Watson-Crick pyrimidine \line \up0 \expndtw0\charscalex102 strand (T16 and A17)
except crosspeak l, which is \line \up0 \expndtw0\charscalex102 to A5.\par\pard\
ql \li219\sb1\sl-217\slmult0\tx1214 \up0 \expndtw-2\charscalex100 Figure \up0 \
expndtw-2\charscalex100 4\tab \up0 \expndtw0\charscalex102 shows the H2',2",Me-
aromatic, H1'\par\pard\qj \li20\ri1643\sb1\sl-219\slmult0 \up0 \expndtw-2\
charscalex100 region of the\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 2\ul0\
nosupersub\cf7\f8\fs20 H\ul0\sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 O
NOESY spectrum. Crosspeaks a \line \up0 \expndtw-1\charscalex100 through c involve
the A ring of D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28, crosspeaks
d \line \up0 \expndtw0\charscalex100 through h involve the B ring and
crosspeaks i \line \up0 \expndtw0\charscalex105 through m involve the C ring. Just
as in the H1', \line \up0 \expndtw-1\charscalex100 H5-aromatic region, each ring
primarily has NOEs \line \up0 \expndtw0\charscalex102 to a different strand of the
triplex. The A ring has \line \up0 \expndtw-2\charscalex100 crosspeaks to only T29
(third strand), the B ring has \line \up0 \expndtw-2\charscalex100 crosspeaks to
only T4 (Watson-Crick purine strand) \line \up0 \expndtw0\charscalex109 and the C
ring has crosspeaks to only T16 \line \up0 \expndtw0\charscalex100 (Watson-
Crick pyrimidine strand). The one excep-\line \up0 \expndtw-1\charscalex100 tion
is the T4Me, which has crosspeaks to both \line \up0 \expndtw0\charscalex103
A and B rings. Both the T4Me and the T4H6 \line \up0 \expndtw-4\
charscalex100 resonances have large upfield shifts compared to \line \up0 \
expndtw-1\charscalex100 the usual triplex TMe and TH6 chemical shifts, \line
\up0 \expndtw0\charscalex103 as is illustrated by the position of their crosspeak \
line \up0 \expndtw0\charscalex102 (Figure 4, peak n); for comparison, the
crosspeak
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145140051451401ffd9}}}}}\pard\sb0\sl-240{\bkmkstart Pg5}{\bkmkend Pg5}\par\pard\
li956\sb0\sl-230\slmult0\par\pard\li956\sb100\sl-230\slmult0\fi0\tx6448 \up0 \
expndtw-1\charscalex100 \ul0\nosupersub\cf22\f23\fs20 1056\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\
cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\par\pard\qj \
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\ri1685\sb55\sl-200\slmult0\fi179 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf19\f20\fs18 Figure 3.\ul0\nosupersub\cf13\f14\fs18 H1', H5 aromatic
region \line \up0 \expndtw0\charscalex108 of the \up0 \expndtw0\charscalex105 2D
NOESY spectrum of \line \up0 \expndtw0\charscalex100 the DTA triplex in\ul0\
super\cf8\f9\fs16 2\ul0\nosupersub\cf13\f14\fs18 H\ul0\nosupersub\cf8\f9\fs11 2\
ul0\nosupersub\cf13\f14\fs18 O at 25\ul0\nosupersub\cf27\f28\fs18 \u-3920?\ul0\
nosupersub\cf13\f14\fs18 C \line \up0 \expndtw0\charscalex100 and\ul0\nosupersub\
cf12\f13\fs18 t\ul0\nosupersub\cf8\f9\fs11 m\ul0\nosupersub\cf13\f14\fs18 =
200 ms. The sequential \line \up0 \expndtw0\charscalex102 assignments are
indicated with \line \up0 \expndtw0\charscalex100 continuous lines.
Disruptions in \line \up0 \expndtw0\charscalex100 the sequential
connectivities be-\line \up0 \expndtw-1\charscalex100 tween T4 and A5, T16 and
A17, and \line \up0 \expndtw-2\charscalex100 T27 and D\ul0\nosupersub\cf8\f9\fs11
3\ul0\nosupersub\cf13\f14\fs18 28 are connected with \line \up0 \expndtw0\
charscalex102 broken lines, and the intra-residue \line \up0 \expndtw0\
charscalex100 (aromatic-H1') crosspeak is labeled \line \up0 \expndtw0\
charscalex103 with the residue number. The \line \up0 \expndtw0\
charscalex102 missing crosspeaks are indicated \line \up0 \expndtw-2\
charscalex100 with boxes. Inter-residue crosspeaks \line \dn2 \expndtw-2\
charscalex100 involving the D\ul0\nosupersub\cf8\f9\fs11 3 \up0
\expndtw-2\charscalex100 \ul0\nosupersub\cf13\f14\fs18 aromatic rings \par\pard\
qj \li7529\ri1699\sb2\sl-198\slmult0 \up0 \expndtw0\charscalex103 are: a,
T29H6-H2A; b, T29H6-\line \up0 \expndtw0\charscalex102 H5A; c, T29H1'-H5A;
d, T29H1'-\line \up0 \expndtw-1\charscalex100 H6B; e, T4H1'-H5B; f, T4H1'-H4B;
\line \up0 \expndtw0\charscalex100 g, T4H6-H5B; h, T4H6-H6B; i, H6B-\line \up0 \
expndtw0\charscalex101 A5H8; j, H5B-A5H8; k, H4B-A5H8; \line \up0 \expndtw0\
charscalex104 l, H3/5C-A5H2; m, T16H1'-H4C; \line \up0 \expndtw0\charscalex102
n, T16H1'-H3/5C; o, H4C-T16H6; \line \up0 \expndtw0\charscalex100 p, H3/5C-
T16H6; q, A17H1'-H3/5C; \line \up0 \expndtw0\charscalex102 r, H3/5C-A17H2; s,
H2/6C-A17H2; \line \up0 \expndtw0\charscalex103 t, H4C-A17H8; and u,
H3/5C-\line \up0 \expndtw0\charscalex100 A17H8. Crosspeak v is the large, \
line \up0 \expndtw0\charscalex100 intra-residue T27H3'-H6 \up0 \expndtw-2\
charscalex100 NOE. \par\pard\qj \li7529\ri1639\sb1\sl-200\slmult0\fi0 \up0 \
expndtw-2\charscalex100 Intra- and inter-ring crosspeaks of \line \up0 \
expndtw-3\charscalex100 the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\
f14\fs18 base are marked with a *. \line \up0 \expndtw0\charscalex102 The
spectrum was acquired with a \line \up0 \expndtw-2\charscalex100 spectral width
of 5000 Hz in both \line \up0 \expndtw-4\charscalex100 dimensions; 1024 and
400 complex \line \up0 \expndtw-4\charscalex100 points were collected in t\
ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 and t\ul0\nosupersub\
cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 , \line \up0 \expndtw-4\charscalex100
respectively, with \dn3 \expndtw-4\charscalex100 32 scans per t\ul0\nosupersub\
cf8\f9\fs11 1 \par\pard\qj \li7529\ri1663\sb1\sl-200\slmult0 \up0 \expndtw-3\
charscalex100 \ul0\nosupersub\cf13\f14\fs18 block. In both dimensions 400 points \
up0 \expndtw-2\charscalex100 were apodized using a 45\ul0\nosupersub\cf27\f28\
fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 -phase-\line \up0 \expndtw0\
charscalex100 shifted squared sinebell; both di\up0 \expndtw-1\charscalex100
mensions were zero-filled to 2048 \up0 \expndtw-1\charscalex100 complex
points.\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\colw6244\
colsr160\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb0\sl-230\slmult0 \par\
pard\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb69\sl-230\slmult0 \up0 \
expndtw-2\charscalex100 \ul0\nosupersub\cf7\f8\fs20 between T18Me and T18H6 is
also labeled (Fig-\par\pard\ql \li956\sb1\sl-216\slmult0 \up0 \expndtw0\
charscalex104 ure 4, peak o).\par\pard\qj \li956\ri149\sb1\sl-219\slmult0\fi199 \
up0 \expndtw-2\charscalex100 Just as in the imino-imino region of the H\
ul0\sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 O \up0 \expndtw-1\charscalex100
NOESY spectrum, some disruptions in the sequen-\line \up0 \expndtw-1\charscalex100
tial connectivities are observed. No base-H1' or \up0 \expndtw-2\
charscalex100 base-H2',H2" sequential connectivities are observed \up0 \expndtw-2\
charscalex100 between D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28
and T27, between T4 and A5, or \up0 \expndtw0\charscalex102 between A17 and
T16 (Figure 3).\par\pard\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb60\sl-
230\slmult0 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf24\f25\fs20 NOE
restraints\par\pard\qj \li956\ri149\sb138\sl-219\slmult0\fi199 \up0 \expndtw-4\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 A total of 728 distance restraints were
used for the \line \up0 \expndtw0\charscalex101 refinement steps prior to
relaxation matrix refine-\line \up0 \expndtw-4\charscalex100 ment. Of these, 62 are
hydrogen-bond restraints, 408 \line \up0 \expndtw-1\charscalex100 are derived
from\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 2\ul0\nosupersub\cf7\f8\fs20
H\ul0\sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 O NOESY spectra, 132
are \line \up0 \expndtw0\charscalex100 derived from the H\ul0\sub\cf16\f17\fs18 2\
ul0\nosupersub\cf7\f8\fs20 O NOESY spectrum, and 126 \line \up0 \expndtw0\
charscalex101 are repulsive restraints derived from predicted \line \up0 \
expndtw-1\charscalex100 \ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 2\ul0\
nosupersub\cf7\f8\fs20 H\ul0\sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 O
NOESY crosspeak volumes. The distribution \line \up0 \expndtw0\charscalex104 of
distance restraints by residue is shown in Fig-\line \up0 \expndtw0\charscalex102
ure 5(a). In Figure 5(b), the distance restraints are \line \up0 \expndtw0\
charscalex100 classified as intra-residue, sequential and inter-\line \up0 \
expndtw-2\charscalex100 residue (involving residues other than neighboring \line \
up0 \expndtw-2\charscalex100 residues) restraints. For relaxation matrix
refine-\line \up0 \expndtw0\charscalex102 ment, the \up0 \expndtw0\charscalex102 \
ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 2\ul0\nosupersub\cf7\f8\fs20 H\ul0\
sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 O and repulsive restraints
were\par\pard\column \ql \li5856\sb0\sl-230\slmult0 \par\pard\ql \li5856\sb0\sl-
230\slmult0 \par\pard\ql \li5856\sb0\sl-230\slmult0 \par\pard\ql \li20\sb69\sl-230\
slmult0 \up0 \expndtw0\charscalex103 converted to volume restraints at all five
NOESY\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex100
mixing times yielding 2670 volume restraints. The \up0 \expndtw-2\charscalex100
remaining 194 water and hydrogen-bond distance \up0 \expndtw0\charscalex101
restraints were left as distance restraints.\par\pard\ql \li5856\sb0\sl-230\slmult0
\par\pard\ql \li20\sb59\sl-230\slmult0 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf24\f25\fs20 Torsion angle restraints\par\pard\qj \li20\ri1643\sb139\
sl-219\slmult0\fi199 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\cf7\f8\fs20
Torsion angle restraints for the sugar puckers and \up0 \expndtw-1\charscalex100 \
ul0\nosupersub\cf10\f11\fs20 d\ul0\nosupersub\cf7\f8\fs20 backbone angles were
calculated from H1' to \up0 \expndtw-3\charscalex100 H2',2" crosspeaks in a\ul0\
super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 2\ul0\nosupersub\cf7\f8\fs20 H\ul0\
sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 O P.COSY spectrum (data \up0 \
expndtw0\charscalex102 not shown). The residues that had sufficiently \up0 \
expndtw0\charscalex101 resolved crosspeaks to obtain reliable coupling \up0 \
expndtw-1\charscalex100 constants using CHEOPS are indicated in Figure 5. \up0 \
expndtw0\charscalex104 The peak fits had correlation coefficients that \up0 \
expndtw0\charscalex102 ranged from 90 to 96%.\par\pard\qj \li20\ri1643\sb0\sl-219\
slmult0\fi199 \up0 \expndtw0\charscalex100 To restrain the\ul0\nosupersub\cf10\f11\
fs20 e\ul0\nosupersub\cf7\f8\fs20 backbone angle, a\ul0\super\cf16\f17\fs18\ul0\
super\cf16\f17\fs17 31\ul0\nosupersub\cf7\f8\fs20 P-\ul0\super\cf16\f17\fs18\ul0\
super\cf16\f17\fs17 1\ul0\nosupersub\cf7\f8\fs20 H\ul0\super\cf16\f17\fs18\ul0\
super\cf16\f17\fs17 2\ul0\nosupersub\cf7\f8\fs20 H\ul0\sub\cf16\f17\fs18 2\ul0\
nosupersub\cf7\f8\fs20 O \up0 \expndtw0\charscalex100 heteroCOSY was collected
(data not shown) from \up0 \expndtw-2\charscalex100 which the\ul0\nosupersub\cf9\
f10\fs20 J\ul0\super\cf8\f9\fs17\ul0\super\cf8\f9\fs16 P,H3'\ul0\nosupersub\cf7\
f8\fs20 couplings were determined to be no \up0 \expndtw0\charscalex101 greater
than 14 Hz, indicating that the\ul0\nosupersub\cf10\f11\fs20 e\ul0\nosupersub\
cf7\f8\fs20 dihedral \up0 \expndtw0\charscalex108 angles were not in the \
up0 \expndtw0\charscalex100 +\ul0\nosupersub\cf9\f10\fs20 gauche\ul0\nosupersub\
cf7\f8\fs20 conformation\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0\fi0 \up0 \
expndtw-2\charscalex100 (Blommers\ul0\nosupersub\cf9\f10\fs20 et al\ul0\
nosupersub\cf7\f8\fs20 ., 1991; Roongta\ul0\nosupersub\cf9\f10\fs20 et al\ul0\
nosupersub\cf7\f8\fs20 ., 1990). All \up0 \expndtw-1\charscalex100 residues were
restrained to exclude the +\ul0\nosupersub\cf9\f10\fs20 gauche \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 conformation for the\ul0\nosupersub\cf10\
f11\fs20 e\ul0\nosupersub\cf7\f8\fs20 angle.\par\pard\ql \li219\sb0\sl-219\
slmult0 \up0 \expndtw0\charscalex105 We are aware that there has been some recent \
par\pard\sect\sectd\fs24\paperw12240\paperh15840{\shp
{\*\shpinst\shpleft0\shptop0\shpright12240\shpbottom15840\shpwr3\shpfblwtxt0\shpz-
10000\shplid5
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28a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a
28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a
0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a002
8a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a2
8a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0
028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028
a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28
a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a00
28a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a
28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a
0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a002
8a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a2
8a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0
028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028
a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28
a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a00
28a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a
28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a
0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a002
8a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a2
8a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0
028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028
a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28
a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a00
28a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a
28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a
0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a002
8a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a2
8a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0
028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028
a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28
a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a00
28a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a0028a28a00ffd9}}}}}\
pard\sb0\sl-240{\bkmkstart Pg6}{\bkmkend Pg6}\par\pard\li956\sb0\sl-218\slmult0\
par\pard\li956\sb151\sl-218\slmult0\fi0\tx9955 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\
ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1057\par\pard\qj \li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\
slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\ri1699\sb108\sl-
200\slmult0\fi179 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf19\f20\fs18
Figure 4.\ul0\nosupersub\cf13\f14\fs18 The H2',2",Me-aromatic, \line \up0 \
expndtw0\charscalex101 H1' region of the same 2D NOESY \line \up0 \expndtw0\
charscalex102 spectrum as in Figure \up0 \expndtw0\charscalex102 3. Inter-\par\
pard\qj \li7529\ri1655\sb24\sl-196\slmult0 \up0 \expndtw-1\charscalex100 residue
crosspeaks involving the D\ul0\nosupersub\cf8\f9\fs11 3 \line \up0 \expndtw0\
charscalex103 \ul0\nosupersub\cf13\f14\fs18 aromatic protons are: a, T29Me-\
line \up0 \expndtw0\charscalex101 H2A; b, T4Me-H5A; c, T4Me-H2A; \line \up0 \
expndtw0\charscalex100 d, T4Me-H6B (partially overlapp-\line \up0 \expndtw0\
charscalex100 ing T4Me-A3H8); e, T4Me-H2B; \line \up0 \expndtw0\charscalex100
f, T4H2',2"-H4B; g, T4H2',2"-H5B; \line \up0 \expndtw-3\charscalex100 h,
T4H2',2"-H6B; i, T16Me-H4C (par-\line \up0 \expndtw-1\charscalex100 tially
overlapping T29Me-T29H1'); \line \up0 \expndtw0\charscalex104 j, T16Me-H3/5C; k,
T16Me-H2/6C; \line \up0 \expndtw-2\charscalex100 l, T16H2',2"-H4C; and m,
T16H2',2"-\line \up0 \expndtw-2\charscalex100 H3/5C. Crosspeak n is the upfield \
par\pard\li7529\sb8\sl-207\slmult0\fi0\tx9473 \up0 \expndtw0\charscalex101 shifted
T4Me-T4H6\tab \up0 \expndtw0\charscalex101 NOE and\par\pard\li7529\sb1\sl-197\
slmult0\fi0 \up0 \expndtw0\charscalex101 crosspeak o, is a typical TH6-TMe\par\
pard\li7529\sb1\sl-199\slmult0\fi0 \up0 \expndtw0\charscalex101 NOE (T18Me-T18H6).\
par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\colw6244\
colsr160\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb0\sl-230\slmult0 \par\
pard\ql \li956\sb93\sl-230\slmult0 \up0 \expndtw0\charscalex102 \ul0\nosupersub\
cf7\f8\fs20 debate concerning the validity of fitting coupling\par\pard\qj \li956\
ri149\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex106 constants to a two-state
sugar pucker model \up0 \expndtw-2\charscalex100 (Harbison, 1993; Zhu\ul0\
nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1994). However, most
of \up0 \expndtw0\charscalex102 the measurable sugar puckers were almost exclu-\
line \up0 \expndtw0\charscalex103 sively S-type, with the exception of T27, which
is \up0 \expndtw-1\charscalex100 predominantly N-type.\par\pard\ql \li956\sb0\sl-
230\slmult0 \par\pard\ql \li956\sb59\sl-230\slmult0 \up0 \expndtw-1\charscalex100 \
ul0\nosupersub\cf24\f25\fs20 DTA triplex structure\par\pard\qj \li956\ri149\sb138\
sl-219\slmult0\fi199 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf7\f8\fs20
Figure 6 shows several views of the refined DTA \line \up0 \expndtw0\charscalex102
triplex structures. The seven lowest energy struc-\line \up0 \expndtw0\
charscalex101 tures are shown superimposed in Figure 6(a). The \line \up0 \expndtw-
4\charscalex100 average RMS deviations from ideal geometry for the \line \up0 \
expndtw-5\charscalex100 bonds, angles and impropers are 0.008 A\u730?, 1.592\ul0\
nosupersub\cf25\f26\fs20 \u-3920?\ul0\nosupersub\cf7\f8\fs20 and \line \up0 \
expndtw-2\charscalex100 0.276\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\nosupersub\
cf7\f8\fs20 , respectively, indicating that these structures \line \up0 \expndtw-1\
charscalex100 have very good covalent geometry. The loops have \line \up0 \
expndtw0\charscalex100 few restraints (Figure 5) and adopt many different \line \
up0 \expndtw-4\charscalex100 conformations (not shown). The terminal triplets are \
line \up0 \expndtw0\charscalex101 strongly perturbed by the conformation of
the \line \up0 \expndtw0\charscalex100 loops, which artificially increases the
variability of \line \up0 \expndtw0\charscalex101 these triplets.
In addition, the two triplets at the 5' \line \up0 \expndtw-3\charscalex100 end of
the triplex (with respect to the purine strand) \line \up0 \expndtw-4\charscalex100
are only partially assigned (Table 1) leading to many \line \up0 \expndtw-2\
charscalex100 fewer restraints and greater conformational free-\line \up0 \
expndtw0\charscalex100 dom. For these reasons, only the atoms in this \line
\up0 \expndtw0\charscalex103 \u8216?\u8216?core\u8217?\u8217? of the triplex
(triplets 3 to 7) were used to \line \up0 \expndtw0\charscalex101 calculate the
superposition of structures. These \line \up0 \expndtw0\charscalex104 effects
are also apparent in the RMSD of the \line \up0 \expndtw0\charscalex100
individual residues (Figure 7). The loops and the \line \up0 \expndtw0\
charscalex100 terminal triplets have a larger RMSD compared to\par\pard\column \
ql \li5856\sb0\sl-230\slmult0 \par\pard\ql \li5856\sb0\sl-230\slmult0 \par\pard\
ql \li20\sb93\sl-230\slmult0 \up0 \expndtw-1\charscalex100 the core of the triplex.
The average pairwise RMSD\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0\fi0 \up0 \
expndtw-1\charscalex100 and the average\ul0\nosupersub\cf9\f10\fs20 R\ul0\sub\
cf16\f17\fs18 1/6\ul0\nosupersub\cf7\f8\fs20 -factor (Brunger, 1992) for the \up0
\expndtw0\charscalex103 core of the DTA triplex are \up0 \expndtw-2\
charscalex100 1.3 \up0 \expndtw0\charscalex101 (\ul0\nosupersub\cf10\f11\fs20 2\
ul0\nosupersub\cf7\f8\fs20 0.19) A\u730? and\par\pard\ql \li20\sb1\sl-217\
slmult0 \up0 \expndtw-2\charscalex100 3.9 \up0 \expndtw0\charscalex104 (\ul0\
nosupersub\cf10\f11\fs20 2\ul0\nosupersub\cf7\f8\fs20 0.1)%, respectively. The
number of NOE\par\pard\qj \li20\ri1643\sb1\sl-219\slmult0\fi0 \up0 \expndtw-1\
charscalex100 distance violations greater than 0.2 A\u730? varied from \line \
up0 \expndtw0\charscalex102 one to three per structure and the number of \
line \up0 \expndtw-1\charscalex100 dihedral angle violations greater than \
up0 \expndtw-1\charscalex100 5\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\
nosupersub\cf7\f8\fs20 varied\par\pard\ql \li20\sb0\sl-219\slmult0 \up0 \
expndtw0\charscalex101 from four to seven per structure.\par\pard\qj \li20\ri1643\
sb0\sl-219\slmult0\fi199 \up0 \expndtw-1\charscalex100 The backbone angles,
glycosidic angles, sugar \up0 \expndtw-4\charscalex100 puckers and angles
specific to the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base are
shown \up0 \expndtw0\charscalex102 in Figure 8 for all seven lowest energy
structures. \up0 \expndtw0\charscalex100 Most torsion angles fall into the standard
range of \up0 \expndtw-4\charscalex100 conformations \up0 \expndtw-3\charscalex100
(Saenger, \up0 \expndtw-2\charscalex100 1984). However, several\par\pard\qj \
li20\ri1643\sb0\sl-219\slmult0\fi0 \up0 \expndtw-2\charscalex100 angles
consistently adopt unusual conformations in \up0 \expndtw-3\charscalex100 many of
the refined structures: the glycosidic angle, \up0 \expndtw-3\charscalex100 \ul0\
nosupersub\cf10\f11\fs20 x\ul0\nosupersub\cf7\f8\fs20 , in residues A5, A17 and
T27, prefers the high-anti \up0 \expndtw0\charscalex100 conformation; C19, C\ul0\
super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 26 and
T27 all have N-type \up0 \expndtw-1\charscalex100 sugar puckers; and the T27\
ul0\nosupersub\cf10\f11\fs20 b\ul0\nosupersub\cf7\f8\fs20 angle prefers the \
up0 \expndtw-2\charscalex100 +\ul0\nosupersub\cf9\f10\fs20 gauche\ul0\nosupersub\
cf7\f8\fs20 conformation.\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0\fi199 \up0 \
expndtw0\charscalex100 The helix parameters are shown in Figure 9 as a \line \up0 \
expndtw-4\charscalex100 function of residue or base step. The X-displacement \
line \up0 \expndtw0\charscalex100 is very uniform with good precision, although the
\line \up0 \expndtw-3\charscalex100 precision decreases towards the 5' end (with
respect \line \up0 \expndtw-1\charscalex100 to the purine strand) of the
triplex due to sub-\line \up0 \expndtw-2\charscalex100 stantially fewer
restraints on the two 5'-terminal \line \up0 \expndtw0\charscalex100 triplets.
The axial rise is also fairly uniform except \line \up0 \expndtw0\charscalex102 for
the T4-A5 base step, where the rise more than \line \up0 \expndtw-1\charscalex100
doubles as a result of the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\
fs20 intercalation. The \line \up0 \expndtw-2\charscalex100 helical twist
exhibits the greatest stepwise variation \line \up0 \expndtw0\charscalex101 of all
the helix parameters and also has the lowest \par\pard\sect\sectd\fs24\paperw12240\
paperh15840{\shp
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9}}}}}\pard\sb0\sl-240{\bkmkstart Pg7}{\bkmkend Pg7}\par\pard\li956\sb0\sl-230\
slmult0\par\pard\li956\sb100\sl-230\slmult0\fi0\tx6448 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1058\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\
cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\par\pard\qj \
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\sb0\sl-200\slmult0 \par\pard\qj\
li7529\sb0\sl-200\slmult0 \par\pard\qj\li7529\ri1699\sb75\sl-200\slmult0\fi179 \up0
\expndtw-1\charscalex100 \ul0\nosupersub\cf19\f20\fs18 Figure 5.\ul0\nosupersub\
cf13\f14\fs18 Number of NOE dis-\line \up0 \expndtw0\charscalex100 tance
restraints per residue. (a) The \line \up0 \expndtw0\charscalex101 distance
restraints are classified by \line \up0 \expndtw-2\charscalex100 type as:
quantitative, non-exchange-\line \up0 \expndtw-2\charscalex100 able NOEs from \
dn3 \expndtw-2\charscalex100 \ul0\super\cf8\f9\fs16 2\ul0\nosupersub\cf13\f14\fs18
H\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O NOESY \par\pard\qj
\li7529\ri1664\sb1\sl-200\slmult0\fi0 \up0 \expndtw-1\charscalex100 spectra;
qualitative, exchangeable \line \up0 \expndtw0\charscalex101 NOEs from the H\ul0\
nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O NOESY spec-\line \up0 \
expndtw-3\charscalex100 trum; hydrogen bonds; and repul-\line \up0 \expndtw0\
charscalex100 sive. (b) The distance restraints are \line \up0 \expndtw0\
charscalex100 classified by their range: intra-\line \up0 \expndtw-3\
charscalex100 residue, sequential and inter-residue \line \up0 \expndtw0\
charscalex100 (other than sequential). The light \line \up0 \expndtw0\
charscalex100 gray regions correspond to the \line \up0 \expndtw-1\
charscalex100 loop residues of the DTA triplex. \line \up0 \expndtw-1\
charscalex100 Residues with restraints on the\ul0\nosupersub\cf12\f13\fs18
d \line \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf13\f14\fs18 torsion angle
are marked with a *.\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\
colno2\colw6244\colsr160\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb0\sl-
230\slmult0 \par\pard\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb67\sl-230\
slmult0 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf7\f8\fs20 precision,
indicating that it is the least well-defined\par\pard\qj \li956\ri149\sb0\sl-219\
slmult0 \up0 \expndtw0\charscalex101 helical parameter. Again, the 5' end of the
triplex \up0 \expndtw-1\charscalex100 displays the most variation.\par\pard\qj \
li956\ri149\sb0\sl-219\slmult0\fi199 \up0 \expndtw-4\charscalex100 The conformation
of the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base is best
illustrated \line \up0 \expndtw-1\charscalex100 by the superposition of the D\ul0\
sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base from the seven \line \up0 \
expndtw0\charscalex100 lowest energy structures (Figure 6(c)). The C ring \line \
up0 \expndtw0\charscalex103 and peptide group are clearly not as restricted in \
line \up0 \expndtw0\charscalex102 their conformation as the rest of the D\ul0\sub\
cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base. The \line \up0 \expndtw-1\
charscalex100 major conformation is depicted schematically in \line \up0 \
expndtw0\charscalex100 Figure 1(a).\par\pard\qj \li956\ri149\sb0\sl-219\slmult0\
fi199 \up0 \expndtw-3\charscalex100 The stacking of the D\ul0\sub\cf16\f17\fs18 3\
ul0\nosupersub\cf7\f8\fs20 28 base on the neighboring \line \up0 \expndtw-2\
charscalex100 T16�A5�T29 triplet and T4�A17 base-pair is illus-\line \up0 \
expndtw0\charscalex102 trated in Figure 10. The sequence specificity of D\ul0\sub\
cf16\f17\fs18 3 \line \up0 \expndtw0\charscalex103 \ul0\nosupersub\cf7\f8\fs20
intercalation is also addressed, where the T4�A17 \line \up0 \expndtw0\
charscalex102 base-pair has been isosterically replaced with the \line \up0 \
expndtw0\charscalex101 three other possible Watson-Crick base-pairs, and \line \up0
\expndtw0\charscalex100 the T16�A5�T29 triplet has been isosterically re-\
line \up0 \expndtw-3\charscalex100 placed with a C\ul0\super\cf16\f17\fs18\ul0\
super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 �G�C triplet. The D\ul0\sub\cf16\
f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base stacks with \line \up0 \expndtw0\
charscalex100 greater overlap and the peptide group is more \line \up0 \
expndtw0\charscalex100 centered over the polar groups between the bases, \line \up0
\expndtw-1\charscalex100 when the target base-pair is a T�A or C�G base-pair \
line \up0 \expndtw-2\charscalex100 instead of a A�T or G�C base-pair. The
D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base\par\pard\column \ql \
li5856\sb0\sl-230\slmult0 \par\pard\ql \li5856\sb0\sl-230\slmult0 \par\pard\ql \
li5856\sb0\sl-230\slmult0 \par\pard\ql \li20\sb67\sl-230\slmult0 \up0 \expndtw0\
charscalex101 stacking is illustrated from a different view in\par\pard\ql \
li20\sb1\sl-216\slmult0 \up0 \expndtw0\charscalex101 Figure 6(b), highlighting its
similarity to a triplet.\par\pard\ql \li20\sb214\sl-276\slmult0 \up0 \expndtw-3\
charscalex100 \ul0\nosupersub\cf15\f16\fs24 Discussion\par\pard\ql \li5856\sb0\sl-
230\slmult0 \par\pard\ql \li20\sb10\sl-230\slmult0 \up0 \expndtw-1\charscalex100 \
ul0\nosupersub\cf24\f25\fs20 Intramolecular triplex formation\par\pard\qj \li20\
ri1560\sb138\sl-219\slmult0\fi199 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\
cf7\f8\fs20 The data presented here demonstrate that the \line \up0 \expndtw-
3\charscalex100 DTA sequence forms a stable intramolecular triplex. \line \up0 \
expndtw0\charscalex102 The NOESY spectrum of the exchangeable reson-\line \up0 \
expndtw0\charscalex101 ances (Figure 2) strongly resembles those of other \line \
up0 \expndtw-2\charscalex100 triplexes (Sklena�\u345? & Feigon, 1990). Fifteen
sharp, \line \up0 \expndtw-4\charscalex100 well-defined resonances are observed in
the spectral \line \up0 \expndtw0\charscalex100 region where hydrogen-bonded imino
protons are \line \up0 \expndtw0\charscalex101 found. These have been assigned
to the imino \line \up0 \expndtw0\charscalex104 protons of the eight Watson-Crick
and the seven \line \up0 \expndtw0\charscalex100 Hoogsteen base-pairs. Further
evidence for triplex \line \up0 \expndtw-2\charscalex100 formation is indicated by
the presence of C\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\
cf7\f8\fs20 amino \line \up0 \expndtw0\charscalex102 resonances, which are
characteristically shifted \line \up0 \expndtw-2\charscalex100 downfield. With
the exceptions discussed above, \line \up0 \expndtw-2\charscalex100 sequential
imino-imino NOE connectivities may be \line \up0 \expndtw0\charscalex103 traced, as
is seen in Figure 2(a). \par\pard\sect\sectd\fs24\paperw12240\paperh15840{\shp
{\*\shpinst\shpleft0\shptop0\shpright12240\shpbottom15840\shpwr3\shpfblwtxt0\shpz-
10000\shplid7
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ffd9}}}}}\pard\sb0\sl-240{\bkmkstart Pg8}{\bkmkend Pg8}\par\pard\ql \li1673\sb0\sl-
230\slmult0 \par\pard\ql\li1673\sb220\sl-230\slmult0 \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf26\f27\fs20 (a) \par\pard\ql \li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb100\sl-230\slmult0 \up0 \expndtw-2\charscalex100
(b) \par\pard\ql \li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb0\sl-230\
slmult0 \par\pard\ql\li1673\sb0\sl-230\slmult0 \par\pard\ql\li1673\sb200\sl-230\
slmult0 \up0 \expndtw-2\charscalex100 (c) \par\pard\qj \li956\sb0\sl-205\slmult0 \
par\pard\qj\li956\sb0\sl-205\slmult0 \par\pard\qj\li956\sb0\sl-205\slmult0 \par\
pard\qj\li956\sb0\sl-205\slmult0 \par\pard\qj\li956\sb0\sl-205\slmult0 \par\pard\
qj\li956\sb0\sl-205\slmult0 \par\pard\qj\li956\sb0\sl-205\slmult0 \par\pard\qj\
li956\sb0\sl-205\slmult0 \par\pard\qj\li956\sb0\sl-205\slmult0 \par\pard\qj\li956\
sb0\sl-205\slmult0 \par\pard\qj\li956\sb0\sl-205\slmult0 \par\pard\qj\li956\sb0\sl-
205\slmult0 \par\pard\qj\li956\ri1638\sb131\sl-205\slmult0\fi179 \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf19\f20\fs18 Figure 6.\ul0\nosupersub\cf13\f14\fs18
Solution structures of the DTA triplex. The Watson-Crick purine strand is
yellow, the Watson-Crick \line \up0 \expndtw0\charscalex103 pyrimidine strand is
red and the third strand is blue. (a) Stereo view of the seven lowest energy
structures looking \line \up0 \expndtw-2\charscalex100 into the groove formed by
the Watson-Crick pyrimidine strand and the third strand. The D\ul0\nosupersub\cf8\
f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base is green. Loop residues \line \up0 \
expndtw0\charscalex100 are not shown. (b) Similar view as in (a) but of a single
structure to illustrate how the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\
f14\fs18 base mimics a triplet. Rings \line \up0 \expndtw0\charscalex100 A, B and
C of the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base are
blue, yellow and red, respectively, and the base of the D\ul0\nosupersub\cf8\f9\
fs11 3\ul0\nosupersub\cf13\f14\fs18 base is shown as filled sticks. \par\pard\
qj \li956\ri1698\sb16\sl-180\slmult0\fi0 \up0 \expndtw0\charscalex100 (c) View of
the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base of the seven
lowest energy structures looking into the major groove of the duplex portion of \
line \up0 \expndtw0\charscalex100 the triplex. The rings are colored as in (b). The
superpositions involved all heavy atoms shown in each Figure except \par\pard\ql \
li956\sb18\sl-207\slmult0 \up0 \expndtw0\charscalex100 for the terminal triplets,
the C\ul0\super\cf8\f9\fs16 +\ul0\nosupersub\cf13\f14\fs18 26 �G2 �C19 triplet and
the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 28 peptide group
and C-ring. \par\pard\sect\sectd\fs24\paperw12240\paperh15840{\shp
{\*\shpinst\shpleft0\shptop0\shpright12240\shpbottom15840\shpwr3\shpfblwtxt0\shpz-
10000\shplid8
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0014514500145145001451450014514500145145007ffd9}}}}}\pard\sb0\sl-240{\bkmkstart
Pg9}{\bkmkend Pg9}\par\pard\li956\sb0\sl-230\slmult0\par\pard\li956\sb100\sl-230\
slmult0\fi0\tx6448 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf22\f23\fs20
1060\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution
Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -
containing DNA Triplex\par\pard\qj \li7529\sb0\sl-201\slmult0 \par\pard\qj\li7529\
sb0\sl-201\slmult0 \par\pard\qj\li7529\sb0\sl-201\slmult0 \par\pard\qj\li7529\sb0\
sl-201\slmult0 \par\pard\qj\li7529\sb0\sl-201\slmult0 \par\pard\qj\li7529\sb0\sl-
201\slmult0 \par\pard\qj\li7529\sb0\sl-201\slmult0 \par\pard\qj\li7529\sb0\sl-201\
slmult0 \par\pard\qj\li7529\ri1642\sb146\sl-201\slmult0\fi179 \up0 \expndtw0\
charscalex100 \ul0\nosupersub\cf19\f20\fs18 Figure 7.\ul0\nosupersub\cf13\f14\fs18
Root-mean-squared de-\line \up0 \expndtw0\charscalex100 viation (RMSD) of the seven
lowest \line \up0 \expndtw0\charscalex103 energy structures on a per residue \
line \up0 \expndtw-2\charscalex100 basis. The RMSD is shown for all \line \
up0 \expndtw0\charscalex101 atoms, only the backbone atoms, \line \up0 \
expndtw-4\charscalex100 and only the base atoms. The shaded \line \up0 \expndtw-2\
charscalex100 regions mark the loop residues of \line \up0 \expndtw0\
charscalex110 the triplex. The best fit of the \line \up0 \expndtw-1\
charscalex100 structures was determined using all \line \up0 \expndtw-2\
charscalex100 atoms except the loops, the terminal \line \up0 \expndtw-3\
charscalex100 triplets, the C\ul0\super\cf8\f9\fs16 +\ul0\nosupersub\cf13\f14\fs18
26 �G2 �C19 triplet and \line \up0 \expndtw-3\charscalex100 the D\ul0\nosupersub\
cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 28 peptide group and C-ring.\par\pard\
sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\colw6244\colsr160\ql \
li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb227\sl-230\slmult0 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf24\f25\fs20 Helix morphology\par\pard\qj \li956\
ri149\sb218\sl-219\slmult0\fi199 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\cf7\
f8\fs20 The DTA triplex forms a regular helix that, in \line \up0 \expndtw-
3\charscalex100 many ways, is more similar to\ul0\nosupersub\cf9\f10\fs20 B\ul0\
nosupersub\cf7\f8\fs20 -DNA than\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\
f8\fs20 -DNA. \line \up0 \expndtw-2\charscalex100 This can be seen in the axial
rise, which shows little \line \up0 \expndtw-2\charscalex100 variation except at
the T4�A17-A5�T16 base step, \line \up0 \expndtw-1\charscalex100 where the rise
more than doubles to accommodate \line \up0 \expndtw-3\charscalex100 D\ul0\sub\
cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 intercalation (Figure 9(a)). If
the intercalation \line \up0 \expndtw0\charscalex101 step is ignored, the average
rise is 3.2 A\u730?, which is \line \up0 \expndtw-4\charscalex100 significantly
closer to the rise in\ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -
DNA (3.4 A\u730?) than \line \up0 \expndtw-2\charscalex100
in\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -DNA (2.6 A\u730?).\
par\pard\qj \li956\ri149\sb0\sl-219\slmult0\fi199 \up0 \expndtw0\charscalex105 In
contrast to the axial rise, the helical twist of \up0 \expndtw-3\charscalex100 the
DTA triplex is less regular (Figure 9(b)) and \up0 \expndtw0\charscalex102
resembles\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -DNA more than\
ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -DNA. The helical \up0 \
expndtw0\charscalex100 twist displays greater variation because only the\ul0\
nosupersub\cf10\f11\fs20 e \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf7\f8\
fs20 and\ul0\nosupersub\cf10\f11\fs20 d\ul0\nosupersub\cf7\f8\fs20 backbone
angles are restrained. In addition, \up0 \expndtw-1\charscalex100 the initial
base step \up0 \expndtw-1\charscalex100 (with respect to the purine\par\pard\
ql \li956\sb0\sl-219\slmult0 \up0 \expndtw-2\charscalex100 strand) is especially
variable for several reasons:\par\pard\column \ql \li5856\sb0\sl-230\slmult0 \
par\pard\ql \li20\sb227\sl-230\slmult0 \up0 \expndtw0\charscalex107 (1) it is the
terminal triplet that tends to be less\par\pard\qj \li20\ri1643\sb0\sl-219\
slmult0 \up0 \expndtw-3\charscalex100 stable; (2) the terminal triplet has
few resonance \up0 \expndtw-3\charscalex100 assignments \up0 \expndtw-8\
charscalex100 (Table \up0 \expndtw0\charscalex101 1) and, thus, few
restraints;\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-3\
charscalex100 and (3) even though T20 and T25 are connected \line \up0 \
expndtw0\charscalex103 by a loop, the loop is unassignable and therefore \line \up0
\expndtw-3\charscalex100 unrestrained during refinement, so it adopts a wide \
line \up0 \expndtw-4\charscalex100 range of conformations, which strongly perturbs
the \line \up0 \expndtw-2\charscalex100 conformation of the initial triplet. A
similar effect is \line \up0 \expndtw-1\charscalex100 seen for the second base
step, but to a lesser extent. \line \up0 \expndtw0\charscalex103 The intercalation
site also displays substantial \line \up0 \expndtw-2\charscalex100 variability,
which is related to the multiple con-\line \up0 \expndtw0\charscalex103
formations of the C ring of the D\ul0\sub\cf16\f17\fs18 3 \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 base \up0 \expndtw-2\charscalex100 (dis-\
par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex100 cussed
below). If we ignore the A1�T20-G2�C19 \up0 \expndtw-1\charscalex100 terminal
step and the T4�A17-A5�T16 intercalation \up0 \expndtw-3\charscalex100 step, then
the average twist is 31\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\nosupersub\cf7\
f8\fs20 , which, unlike the \up0 \expndtw0\charscalex105 axial rise, is more
similar to the twist in\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -
DNA \up0 \expndtw0\charscalex102 (33\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\
nosupersub\cf7\f8\fs20 ) than in\ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\
f8\fs20 -DNA (36\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\nosupersub\cf7\f8\
fs20 ).\par\pard\ql \li219\sb1\sl-217\slmult0 \up0 \expndtw-2\charscalex100 The X-
displacement of the Watson-Crick base-\par\pard\sect\sectd\sbknone \qj \li956\
sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-
210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\
slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0
\par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\
pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\
qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\
li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\
sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-
210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\
slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0
\par\pard\qj\li956\sb0\sl-210\slmult0 \par\pard\qj\li956\sb0\sl-210\slmult0 \par\
pard\qj\li956\ri1638\sb23\sl-210\slmult0\fi179 \up0 \expndtw-2\charscalex100 \ul0\
nosupersub\cf19\f20\fs18 Figure 8.\ul0\nosupersub\cf13\f14\fs18 Torsion angles
and sugar puckers of all seven lowest energy structures, listed by
residue. (P) is the \up0 \expndtw0\charscalex102 pseudo-rotation angle of the
sugars with the N-type and S-type pucker ranges indicated. D\ul0\nosupersub\cf8\f9\
fs11 3\ul0\nosupersub\cf13\f14\fs18 28 has three additional \up0 \expndtw0\
charscalex100 angles,\ul0\nosupersub\cf12\f13\fs18 u\ul0\nosupersub\cf8\f9\fs11 1\
ul0\nosupersub\cf13\f14\fs18 ,\ul0\nosupersub\cf12\f13\fs18 u\ul0\nosupersub\cf8\
f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 and\ul0\nosupersub\cf12\f13\fs18 u\ul0\
nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 , as defined in the legend
to Figure 1(a). \par\pard\sect\sectd\fs24\paperw12240\paperh15840{\shp
{\*\shpinst\shpleft0\shptop0\shpright12240\shpbottom15840\shpwr3\shpfblwtxt0\shpz-
10000\shplid9
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2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a280
0a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a2
8a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2
800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2800a28a2803ffd9}}}}}\pard\
sb0\sl-240{\bkmkstart Pg10}{\bkmkend Pg10}\par\pard\li956\sb0\sl-218\slmult0\par\
pard\li956\sb151\sl-218\slmult0\fi0\tx9955 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\
ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1061\par\pard\qj \li5856\sb0\sl-220\
slmult0 \par\pard\qj\li5856\ri1665\sb192\sl-220\slmult0\fi199 \up0 \expndtw0\
charscalex103 \ul0\nosupersub\cf7\f8\fs20 The sugar puckers of the DTA triplex are
more \up0 \expndtw-3\charscalex100 similar to those in\ul0\nosupersub\cf9\f10\fs20
B\ul0\nosupersub\cf7\f8\fs20 -DNA than in\ul0\nosupersub\cf9\f10\fs20 A\ul0\
nosupersub\cf7\f8\fs20 -DNA. With the \up0 \expndtw0\charscalex100 exception of
three residues in the third strand, the \up0 \expndtw-2\charscalex100 sugars in
the core of the DTA triplex prefer an \up0 \expndtw-2\charscalex100 S-type
pucker (Figure 8). \par\pard\ql \li5856\sb0\sl-230\slmult0 \par\pard\ql\li5856\
sb62\sl-230\slmult0 \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf24\f25\fs20
Comparison with other triplex structures \par\pard\qj \li5856\ri1623\sb140\sl-218\
slmult0\fi199 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\cf7\f8\fs20 Taken
together, the helix parameters indicate that \line \up0 \expndtw-4\charscalex100
the DTA triplex has a morphology more like\ul0\nosupersub\cf9\f10\fs20 B\ul0\
nosupersub\cf7\f8\fs20 -DNA \line \up0 \expndtw0\charscalex101 than\ul0\nosupersub\
cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -DNA. This is in contrast to
early fiber \line \up0 \expndtw0\charscalex100 diffraction studies on
poly(dT)�poly(dA)�poly(dT), \line \up0 \expndtw0\charscalex100 which concluded that
the helical morphology was \line \up0 \expndtw0\charscalex101 similar to that of\
ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -form DNA (Arnott &
Selsing, \line \up0 \expndtw-2\charscalex100 1974). More recently, fiber
diffraction studies on \line \up0 \expndtw-2\charscalex100 two different
sequences have suggested that the \line \up0 \expndtw-1\charscalex100
diffraction patterns are more characteristic of \line \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -form DNA
than\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -form DNA (Liu\ul0\
nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1994). In \line \up0 \
expndtw-3\charscalex100 addition, NMR-derived structures of intramolecular \line \
up0 \expndtw-3\charscalex100 pyrimidine�purine�pyrimidine triplexes containing \
line \up0 \expndtw0\charscalex100 a non-canonical G�T�A triplet at a single site
(GTA \line \up0 \expndtw-2\charscalex100 triplex) (Radhakrishnan & Patel, 1994b;
Wang\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., \line \up0 \
expndtw0\charscalex101 1992) and a non-canonical T�C�G triplet at a single \line \
up0 \expndtw-2\charscalex100 site (TCG triplex) (Radhakrishnan & Patel, 1994a) \
line \up0 \expndtw0\charscalex104 have been solved. A comparison of the
helix \line \up0 \expndtw-1\charscalex100 parameters is given in Table \up0 \
expndtw0\charscalex102 2. In general, the \par\pard\qj \li5856\ri1632\sb1\sl-
220\slmult0 \up0 \expndtw-3\charscalex100 triplexes have similar helix parameters.
The greatest \line \up0 \expndtw0\charscalex102 difference is found in the X-
displacement; the \line \up0 \expndtw0\charscalex106 Arnott fiber diffraction
structure has a large \line \up0 \expndtw-1\charscalex100 X-displacement, while
the DTA, GTA and TCG \line \up0 \expndtw0\charscalex101 triplexes all have
significantly smaller X-displace-\line \up0 \expndtw0\charscalex101 ments. As a
result, the Arnott fiber diffraction \line \up0 \expndtw0\charscalex102
structure has a significantly deeper major groove \line \up0 \expndtw-1\
charscalex100 than the solution structures. Similarly, the DTA \line \up0 \
expndtw0\charscalex101 triplex has the shallowest major groove because it \line \
up0 \expndtw0\charscalex103 has the smallest X-displacement of all the triplex \
line \up0 \expndtw-3\charscalex100 structures. An earlier NOE-derived model
structure \line \up0 \expndtw0\charscalex100 of a triplex, similar in sequence to
the DTA triplex \line
\up0 \expndtw-1\charscalex100 but containing only canonical T�A�T and C\ul0\
super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 �G�C \line
\up0 \expndtw0\charscalex100 triplets, also has a similar rise (3.1 A\u730?),
twist (32\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\nosupersub\cf7\f8\fs20 ) \line
\up0 \expndtw-2\charscalex100 and X-displacement (\ul0\nosupersub\cf25\f26\fs20 -\
ul0\nosupersub\cf7\f8\fs20 2.2 A\u730?) (Macaya\ul0\nosupersub\cf9\f10\fs20 et al\
ul0\nosupersub\cf7\f8\fs20 ., 1992b).\par\pard\sect\sectd\sbknone\cols2\colno1\
colw5696\colsr160\colno2\colw6244\colsr160\ql \li1135\sb72\sl-207\slmult0 \up0 \
expndtw-2\charscalex100 \ul0\nosupersub\cf19\f20\fs18 Figure \up0 \expndtw-1\
charscalex100 9.\ul0\nosupersub\cf13\f14\fs18 Helical parameters as a function of
base step\par\pard\ql \li956\sb1\sl-197\slmult0 \up0 \expndtw0\charscalex102 or
residue, averaged over the \up0 \expndtw0\charscalex101 seven lowest energy\
par\pard\qj \li956\ri149\sb1\sl-199\slmult0 \up0 \expndtw-3\charscalex100
structures. Error bars indicate the standard deviation. The \up0 \expndtw0\
charscalex100 average value for the DTA triplex along with the values \up0 \
expndtw0\charscalex100 for\ul0\nosupersub\cf14\f15\fs18 A\ul0\nosupersub\cf13\
f14\fs18 - and\ul0\nosupersub\cf14\f15\fs18 B\ul0\nosupersub\cf13\f14\fs18 -DNA
are indicated. (a) Axial rise. The \up0 \expndtw-4\charscalex100 average value
was calculated omitting the T4 �A17-A5 �T16 \up0 \expndtw0\charscalex101 base
step. \up0 \expndtw0\charscalex101 (b) Helical twist. The average value was\
par\pard\ql \li956\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100 calculated
omitting the A1 �T20-G2 �C19 \up0 \expndtw-1\charscalex100 and T4 �A17-\par\
pard\ql \li956\sb1\sl-199\slmult0 \up0 \expndtw-1\charscalex100 A5 �T16 base steps.
(c) X-displacement.\par\pard\qj \li956\sb0\sl-219\slmult0 \par\pard\qj \li956\sb0\
sl-219\slmult0 \par\pard\qj \li956\sb0\sl-219\slmult0 \par\pard\qj \li956\ri149\
sb104\sl-219\slmult0\fi0 \up0 \expndtw0\charscalex101 \ul0\nosupersub\cf7\f8\fs20
pairs from the global axis has an average value of \line \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf25\f26\fs20 -\ul0\nosupersub\cf7\f8\fs20 1.4 A\
u730? for the DTA triplex (Figure 9(c)), and is \line \up0 \expndtw0\
charscalex102 intermediate between\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\
cf7\f8\fs20 -DNA (\ul0\nosupersub\cf25\f26\fs20 -\ul0\nosupersub\cf7\f8\fs20 5.4)
and\ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -DNA \line \up0 \
expndtw0\charscalex101 (\ul0\nosupersub\cf25\f26\fs20 -\ul0\nosupersub\cf7\f8\fs20
0.7) but is more similar to\ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\
fs20 -DNA. The negative \line \up0 \expndtw0\charscalex102 X-displacement means
that the DTA triplex has a \line \up0 \expndtw0\charscalex101 deep major groove,
induced by the binding of the \line \up0 \expndtw-2\charscalex100 third strand to
the Watson-Crick purine strand, but \line \up0 \expndtw-1\charscalex100 not as deep
as in\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -DNA. The Y-
displacement (not \line \up0 \expndtw0\charscalex102 shown) is very small, which is
in agreement with \line \up0 \expndtw0\charscalex102 both\ul0\nosupersub\cf9\f10\
fs20 A\ul0\nosupersub\cf7\f8\fs20 - and\ul0\nosupersub\cf9\f10\fs20 B\ul0\
nosupersub\cf7\f8\fs20 -DNA.\par\pard\column \ql \li219\sb1\sl-221\slmult0 \up0 \
expndtw0\charscalex101 It is worth noting that the NMR-derived triplex\par\pard\
qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-2\charscalex100 structures were
refined by different methodologies. \line \up0 \expndtw-3\charscalex100 The GTA
and TCG structures were both refined \line \up0 \expndtw0\charscalex103 from\
ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 - and\ul0\nosupersub\cf9\
f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -DNA starting models. In contrast, \line \
up0 \expndtw-3\charscalex100 the DTA structure presented here was refined using \
line \up0 \expndtw0\charscalex100 distance geometry, which samples a larger area of
\line \up0 \expndtw-3\charscalex100 conformational space (and results in a larger
RMSD \line \up0 \expndtw0\charscalex100 between structures). Although these
structures all \line \up0 \expndtw0\charscalex103 have similar helical
parameters, they do have \line \up0 \expndtw0\charscalex101 significant
differences. It is unclear to what extent \line \up0 \expndtw0\charscalex100 the
refinement method contributes to these differ-\line \up0 \expndtw-2\charscalex100
ences.\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0\fi199 \up0 \expndtw0\
charscalex102 The sugars in triplexes were originally thought \line \up0 \expndtw-
1\charscalex100 to be C3'-\ul0\nosupersub\cf9\f10\fs20 endo\ul0\nosupersub\cf7\
f8\fs20 because Arnott\u8217?s fiber diffraction \line \up0 \expndtw0\
charscalex104 structure was very similar to\ul0\nosupersub\cf9\f10\fs20 A\
ul0\nosupersub\cf7\f8\fs20 -DNA \up0 \expndtw-4\charscalex100 (Arnott\par\pard\ql \
li20\sb0\sl-219\slmult0 \up0 \expndtw-1\charscalex100 & Selsing, \up0 \expndtw0\
charscalex100 1974). However, NMR studies of\par\pard\qj \li20\ri1643\sb0\
sl-219\slmult0 \up0 \expndtw-1\charscalex100 intramolecular triplexes have
shown that the \line \up0 \expndtw-1\charscalex100 sugars are predominantly
S-type (Macaya\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\
fs20 ., \line \up0 \expndtw0\charscalex100 1991, 1992a,b; Radhakrishnan & Patel,
1992). The \line \up0 \expndtw0\charscalex104 DTA triplex and the GTA and TCG
triplexes \line \up0 \expndtw-2\charscalex100 (Radhakrishnan & Patel, 1994a,b)
also have pre-\line \up0 \expndtw-3\charscalex100 dominantly S-type sugar
puckers. C2'-\ul0\nosupersub\cf9\f10\fs20 endo\ul0\nosupersub\cf7\f8\fs20
sugar \par\pard\sect\sectd\fs24\paperw12240\paperh15840{\shp
{\*\shpinst\shpleft0\shptop0\shpright12240\shpbottom15840\shpwr3\shpfblwtxt0\shpz-
10000\shplid10
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05145140051451400514514005145140051451400514514005145140051451400514514005145140051
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40051451400514514005145140051451400514514005145140051451400514514005145140051451400
51451400514514005145140051451400514514005145140051451400514514005145140051451400514
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05145140051451400514514005145140051451400514514005145140051451400514514005145140051
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51451400514514005145140051451400514514005145140051451400514514005145140051451400514
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fd9}}}}}\pard\sb0\sl-240{\bkmkstart Pg11}{\bkmkend Pg11}\par\pard\li956\sb0\sl-230\
slmult0\par\pard\li956\sb100\sl-230\slmult0\fi0\tx6448 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1062\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\
cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\par\pard\qj \
li7529\sb0\sl-197\slmult0 \par\pard\qj\li7529\sb0\sl-197\slmult0 \par\pard\qj\
li7529\ri1656\sb104\sl-197\slmult0\fi179 \up0 \expndtw-2\charscalex100 \ul0\
nosupersub\cf19\f20\fs18 Figure 10.\ul0\nosupersub\cf13\f14\fs18 Stacking of the
D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base \line \up0 \
expndtw-2\charscalex100 on the target T4 �A17 base-pair or \line \up0 \
expndtw-2\charscalex100 the neighboring T29 �A5 �T26 triplet, \line \up0 \expndtw0\
charscalex102 and comparison to the stacking on \line \up0 \expndtw0\charscalex101
alternate base-pairs or triplets. The \line \up0 \expndtw0\charscalex100 D\ul0\
nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base is blue and the other
bases \line \up0 \expndtw-2\charscalex100 are orange. Atoms that could poten-\
line \up0 \expndtw0\charscalex101 tially act as hydrogen bond donors \line \up0 \
expndtw-2\charscalex100 and acceptors are purple (nitrogen), \line \up0 \expndtw-3\
charscalex100 red (oxygen) and white (hydrogens). \par\pard\qj \li7529\ri1644\sb23\
sl-198\slmult0\fi0 \up0 \expndtw0\charscalex104 (a) Stacking of the D\ul0\
nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base on the \line \up0 \
expndtw-3\charscalex100 native T �A base-pair. (b) Same as (a) \line \up0 \expndtw-
1\charscalex100 except the native T �A base-pair has \line \up0 \expndtw-2\
charscalex100 been isosterically
replaced by a C �G \line \up0 \expndtw0\charscalex100 base-pair. (c) The native T
�A base-\line \up0 \expndtw0\charscalex105 pair has been replaced by an A �T \
line \up0 \expndtw0\charscalex101 base-pair. (d) The native T �A base-\line \up0 \
expndtw-1\charscalex100 pair has been replaced by a G �C \line \up0 \expndtw-
4\charscalex100 base-pair. (e) Stacking of the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\
nosupersub\cf13\f14\fs18 base \line \up0 \expndtw-3\charscalex100 on the
neighboring T �A �T triplet. (f) \line \up0 \expndtw-4\charscalex100 The
neighboring T �A �T triplet has \line \up0 \expndtw-1\charscalex100 been
isosterically replaced with a \line \up0 \expndtw-3\charscalex100 C\ul0\
nosupersub\cf8\f9\fs11 +\ul0\nosupersub\cf13\f14\fs18 �G �C triplet.\par\pard\
sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\colw6244\colsr160\ql \
li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb173\sl-230\slmult0 \up0 \expndtw0\
charscalex103 \ul0\nosupersub\cf7\f8\fs20 puckers are also claimed in the more
recent fiber\par\pard\ql \li956\sb1\sl-216\slmult0 \up0 \expndtw0\charscalex101
diffraction results (Liu\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\
fs20 ., 1994).\par\pard\qj \li956\ri149\sb1\sl-219\slmult0\fi199 \up0 \expndtw0\
charscalex102 In summary, the general morphology of the \up0 \expndtw0\
charscalex106 triplexes falls into a distinct family with the \up0 \expndtw-
2\charscalex100 following characteristics: \up0 \expndtw0\charscalex105 (1) an
axial rise very\par\pard\qj \li956\ri149\sb0\sl-219\slmult0\fi0 \up0 \expndtw-2\
charscalex100 similar to that in\ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\
f8\fs20 -DNA; (2) a low helical twist that \line \up0 \expndtw0\charscalex100 is
similar to that in\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 -DNA;
(3) an X-displacement \line \up0 \expndtw-1\charscalex100 that is intermediate
between that in\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 and\ul0\
nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -DNA, \line \up0 \expndtw0\
charscalex103 but generally closer to\ul0\nosupersub\cf9\f10\fs20 B\ul0\
nosupersub\cf7\f8\fs20 -DNA; and \up0 \expndtw0\charscalex106 (4) a\par\pard\qj
\li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex106 predominance of S-
type sugar puckers as in \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf9\f10\
fs20 B\ul0\nosupersub\cf7\f8\fs20 -DNA. These characteristics suggest that
triplexes \up0 \expndtw0\charscalex101 resemble\ul0\nosupersub\cf9\f10\fs20 B\ul0\
nosupersub\cf7\f8\fs20 -DNA more than\ul0\nosupersub\cf9\f10\fs20 A\ul0\
nosupersub\cf7\f8\fs20 -DNA.\par\pard\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \
li956\sb59\sl-230\slmult0 \up0 \expndtw-4\charscalex100 \ul0\nosupersub\cf24\f25\
fs20 D\ul0\sub\cf23\f24\fs18 3\ul0\nosupersub\cf24\f25\fs20 intercalation\par\
pard\qj \li956\ri149\sb139\sl-219\slmult0\fi199 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf7\f8\fs20 As previously reported, D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 intercalates on the 3' \up0 \expndtw-4\charscalex100
side \up0 \expndtw-1\charscalex100 (relative to the purine strand) of its
target\par\pard\qj \li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex101
base-pair rather than forming sequence-specific \line \up0 \expndtw-4\
charscalex100 hydrogen-bond interactions (Koshlap\ul0\nosupersub\cf9\f10\fs20
et al\ul0\nosupersub\cf7\f8\fs20 ., 1993). \line \up0 \expndtw0\charscalex101
Disruptions in the sequential connectivities in the\par\pard\ql \li2330\sb0\sl-207\
slmult0 \par\pard\ql \li2330\sb0\sl-207\slmult0 \par\pard\ql \li2330\sb5\sl-207\
slmult0 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf19\f20\fs18 Table 2.\ul0\
nosupersub\cf13\f14\fs18 Helix parameters\par\pard\column \ql \li5856\sb0\sl-230\
slmult0 \par\pard\ql \li20\sb173\sl-230\slmult0 \up0 \expndtw0\charscalex100 \ul0\
nosupersub\cf7\f8\fs20 imino region (Figure 2(a)) and the aromatic to H1'\par\pard\
ql \li20\sb1\sl-216\slmult0 \up0 \expndtw-3\charscalex100 region \up0 \expndtw-2\
charscalex100 (Figure \up0 \expndtw0\charscalex103 3) of NOESY spectra
indicated\par\pard\qj \li20\ri1643\sb1\sl-219\slmult0 \up0 \expndtw-2\charscalex100
intercalation (Koshlap\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\
fs20 ., 1993). The intercalation \line \up0 \expndtw0\charscalex100 explains the
strong sequence dependence on the 3' \line \up0 \expndtw-1\charscalex100
neighboring triplet and the relative insensitivity to \line \up0 \expndtw-2\
charscalex100 the \up0 \expndtw-1\charscalex100 5' neighboring triplet observed
by Kiessling\par\pard\ql \li20\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex103 \
ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., (1992).\par\pard\qj
\li20\ri1560\sb0\sl-219\slmult0\fi199 \up0 \expndtw-4\charscalex100 The D\ul0\sub\
cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base is readily accommodated into
the \line \up0 \expndtw-3\charscalex100 triplex, although the intercalation
perturbs the helix \line \up0 \expndtw-1\charscalex100 in several ways. In
comparison to our previous \line \up0 \expndtw-3\charscalex100 studies on a
similar triplex that does not contain the \line \up0 \expndtw-3\charscalex100 D\
ul0\nosupersub\cf16\f17\fs12 3\ul0\nosupersub\cf7\f8\fs20 base (Macaya\ul0\
nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1992b; Sklena�\
u345? & Feigon, \line \up0 \expndtw0\charscalex101 1990), the resonances for the
T25�A1�T20 and the \line \up0 \expndtw-4\charscalex100 C\ul0\nosupersub\cf16\f17\
fs12 +\ul0\nosupersub\cf7\f8\fs20 26�G2�C19 triplets and the TATA loop
residues \line \up0 \expndtw0\charscalex102 are much broader, even to the
point of being \line \up0 \expndtw-2\charscalex100 unobservable, indicating that
intercalation of the D\ul0\sub\cf16\f17\fs18 3 \line \up0 \expndtw0\charscalex101 \
ul0\nosupersub\cf7\f8\fs20 base destabilizes the 5' end of the triplex. Another \
line \up0 \expndtw0\charscalex100 effect of D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 intercalation is an increase in the axial \line \up0 \
expndtw0\charscalex102 rise with a concomitant unwinding of the helix at \line \up0
\expndtw0\charscalex102 the intercalation site (Figure 9(b)). In fact, the low \
par\pard\sect\sectd\sbknone \li2330\sb79\sl-184\slmult0\fi0\tx3709\tx4656\tx5656\
tx7351 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\fs16 Structure\ul0\
super\cf28\f29\fs14 a\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\
fs16 Rise (A\u730?)\tab \up0 \expndtw-1\charscalex100 Twist (\ul0\nosupersub\cf29\
f30\fs16 \u-3920?\ul0\nosupersub\cf11\f12\fs16 )\tab \up0 \expndtw-1\charscalex100
X-disp (A\u730?)\tab \up0 \expndtw-1\charscalex100 Sugar pucker\par\pard\sect\
sectd\sbknone \li2330\sb85\sl-184\slmult0\fi0\tx3913\tx4898\tx5892\tx7223 \up0 \
expndtw-1\charscalex100 DTA\tab \up0 \expndtw-1\charscalex100 3.2\ul0\super\cf28\
f29\fs14 b\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\fs16 31\ul0\
super\cf28\f29\fs14 c\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf29\f30\
fs16 -\ul0\nosupersub\cf11\f12\fs16 1.4\tab \up0 \expndtw-1\charscalex100 Generally
S-type\par\pard\sect\sectd\sbknone \li2330\sb0\sl-179\slmult0\fi0\tx3904\tx4880\
tx5892\tx7223 \up0 \expndtw-1\charscalex100 GTA\tab \up0 \expndtw-1\charscalex100
3.4\tab \up0 \expndtw-1\charscalex100 31\tab \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf29\f30\fs16 -\ul0\nosupersub\cf11\f12\fs16 1.9\tab \up0 \expndtw-1\
charscalex100 Generally S-type\par\pard\sect\sectd\sbknone \li2330\sb0\sl-179\
slmult0\fi0\tx3904\tx4880\tx5892\tx7223 \up0 \expndtw-1\charscalex100 TCG\tab \
up0 \expndtw-1\charscalex100 3.4\tab \up0 \expndtw-1\charscalex100 32\tab \up0 \
expndtw-1\charscalex100 \ul0\nosupersub\cf29\f30\fs16 -\ul0\nosupersub\cf11\f12\
fs16 2.1\tab \up0 \expndtw-1\charscalex100 Generally S-type\par\pard\sect\sectd\
sbknone \li2330\sb1\sl-180\slmult0\fi0\tx3904\tx4880\tx5828\tx7613 \up0 \expndtw-1\
charscalex100 Liu (TAT)\tab \up0 \expndtw-1\charscalex100 3.3\tab \up0 \expndtw-1\
charscalex100 28\tab \up0 \expndtw-1\charscalex100 N/A\ul0\super\cf28\f29\fs14 d\
tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\fs16 S-type\ul0\super\
cf28\f29\fs14 e\par\pard\sect\sectd\sbknone \li2330\sb0\sl-179\slmult0\fi0\tx3904\
tx4880\tx5828\tx7613 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\fs16
Liu (hetero)\tab \up0 \expndtw-1\charscalex100 3.2\tab \up0 \expndtw-1\
charscalex100 30\tab \up0 \expndtw-1\charscalex100 N/A\ul0\super\cf28\f29\fs14 d\
tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\fs16 S-type\ul0\super\
cf28\f29\fs14 e\par\pard\sect\sectd\sbknone \li2330\sb0\sl-179\slmult0\fi0\tx3904\
tx4880\tx5892\tx7211 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf11\f12\fs16
Arnott\tab \up0 \expndtw-1\charscalex100 3.3\tab \up0 \expndtw-1\charscalex100 30\
tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf29\f30\fs16 -\ul0\nosupersub\
cf11\f12\fs16 3.6\tab \up0 \expndtw-1\charscalex100 Assumed N-type\par\pard\sect\
sectd\sbknone \li2330\sb0\sl-179\slmult0\fi0\tx3904\tx4880\tx5892\tx7598 \up0 \
expndtw-1\charscalex100 \ul0\nosupersub\cf30\f31\fs16 B\ul0\nosupersub\cf11\f12\
fs16 -DNA\tab \up0 \expndtw-1\charscalex100 3.4\tab \up0 \expndtw-1\charscalex100
36\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf29\f30\fs16 -\ul0\
nosupersub\cf11\f12\fs16 0.7\tab \up0 \expndtw-1\charscalex100 S-type\par\pard\
sect\sectd\sbknone \li2330\sb1\sl-180\slmult0\fi0\tx3904\tx4880\tx5892\tx7574 \
up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf30\f31\fs16 A\ul0\nosupersub\cf11\
f12\fs16 -DNA\tab \up0 \expndtw-1\charscalex100 2.6\tab \up0 \expndtw-1\
charscalex100 33\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf29\f30\fs16 -\
ul0\nosupersub\cf11\f12\fs16 5.4\tab \up0 \expndtw-1\charscalex100 N-type\par\pard\
qj \li2330\ri3029\sb94\sl-175\slmult0\fi159
\up0 \expndtw-2\charscalex100 \ul0\super\cf28\f29\fs14 a\ul0\nosupersub\cf11\f12\
fs16 DTA refers to the DTA triplex structure. GTA and TCG refer to the two NMR-
derived triplex \up0 \expndtw0\charscalex100 structures containing a non-canonical
triplet (Radhakrishnan & Patel, 1994a,b). Liu (TAT) and \up0 \expndtw0\
charscalex100 Liu (hetero) refer to the two DNA sequences used in fiber diffraction
studies (Liu\ul0\nosupersub\cf30\f31\fs16 et al\ul0\nosupersub\cf11\f12\fs16 .,
1994). \up0 \expndtw0\charscalex100 Arnott refers to the original fiber diffraction
structure (Arnott & Selsing, 1974).\ul0\nosupersub\cf30\f31\fs16 B\ul0\
nosupersub\cf11\f12\fs16 -DNA and \up0 \expndtw0\charscalex100 \ul0\nosupersub\
cf30\f31\fs16 A\ul0\nosupersub\cf11\f12\fs16 -DNA refer to the standard DNA duplex
conformations (Saenger, 1984). \par\pard\ql \li2490\sb3\sl-178\slmult0 \up0 \
expndtw0\charscalex103 \ul0\super\cf28\f29\fs14 b\ul0\nosupersub\cf11\f12\fs16 The
axial rise for the DTA triplex is calculated omitting the T4 A17-G2 T16 base
step. \par\pard\qj \li2330\ri3029\sb1\sl-180\slmult0\fi159 \up0 \expndtw-2\
charscalex100 \ul0\super\cf28\f29\fs14 c\ul0\nosupersub\cf11\f12\fs16 The helical
twist for the DTA triplex is calculated omitting the A1 T20-G2 C19 and T4 A17-A5 \
up0 \expndtw-3\charscalex100 T16 base steps. \par\pard\ql \li2490\sb1\sl-179\
slmult0 \up0 \expndtw0\charscalex102 \ul0\super\cf28\f29\fs14 d\ul0\nosupersub\
cf11\f12\fs16 N/A, not available. \par\pard\ql \li2490\sb1\sl-179\slmult0 \up0 \
expndtw-1\charscalex100 \ul0\super\cf28\f29\fs14 e\ul0\nosupersub\cf11\f12\fs16
The sugar conformation is claimed by the authors, but no evidence is given (Liu\
ul0\nosupersub\cf30\f31\fs16 et al\ul0\nosupersub\cf11\f12\fs16 ., 1994). \par\
pard\sect\sectd\fs24\paperw12240\paperh15840\pard\sb0\sl-240{\bkmkstart Pg12}{\
bkmkend Pg12}\par\pard\li956\sb0\sl-218\slmult0\par\pard\li956\sb151\sl-218\
slmult0\fi0\tx9955 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf1\f2\fs18
Solution Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18
-containing DNA Triplex\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf22\f23\
fs20 1063\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\
colw6244\colsr160\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb191\sl-230\
slmult0 \up0 \expndtw0\charscalex101 \ul0\nosupersub\cf7\f8\fs20 twist observed at
the A3-T4 step is even smaller if\par\pard\qj \li956\ri149\sb0\sl-219\slmult0\fi0 \
up0 \expndtw-4\charscalex100 one considers that the D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 base acts like another base, \up0 \expndtw0\charscalex105
so that the A3-T4 \up0 \expndtw0\charscalex106 base step is really a dual\
par\pard\qj \li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex102 A3-D\ul0\
sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28-T4 base step. Similar effects
are seen in \up0 \expndtw0\charscalex100 intercalating drug-DNA complexes (Addess\
ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., \up0 \expndtw0\
charscalex103 1992; Gao & Patel, 1988; Gilbert\ul0\nosupersub\cf9\f10\fs20 et al\
ul0\nosupersub\cf7\f8\fs20 ., 1989).\par\pard\qj \li956\ri149\sb0\sl-219\slmult0\
fi199 \up0 \expndtw0\charscalex100 Other effects of D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 intercalation are manifested \line \up0 \expndtw0\
charscalex101 in unusual torsion angles and sugar puckers (Fig-\line \up0 \expndtw-
3\charscalex100 ure 8). Backbone restraints were only applied to \line \
up0 \expndtw0\charscalex103 some of the\ul0\nosupersub\cf10\f11\fs20 d\ul0\
nosupersub\cf7\f8\fs20 angles and loosely applied to the\ul0\nosupersub\cf10\f11\
fs20 e \line \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf7\f8\fs20 angles. As a
result, most backbone angles are only \line \up0 \expndtw0\charscalex102 indirectly
determined and the precision of the \line \up0 \expndtw-2\charscalex100
backbone angles varies from well defined to almost \line \up0 \expndtw0\
charscalex100 random (Figure 8). Nevertheless, most angles are \line \up0 \
expndtw0\charscalex101 predominantly within normal ranges \up0 \expndtw-3\
charscalex100 (Saenger,\par\pard\qj \li956\ri149\sb0\sl-219\slmult0\fi0 \up0 \
expndtw0\charscalex102 1984). In several of the structures, the T27\ul0\nosupersub\
cf10\f11\fs20 b\ul0\nosupersub\cf7\f8\fs20 angle \line \up0 \expndtw0\
charscalex104 is in the +\ul0\nosupersub\cf9\f10\fs20 gauche\ul0\nosupersub\cf7\
f8\fs20 range instead of the usual\ul0\nosupersub\cf9\f10\fs20 trans \line \up0 \
expndtw-2\charscalex100 \ul0\nosupersub\cf7\f8\fs20 conformation. The +\ul0\
nosupersub\cf9\f10\fs20 gauche\ul0\nosupersub\cf7\f8\fs20 conformation places
T27 \line \up0 \expndtw-3\charscalex100 in a more lateral position (with respect to
the global \line \up0 \expndtw-2\charscalex100 helical axis) from C\ul0\super\cf16\
f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 26. Also, the T27\
ul0\nosupersub\cf10\f11\fs20 x\ul0\nosupersub\cf7\f8\fs20 angle is very \line \
up0 \expndtw-3\charscalex100 close to the high-anti conformation, which
effec-\line \up0 \expndtw-2\charscalex100 tively rotates the T27 sugar and
phosphate closer to \line \up0 \expndtw0\charscalex103 C\ul0\nosupersub\cf16\f17\
fs12 +\ul0\nosupersub\cf7\f8\fs20 26. The sugar pucker of T27 is also unusual in \
line \up0 \expndtw0\charscalex101 that it adopts an N-type conformation while
most \line \up0 \expndtw-2\charscalex100 other residues are S-type. This N-type
sugar pucker \line \up0 \expndtw0\charscalex102 creates a large T27H6 \up0 \
expndtw0\charscalex103 to T27H3' crosspeak in\par\pard\qj \li956\ri149\sb1\sl-
219\slmult0\fi0 \up0 \expndtw0\charscalex100 the NOESY spectrum (Figure 3,
peak v) and a \line \up0 \expndtw0\charscalex104 \u8216?\u8216?reversed\u8217?\
u8217? coupling pattern in the T27H1' to \line \up0 \expndtw-1\charscalex100
T27H2',2" crosspeaks in the P.COSY spectrum (not \line \up0 \expndtw-3\
charscalex100 shown). These structural changes are a consequence \line \up0 \
expndtw-3\charscalex100 of the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20
28 base skipping over the T4�A17 base-pair \line \up0 \expndtw-2\charscalex100 to
intercalate, thereby pulling T27 out of plane with \line \up0 \expndtw-2\
charscalex100 A3 and T18. The N-type sugar conformation of T27 \line \up0 \expndtw-
1\charscalex100 also results in a decrease in the twist of D\ul0\sub\cf16\
f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28, \line \up0 \expndtw0\charscalex103
positioning the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 base so
that it more closely \line \up0 \expndtw0\charscalex100 mimics a triplet.\par\pard\
qj \li956\ri149\sb0\sl-219\slmult0\fi199 \up0 \expndtw-1\charscalex100 The\ul0\
nosupersub\cf10\f11\fs20 x\ul0\nosupersub\cf7\f8\fs20 angles of A5 and A17, which
are both 3' to \up0 \expndtw0\charscalex100 the intercalation site relative to
their respective \up0 \expndtw-1\charscalex100 strands, adopt a high-anti
conformation. This \up0 \expndtw0\charscalex100 enables the backbone to stretch
further than usual, \up0 \expndtw-2\charscalex100 allowing a greater axial rise at
the intercalation site. \up0 \expndtw-2\charscalex100 The base in the
equivalent position in the third \up0 \expndtw-3\charscalex100 strand is D\
ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28, which does not have a
high-\ul0\nosupersub\cf9\f10\fs20 anti \up0 \expndtw0\charscalex102 \ul0\
nosupersub\cf7\f8\fs20 conformation, but instead pulls on and induces a \up0 \
expndtw-1\charscalex100 high-anti conformation in T27.\par\pard\qj \li956\ri149\
sb0\sl-219\slmult0\fi199 \up0 \expndtw-3\charscalex100 In the refined structures,
the C19 and C\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\
f8\fs20 26 sugars \line \up0 \expndtw-1\charscalex100 have predominantly N-type
puckers. However, no \line \up0 \expndtw0\charscalex100 dihedral angle restraints
were applied to these \line \up0 \expndtw-1\charscalex100 sugars and there is
no direct NMR evidence to \line \up0 \expndtw-3\charscalex100 support this
result. The P.COSY H1'-H2',2" coupling \line \up0 \expndtw-1\charscalex100 patterns
could not be used to confirm these results \line \up0 \expndtw-1\charscalex100
because they are poorly resolved (data not shown). \line \up0 \expndtw-1\
charscalex100 In the aromatic H3' region of the NOESY spectrum \line \up0 \expndtw-
2\charscalex100 (Figure \up0 \expndtw0\charscalex100 3), both the C19 \up0 \
expndtw-1\charscalex100 and C\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\
ul0\nosupersub\cf7\f8\fs20 26 intra-residue\par\pard\qj \li956\ri149\sb0\sl-219\
slmult0 \up0 \expndtw0\charscalex102 crosspeaks are weak, indicating that these
sugars \up0 \expndtw0\charscalex101 are not N-type. However, both residues
generally \up0 \expndtw-3\charscalex100 have weaker crosspeaks than other
residues and \up0 \expndtw-1\charscalex100 C\ul0\super\cf16\f17\fs18\ul0\super\
cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 26 has especially broad crosspeaks and
no imino \up0 \expndtw0\charscalex100 NOE crosspeaks (Figure 2(a)), indicating
that the \up0 \expndtw-1\charscalex100 C\ul0\nosupersub\cf16\f17\fs12 +\ul0\
nosupersub\cf7\f8\fs20 26�G2�C19 \up0 \expndtw0\charscalex100 triplet is in
intermediate exchange\par\pard\qj \li956\ri149\sb1\sl-219\slmult0 \up0 \expndtw-2\
charscalex100 with an alternate (probably non-hydrogen bonded) \line \up0 \
expndtw0\charscalex103 state. A protonated cytosine in the same position \line \up0
\expndtw0\charscalex101 has been previously found to prefer N-type sugar\par\pard\
column \ql \li5856\sb0\sl-230\slmult0 \par\pard\ql \li20\sb191\sl-230\slmult0 \
up0 \expndtw-2\charscalex100 puckers (Macaya\ul0\nosupersub\cf9\f10\fs20 et al\
ul0\nosupersub\cf7\f8\fs20 ., 1992a). It is unclear
whether\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-3\charscalex100
the N-type sugar puckers are a result of the D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 base \up0 \expndtw0\charscalex100 intercalation or a
sequence effect.\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0\fi199 \up0 \expndtw-3\
charscalex100 There are other unusual torsion angles in the loop \up0 \expndtw0\
charscalex100 residues and the terminal triplets, but they are \up0 \
expndtw0\charscalex101 probably not due to D\ul0\sub\cf16\f17\fs18 3 \up0 \
expndtw-1\charscalex100 \ul0\nosupersub\cf7\f8\fs20 intercalation. The loop\par\
pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-1\charscalex100 residues do
not necessarily conform to standard\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\
cf7\f8\fs20 -\line \up0 \expndtw-1\charscalex100 or\ul0\nosupersub\cf9\f10\fs20 B\
ul0\nosupersub\cf7\f8\fs20 -DNA-like angles, and the terminal triplets are \up0 \
expndtw-1\charscalex100 only partially assigned (Table 1), have many fewer \up0 \
expndtw-1\charscalex100 restraints (Figure 5), and are strongly perturbed by \up0 \
expndtw0\charscalex100 the conformation of the loops.\par\pard\ql \li5856\sb0\sl-
230\slmult0 \par\pard\ql \li20\sb60\sl-230\slmult0 \up0 \expndtw-3\charscalex100 \
ul0\nosupersub\cf24\f25\fs20 D\ul0\sub\cf23\f24\fs18 3\ul0\nosupersub\cf24\f25\fs20
base conformation\par\pard\qj \li20\ri1643\sb138\sl-219\slmult0\fi199 \up0 \
expndtw0\charscalex100 \ul0\nosupersub\cf7\f8\fs20 The conformation of the D\ul0\
sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base is important in \line \up0 \
expndtw0\charscalex100 determining the interactions between the D\ul0\sub\cf16\f17\
fs18 3\ul0\nosupersub\cf7\f8\fs20 base \line \up0 \expndtw-3\charscalex100 and
its neighboring bases. Figure 6(c) shows the \line \up0 \expndtw-2\
charscalex100 superposition of the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\
fs20 base from the seven lowest \line \up0 \expndtw-1\charscalex100 energy
structures. The orientation of rings A and B \line \up0 \expndtw-1\charscalex100
are well defined by their numerous NOE inter-\line \up0 \expndtw0\
charscalex103 actions with the T4, A5, T16, A17 and T29 sugars \line \up0 \
expndtw0\charscalex100 and with each other (Figures 3 and 4). The\ul0\nosupersub\
cf10\f11\fs20 x\ul0\nosupersub\cf7\f8\fs20 angle \line \up0 \expndtw0\
charscalex101 adopts an\ul0\nosupersub\cf9\f10\fs20 anti\ul0\nosupersub\cf7\f8\
fs20 conformation \up0 \expndtw-2\charscalex100 (Figure \up0 \expndtw0\
charscalex104 8; where\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-
2\charscalex100 the N1A, C2A and H2A atoms are analogous to the \up0 \expndtw0\
charscalex104 N9, C8 and H8 atoms in a purine) that fixes the \up0 \expndtw-1\
charscalex100 orientation of the A ring parallel to its neighboring \up0 \expndtw0\
charscalex101 bases and points the B ring into the major groove. \up0 \expndtw0\
charscalex100 In this configuration, the position of rings A and B \up0 \expndtw-3\
charscalex100 are similar to those of a third strand pyrimidine and \up0 \expndtw0\
charscalex102 its Hoogsteen base-paired residue in the Watson-\line \up0 \expndtw-
1\charscalex100 Crick purine strand, respectively.\par\pard\qj \li20\ri1643\sb0\sl-
219\slmult0\fi199 \up0 \expndtw-4\charscalex100 The\ul0\nosupersub\cf10\f11\fs20
u\ul0\sub\cf16\f17\fs18 1\ul0\nosupersub\cf7\f8\fs20 torsion angle (Figure 1(a)),
which connects \up0 \expndtw-2\charscalex100 rings A and B, determines the
rotational position of \up0 \expndtw0\charscalex106 the B ring and, thus, the
position of the peptide \up0 \expndtw-1\charscalex100 group and the C ring. In all
seven structures, the\ul0\nosupersub\cf10\f11\fs20 u\ul0\sub\cf16\f17\fs18 1 \
up0 \expndtw0\charscalex103 \ul0\nosupersub\cf7\f8\fs20 torsion angle positions the
B ring to be co-planar \up0 \expndtw0\charscalex101 with the A ring and points the
peptide group and \up0 \expndtw-3\charscalex100 C ring towards the Watson-Crick
pyrimidine strand \up0 \expndtw-2\charscalex100 (Figures \up0 \expndtw0\
charscalex100 6(c) and \up0 \expndtw0\charscalex101 8). Neither the rings nor
the\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-2\charscalex100
peptide group were restrained to be co-planar. This \up0 \expndtw-1\charscalex100
configuration places rings B and C in a similar \up0 \expndtw0\
charscalex100 position to a Watson-Crick base-pair.\par\pard\ql \li20\ri1643\sb0\
sl-219\slmult0\fi199\tx229 \up0 \expndtw-1\charscalex100 The\ul0\nosupersub\cf10\
f11\fs20 u\ul0\sub\cf16\f17\fs18 2\ul0\nosupersub\cf7\f8\fs20 torsion angle
adopts several orientations \line \up0 \expndtw-1\charscalex100 (Figures 6(c) and
8) but predominantly favors the \line \up0 \expndtw-2\charscalex100 orientation
with the carbonyl group pointing out of \line \up0 \expndtw0\charscalex100 the
major groove. The\ul0\nosupersub\cf10\f11\fs20 u\ul0\sub\cf16\f17\fs18 2\ul0\
nosupersub\cf7\f8\fs20 torsion angle affects the \line \up0 \expndtw0\
charscalex103 position of the C ring, but only by\ul0\nosupersub\cf10\f11\fs20 0\
ul0\nosupersub\cf7\f8\fs20 2 A\u730? at most. \line \up0 \expndtw0\charscalex103 In
theory, the conformation of the peptide group \line \up0 \expndtw-3\charscalex100
could be determined by NOE interactions involving \line \up0 \expndtw-2\
charscalex100 the amide proton, but the amide resonance was not \line \up0 \
expndtw0\charscalex100 observed due to rapid chemical exchange with \line \
up0 \expndtw0\charscalex101 water. This also suggests that the amide proton is \
line \up0 \expndtw0\charscalex106 not involved in a hydrogen bond. Thus, the
\line \up0 \expndtw0\charscalex101 orientation of the peptide group is only
indirectly \line \up0 \expndtw0\charscalex102 determined by restraints to rings B
and C. \line\tab \up0 \expndtw-4\charscalex100 The\ul0\nosupersub\cf10\f11\fs20 u\
ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 torsion angle is the most
variable and least \line \up0 \expndtw-3\charscalex100 well defined in the D\ul0\
sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base (Figure 8). The chemical \
line \up0 \expndtw-3\charscalex100 shift degeneracy of the C ring protons indicates
that \line \up0 \expndtw-4\charscalex100 the chemical shifts are motionally
averaged and that \line \up0 \expndtw0\charscalex103 the C ring is rotating fast on
the NMR time scale. \line \up0 \expndtw-4\charscalex100 Interestingly, significant
conformational variation of \line \up0 \expndtw-1\charscalex100 the C ring is also
observed in the refined structures \line \up0 \expndtw-2\charscalex100 (Figures \
up0 \expndtw0\charscalex101 6(c) and \up0 \expndtw0\charscalex101 8). However,
since the NOE

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}}\par\pard\sect\sectd\fs24\paperw12240\paperh15840\pard\sb0\sl-240{\bkmkstart
Pg13}{\bkmkend Pg13}\par\pard\li956\sb0\sl-230\slmult0\par\pard\li956\sb100\sl-230\
slmult0\fi0\tx6448 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf22\f23\fs20
1064\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution
Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -
containing DNA Triplex\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\
colno2\colw6244\colsr160\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb217\sl-
230\slmult0 \up0 \expndtw0\charscalex102 \ul0\nosupersub\cf7\f8\fs20 restraints
used during the refinement are also\par\pard\qj \li956\ri149\sb0\sl-219\
slmult0 \up0 \expndtw0\charscalex101 degenerate, it is unclear whether the
variability of \up0 \expndtw0\charscalex100 the C ring seen in the calculated
structures reflects \up0 \expndtw0\charscalex101 actual rotation of the C ring or
if it simply reflects \up0 \expndtw-2\charscalex100 the degeneracy of the
restraints. The large standard \up0 \expndtw0\charscalex104 deviation in the axial
rise at the T4-A5 base step \up0 \expndtw-2\charscalex100 (Figure 9(a)) is a
direct consequence of the con-\line \up0 \expndtw-3\charscalex100 formational
variability of the C ring. Even if the \up0 \expndtw0\charscalex101 rise is
halved (to account for the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20
base), the rise \up0 \expndtw-2\charscalex100 is still large \up0 \expndtw-2\
charscalex100 (\ul0\nosupersub\cf10\f11\fs20 0\ul0\nosupersub\cf7\f8\fs20 4.3 A\
u730?) due to those structures in\par\pard\qj \li956\ri149\sb1\sl-219\
slmult0 \up0 \expndtw0\charscalex100 which the C ring is in a perpendicular
(unstacked) \up0 \expndtw-4\charscalex100 conformation.\par\pard\ql \li956\sb0\sl-
230\slmult0 \par\pard\ql \li956\sb60\sl-230\slmult0 \up0 \expndtw-1\charscalex100 \
ul0\nosupersub\cf24\f25\fs20 Stacking of the D\ul0\sub\cf23\f24\fs18 3\ul0\
nosupersub\cf24\f25\fs20 base\par\pard\ql \li956\ri149\sb138\sl-219\slmult0\
fi199\tx1155 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\cf7\f8\fs20 As
previously reported, the stacking of the D\ul0\sub\cf16\f17\fs18 3 \line \up0
\expndtw0\charscalex103 \ul0\nosupersub\cf7\f8\fs20 base causes upfield ring
current shifts of\ul0\nosupersub\cf10\f11\fs20 0\ul0\nosupersub\cf7\f8\fs20 1
ppm \line \up0 \expndtw0\charscalex100 for the T4H6 and T4Me relative to other TH6-
TMe \line \up0 \expndtw-2\charscalex100 crosspeaks (Figure 4 and Table 1)
(Koshlap\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., \line \
up0 \expndtw-1\charscalex100 1993). This effect can be rationalized by examining \
line \up0 \expndtw0\charscalex102 Figure 10(a), where the stacking of the D\ul0\
sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base in \line \up0 \expndtw-2\
charscalex100 relationship to the neighboring T4�A17 base-pair \line \up0 \
expndtw0\charscalex101 and T29�A5�T16 triplet is shown. The B ring (and \line \
up0 \expndtw0\charscalex100 partially the A ring) stacks directly over the T4Me \
line \up0 \expndtw0\charscalex101 and T4H6, which induces an upfield shift. \line\
tab \up0 \expndtw-2\charscalex100 The most prominent feature of the stacking is the
\line \up0 \expndtw-3\charscalex100 relative disorder of the D\ul0\sub\cf16\f17\
fs18 3\ul0\nosupersub\cf7\f8\fs20 base position. Compared \line \up0 \expndtw-4\
charscalex100 to the neighboring base-pair and triplet, the position \line \up0 \
expndtw0\charscalex104 of the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20
base is less well defined. In fact, the D\ul0\sub\cf16\f17\fs18 3 \line \up0 \
expndtw-4\charscalex100 \ul0\nosupersub\cf7\f8\fs20 base has the largest RMSD of
any residue in the core \line \up0 \expndtw-4\charscalex100 of the triplex and is
also the only residue (other than \line \up0 \expndtw0\charscalex100 the loops)
that has a greater RMSD of its base than \line \up0 \expndtw-1\charscalex100 its
backbone (Figure 7). The major contribution to \line \up0 \expndtw0\charscalex102
the RMSD comes from the peptide group and the \line \up0 \expndtw-2\charscalex100 C
ring, as already discussed. The D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\
fs20 base generally \line \up0 \expndtw0\charscalex100 has some overlap with the
T29�A5�T16 triplet and \line \up0 \expndtw0\charscalex104 substantial overlap
with the T4�A17 \up0 \expndtw-2\charscalex100 base-pair\par\pard\qj \li956\ri149\
sb0\sl-219\slmult0\fi0 \up0 \expndtw0\charscalex102 (Figure 10(a) and (e)). This
may explain why the \up0 \expndtw-1\charscalex100 stability of D\ul0\sub\cf16\
f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 -containing triplexes is strongly \
up0 \expndtw0\charscalex100 affected by the sequence of the adjacent base-pair, \
up0 \expndtw-2\charscalex100 but are less affected by the sequence of the
adjacent \up0 \expndtw0\charscalex101 triplet (Kiessling\ul0\nosupersub\cf9\f10\
fs20 et al\ul0\nosupersub\cf7\f8\fs20 ., 1992).\par\pard\qj \li956\ri149\sb0\sl-
219\slmult0\fi199 \up0 \expndtw-2\charscalex100 An interesting result is that the
D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base mimics a \line \up0 \
expndtw0\charscalex105 triplet with each ring assuming the position of a \line \up0
\expndtw-2\charscalex100 base in each strand (Figure 6(b)). From the 3' end of \
line \up0 \expndtw0\charscalex101 the triplex (with respect to the purine strand),
the \line \up0 \expndtw-3\charscalex100 first four triplets form a regular
stacking pattern \line \up0 \expndtw-3\charscalex100 with the D\ul0\sub\cf16\
f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base mimicking a fifth triplet.
Then \line \up0 \expndtw0\charscalex102 there is large unwinding of the helix
between the \line \up0 \expndtw-2\charscalex100 D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 base and the adjacent T4�A17 base-pair (Fig-\line \
up0 \expndtw0\charscalex103 ure 9(b)), so the mimicry is not perfect. After the \
line \up0 \expndtw-2\charscalex100 T4�A17 base-pair, the helix continues with a
regular \line \up0 \expndtw0\charscalex101 twist again (excluding the A1-G2 step,
which is ill \line \up0 \expndtw-2\charscalex100 defined). As discussed above, the
unwinding at the \line \up0 \expndtw0\charscalex100 T4-A5 step is more severe
than is indicated in \line \up0 \expndtw-3\charscalex100 Figure 9(b), since
the step is really two steps of \line \up0 \expndtw-3\charscalex100 T4-D\ul0\
sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 and D\ul0\sub\cf16\f17\fs18 3\
ul0\nosupersub\cf7\f8\fs20 28-A5. In fact, rings B and C (which \line \up0 \
expndtw-2\charscalex100 mimic a Watson-Crick base-pair) have almost 0\ul0\
nosupersub\cf25\f26\fs20 \u-3920? \line \up0 \expndtw0\charscalex101 \ul0\
nosupersub\cf7\f8\fs20 twist relative to the T4�A17 \up0 \expndtw0\
charscalex100 base-pair. The un-\par\pard\ql \li956\ri149\sb0\sl-219\slmult0\fi0\
tx1155 \up0 \expndtw0\charscalex102 winding is expected because the helical rise
must \line \up0 \expndtw-1\charscalex100 increase to accommodate the D\ul0\sub\
cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 intercalation. \line\tab \up0 \
expndtw-2\charscalex100 The D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20
base superimposes on a triplet best when \line \up0 \expndtw-1\charscalex100 the
angles\ul0\nosupersub\cf10\f11\fs20 u\ul0\sub\cf16\f17\fs18 1\ul0\nosupersub\cf7\
f8\fs20 and\ul0\nosupersub\cf10\f11\fs20 u\ul0\sub\cf16\f17\fs18 2\ul0\
nosupersub\cf7\f8\fs20 are both in the conformation\par\pard\column \ql \li5856\
sb0\sl-230\slmult0 \par\pard\ql \li20\sb217\sl-230\slmult0 \up0 \expndtw0\
charscalex102 shown in Figure 1(a), which is also the major\par\pard\qj \
li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-3\charscalex100 conformation of the
seven lowest energy structures. \up0 \expndtw0\charscalex100 In such a
superposition, the glycosidic bond of the \up0 \expndtw-3\charscalex100 D\ul0\sub\
cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base is rotated away from the
purine strand \up0 \expndtw0\charscalex102 relative to a canonical triplet. This
is precisely the \up0 \expndtw0\charscalex103 effect that the N-type sugar pucker
of T27 has on \up0 \expndtw0\charscalex104 D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 28, as discussed above. These observations \up0 \
expndtw-2\charscalex100 suggest that it may be possible to design a base that \
up0 \expndtw0\charscalex100 confers greater stability to the triplex by designing \
up0 \expndtw0\charscalex101 it to mimic a triplet more closely.\par\pard\ql \
li5856\sb0\sl-230\slmult0 \par\pard\ql \li20\sb60\sl-230\slmult0 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf24\f25\fs20 Sequence specificity\par\pard\ql \
li219\sb129\sl-230\slmult0 \up0 \expndtw0\charscalex107 \ul0\nosupersub\cf7\f8\fs20
The sequence specificity of D\ul0\sub\cf16\f17\fs18 3 \up0 \expndtw-4\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 intercalation\par\pard\qj \li20\ri1643\
sb0\sl-219\slmult0\fi0 \up0 \expndtw0\charscalex101 appears to be derived
primarily from stacking \line \up0 \expndtw-1\charscalex100 interactions between
the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base and its neighbor-\
line \up0 \expndtw-1\charscalex100 ing bases. Although stacking
interactions are \line \up0 \expndtw-4\charscalex100 difficult to determine, the
D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base does have slightly \
line \up0 \expndtw0\charscalex101 more overlap with T�A and C�G base-pairs (good \
line \up0 \expndtw0\charscalex102 targets for the D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 base) than it does with A�T and \line \up0 \expndtw0\
charscalex100 G�C base-pairs (poor targets for the D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 base; Fig-\line \up0 \expndtw-4\charscalex100
ure 10). Sequence-specific hydrogen bond formation \line \up0 \expndtw0\
charscalex101 cannot be unambiguously ruled out, although the \line \up0 \expndtw0\
charscalex101 three chemical groups of the D\ul0\sub\cf16\f17\fs18 3 \up0 \
expndtw0\charscalex100 \ul0\nosupersub\cf7\f8\fs20 base that can\par\pard\qj \
li20\ri1643\sb0\sl-219\slmult0 \up0 \expndtw-4\charscalex100 potentially form
hydrogen bonds (the amide proton, \line \up0 \expndtw0\charscalex105 the carbonyl
oxygen and the N3A imidazole \line \up0 \expndtw0\charscalex105 nitrogen) do
not show evidence of hydrogen \line \up0 \expndtw0\charscalex100 bonding. The
amide proton is exchanging rapidly, \line \up0 \expndtw0\charscalex101 which is
inconsistent with hydrogen bond for-\line \up0 \expndtw-2\charscalex100 mation.
The imidazole N3A nitrogen faces outward \line \up0 \expndtw-2\charscalex100 into
the major groove with no nearby hydrogen \line \up0 \expndtw-3\charscalex100
bond acceptors (Figure 10). In addition, the only \line \up0 \expndtw-3\
charscalex100 available acceptors for the peptide amide proton are \line \up0 \
expndtw0\charscalex101 the A5 and A17N1, the A5N7 and the T4O2, all of \line \up0 \
expndtw-1\charscalex100 which are out of plane with the peptide group and \line \
up0 \expndtw0\charscalex100 could form only weak hydrogen bonds. Similarly, \line \
up0 \expndtw0\charscalex103 the only hydrogen bond donors near the peptide \line \
up0 \expndtw0\charscalex101 carbonyl group are the A5 and A17 amino groups \line \
up0 \expndtw-2\charscalex100 and the T4 and T16 imino protons, which would all \
line \up0 \expndtw-1\charscalex100 yield weak hydrogen bonds.\par\pard\qj \li20\
ri1643\sb0\sl-219\slmult0\fi199 \up0 \expndtw0\charscalex100 Electrostatic
interactions may also be important, \up0 \expndtw0\charscalex102 although the exact
nature of the interaction is not \up0 \expndtw-2\charscalex100 clear. For example,
in the major groove, the peptide \up0 \expndtw0\charscalex102 polar groups are near
several polar groups of the \up0 \expndtw-2\charscalex100 T�A base-pair (Figure
10(a)). However, in the major \up0 \expndtw0\charscalex101 groove of a G�C base-
pair (a poor target for the D\ul0\sub\cf16\f17\fs18 3 \up0 \expndtw-2\charscalex100
\ul0\nosupersub\cf7\f8\fs20 base) the same polar groups are present in a similar \
up0 \expndtw-2\charscalex100 arrangement (Figure \up0 \expndtw-1\charscalex100
10(d)). Similarly, the major\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0 \up0 \
expndtw-2\charscalex100 groove of a C�G and on A�T base-pair resemble one \line \
up0 \expndtw0\charscalex101 another, although a C�G base-pair is a good target \
line \up0 \expndtw-4\charscalex100 for the D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 base and an A�T base-pair is a poor target. \line \up0 \
expndtw-2\charscalex100 In an effort to elucidate further the determinants of \line
\up0 \expndtw0\charscalex102 sequence specificity, we are currently solving the \
line \up0 \expndtw0\charscalex100 solution structure of the D\ul0\sub\cf16\f17\fs18
3\ul0\nosupersub\cf7\f8\fs20 base targeted to a C�G \line \up0 \expndtw-2\
charscalex100 base-pair.\par\pard\qj \li20\ri1643\sb0\sl-219\slmult0\fi199 \up0 \
expndtw-3\charscalex100 D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20
intercalation strongly prefers a neighboring \line \up0 \expndtw0\charscalex102
T�A�T triplet over a C\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\
nosupersub\cf7\f8\fs20 �G�C triplet. Comparison of \line \up0 \expndtw-4\
charscalex100 the D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base
stacked over a T�A�T and a C\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\
nosupersub\cf7\f8\fs20 �G�C triplet \line \up0 \expndtw0\charscalex104 does not
present any obvious reason for this \line \up0 \expndtw-2\charscalex100
preference \up0 \expndtw-2\charscalex100 (Figure \up0 \expndtw0\charscalex100 10(e)
and \up0 \expndtw0\charscalex100 (f)). However, the\par\pard\qj \li20\ri1643\sb0\
sl-219\slmult0 \up0 \expndtw0\charscalex102 preference for a neighboring T�A�T
triplet may be \line \up0 \expndtw0\charscalex103 more general than just for the D\
ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base, since the \line \up0 \
expndtw0\charscalex100 canonical triplets also prefer neighboring T�A�T

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shpbxpage\shpbypage\shpwr3\shpwrk0\shpfblwtxt1\shpz445\shplid0
{\sp{\sn shapeType}{\sv 0}}{\sp{\sn fFlipH}{\sv 0}}{\sp{\sn fFlipV}{\sv 0}}{\sp{\sn
geoRight}{\sv 9442}}{\sp{\sn geoBottom}{\sv 20}}
{\sp{\sn pVerticies}{\sv 8;4;(0,20);(9442,20);(9442,0);(0,0)}}
{\sp{\sn pSegmentInfo}{\sv 2;10;16384;45824;1;45824;1;45824;1;45824;24577;32768}}
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sn fLine}{\sv 0}}{\sp{\sn lineType}{\sv 0}}{\sp{\sn fArrowheadsOK}{\sv 1}}{\sp{\sn
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}}\par\pard\sect\sectd\fs24\paperw12240\paperh15840\pard\sb0\sl-240{\bkmkstart
Pg14}{\bkmkend Pg14}\par\pard\li956\sb0\sl-218\slmult0\par\pard\li956\sb151\sl-218\
slmult0\fi0\tx9955 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf1\f2\fs18
Solution Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18
-containing DNA Triplex\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf22\f23\
fs20 1065\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\
colw6244\colsr160\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb191\sl-230\
slmult0 \up0 \expndtw0\charscalex101 \ul0\nosupersub\cf7\f8\fs20 triplets over C\
ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\fs17 +\ul0\nosupersub\cf7\f8\fs20 �G�C
triplets (Kiessling\ul0\nosupersub\cf9\f10\fs20 et al\ul0\nosupersub\cf7\f8\
fs20 ., 1992).\par\pard\qj \li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw-2\
charscalex100 This preference may be an effect of the positive \up0 \
expndtw0\charscalex103 charge in a C\ul0\super\cf16\f17\fs18\ul0\super\cf16\f17\
fs17 +\ul0\nosupersub\cf7\f8\fs20 �G�C triplet.\par\pard\qj \li956\ri149\sb0\sl-
219\slmult0\fi199 \up0 \expndtw0\charscalex103 Intercalation occurs on the 3' side
of the target \line \up0 \expndtw0\charscalex104 base-pair instead of the 5' side.
This is due to the \line \up0 \expndtw-1\charscalex100 right-handedness of the
triplex. If one observes the \line \up0 \expndtw-3\charscalex100 helix in Figure
6(b), the third strand proceeds 5' to 3' \line \up0 \expndtw-2\charscalex100 from
top to bottom of the figure. In this orientation, \line \up0 \expndtw0\
charscalex102 D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 stacks below
and to the left of T27, between \line \up0 \expndtw0\charscalex100 the T27 and the
A3 sugars. D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 also stacks
above \line \up0 \expndtw0\charscalex103 and to the right of the T29 sugar. If D\
ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 were to \line \up0 \expndtw-
3\charscalex100 intercalate on the 5' side of (above) T4, the base step \line \
up0 \expndtw0\charscalex101 between T27 and D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 28 would be compressed and \line \up0 \expndtw-1\
charscalex100 overwound, which would force D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 28 towards the \line \up0 \expndtw0\charscalex102 purine
strand. Since D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 stacks
between the A3 \line \up0 \expndtw-2\charscalex100 and T27 sugars, the compression
in the rise and the \line \up0 \expndtw-2\charscalex100 overwinding of the twist
would force D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 into the \line
\up0 \expndtw-4\charscalex100 A3 sugar causing interference with the intercalation.
\line \up0 \expndtw-1\charscalex100 However, if D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 28 intercalates on the \up0 \expndtw0\charscalex102 3'
side of\par\pard\qj \li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex101
(below) T4 (as is observed), the base step between \up0 \expndtw-1\charscalex100 D\
ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 and T29 would be
compressed and over-\line \up0 \expndtw-3\charscalex100 wound, which would
force D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 away from the \
up0 \expndtw0\charscalex100 purine strand. Since D\ul0\sub\cf16\f17\fs18 3\ul0\
nosupersub\cf7\f8\fs20 28 does not stack between \up0 \expndtw0\charscalex108 two
sugars on the \up0 \expndtw0\charscalex109 3' side and because the\par\pard\
qj \li956\ri149\sb0\sl-219\slmult0\fi0 \up0 \expndtw-1\charscalex100 overwinding
rotates D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 28 further from the
purine \line \up0 \expndtw-1\charscalex100 strand, there is no obstruction from
other residues.\par\pard\ql \li956\sb0\sl-230\slmult0 \par\pard\ql \li956\sb100\sl-
230\slmult0 \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf24\f25\fs20
Conclusions\par\pard\qj \li956\ri149\sb139\sl-219\slmult0\fi199 \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf7\f8\fs20 In summary, a
pyrimidine�purine�pyrimidine \line \up0 \expndtw-3\charscalex100 triplex containing
a D\ul0\sub\cf16\f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base forms a stable
structure \line \up0 \expndtw-1\charscalex100 resembling other triplex structures,
despite having \line \up0 \expndtw-4\charscalex100 to accommodate D\ul0\sub\cf16\
f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 intercalation. The stability is \line \
up0 \expndtw-1\charscalex100 partially due to the ability of the D\ul0\sub\cf16\
f17\fs18 3\ul0\nosupersub\cf7\f8\fs20 base to imitate \line \up0 \expndtw0\
charscalex102 a triplet, although imperfectly. This suggests that \line \up0 \
expndtw-3\charscalex100 greater stability may be achieved by designing a \
line \up0 \expndtw0\charscalex106 base to more closely mimic a triplet.
Pyrim-\line \up0 \expndtw0\charscalex102 idine�purine�pyrimidine triplexes seem
to have \line \up0 \expndtw-1\charscalex100 several features in common, including
an axial rise \line \up0 \expndtw0\charscalex100 of\ul0\nosupersub\cf10\f11\fs20
0\ul0\nosupersub\cf7\f8\fs20 3.2 to 3.4 A\u730?, a low helical twist of\ul0\
nosupersub\cf10\f11\fs20 0\ul0\nosupersub\cf7\f8\fs20 30 to \line \up0 \expndtw-
1\charscalex100 32\ul0\nosupersub\cf25\f26\fs20 \u-3920?\ul0\nosupersub\cf7\f8\fs20
, an X-displacement of \up0 \expndtw0\charscalex103 \ul0\nosupersub\cf10\f11\
fs20 0\ul0\nosupersub\cf25\f26\fs20 -\ul0\nosupersub\cf7\f8\fs20 1 to\ul0\
nosupersub\cf25\f26\fs20 -\ul0\nosupersub\cf7\f8\fs20 3 A\u730?, and a\par\
pard\qj \li956\ri149\sb0\sl-219\slmult0 \up0 \expndtw0\charscalex105 predominance
of S-type sugar puckers. Since \up0 \expndtw0\charscalex101 triplexes conform
to neither\ul0\nosupersub\cf9\f10\fs20 A\ul0\nosupersub\cf7\f8\fs20 - nor\
ul0\nosupersub\cf9\f10\fs20 B\ul0\nosupersub\cf7\f8\fs20 -DNA \up0 \expndtw0\
charscalex103 exclusively, they might best be considered a new \up0 \expndtw-2\
charscalex100 form of DNA,\ul0\nosupersub\cf9\f10\fs20 T\ul0\nosupersub\cf7\f8\
fs20 -form DNA, a separate, distinct \up0 \expndtw0\charscalex100 family of
structures.\par\pard\ql \li956\sb0\sl-276\slmult0 \par\pard\ql \li956\sb15\sl-276\
slmult0 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf15\f16\fs24 Materials and
Methods\par\pard\ql \li956\sb160\sl-207\slmult0 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf2\f3\fs18 Sample preparation\par\pard\qj \li956\ri149\sb158\sl-199\
slmult0\fi179 \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf13\f14\fs18 The
phosphoramidite derivative of the artificial \line \up0 \expndtw-1\
charscalex100 nucleoside, D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\
fs18 , was prepared as described (Griffin\ul0\nosupersub\cf14\f15\fs18 et al\ul0\
nosupersub\cf13\f14\fs18 ., \line \up0 \expndtw-2\charscalex100 1992). The DNA
oligonucleotides were synthesized on an \line \up0 \expndtw0\charscalex101 ABI
380B DNA synthesizer. The oligonucleotides were \line \up0 \expndtw0\charscalex100
deprotected with concentrated ammonia at \up0 \expndtw0\charscalex101 55\ul0\
nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 C for\par\pard\qj \
li956\ri149\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 24 hours, and
subsequently desalted on a Sephadex G10 \up0 \expndtw-1\charscalex100 column. FPLC
purification \up0 \expndtw-1\charscalex100 (DMT-on) was performed\par\pard\qj \
li956\ri149\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100 using a gradient of
0 to 40% acetonitrile/100 mM tri-\line \up0 \expndtw-3\charscalex100
ethylammonium acetate over 40 minutes. Detritylation \line \up0 \expndtw-1\
charscalex100 was accomplished with 80% acetic acid for 30 minutes. \line \up0 \
expndtw-2\charscalex100 Final FPLC purification (DMT-off) used a gradient of 0 to \
line \up0 \expndtw-2\charscalex100 27% acetonitrile/100 mM triethylammonium acetate
over \line \up0 \expndtw-3\charscalex100 30 minutes. To remove the triethylammonium
acetate, the\par\pard\column \ql \li5856\sb0\sl-207\slmult0 \par\pard\ql \li5856\
sb0\sl-207\slmult0 \par\pard\ql \li20\sb6\sl-207\slmult0 \up0 \expndtw-2\
charscalex100 sample was run over a BioRad AG 50W-X8 ion-exchange\par\pard\qj \
li20\ri1643\sb0\sl-205\slmult0 \up0 \expndtw-3\charscalex100 column, followed by
chromatography on a Sephadex G15 \line \up0 \expndtw-1\charscalex100 column. The
appropriate fractions were then pooled and \line \up0 \expndtw-1\charscalex100
dried by lyophilization. The final conditions of the NMR \line \up0 \expndtw0\
charscalex101 samples were 100 mM NaCl, 5 mM MgCl\ul0\nosupersub\cf8\f9\fs11 2\ul0\
nosupersub\cf13\f14\fs18 , and\ul0\nosupersub\cf12\f13\fs18 0\ul0\nosupersub\
cf13\f14\fs18 2 mM\par\pard\ql \li20\sb1\sl-191\slmult0 \up0 \expndtw-1\
charscalex100 DNA in 400\ul0\nosupersub\cf12\f13\fs18 m\ul0\nosupersub\cf13\f14\
fs18 l of either 99.996%\ul0\super\cf8\f9\fs16 2\ul0\nosupersub\cf13\f14\fs18 H\
ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O or 90% H\ul0\
nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O/10%\par\pard\ql \li20\sb0\
sl-101\slmult0 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf8\f9\fs11 2\par\
pard\ql \li175\sb0\sl-162\slmult0 \up0 \expndtw0\charscalex102 \ul0\nosupersub\
cf13\f14\fs18 H\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O; the
pH was adjusted to 5.2 with NaOH/HCl.\par\pard\ql \li5856\sb0\sl-207\slmult0 \par\
pard\ql \li20\sb5\sl-207\slmult0 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf2\
f3\fs18 NMR spectroscopy\par\pard\qj \li20\ri1643\sb158\sl-199\slmult0\fi179 \up0 \
expndtw0\charscalex103 \ul0\nosupersub\cf13\f14\fs18 All NMR experiments were
performed on a General \up0 \expndtw0\charscalex100 Electric GN500 \up0 \expndtw0\
charscalex100 spectrometer.
Phase-sensitive nuclear\par\pard\qj \li20\ri1643\sb1\sl-199\slmult0 \up0 \
expndtw-1\charscalex100 Overhauser effect (NOESY) spectra (Kumar\ul0\nosupersub\
cf14\f15\fs18 et al\ul0\nosupersub\cf13\f14\fs18 ., 1980; \up0 \expndtw-1\
charscalex100 Macura & Ernst, 1980) were obtained employing the \up0 \
expndtw0\charscalex103 method of States\ul0\nosupersub\cf14\f15\fs18 et al\ul0\
nosupersub\cf13\f14\fs18 . (1982). For spectra in\ul0\super\cf8\f9\fs16 2\ul0\
nosupersub\cf13\f14\fs18 H\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\
fs18 O, the \up0 \expndtw-3\charscalex100 residual\ul0\super\cf8\f9\fs16 2\ul0\
nosupersub\cf13\f14\fs18 H\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\
fs18 O peak was suppressed by irradiation during \up0 \expndtw-2\charscalex100 the
recycle delay. Water suppression for samples in H\ul0\nosupersub\cf8\f9\fs11 2\ul0\
nosupersub\cf13\f14\fs18 O \up0 \expndtw0\charscalex104 was achieved by using
a \up0 \expndtw0\charscalex104 11-spin echo read pulse\par\pard\qj \li20\ri1568\
sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 (11ECHO; Sklena�\u345? & Bax,
1987). The carrier was centered \up0 \expndtw0\charscalex104 at the water
resonance, and the imino and amino \up0 \expndtw-1\charscalex100 resonances
were maximized by setting\ul0\nosupersub\cf12\f13\fs18 t\ul0\nosupersub\cf13\f14\
fs18 = 50 ms. Further \up0 \expndtw0\charscalex101 elimination of the residual
water was accomplished \up0 \expndtw0\charscalex101 during processing using a
time-domain convolution \up0 \expndtw0\charscalex101 routine (Marion\ul0\
nosupersub\cf14\f15\fs18 et al\ul0\nosupersub\cf13\f14\fs18 ., 1989).\par\pard\
qj \li20\ri1643\sb0\sl-199\slmult0\fi179 \up0 \expndtw-2\charscalex100 For NOE
restraints involving non-exchangeable reson-\line \up0 \expndtw-2\charscalex100
ances, a set of\ul0\super\cf8\f9\fs16 2\ul0\nosupersub\cf13\f14\fs18 H\ul0\
nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O NOESY spectra was
collected at 25\ul0\nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18
C \line \up0 \expndtw-1\charscalex100 with mixing times of 40, 80, 120, 160 and 200
ms without \line \up0 \expndtw0\charscalex101 removing the sample from the
magnet. All NOESY \line \up0 \expndtw0\charscalex104 spectra in the series
were collected and processed \line \up0 \expndtw-3\charscalex100 identically
except for the mixing time. The acquisition \line \up0 \expndtw-3\
charscalex100 parameters were a sweep width of 5000 Hz in both t\ul0\nosupersub\
cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 and \line \up0 \expndtw-3\
charscalex100 t\ul0\nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 , 1024
points in t\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 , 350 points
in t\ul0\nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 , 32 scans per t\
ul0\nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 block, \line \up0 \
expndtw0\charscalex102 and a recycle delay of two seconds. The t\ul0\nosupersub\
cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 apodization \line \up0 \expndtw-1\
charscalex100 was a 450 point, 45\ul0\nosupersub\cf27\f28\fs18 \u-3920?\ul0\
nosupersub\cf13\f14\fs18 phase shifted, squared sinebell with \line \up0 \expndtw-
2\charscalex100 a first-order polynomial baseline flattening and the t\ul0\
nosupersub\cf8\f9\fs11 1 \line \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf13\
f14\fs18 apodization was a 350 point, 45\ul0\nosupersub\cf27\f28\fs18 \u-3920?\ul0\
nosupersub\cf13\f14\fs18 phase shifted, squared \line \up0 \expndtw-1\
charscalex100 sinebell with a second-order polynomial baseline flatten-\line \up0 \
expndtw-3\charscalex100 ing. The resulting datasets were zero filled to 4096 by
4096 \line \up0 \expndtw0\charscalex103 complex points for ample digital
resolution during \line \up0 \expndtw0\charscalex100 integration of the crosspeak
volumes.\par\pard\qj \li20\ri1643\sb0\sl-199\slmult0\fi179 \up0 \expndtw-2\
charscalex100 For NOE restraints involving exchangeable resonances, \line \up0 \
expndtw0\charscalex103 an H\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\
fs18 O NOESY spectrum was collected at 1\ul0\nosupersub\cf27\f28\fs18 \u-3920?\
ul0\nosupersub\cf13\f14\fs18 C with a \line \up0 \expndtw0\charscalex100 mixing
time of 100 ms. The excitation maximum for the \line \up0 \expndtw-1\charscalex100
11ECHO water suppression was set to 13.9 ppm. All \line \up0 \expndtw-2\
charscalex100 processing, peak picking and integration were performed \line \up0 \
expndtw0\charscalex100 using FELIX 2.3 (Biosym Technologies/MSI) running on \line \
up0 \expndtw0\charscalex100 Silicon Graphics workstations. Further details of
the \line \up0 \expndtw0\charscalex102 acquisition and processing parameters are
given in the \line \up0 \expndtw-2\charscalex100 Figure captions.\par\pard\qj \
li20\ri1643\sb0\sl-203\slmult0\fi179 \up0 \expndtw-2\charscalex100 For proton
coupling data, a P.COSY spectrum (Marion \line \up0 \expndtw0\charscalex100 & Bax,
1988; Mueller, 1987) was collected at 25\ul0\nosupersub\cf27\f28\fs18 \u-3920?\ul0\
nosupersub\cf13\f14\fs18 C with a \line \up0 \expndtw-1\charscalex100 90\ul0\
nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 mixing pulse.
The acquisition parameters were a \line \up0 \expndtw-1\charscalex100 sweep
width of 5000 Hz in both t\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\
fs18 and t\ul0\nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 , 1024
points in \line \up0 \expndtw-8\charscalex87 t\ul0\nosupersub\cf8\f9\fs11 2\ul0\
nosupersub\cf13\f14\fs18 , \up0 \expndtw0\charscalex100 550 points in t\ul0\
nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 , 96 scans per t\ul0\
nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 block, and a recycle\par\
pard\qj \li20\ri1643\sb0\sl-199\slmult0\fi0 \up0 \expndtw0\charscalex101 delay of
1.8 seconds. Using the technique of Marion & \line \up0 \expndtw-2\charscalex100
Bax (1988), a one-dimensional reference spectrum was \line \up0 \expndtw-1\
charscalex100 collected to subtract the dispersive component of the \line \
up0 \expndtw-2\charscalex100 diagonal. The same parameters as the P.COSY were
used \line \up0 \expndtw-1\charscalex100 except that 1536 scans were collected and
the acquisition \line \up0 \expndtw-4\charscalex100 time was doubled. To insure
that the total relaxation delay \line \up0 \expndtw0\charscalex101 and H\ul0\
nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O pre-saturation between
scans was the same in \line \up0 \expndtw0\charscalex100 both the reference and
P.COSY spectrum, an additional \line \up0 \expndtw-1\charscalex100 delay equal to
the acquisition time was added to the end \line \up0 \expndtw-1\charscalex100 of
the P.COSY pulse sequence. The t\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\
f14\fs18 apodization was a \line \up0 \expndtw0\charscalex100 700 point, 35\ul0\
nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 phase shifted,
squared sinebell; and the t\ul0\nosupersub\cf8\f9\fs11 1 \line \up0 \expndtw0\
charscalex100 \ul0\nosupersub\cf13\f14\fs18 apodization was a 550 point, 45\ul0\
nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 phase shifted,
squared \line \up0 \expndtw-3\charscalex100 sinebell. Selective regions of the
spectrum were processed \line \up0 \expndtw0\charscalex101 and zero filled to a
resolution of \up0 \expndtw-2\charscalex100 0.82 \up0 \expndtw0\charscalex103
point/Hz for\par\pard\ql \li20\sb1\sl-172\slmult0 \up0 \expndtw-1\charscalex100
crosspeak pattern fitting.

{\shp {\*\shpinst\shpleft956\shptop899\shpright10398\shpbottom919\shpfhdr0\
shpbxpage\shpbypage\shpwr3\shpwrk0\shpfblwtxt1\shpz638\shplid0
{\sp{\sn shapeType}{\sv 0}}{\sp{\sn fFlipH}{\sv 0}}{\sp{\sn fFlipV}{\sv 0}}{\sp{\sn
geoRight}{\sv 9442}}{\sp{\sn geoBottom}{\sv 20}}
{\sp{\sn pVerticies}{\sv 8;4;(0,20);(9442,20);(9442,0);(0,0)}}
{\sp{\sn pSegmentInfo}{\sv 2;10;16384;45824;1;45824;1;45824;1;45824;24577;32768}}
{\sp{\sn fFillOK}{\sv 1}}{\sp{\sn fFilled}{\sv 1}}{\sp{\sn fillColor}{\sv 0}}{\sp{\
sn fLine}{\sv 0}}{\sp{\sn lineType}{\sv 0}}{\sp{\sn fArrowheadsOK}{\sv 1}}{\sp{\sn
fBehindDocument}{\sv 1}}{\sp{\sn lineColor}{\sv 0}}
}}\par\pard\sect\sectd\fs24\paperw12240\paperh15840\pard\sb0\sl-240{\bkmkstart
Pg15}{\bkmkend Pg15}\par\pard\li956\sb0\sl-230\slmult0\par\pard\li956\sb100\sl-230\
slmult0\fi0\tx6448 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf22\f23\fs20
1066\tab \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution
Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -
containing DNA Triplex\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\colsr160\
colno2\colw6244\colsr160\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \li956\sb0\sl-
207\slmult0 \par\pard\ql \li956\sb32\sl-207\slmult0 \up0 \expndtw-1\charscalex100 \
ul0\nosupersub\cf2\f3\fs18 NOE restraints\par\pard\qj \li956\ri149\sb179\sl-198\
slmult0\fi179 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\cf13\f14\fs18 Crosspeak
volumes from the\ul0\super\cf8\f9\fs16 2\ul0\nosupersub\cf13\f14\fs18 H\ul0\
nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\f14\fs18 O NOESY mixing time \line \
up0 \expndtw0\charscalex103 series were integrated for each mixing time.
These \line \up0 \expndtw-3\charscalex100 volumes were either used for
relaxation matrix refine-\line \up0 \expndtw-2\charscalex100 ment directly or
converted to distances for restrained \line \up0 \expndtw-1\charscalex100
distance refinement. Short mixing time data can be used \line \up0 \expndtw0\
charscalex102 to estimate the initial build-up rates of these crosspeak \line \
up0 \expndtw-3\charscalex100 volumes, which are inversely correlated to their
distances. \line \up0 \expndtw0\charscalex100 Only the 40 ms mixing time data were
used to calculate \line \up0 \expndtw-1\charscalex100 the distances because the
data from longer mixing times \line \up0 \expndtw0\charscalex100 indicated
significant spin diffusion. The 40 ms volumes \line \up0 \expndtw-2\charscalex100
were converted into distances using a set of known, fixed \line \up0 \expndtw-1\
charscalex100 distances for calibration and the relationship\ul0\nosupersub\cf14\
f15\fs18 Vol\ul0\nosupersub\cf8\f9\fs11 ij\ul0\nosupersub\cf12\f13\fs18 A\ul0\
nosupersub\cf13\f14\fs18 1/\ul0\nosupersub\cf14\f15\fs18 r\ul0\super\cf17\f18\
fs15\ul0\super\cf17\f18\fs14 ij\ul0\super\cf13\f14\fs26 , \line \up0 \expndtw0\
charscalex100 where\ul0\nosupersub\cf14\f15\fs18 Vol\ul0\nosupersub\cf8\f9\fs11
ij\ul0\nosupersub\cf13\f14\fs18 is the volume of the crosspeak between \
line \up0 \expndtw0\charscalex100 protons i and j, and\ul0\nosupersub\cf14\f15\fs18
r\ul0\nosupersub\cf8\f9\fs11 ij\ul0\nosupersub\cf13\f14\fs18 is the distance
between protons i \line \up0 \expndtw-3\charscalex100 and j. The crosspeaks used
for calibration were C9 H5-H6, \line \up0 \expndtw0\charscalex100 C19 H5-H6, C30
H5-H6 and D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 28 H5B-
H6B, chosen \line \up0 \expndtw0\charscalex100 because they were isolated
and could be cleanly \line \up0 \expndtw-3\charscalex100 integrated.\par\
pard\qj \li956\ri149\sb2\sl-199\slmult0\fi179 \up0 \expndtw-3\charscalex100 The
exchangeable crosspeaks were qualitatively catego-\line \up0 \expndtw-3\
charscalex100 rized as strong, medium or weak corresponding to 3.0, 4.0 \up0 \
expndtw-1\charscalex100 and 5.0 A\u730?, respectively. The crosspeak
intensities for \up0 \expndtw0\charscalex100 exchangeable resonances are not
accurately quantifiable \up0 \expndtw0\charscalex100 because they exchange with
water at differing rates and \up0 \expndtw-2\charscalex100 because correction for
the 11ECHO sin\ul0\super\cf8\f9\fs16 3\ul0\nosupersub\cf13\f14\fs18 excitation
profile \up0 \expndtw0\charscalex101 is only accurate near the maximum.\par\pard\qj
\li956\ri149\sb0\sl-199\slmult0\fi179 \up0 \expndtw-1\charscalex100 Crosspeaks that
overlapped each other and that could \line \up0 \expndtw0\charscalex100 not be
integrated separately were, nevertheless, utilized \line \up0 \expndtw-2\
charscalex100 by integrating the overlapping crosspeaks as a single \line \
up0 \expndtw0\charscalex101 crosspeak and converting the total volume into a single
\line \up0 \expndtw-2\charscalex100 distance restraint. The resulting distance
restraint was \line \up0 \expndtw-1\charscalex100 entered into XPLOR by using a \
u8216?\u8216?sum\u8217?\u8217? averaging, which \line \up0 \expndtw-2\charscalex100
allows multiple assignments to be defined and which \line \up0 \expndtw0\
charscalex100 correctly handles degenerate crosspeaks. Several reson-\line \up0 \
expndtw-3\charscalex100 ances in the C ring of the D\ul0\nosupersub\cf8\f9\fs11 3\
ul0\nosupersub\cf13\f14\fs18 base are degenerate and were \line \up0 \expndtw-1\
charscalex100 also averaged using the sum averaging method. Any \line \up0 \
expndtw-2\charscalex100 crosspeaks involving methyl groups had a 1/\ul0\nosupersub\
cf14\f15\fs18 r\ul0\super\cf8\f9\fs16 3\ul0\nosupersub\cf13\f14\fs18 averaging \
line \up0 \expndtw-2\charscalex100 in XPLOR (James\ul0\nosupersub\cf14\f15\fs18 et
al\ul0\nosupersub\cf13\f14\fs18 ., 1991). All other distance restraints \line \
up0 \expndtw-2\charscalex100 were calculated using \u8216?\u8216?center\u8217?\
u8217? averaging. In all cases \line \up0 \expndtw-1\charscalex100 except
overlapping crosspeaks, the lower bound was the \line \up0 \expndtw0\charscalex101
van der Waals\u8217? (VDW) radii and the upper bound was \line \up0 \expndtw-1\
charscalex100 +10% of the distance. For overlapping crosspeaks the \line \
up0 \expndtw-2\charscalex100 lower bound could potentially be less than the
VDW \line \up0 \expndtw-2\charscalex100 radii when using the sum averaging and
requires that the \line \up0 \expndtw0\charscalex103 lower bound be determined
by the formula: lower \line \up0 \expndtw-1\charscalex100 bound = VDW/(\ul0\
nosupersub\cf14\f15\fs18 n\ul0\super\cf8\f9\fs16 1/6\ul0\nosupersub\cf13\f14\
fs18 ), where\ul0\nosupersub\cf14\f15\fs18 n\ul0\nosupersub\cf13\f14\fs18 is
the number of over-\line \up0 \expndtw-1\charscalex100 lapping crosspeaks
integrated as a single crosspeak. The \line \up0 \expndtw0\charscalex102 upper
bound was +20% of the distance.\par\pard\qj \li956\ri149\sb0\sl-199\slmult0\fi179 \
up0 \expndtw-1\charscalex100 Background noise was integrated at various regions
of \up0 \expndtw-1\charscalex100 the spectrum and the average value was subtracted
from \up0 \expndtw-1\charscalex100 each crosspeak before converting them to
distances. The \up0 \expndtw-2\charscalex100 standard deviation of the
background noise level also \up0 \expndtw-2\charscalex100 gave an estimate of
the smallest measurable volume and, \up0 \expndtw-3\charscalex100 thus, the
longest measurable distance. Crosspeaks that \up0 \expndtw-2\charscalex100 were
below the noise level in the 40 ms NOESY spectrum \up0 \expndtw0\charscalex104 but
were visible at longer mixing times were given an \up0 \expndtw-1\charscalex100
upper bound restraint of 6 A\u730?.\par\pard\qj \li956\ri149\sb0\sl-199\slmult0\
fi179 \up0 \expndtw0\charscalex105 Repulsive restraints, which were obtained
in an \up0 \expndtw0\charscalex100 iterative approach (see Structure
determination, below) \up0 \expndtw0\charscalex100 were also utilized. When used as
distance restraints, the \up0 \expndtw-1\charscalex100 lower bound was 4 A\u730?
and the upper bound was 99 A\u730?. \up0 \expndtw0\charscalex100 When used as
volume restraints, the target volume was \up0 \expndtw0\charscalex102 set to the
noise level.\par\pard\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \li956\sb126\sl-
207\slmult0 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf2\f3\fs18 Torsion angle
restraints\par\pard\qj \li956\ri149\sb159\sl-199\slmult0\fi179 \up0 \expndtw-3\
charscalex100 \ul0\nosupersub\cf13\f14\fs18 To determine the coupling constants
in the deoxyri-\line \up0 \expndtw0\charscalex101 boses, the H1'-H2' and H1'-H2"
crosspeaks of a P.COSY\par\pard\column \ql \li5856\sb0\sl-207\slmult0 \par\pard\
ql \li5856\sb0\sl-207\slmult0 \par\pard\ql \li20\sb32\sl-207\slmult0 \up0 \
expndtw0\charscalex101 spectrum were fit using CHEOPS (Macaya\ul0\nosupersub\cf14\
f15\fs18 et al\ul0\nosupersub\cf13\f14\fs18 ., 1992a;\par\pard\qj \li20\ri1643\
sb0\sl-199\slmult0\fi0 \up0 \expndtw-1\charscalex100 Schultze & Feigon, unpublished
program). The dihedral \line \up0 \expndtw0\charscalex100 angles\ul0\nosupersub\
cf12\f13\fs18 n\ul0\nosupersub\cf8\f9\fs11 1\ul0\nosupersub\cf13\f14\fs18 and\
ul0\nosupersub\cf12\f13\fs18 n\ul0\nosupersub\cf8\f9\fs11 2\ul0\nosupersub\cf13\
f14\fs18 were determined from these coupling \line \up0 \expndtw-3\charscalex100
constants by fitting them to a two-state model for the \line \up0 \
expndtw0\charscalex100 sugar pucker with the program PSEUROT (de Leeuw & \line \up0
\expndtw-2\charscalex100 Altona, 1983) and using the dihedrals from the
major \line \up0 \expndtw-1\charscalex100 conformation. The dihedrals were
restrained with an \line \up0 \expndtw0\charscalex101 error of \up0 \expndtw0\
charscalex105 \ul0\nosupersub\cf12\f13\fs18 2\ul0\nosupersub\cf13\f14\fs18 5\ul0\
nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\cf13\f14\fs18 . These two
dihedral restraints fix the\par\pard\qj \li20\ri1643\sb0\sl-199\slmult0 \up0 \
expndtw-2\charscalex100 backbone torsion angle\ul0\nosupersub\cf12\f13\fs18 d\ul0\
nosupersub\cf13\f14\fs18 . Twelve residues were resolved \line \up0 \expndtw-3\
charscalex100 enough to determine coupling constants, leading to 24 \line \
up0 \expndtw0\charscalex101 dihedral angle restraints. The\ul0\nosupersub\cf12\f13\
fs18 e\ul0\nosupersub\cf13\f14\fs18 dihedrals were derived \line \up0 \expndtw0\
charscalex102 from a\ul0\super\cf8\f9\fs16 1\ul0\nosupersub\cf13\f14\fs18 H-\ul0\
super\cf8\f9\fs16 31\ul0\nosupersub\cf13\f14\fs18 P heteroCOSY spectrum from which
it was \line \up0 \expndtw-2\charscalex100 determined that no\ul0\super\cf8\f9\
fs16
3\ul0\nosupersub\cf14\f15\fs18 J\ul0\nosupersub\cf8\f9\fs11 P,H3'\ul0\
nosupersub\cf13\f14\fs18 couplings were greater than \line \up0 \expndtw-2\
charscalex100 14 Hz, which excludes the +\ul0\nosupersub\cf14\f15\fs18 gauche\ul0\
nosupersub\cf13\f14\fs18 conformation for the\ul0\nosupersub\cf12\f13\fs18 e \
line \up0 \expndtw0\charscalex101 \ul0\nosupersub\cf13\f14\fs18 dihedral angle.
Therefore, the\ul0\nosupersub\cf12\f13\fs18 e\ul0\nosupersub\cf13\f14\fs18 angle
was restrained to \line \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf27\f28\fs18
-\ul0\nosupersub\cf13\f14\fs18 120 \up0 \expndtw0\charscalex102 (\ul0\nosupersub\
cf12\f13\fs18 2\ul0\nosupersub\cf13\f14\fs18 120)\ul0\nosupersub\cf27\f28\fs18 \u-
3920?\ul0\nosupersub\cf13\f14\fs18 for all 31 phosphate groups. Twenty three\par\
pard\qj \li20\ri1643\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex100 residues from
the core of the triplex and the CCCC \up0 \expndtw0\charscalex100 loop had
their\ul0\nosupersub\cf12\f13\fs18 x\ul0\nosupersub\cf13\f14\fs18 angle
loosely restrained to the\ul0\nosupersub\cf14\f15\fs18 anti \up0 \expndtw0\
charscalex101 \ul0\nosupersub\cf13\f14\fs18 conformation (\ul0\nosupersub\cf27\
f28\fs18 -\ul0\nosupersub\cf13\f14\fs18 120(\ul0\nosupersub\cf12\f13\fs18 2\ul0\
nosupersub\cf13\f14\fs18 90)\ul0\nosupersub\cf27\f28\fs18 \u-3920?\ul0\nosupersub\
cf13\f14\fs18 ). The\ul0\nosupersub\cf12\f13\fs18 x\ul0\nosupersub\cf13\f14\fs18
angles for G2, the \up0 \expndtw-2\charscalex100 T25�A1�T20 \up0 \expndtw0\
charscalex100 triplet, and the TATA loop were not\par\pard\qj \li20\
ri1643\sb0\sl-199\slmult0\fi0 \up0 \expndtw0\charscalex100 restrained, since the
conformation of their glycosidic \line \up0 \expndtw-3\charscalex100 bond could
not be determined from their base to H1' \line \up0 \expndtw-1\charscalex100
crosspeaks. The\ul0\nosupersub\cf12\f13\fs18 x\ul0\nosupersub\cf13\f14\fs18 angle
for D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 28 was also not
restrained \line \up0 \expndtw-4\charscalex100 so as not to bias the
conformation of the D\ul0\nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18
base. To \line \up0 \expndtw-3\charscalex100 maintain proper chirality, an
additional dihedral angle \line \up0 \expndtw0\charscalex102 restraint was
applied to each chiral center, C1', C3' and \line \up0 \expndtw0\charscalex102 C4',
and to each prochiral center, C2', C5' and P.\par\pard\ql \li5856\sb0\sl-207\
slmult0 \par\pard\ql \li20\sb86\sl-207\slmult0 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf2\f3\fs18 Structure determination\par\pard\ql \li20\ri1643\sb158\sl-
199\slmult0\fi179\tx209 \up0 \expndtw0\charscalex103 \ul0\nosupersub\cf13\f14\fs18
Structure calculations were performed on Digital \line \up0 \expndtw0\
charscalex101 Equipment Corporation Alpha workstations using \line \up0 \
expndtw-3\charscalex100 XPLOR V3.1 (Brunger, 1992). The structure determination \
line \up0 \expndtw0\charscalex103 is composed of an initial refinement, which
essentially \line \up0 \expndtw-3\charscalex100 follows the protocols outlined in
the XPLOR V3.1 manual, \line \up0 \expndtw0\charscalex102 with only minor changes,
followed by an iterative, full \line \up0 \expndtw0\charscalex100 relaxation matrix
refinement. Iterative relaxation matrix \line \up0 \expndtw-3\charscalex100
refinement involves back-calculating the NOE volumes \line \up0 \expndtw0\
charscalex102 from the structures produced by the initial XPLOR \line \up0 \
expndtw-1\charscalex100 protocols and refining these back calculated
volumes \line \up0 \expndtw-1\charscalex100 against the observed volumes (Yip &
Case, 1989). After \line \up0 \expndtw0\charscalex100 one round of
relaxation matrix refinement, those \line \up0 \expndtw0\charscalex102
crosspeaks that are observed in the back-calculated \line \up0 \expndtw-3\
charscalex100 spectra but are clearly not observed in the NOESY spectra \line \
up0 \expndtw0\charscalex100 are entered as repulsive restraints and the structures
are \line \up0 \expndtw0\charscalex100 re-calculated. Several rounds of this
procedure are done \line \up0 \expndtw0\charscalex101 until no further repulsive
terms are found. \line\tab \up0 \expndtw-2\charscalex100 The XPLOR protocols
essentially consist of distance \line \up0 \expndtw-1\charscalex100 geometry
embedding of the structure consistent with the \line \up0 \expndtw-3\charscalex100
NOE distance and dihedral angle restraints, regulariz-\line \up0 \expndtw-2\
charscalex100 ation of the structure, further refinement using simulated \line \up0
\expndtw-3\charscalex100 annealing \up0 \expndtw0\charscalex101 (SA) with a
simplified VDW energy term\par\pard\qj \li20\ri1643\sb1\sl-199\slmult0\fi0 \
up0 \expndtw-1\charscalex100 and a final refinement with a long SA protocol and a
full \line \up0 \expndtw0\charscalex105 VDW energy term. In addition, we
supplemented \line \up0 \expndtw-1\charscalex100 these protocols with a final
relaxation matrix refinement. \line \up0 \expndtw0\charscalex102 The following
changes to the protocols were made: (1) \line \up0 \expndtw-1\charscalex100
distance geometry sub-embedding (dg sub embed.inp), \line \up0 \expndtw0\
charscalex100 which used atoms N1A, C1B, N and C1C of the D\ul0\
nosupersub\cf8\f9\fs11 3 \line \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf13\
f14\fs18 base for sub-embedding \up0 \expndtw-2\charscalex100 (Figure \up0 \
expndtw-2\charscalex100 1(a)); \up0 \expndtw-2\charscalex100 100 \up0 \expndtw-2\
charscalex100 structures\par\pard\qj \li20\ri1643\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex100 were calculated; (2) regularization (dgsa.inp), which de-\
line \up0 \expndtw0\charscalex108 creased the time step to \up0 \expndtw0\
charscalex105 2.5 fs to prevent wildly\par\pard\qj \li20\ri1643\sb0\sl-199\
slmult0 \up0 \expndtw-1\charscalex100 oscillating structures during dynamics, but
increased the \line \up0 \expndtw0\charscalex100 number of steps to 2000 to
maintain the same total \line \up0 \expndtw-1\charscalex100 simulation time; \
up0 \expndtw-2\charscalex100 100 \up0 \expndtw0\charscalex101 structures were
calculated; \up0 \expndtw-2\charscalex100 (3)\par\pard\qj \li20\ri1643\sb0\sl-199\
slmult0 \up0 \expndtw-2\charscalex100 refinement (refine.inp), which decreased
the time step \line \up0 \expndtw-2\charscalex100 to \up0 \expndtw0\charscalex100
2.0 fs and increased the number of steps to \up0 \expndtw-2\charscalex100
5000\par\pard\qj \li20\ri1643\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100
during dynamics; 100 structures were calculated; (4) full \line \up0 \expndtw-2\
charscalex100 VDW refinement (refine gentle.inp), which increased the \line \up0 \
expndtw-1\charscalex100 temperature during dynamics to 500 K. Included hydro-
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{\shp {\*\shpinst\shpleft6075\shptop13222\shpright8082\shpbottom13601\shpfhdr0\
shpbxpage\shpbypage\shpwr3\shpwrk0\shpfblwtxt1\shpz10001\shplid10001
{\sp{\sn shapeType}{\sv 202}}{\sp{\sn fFlipH}{\sv 0}}{\sp{\sn fFlipV}{\sv 0}}{\sp{\
sn fRecolorFillAsPicture}{\sv 0}}{\sp{\sn fUseShapeAnchor}{\sv 0}}{\sp{\sn fLine}{\
sv 0}}{\sp{\sn fFilled}{\sv 0}}{\sp{\sn fLayoutInCell}{\sv 1}}{\sp{\sn
fBehindDocument}{\sv 1}}{\shptxt\pard\plain \qj\sl132 \li0\ri0 \expndtw0\
charscalex100\ul0\nosupersub\cf13\f14\fs18 N. T., He�le{\par}}}}\pard\sb0\sl-240{\
bkmkstart Pg16}{\bkmkend Pg16}\par\pard\li956\sb0\sl-218\slmult0\par\pard\li956\
sb151\sl-218\slmult0\fi0\tx9955 \up0 \expndtw-1\charscalex100 \ul0\nosupersub\cf1\
f2\fs18 Solution Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\ul0\nosupersub\
cf1\f2\fs18 -containing DNA Triplex\tab \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf22\f23\fs20 1067\par\pard\sect\sectd\sbknone\cols2\colno1\colw5696\
colsr160\colno2\colw6244\colsr160\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \li956\
sb0\sl-207\slmult0 \par\pard\ql \li956\sb6\sl-207\slmult0 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf13\f14\fs18 gen bond energy term and used the
planarity restraint to\par\pard\qj \li956\ri149\sb20\sl-198\slmult0\fi0 \up0 \
expndtw-3\charscalex100 keep the individual bases and the rings of the D\ul0\
nosupersub\cf8\f9\fs11 3\ul0\nosupersub\cf13\f14\fs18 base flat; \line \up0 \
expndtw0\charscalex100 the 40 lowest energy structures from the previous stage \
line \up0 \expndtw-1\charscalex100 of refinement were refined; and (5)
relaxation matrix \line \up0 \expndtw0\charscalex101 refinement, in which
volumes from all five NOESY \line \up0 \expndtw0\charscalex101 mixing times
were used. The non-exchangeable and \line \up0 \expndtw-2\charscalex100
repulsive NOE distance restraints were replaced with the \line \up0 \expndtw-1\
charscalex100 corresponding volume integrals. The exchangeable (and \line \up0 \
expndtw0\charscalex103 hydrogen bond) NOEs were left as distance restraints. \
line \up0 \expndtw-3\charscalex100 The NOE energy scale was increased to
100. Isotropic \line \up0 \expndtw0\charscalex102 tumbling was assumed with a
correlation time of 5 ns. \line \up0 \expndtw0\charscalex107 The NOE integrals
were scaled to the same four \line \up0 \expndtw0\charscalex100 crosspeaks as
in the distance refinement. The relaxation \line \up0 \expndtw-2\charscalex100
energy parameters were set to cutoff = all, value = 6.0, \line \up0 \
expndtw0\charscalex101 potential = well, iexp = 1/6, eexp = 2, expo = 2, weight
\line \up0 \expndtw-2\charscalex100 = 0.5. This is essentially a\ul0\nosupersub\
cf14\f15\fs18 Vol\ul0\super\cf8\f9\fs16 1/6\ul0\nosupersub\cf13\f14\fs18
weighting of the integrals \line \up0 \expndtw0\charscalex101 (Brunger, 1992;
James\ul0\nosupersub\cf14\f15\fs18 et al\ul0\nosupersub\cf13\f14\fs18 ., 1991).
All other parameters \line \up0 \expndtw0\charscalex100 are the same as in the full
VDW refinement. The overall \line \up0 \expndtw0\charscalex100 relaxation matrix
refinement protocol is: (1) 100 steps of \line \up0 \expndtw0\charscalex100 energy
minimization with relaxation energy calibration \line \up0 \expndtw-1\charscalex100
turned off; (2) 1000 steps of dynamics with a time step of \line \up0 \expndtw0\
charscalex100 1.0 fs at 300 K with temperature bath coupling and auto \line \up0 \
expndtw-1\charscalex100 calibration turned on for the relaxation energy
term; \line \up0 \expndtw0\charscalex100 (3) the dynamics trajectory is
averaged over the last \line \up0 \expndtw0\charscalex102 half of the dynamics
run taken every 10 steps to obtain \line \up0 \expndtw0\charscalex102 an average
structure; and \up0 \expndtw-2\charscalex100 (4) \up0 \expndtw-2\charscalex100 200
\up0 \expndtw0\charscalex104 steps of energy\par\pard\qj \li956\ri149\sb2\sl-199\
slmult0 \up0 \expndtw-3\charscalex100 minimization done in two 100-step phases with
relaxation \up0 \expndtw0\charscalex100 matrix calibration done after each phase.
The 20 lowest \up0 \expndtw0\charscalex100 energy structures from the previous
stage of refinement \up0 \expndtw-1\charscalex100 were refined.\par\pard\ql \li956\
sb0\sl-207\slmult0 \par\pard\ql \li956\sb126\sl-207\slmult0 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf2\f3\fs18 Structure analysis\par\pard\qj \li956\
ri149\sb159\sl-199\slmult0\fi179 \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf13\
f14\fs18 The program CURVES (Lavery & Sklenar, 1988) was \line \up0 \expndtw0\
charscalex105 used to calculate the helical parameters in all the \line \
up0 \expndtw0\charscalex100 structures. Only the Watson-Crick duplex portion of the
\line \up0 \expndtw0\charscalex100 triplex was used in these calculations. XPLOR
V3.1 was \line \up0 \expndtw0\charscalex101 used to measure all the backbone
angles and sugar \line \up0 \expndtw-3\charscalex100 puckers.\par\pard\ql \li956\
sb0\sl-276\slmult0 \par\pard\ql \li956\sb0\sl-276\slmult0 \par\pard\ql \li956\
sb142\sl-276\slmult0 \up0 \expndtw-3\charscalex100 \ul0\nosupersub\cf15\f16\fs24
Acknowledgements\par\pard\qj \li956\ri149\sb87\sl-199\slmult0\fi179 \up0 \expndtw-
1\charscalex100 \ul0\nosupersub\cf13\f14\fs18 This work was supported by NIH grant
R01 GM37254 \line \up0 \expndtw-4\charscalex100 to J.F., and an Office of Naval
Research grant to P.B.D. The \line \up0 \expndtw0\charscalex100 coordinates for the
structures have been deposited with \line \up0 \expndtw-2\charscalex100 the
Brookhaven Protein Data Base (accession no. 1WAN).\par\pard\ql \li956\sb0\sl-276\
slmult0 \par\pard\ql \li956\sb20\sl-276\slmult0 \up0 \expndtw-3\charscalex100 \ul0\
nosupersub\cf15\f16\fs24 References\par\pard\ql \li956\sb120\sl-207\slmult0 \up0 \
expndtw0\charscalex107 \ul0\nosupersub\cf13\f14\fs18 Addess, K. J., Gilbert, D. E.,
Olsen, R. K. & Feigon, J.\par\pard\ql \li1314\sb1\sl-197\slmult0 \up0 \expndtw0\
charscalex104 (1992). Proton NMR studies of \up0 \expndtw0\charscalex101 [N-
MeCys\ul0\super\cf8\f9\fs16 3\ul0\nosupersub\cf13\f14\fs18 , N-\par\pard\ql \
li1314\sb1\sl-199\slmult0 \up0 \expndtw-4\charscalex100 MeCys\ul0\super\cf8\f9\fs16
7\ul0\nosupersub\cf13\f14\fs18 ]TANDEM binding to DNA oligonucleotides:\par\pard\
ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 sequence specific
binding at the TpA site.\ul0\nosupersub\cf14\f15\fs18 Biochem-\par\pard\ql \
li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 istry,\ul0\nosupersub\cf19\
f20\fs18 31\ul0\nosupersub\cf13\f14\fs18 , 339-350.\par\pard\ql \li956\sb1\sl-199\
slmult0 \up0 \expndtw0\charscalex107 Arnott, S. & Selsing, E. \up0 \expndtw0\
charscalex104 (1974). Structures for the\par\pard\ql \li1314\sb0\sl-199\
slmult0 \up0 \expndtw0\charscalex100 polynucleotide complexes poly(dA)�poly(dT)
and\par\pard\qj \li956\ri149\sb0\sl-199\slmult0\fi358 \up0 \expndtw-1\charscalex100
poly(dT)�poly(dA)�poly(dT).\ul0\nosupersub\cf14\f15\fs18 J. Mol. Biol.\ul0\
nosupersub\cf19\f20\fs18 88\ul0\nosupersub\cf13\f14\fs18 , 509-521. \line \up0 \
expndtw-3\charscalex100 Bax, A., Griffey, R. H. & Hawkins, B. L. (1983).
Correlation\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-3\charscalex100 of
proton and nitrogen-15 chemical shifts by multiple\par\pard\ql \li956\ri149\sb1\sl-
199\slmult0\fi358 \up0 \expndtw0\charscalex101 quantum NMR.\ul0\nosupersub\cf14\
f15\fs18 J. Magn. Reson.\ul0\nosupersub\cf19\f20\fs18 55\ul0\nosupersub\cf13\f14\
fs18 (55), 301-315. \line \up0 \expndtw-2\charscalex100 Beal, P. A. & Dervan, P. B.
(1991). Second structural motif\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex100 for recognition of DNA by oligonucleotide-directed\par\pard\
ql \li956\ri149\sb0\sl-199\slmult0\fi358 \up0 \expndtw0\charscalex100 triple-helix
formation.\ul0\nosupersub\cf14\f15\fs18 Science,\ul0\nosupersub\cf19\f20\fs18
251\ul0\nosupersub\cf13\f14\fs18 , 1360-1363. \line \up0 \expndtw-3\charscalex100
Belotserkovskii, B. P., Veselkov, A. G., Filippov, S. A.,\par\pard\ql \
li1314\sb1\sl-199\slmult0 \up0 \expndtw-2\charscalex100 Dobrynin, V. N., Mirkin, S.
M. & Frank-Kamenetskii,\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex100 M. D. (1990). Formation of intramolecular triplex in\par\pard\
column \ql \li5856\sb0\sl-207\slmult0 \par\pard\ql \li5856\sb0\sl-207\slmult0 \par\
pard\ql \li379\sb6\sl-207\slmult0 \up0 \expndtw-1\charscalex100 homopurine-
homopyrimidine mirror repeats with\par\pard\qj \li20\ri1643\sb0\sl-200\slmult0\
fi358 \up0 \expndtw0\charscalex101 point substitutions.\ul0\nosupersub\cf14\f15\
fs18 Nucl. Acids Res.\ul0\nosupersub\cf19\f20\fs18 18\ul0\nosupersub\cf13\f14\
fs18 , 6621-6624. \line \up0 \expndtw0\charscalex103 Blommers, M. J. J., van de
Ven, F. J. M., van der Marel,\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\
charscalex102 G. A., van Boom, J. H. & Hilbers, C. W. (1991). The\par\pard\ql \
li379\sb1\sl-200\slmult0 \up0 \expndtw-1\charscalex100 three-dimensional structure
of a DNA hairpin in\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\
charscalex100 solution. Two-dimensional NMR studies and struc-\par\pard\ql \li379\
sb1\sl-200\slmult0 \up0 \expndtw-5\charscalex100 tural analysis of
d(ATCCTATTTATAGGAT).\ul0\nosupersub\cf14\f15\fs18 Eur. J.\par\pard\ql \li379\
sb1\sl-200\slmult0 \up0 \expndtw0\charscalex102 Biochem.\ul0\nosupersub\cf19\f20\
fs18 181\ul0\nosupersub\cf13\f14\fs18 , 33-51.\par\pard\ql \li20\sb1\sl-200\
slmult0 \up0 \expndtw0\charscalex103 Broitman, S. L., Im, D. D. & Fresco, J. R.
(1987). Form-\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100
ation of the triple-stranded polynucleotide helix,\par\pard\qj \li20\ri1643\
sb1\sl-200\slmult0\fi358 \up0 \expndtw-2\charscalex100 poly(A�A�U).\ul0\nosupersub\
cf14\f15\fs18 Proc. Natl Acad. Sci. USA,\ul0\nosupersub\cf19\f20\fs18 84\ul0\
nosupersub\cf13\f14\fs18 , 5120-5124. \line \up0 \expndtw0\charscalex100 Brunger,
A. T. (1992).\ul0\nosupersub\cf14\f15\fs18 X-PLOR (Version 3.1) Manual\ul0\
nosupersub\cf13\f14\fs18 , Yale\par\pard\ql
\li20\ri1643\sb1\sl-200\slmult0\fi358 \up0 \expndtw-1\charscalex100 University
Press, New Haven and London. \line \up0 \expndtw0\charscalex101 Cooney, M.,
Czernuszewicz, G., Postel, E. H., Flint, S. J.\par\pard\ql \li379\sb2\sl-200\
slmult0 \up0 \expndtw0\charscalex100 & Hogan, M. E. (1988). Site-specific
oligonucleotide\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw-1\charscalex100
binding represses transcription of the human c-myc\par\pard\ql \li379\sb1\sl-200\
slmult0 \up0 \expndtw0\charscalex103 gene\ul0\nosupersub\cf14\f15\fs18 in vitro\
ul0\nosupersub\cf13\f14\fs18 .\ul0\nosupersub\cf14\f15\fs18 Science,\ul0\
nosupersub\cf19\f20\fs18 241\ul0\nosupersub\cf13\f14\fs18 , 456-459.\par\pard\ql \
li20\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex101 de Leeuw, F. A. A.
M. & Altona, C. J. \up0 \expndtw-2\charscalex100 (1983).\par\pard\ql \
li379\sb1\sl-200\slmult0 \up0 \expndtw-3\charscalex100 Computer-assisted
pseudorotation analysis of five-\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \
expndtw0\charscalex103 membered rings by means of proton spin-spin\par\pard\
ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 coupling constants:
Program PSEUROT.\ul0\nosupersub\cf14\f15\fs18 J. Comp.\par\pard\ql \li379\sb1\
sl-200\slmult0 \up0 \expndtw0\charscalex103 Chem.\ul0\nosupersub\cf19\f20\fs18 4\
ul0\nosupersub\cf13\f14\fs18 , 428-437.\par\pard\ql \li20\sb1\sl-200\slmult0 \up0 \
expndtw-3\charscalex100 de los Santos, C., Rosen, M. & Patel, D. (1989).
NMR\par\pard\ql \li379\sb14\sl-207\slmult0 \up0 \expndtw-1\charscalex100 studies
of DNA (R+)\ul0\nosupersub\cf8\f9\fs11 n\ul0\nosupersub\cf13\f14\fs18 �(Y\ul0\
nosupersub\cf27\f28\fs18 -\ul0\nosupersub\cf13\f14\fs18 )\ul0\nosupersub\cf8\f9\
fs11 n\ul0\nosupersub\cf13\f14\fs18 �(Y+)\ul0\nosupersub\cf8\f9\fs11 n\ul0\
nosupersub\cf13\f14\fs18 triple helices in\par\pard\ql \li379\sb1\sl-175\
slmult0 \up0 \expndtw0\charscalex100 solution: Imino and amino proton markers of
T�A�T\par\pard\ql \li379\sb5\sl-200\slmult0 \up0 \expndtw0\charscalex101 and C�G�C+
base-triple formation.\ul0\nosupersub\cf14\f15\fs18 Biochemistry,\ul0\nosupersub\
cf19\f20\fs18 28\ul0\nosupersub\cf13\f14\fs18 ,\par\pard\ql \li379\sb1\sl-200\
slmult0 \up0 \expndtw0\charscalex101 7282-7289.\par\pard\ql \li20\sb1\sl-200\
slmult0 \up0 \expndtw-4\charscalex100 Degols, G., Clarenc, J. P., Lebleu, B. &
Leonetti, J. P. (1994).\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\
charscalex100 Reversible inhibition of gene expression by a\par\pard\ql
\li379\sb1\sl-200\slmult0 \up0 \expndtw-2\charscalex100 psoralen functionalized
triple helix forming oligonu-\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\
charscalex100 cleotide in intact cells.\ul0\nosupersub\cf14\f15\fs18 J.
Biol. Chem. \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf19\f20\fs18 269\ul0\
nosupersub\cf13\f14\fs18 (24),\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \
expndtw0\charscalex100 16933-16937.\par\pard\ql \li20\sb2\sl-200\slmult0 \up0 \
expndtw-1\charscalex100 Felsenfeld, G., Davies, D. R. & Rich, A. (1957). Formation\
par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 of a three-
stranded polynucleotide molecule.\ul0\nosupersub\cf14\f15\fs18 J. Am.\par\pard\
ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex102 Chem. Soc.\ul0\
nosupersub\cf19\f20\fs18 79\ul0\nosupersub\cf13\f14\fs18 , 2023-2024.\par\pard\
ql \li20\sb1\sl-200\slmult0 \up0 \expndtw-2\charscalex100 Gao, X. & Patel, D. J.
(1988). NMR studies of echinomycin\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \
expndtw-2\charscalex100 bisintercalation complexes with d(A1-C2-G3-T4) and\par\
pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 d(T1-C2-G3-A4)
duplexes in aqueous solution:\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \
expndtw0\charscalex100 sequence-dependent formation of Hoogsteen A1�T4\par\pard\
ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 and Watson-Crick
T1�A4 \up0 \expndtw0\charscalex100 base-pairs flanking the\par\pard\ql \li20\
ri1643\sb1\sl-200\slmult0\fi358 \up0 \expndtw0\charscalex100 bisintercalation
site.\ul0\nosupersub\cf14\f15\fs18 Biochemistry,\ul0\nosupersub\cf19\f20\fs18 27\
ul0\nosupersub\cf13\f14\fs18 , 1744-1751. \line \up0 \expndtw0\charscalex104
Gilbert, D. E., van der Marel, G. A., van Boom, J. H. &\par\pard\ql \li379\sb1\sl-
200\slmult0 \up0 \expndtw0\charscalex101 Feigon, J. \up0 \expndtw0\charscalex100
(1989). Unstable Hoogsteen base-pairs\par\pard\ql \li379\sb1\sl-200\slmult0 \up0
\expndtw-2\charscalex100 adjacent to echinomycin binding sites within a DNA\par\
pard\ql \li20\ri1643\sb1\sl-200\slmult0\fi358 \up0 \expndtw0\charscalex102 duplex.\
ul0\nosupersub\cf14\f15\fs18 Proc. Natl Acad. Sci. USA,\ul0\nosupersub\cf19\f20\
fs18 86\ul0\nosupersub\cf13\f14\fs18 , 3006-3010. \line \up0 \expndtw0\
charscalex102 Greenberg, W. A. & Dervan, P. B. (1995). Energetics of\par\pard\ql \
li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex101 formation of sixteen triple
helical complexes which\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw-2\
charscalex100 vary at a single position within a purine motif.\ul0\nosupersub\cf14\
f15\fs18 J. Am.\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex102
Chem. Soc.\ul0\nosupersub\cf19\f20\fs18 117\ul0\nosupersub\cf13\f14\fs18 , 5016-
5022.\par\pard\ql \li20\sb2\sl-200\slmult0 \up0 \expndtw0\charscalex100 Griffin,
L. C. & Dervan, P. B. \up0 \expndtw-1\charscalex100 (1989). Recognition of\
par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 thymine�adenine
base-pairs by guanine in a pyrim-\par\pard\ql \li20\ri1643\sb1\sl-200\slmult0\fi358
\up0 \expndtw0\charscalex102 idine triple helix motif.\ul0\nosupersub\cf14\f15\fs18
Science,\ul0\nosupersub\cf19\f20\fs18 245\ul0\nosupersub\cf13\f14\fs18 , 967-
971. \line \up0 \expndtw0\charscalex101 Griffin, L. C., Kiessling, L. L., Beal, P.
A., Gillespie, P. &\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw-4\
charscalex100 Dervan, P. B. (1992). Recognition of all four base-pairs\par\pard\
ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 of double-helical DNA
by triple-helix formation:\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\
charscalex100 design of nonnatural deoxyribonucleosides for\par\pard\ql \
li379\sb1\sl-200\slmult0 \up0 \expndtw-2\charscalex100 pyrimidine�purine base-pair
binding.\ul0\nosupersub\cf14\f15\fs18 J. Am. Chem.\par\pard\ql \li379\sb1\sl-
200\slmult0 \up0 \expndtw0\charscalex102 Soc.\ul0\nosupersub\cf19\f20\fs18 114\
ul0\nosupersub\cf13\f14\fs18 , 7976-7982.\par\pard\ql \li20\sb1\sl-200\slmult0 \up0
\expndtw0\charscalex105 Grigoriev, M., Praseuth, D., Robin, P., Hemar, A.,\
par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw-1\charscalex100 Saison-
Behmoaras, T., Dautry-Varsat, A., Thuong,\par\pard\ql \li1176\sb1\sl-200\
slmult0 \up0 \expndtw0\charscalex100 `ne, C. & Harel-Bellant, A. (1992). A triple\
par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw-3\charscalex100 helix-forming
oligonucleotide-intercalator conjugate\par\pard\ql \li379\sb1\sl-200\slmult0 \
up0 \expndtw-3\charscalex100 acts as a transcriptional repressor via inhibition of
NF\par\pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 \ul0\
nosupersub\cf12\f13\fs18 k\ul0\nosupersub\cf13\f14\fs18 B binding to
interleukin-2 \up0 \expndtw-2\charscalex100 receptor\ul0\nosupersub\cf12\f13\fs18
a\ul0\nosupersub\cf13\f14\fs18 -regulatory\par\pard\ql \li379\sb1\sl-200\slmult0 \
up0 \expndtw0\charscalex102 sequence.\ul0\nosupersub\cf14\f15\fs18 J. Biol. Chem.\
ul0\nosupersub\cf19\f20\fs18 267\ul0\nosupersub\cf13\f14\fs18 (5), 3389-3395.\par\
pard\ql \li20\sb1\sl-200\slmult0 \up0 \expndtw0\charscalex100 Harbison, G. S.
(1993). Interference between J-couplings\par\pard\ql \li379\sb2\sl-200\slmult0 \up0
\expndtw0\charscalex105 and cross-relaxation in solution NMR spec-\par\
pard\ql \li379\sb1\sl-200\slmult0 \up0 \expndtw-2\charscalex100 troscopy\u8212?
consequences for macromolecular struc-\par\pard\ql \li379\sb1\sl-200\slmult0 \
up0 \expndtw-1\charscalex100 ture determination.\ul0\nosupersub\cf14\f15\fs18 J.
Am. Chem. Soc.\ul0\nosupersub\cf19\f20\fs18 115\ul0\nosupersub\cf13\f14\fs18 ,
3026-3027.
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{\shp {\*\shpinst\shpleft1174\shptop7593\shpright5992\shpbottom7972\shpfhdr0\
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{\sp{\sn shapeType}{\sv 202}}{\sp{\sn fFlipH}{\sv 0}}{\sp{\sn fFlipV}{\sv 0}}{\sp{\
sn fRecolorFillAsPicture}{\sv 0}}{\sp{\sn fUseShapeAnchor}{\sv 0}}{\sp{\sn fLine}{\
sv 0}}{\sp{\sn fFilled}{\sv 0}}{\sp{\sn fLayoutInCell}{\sv 1}}{\sp{\sn
fBehindDocument}{\sv 1}}{\shptxt\pard\plain \qj\sl132 \li0\ri0 \expndtw-2\
charscalex100\ul0\nosupersub\cf13\f14\fs18 Decout, J.-L., Thuong, N. T., Lhomme, J.
& He�le{\par}}}}

{\shp {\*\shpinst\shpleft6075\shptop2214\shpright10292\shpbottom2593\shpfhdr0\
shpbxpage\shpbypage\shpwr3\shpwrk0\shpfblwtxt1\shpz10001\shplid10001
{\sp{\sn shapeType}{\sv 202}}{\sp{\sn fFlipH}{\sv 0}}{\sp{\sn fFlipV}{\sv 0}}{\sp{\
sn fRecolorFillAsPicture}{\sv 0}}{\sp{\sn fUseShapeAnchor}{\sv 0}}{\sp{\sn fLine}{\
sv 0}}{\sp{\sn fFilled}{\sv 0}}{\sp{\sn fLayoutInCell}{\sv 1}}{\sp{\sn
fBehindDocument}{\sv 1}}{\shptxt\pard\plain \qj\sl132 \li0\ri0 \expndtw-1\
charscalex100\ul0\nosupersub\cf13\f14\fs18 T., Barcelo, F., Chomilier, J. &
He�le{\par}}}}\pard\sb0\sl-240{\bkmkstart Pg17}{\bkmkend Pg17}\par\pard\li956\sb0\
sl-230\slmult0\par\pard\li956\sb100\sl-230\slmult0\fi0\tx6448 \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1068\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\
cf21\f22\fs10 3\ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\par\pard\sect\
sectd\sbknone\cols2\colno1\colw5696\colsr160\colno2\colw6244\colsr160\ql \li956\
sb0\sl-207\slmult0 \par\pard\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \li956\sb32\
sl-207\slmult0 \up0 \expndtw-4\charscalex100 \ul0\nosupersub\cf13\f14\fs18 Havre,
P. A., Gunther, E. J., Gasparro, F. P. & Glazer, P. M.\par\pard\ql \li1314\sb0\sl-
199\slmult0 \up0 \expndtw-3\charscalex100 (1993). Targeted mutagenesis of DNA
using triple\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100
helix-forming oligonucleotides linked to psoralen.\par\pard\ql \li956\ri149\
sb0\sl-199\slmult0\fi358 \up0 \expndtw0\charscalex102 \ul0\nosupersub\cf14\f15\fs18
Proc. Natl Acad. Sci. USA,\ul0\nosupersub\cf19\f20\fs18 90\ul0\nosupersub\cf13\
f14\fs18 (16), 7879-7883. \line \up0 \expndtw0\charscalex102 James, T. L., Gochin,
M., Kerwood, D. J., Schmitz, U. &\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \
expndtw-2\charscalex100 Thomas, P. D. (1991).\ul0\nosupersub\cf14\f15\fs18
Computational Aspects of the\par\pard\ql \li1314\sb1\sl-199\slmult0 \up0 \
expndtw-1\charscalex100 Study of Biological Macromolecules by NMR\ul0\
nosupersub\cf13\f14\fs18 (Hoch,\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex101 J. C., ed.), Plenum Press, New York.\par\pard\ql \li956\sb0\
sl-199\slmult0 \up0 \expndtw0\charscalex104 Ji, H. M., Smith, L. M. & Guilfoyle, R.
A. (1994). Rapid\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-2\
charscalex100 isolation of cosmid insert DNA by triple-helix-medi-\par\pard\ql \
li1314\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 ated affinity capture.\
ul0\nosupersub\cf14\f15\fs18 Genet. Anal. Techn. Appl.\ul0\nosupersub\cf19\
f20\fs18 11\ul0\nosupersub\cf13\f14\fs18 ,\par\pard\ql \li1314\sb1\sl-199\slmult0
\up0 \expndtw0\charscalex103 43-47.\par\pard\ql \li956\sb0\sl-199\slmult0 \up0 \
expndtw-2\charscalex100 Kiessling, L. L., Griffin, L. C. & Dervan, P. B.
(1992).\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100
Flanking sequence effects within the pyrimidine\par\pard\ql \li1314\sb0\sl-
199\slmult0 \up0 \expndtw0\charscalex100 triple-helix motif characterized by
affinity cleaving.\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex100 \ul0\nosupersub\cf14\f15\fs18 Biochemistry,\ul0\nosupersub\cf19\f20\
fs18 31\ul0\nosupersub\cf13\f14\fs18 , 2829-2834.\par\pard\ql \li956\sb1\sl-199\
slmult0 \up0 \expndtw0\charscalex103 Koshlap, K. M., Gillespie, P., Dervan, P. B. &
Feigon, J.\par\pard\ql \li1314\sb13\sl-207\slmult0 \up0 \expndtw-4\charscalex100
(1993). Nonnatural deoxyribonucleoside D\ul0\nosupersub\cf8\f9\fs11 3\ul0\
nosupersub\cf13\f14\fs18 incorpor-\par\pard\ql \li1314\sb1\sl-174\slmult0 \up0 \
expndtw0\charscalex100 ated in an intramolecular DNA triplex binds\par\
pard\ql \li1314\sb5\sl-199\slmult0 \up0 \expndtw0\charscalex101 sequence-
specifically by intercalation.\ul0\nosupersub\cf14\f15\fs18 J. Am. Chem.\par\pard\
ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 Soc.\ul0\nosupersub\
cf19\f20\fs18 115\ul0\nosupersub\cf13\f14\fs18 , 7908-7909.\par\pard\ql \li956\
sb1\sl-199\slmult0 \up0 \expndtw0\charscalex105 Kumar, A., Ernst, R. R. &
Wuthrich, K. \up0 \expndtw0\charscalex102 (1980). A\par\pard\ql \li1314\sb0\sl-
199\slmult0 \up0 \expndtw-2\charscalex100 two-dimensional nuclear Overhauser
enhancement\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-3\charscalex100
(2D NOE) experiment for the elucidation of complete\par\pard\ql \li1314\sb0\sl-199\
slmult0 \up0 \expndtw-3\charscalex100 proton-proton cross-relaxation networks in
biological\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100
macromolecules.\ul0\nosupersub\cf14\f15\fs18 Biochem. Biophys. Res. Commun.\ul0\
nosupersub\cf19\f20\fs18 95\ul0\nosupersub\cf13\f14\fs18 ,\par\pard\ql \li1314\
sb1\sl-199\slmult0 \up0 \expndtw0\charscalex108 1-6.\par\pard\ql \li956\sb0\sl-199\
slmult0 \up0 \expndtw0\charscalex104 Lavery, R. & Sklenar, H. \up0 \expndtw0\
charscalex104 (1988). The definition of\par\pard\ql \li1314\sb0\sl-199\slmult0 \
up0 \expndtw0\charscalex101 generalized helicoidal parameters and of
axis\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 curvature
for irregular nucleic acids.\ul0\nosupersub\cf14\f15\fs18 J. Biomol. Struct.\par\
pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 Dynam.\ul0\
nosupersub\cf19\f20\fs18 6\ul0\nosupersub\cf13\f14\fs18 (1), 63-91.\par\pard\ql \
li956\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex102 Le Doan, T., Perrouault, L.,
Praseuth, D., Habhoub, N.,\par\pard\ql \li4976\sb0\sl-199\slmult0 \up0 \expndtw-1\
charscalex100 `ne, C.\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex100 (1987). Sequence-specific recognition, photocross-\par\pard\ql \
li1314\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100 linking and cleavage of the
DNA double helix by an\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-1\
charscalex100 oligo-[\ul0\nosupersub\cf12\f13\fs18 a\ul0\nosupersub\cf13\f14\
fs18 ]-thymidylate covalently linked to an azido-\par\pard\qj \li956\ri149\sb1\sl-
199\slmult0\fi358 \up0 \expndtw-1\charscalex100 proflavine derivative.\ul0\
nosupersub\cf14\f15\fs18 Nucl. Acids Res.\ul0\nosupersub\cf19\f20\fs18 15\ul0\
nosupersub\cf13\f14\fs18 , 7749-7760. \up0 \expndtw0\charscalex106 Lipsett, M. N.
\up0 \expndtw0\charscalex102 (1964). Complex formation between\par\pard\ql \
li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex101 polycytidylic acid and
guanine oligonucleotides.\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex103 \ul0\nosupersub\cf14\f15\fs18 J. Biol. Chem.\ul0\nosupersub\cf19\f20\
fs18 239\ul0\nosupersub\cf13\f14\fs18 , 1256-1260.\par\pard\ql \li956\sb0\sl-199\
slmult0 \up0 \expndtw-3\charscalex100 Liu, K., Miles, H. T., Parris, K. D.
& Sasisekharan, V.\par\pard\ql \li1314\sb1\sl-199\slmult0 \up0 \expndtw-2\
charscalex100 (1994). Fibre-type X-Ray diffraction patterns from\par\pard\ql \
li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 single crystals of triple
helical DNA.\ul0\nosupersub\cf14\f15\fs18 Nature Struct.\par\pard\ql \li1314\sb0\
sl-199\slmult0 \up0 \expndtw0\charscalex105 Biol.\ul0\nosupersub\cf19\f20\fs18 1\
ul0\nosupersub\cf13\f14\fs18 , 11-12.\par\pard\ql \li956\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex101 Luebke, K. J. & Dervan, P. B. \up0 \expndtw-2\
charscalex100 (1991). Nonenzymatic\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \
expndtw-1\charscalex100 sequence-specific ligation of double-helical DNA.\par\
pard\ql \li1314\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex103 \ul0\nosupersub\
cf14\f15\fs18 J. Am. Chem. Soc.\ul0\nosupersub\cf19\f20\fs18 113\ul0\nosupersub\
cf13\f14\fs18 , 7447-7448.\par\pard\ql \li956\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex102 Macaya, R. F., Gilbert, D. E., Malek, S., Sinsheimer, J. &\par\pard\
ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100 Feigon, J. (1991).
Structure and stability of X�G�C\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \
expndtw-1\charscalex100 mismatches in the third strand of intramolecular\par\
pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex101 triplexes.\ul0\
nosupersub\cf14\f15\fs18 Science,\ul0\nosupersub\cf19\f20\fs18 254\ul0\
nosupersub\cf13\f14\fs18 , 270-274.\par\pard\ql \li956\sb1\sl-199\slmult0 \up0 \
expndtw-3\charscalex100 Macaya, R. F., Schultze, P. & Feigon, J. (1992a).
Sugar\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100
conformations in intramolecular DNA triplexes\par\pard\ql \li1314\sb0\sl-
199\slmult0 \up0 \expndtw-1\charscalex100 determined by coupling constants
obtained by\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100
automated simulation of P.COSY crosspeaks.\ul0\nosupersub\cf14\f15\fs18 J. Am.\
par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex103 Chem. Soc.\ul0\
nosupersub\cf19\f20\fs18 114\ul0\nosupersub\cf13\f14\fs18 , 781-783.\par\pard\ql \
li956\sb1\sl-199\slmult0 \up0 \expndtw-3\charscalex100 Macaya, R. F., Wang, E.,
Schultze, P., Sklena�\u345?, V. & Feigon,\par\pard\ql \li1314\sb0\sl-199\slmult0 \
up0 \expndtw-2\charscalex100 J. \up0 \expndtw0\charscalex100 (1992b). Proton NMR
assignments and structural\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-3\
charscalex100 characterization of an intramolecular DNA triplex.\par\pard\ql \
li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex104 \ul0\nosupersub\cf14\f15\
fs18 J. Mol. Biol.\ul0\nosupersub\cf19\f20\fs18 225\ul0\nosupersub\cf13\f14\fs18 ,
755-773.\par\pard\ql \li956\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100
Macura, S. & Ernst, R. R. (1980). Elucidation of cross\par\pard\ql \
li1314\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex100 relaxation in liquids by
two-dimensional N.M.R.\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex100 spectroscopy.\ul0\nosupersub\cf14\f15\fs18 Mol. Phys.\ul0\
nosupersub\cf19\f20\fs18 41\ul0\nosupersub\cf13\f14\fs18 , 95-117.\par\pard\ql \
li956\sb0\sl-199\slmult0 \up0
\expndtw0\charscalex104 Maher, L. J. \up0 \expndtw0\charscalex100 (1992). DNA
triple-helix formation\u8212?an\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex102 approach to artificial gene repressors.\ul0\nosupersub\
cf14\f15\fs18 BioEssays\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex102 \ul0\nosupersub\cf19\f20\fs18 14\ul0\nosupersub\cf13\f14\fs18 (12),
807-815.\par\pard\ql \li956\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex109 Marion,
D. & Bax, A. \up0 \expndtw0\charscalex101 (1988). P.COSY, a sensitive\par\
pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100 alternative for
double-quantum-filtered COSY.\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex103 \ul0\nosupersub\cf14\f15\fs18 J. Magn. Reson.\ul0\
nosupersub\cf19\f20\fs18 80\ul0\nosupersub\cf13\f14\fs18 , 528-533.\par\pard\
column \ql \li5856\sb0\sl-207\slmult0 \par\pard\ql \li5856\sb0\sl-207\slmult0 \par\
pard\ql \li20\sb32\sl-207\slmult0 \up0 \expndtw-1\charscalex100 Marion, D., Ikura,
M. & Bax, A. (1989). Improved solvent\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex101 suppression in one- and two-dimensional NMR\par\pard\ql
\li379\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 spectra by convolution of
time-domain data.\ul0\nosupersub\cf14\f15\fs18 J. Magn.\par\pard\ql \li379\sb0\sl-
199\slmult0 \up0 \expndtw0\charscalex103 Res.\ul0\nosupersub\cf19\f20\fs18 84\ul0\
nosupersub\cf13\f14\fs18 , 425-430.\par\pard\ql \li20\sb0\sl-199\slmult0 \up0 \
expndtw-2\charscalex100 Mergny, J.-L., Sun, J.-S., Rouge�e, M., Montenay-
Garestier,\par\pard\ql \li3363\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex101 `ne,
C. \up0 \expndtw-2\charscalex100 (1991).\par\pard\ql \li379\sb1\sl-199\slmult0 \up0
\expndtw-1\charscalex100 Sequence specificity in triple-helix formation: exper-\
par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex104 imental and
theoretical studies of the effect of\par\pard\ql \li379\sb0\sl-199\slmult0 \
up0 \expndtw0\charscalex100 mismatches on triplex stability.\ul0\nosupersub\
cf14\f15\fs18 Biochemistry, \up0 \expndtw-2\charscalex100 \ul0\nosupersub\cf19\
f20\fs18 30\ul0\nosupersub\cf13\f14\fs18 ,\par\pard\ql \li379\sb0\sl-199\slmult0 \
up0 \expndtw0\charscalex101 9791-9798.\par\pard\ql \li20\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex103 Moser, H. E. & Dervan, P. B. (1987). Sequence-specific\par\
pard\ql \li379\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex102 cleavage of double
helical DNA by triple helix\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex101 formation.\ul0\nosupersub\cf14\f15\fs18 Science,\ul0\
nosupersub\cf19\f20\fs18 238\ul0\nosupersub\cf13\f14\fs18 , 645-650.\par\pard\ql \
li20\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 Mueller, L. \up0 \expndtw-1\
charscalex100 (1987). P.E.COSY, a simple alternative to\par\pard\ql \li379\
sb0\sl-199\slmult0 \up0 \expndtw0\charscalex101 E.COSY.\ul0\nosupersub\cf14\f15\
fs18 J. Magn. Reson.\ul0\nosupersub\cf19\f20\fs18 72\ul0\nosupersub\cf13\f14\fs18
, 191-196.\par\pard\ql \li20\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102
Olivas, W. M. & Maher, L. J. (1994). Analysis of duplex\par\pard\ql \li379\sb1\sl-
199\slmult0 \up0 \expndtw-1\charscalex100 DNA by triple helix formation\
u8212?application to\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw-2\
charscalex100 detection of a P53 microdeletion.\ul0\nosupersub\cf14\f15\fs18
Biotechniques,\ul0\nosupersub\cf19\f20\fs18 16\ul0\nosupersub\cf13\f14\fs18 (1),\
par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 128-132.\par\
pard\ql \li20\sb0\sl-199\slmult0 \up0 \expndtw-1\charscalex100 Radhakrishnan, I.
& Patel, D. J. (1992). Solution con-\par\pard\ql \li379\sb0\sl-199\slmult0 \
up0 \expndtw0\charscalex100 formation of a G�TA triple in an intramolecular\
par\pard\ql \li379\sb1\sl-199\slmult0 \up0 \expndtw-2\charscalex100
pyrimidine�purine�pyrimidine DNA triplex.\ul0\nosupersub\cf14\f15\fs18 J. Am.\
par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 Chem. Soc.\ul0\
nosupersub\cf19\f20\fs18 114\ul0\nosupersub\cf13\f14\fs18 (17), 6913-6915.\par\
pard\ql \li20\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 Radhakrishnan, I.
& Patel, D. J. \up0 \expndtw-2\charscalex100 (1994a). Solution\par\pard\
ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 structure and
hydration patterns of a pyrim-\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \
expndtw-2\charscalex100 idine�purine�pyrimidine DNA triplex containing a\par\
pard\ql \li20\ri1643\sb1\sl-199\slmult0\fi358 \up0 \expndtw0\charscalex102 novel
T�CG base-triple.\ul0\nosupersub\cf14\f15\fs18 J. Mol. Biol.\ul0\nosupersub\cf19\
f20\fs18 241\ul0\nosupersub\cf13\f14\fs18 , 600-619. \line \up0 \expndtw-3\
charscalex100 Radhakrishnan, I. & Patel, D. J. (1994b). Solution structure\par\
pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex103 of a
pyrimidine�purine�pyrimidine DNA triplex\par\pard\ql \li379\sb0\sl-199\slmult0 \
up0 \expndtw-3\charscalex100 containing T�AT, C\ul0\super\cf8\f9\fs16 +\ul0\
nosupersub\cf13\f14\fs18 �GC and G�TA triples.\ul0\nosupersub\cf14\f15\fs18
Structure,\ul0\nosupersub\cf19\f20\fs18 2\ul0\nosupersub\cf13\f14\fs18 ,\par\pard\
ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex103 17-32.\par\pard\ql \li20\
sb1\sl-199\slmult0 \up0 \expndtw0\charscalex100 Radhakrishnan, I., de los Santos,
C. & Patel, D. J. (1991).\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw-1\
charscalex100 Nuclear magnetic resonance structural studies of\par\pard\ql \
li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 intramolecular
purine�purine�pyrimidine DNA\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex100 triplexes in solution. Base triple pairing alignments\par\
pard\ql \li20\ri1643\sb0\sl-199\slmult0\fi358 \up0 \expndtw0\charscalex102 and
strand direction.\ul0\nosupersub\cf14\f15\fs18 J. Mol. Biol.\ul0\nosupersub\cf19\
f20\fs18 221\ul0\nosupersub\cf13\f14\fs18 , 1403-1418. \up0 \expndtw0\
charscalex101 Rajagopal, P. & Feigon, J. \up0 \expndtw0\charscalex102 (1989a).
NMR studies of\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex101
triple-strand formation from the homopurine-\par\pard\ql \li379\sb13\sl-
207\slmult0 \up0 \expndtw-3\charscalex100 homopyrimidine deoxyribonucleotides
d(GA)\ul0\nosupersub\cf8\f9\fs11 4\ul0\nosupersub\cf13\f14\fs18 and\par\pard\
ql \li379\sb1\sl-197\slmult0 \up0 \expndtw0\charscalex100 d(TC)\ul0\nosupersub\cf8\
f9\fs11 4\ul0\nosupersub\cf13\f14\fs18 .\ul0\nosupersub\cf14\f15\fs18
Biochemistry,\ul0\nosupersub\cf19\f20\fs18 28\ul0\nosupersub\cf13\f14\fs18 , 7859-
7870.\par\pard\ql \li20\sb1\sl-176\slmult0 \up0 \expndtw-3\charscalex100 Rajagopal,
P. & Feigon, J. (1989b). Triple strand formation\par\pard\ql \li379\sb5\sl-199\
slmult0 \up0 \expndtw0\charscalex100 in the homopurine:homopyrimidine DNA oligonu-\
par\pard\qj \li20\ri1643\sb35\sl-180\slmult0\fi358 \up0 \expndtw-1\charscalex100
cleotides d(GA)\ul0\nosupersub\cf8\f9\fs11 4\ul0\nosupersub\cf13\f14\fs18 and
d(TC)\ul0\nosupersub\cf8\f9\fs11 4\ul0\nosupersub\cf13\f14\fs18 .\ul0\nosupersub\
cf14\f15\fs18 Nature,\ul0\nosupersub\cf19\f20\fs18 339\ul0\nosupersub\cf13\f14\
fs18 , 637-640. \line \up0 \expndtw0\charscalex101 Roberts, R. W. & Crothers, D. M.
(1991). Specificity and\par\pard\ql \li379\sb4\sl-199\slmult0 \up0 \expndtw-2\
charscalex100 stringency in DNA triplex formation.\ul0\nosupersub\cf14\f15\fs18
Proc. Natl Acad.\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex103
Sci. USA,\ul0\nosupersub\cf19\f20\fs18 88\ul0\nosupersub\cf13\f14\fs18 , 9397-
9401.\par\pard\ql \li20\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex101 Roongta, V.
A., Jones, C. R. & Gorenstein, D. G. (1990).\par\pard\ql \li379\sb0\sl-199\slmult0
\up0 \expndtw-3\charscalex100 Effect of distortions in the deoxyribose
phosphate\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100
backbone conformation of duplex oligodeoxyribonu-\par\pard\ql \li379\sb0\sl-199\
slmult0 \up0 \expndtw-4\charscalex100 cleotide dodecamers containing GT, GG, GA,
AC, and\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex101 GU
base-pair mismatches on \up0 \expndtw0\charscalex103 \ul0\super\cf8\f9\fs16 31\
ul0\nosupersub\cf13\f14\fs18 P NMR spectra.\par\pard\ql \li379\sb1\sl-199\slmult0
\up0 \expndtw0\charscalex100 \ul0\nosupersub\cf14\f15\fs18 Biochemistry,\ul0\
nosupersub\cf19\f20\fs18 29\ul0\nosupersub\cf13\f14\fs18 , 5245-5258.\par\pard\
ql \li20\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 Saenger, W. (1984).\
ul0\nosupersub\cf14\f15\fs18 Principles of Nucleic Acid Structure\ul0\
nosupersub\cf13\f14\fs18 ,\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw-3\
charscalex100 Springer-Verlag, New York.\par\pard\ql \li20\sb0\sl-199\slmult0 \
up0 \expndtw-2\charscalex100 Sklena�\u345?, V. & Bax, A. (1987). Spin-echo water
suppression\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 for
the generation of pure-phase two-dimensional\par\pard\ql \li20\ri1643\sb1\sl-
199\slmult0\fi358 \up0 \expndtw0\charscalex102 NMR spectra.\ul0\nosupersub\cf14\
f15\fs18 J. Magn. Reson.\ul0\nosupersub\cf19\f20\fs18 74\ul0\nosupersub\cf13\f14\
fs18 , 469-479. \up0 \expndtw-1\charscalex100 Sklena�\u345?, V. & Feigon, J. \
up0 \expndtw-2\charscalex100 (1990). Formation of a stable\par\pard\ql \li379\
sb0\sl-199\slmult0 \up0 \expndtw0\charscalex103 triplex from a single DNA
strand.\ul0\nosupersub\cf14\f15\fs18 Nature, \up0 \expndtw-2\charscalex100 \ul0\
nosupersub\cf19\f20\fs18 345\ul0\nosupersub\cf13\f14\fs18 ,\par\pard\ql \li379\sb0\
sl-199\slmult0 \up0 \expndtw0\charscalex102 836-838.\par\pard\ql \li20\sb0\sl-199\
slmult0 \up0 \expndtw0\charscalex103 States, D. J., Haberkorn, R. A. & Ruben, D.
J. (1982). A\par\pard\ql \li379\sb1\sl-199\slmult0 \up0 \expndtw0\charscalex100
two-dimensional nuclear Overhauser experiment\par\pard\ql \li379\sb0\sl-199\
slmult0 \up0 \expndtw0\charscalex103 with pure absorption phase in four
quadrants.\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex103 \ul0\
nosupersub\cf14\f15\fs18 J. Magn. Res.\ul0\nosupersub\cf19\f20\fs18 48\ul0\
nosupersub\cf13\f14\fs18 , 286-292.\par\pard\ql \li20\sb0\sl-199\slmult0 \up0 \
expndtw-3\charscalex100 Strobel, S. A. & Dervan, P. B. (1991). Single-site
enzymatic\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100
cleavage of yeast genomic DNA mediated by triple\par\pard\ql \li379\sb1\sl-199\
slmult0 \up0 \expndtw0\charscalex101 helix formation.\ul0\nosupersub\cf14\f15\fs18
Nature,\ul0\nosupersub\cf19\f20\fs18 350\ul0\nosupersub\cf13\f14\fs18 , 172-174.\
par\pard\ql \li20\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 Strobel, S. A.,
Doucette-Stamm, L. A., Riba, L., Housman,\par\pard\ql \li379\sb0\sl-199\slmult0 \
up0 \expndtw-1\charscalex100 D. E. & Dervan, P. B. (1991). Site-specific cleavage
of

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{\shp {\*\shpinst\shpleft816\shptop1617\shpright3457\shpbottom1996\shpfhdr0\
shpbxpage\shpbypage\shpwr3\shpwrk0\shpfblwtxt1\shpz10001\shplid10001
{\sp{\sn shapeType}{\sv 202}}{\sp{\sn fFlipH}{\sv 0}}{\sp{\sn fFlipV}{\sv 0}}{\sp{\
sn fRecolorFillAsPicture}{\sv 0}}{\sp{\sn fUseShapeAnchor}{\sv 0}}{\sp{\sn fLine}{\
sv 0}}{\sp{\sn fFilled}{\sv 0}}{\sp{\sn fLayoutInCell}{\sv 1}}{\sp{\sn
fBehindDocument}{\sv 1}}{\shptxt\pard\plain \qj\sl132 \li0\ri0 \expndtw0\
charscalex106\ul0\nosupersub\cf13\f14\fs18 Sun, J.-S. & He�le{\par}}}}\pard\sb0\sl-
240{\bkmkstart Pg18}{\bkmkend Pg18}\par\pard\li956\sb0\sl-218\slmult0\par\pard\
li956\sb151\sl-218\slmult0\fi0\tx9955 \up0 \expndtw-1\charscalex100 \ul0\
nosupersub\cf1\f2\fs18 Solution Structure of a D\ul0\nosupersub\cf21\f22\fs10 3\
ul0\nosupersub\cf1\f2\fs18 -containing DNA Triplex\tab \up0 \expndtw-1\
charscalex100 \ul0\nosupersub\cf22\f23\fs20 1069\par\pard\sect\sectd\sbknone\cols2\
colno1\colw5696\colsr160\colno2\colw6244\colsr160\ql \li956\sb0\sl-207\slmult0 \
par\pard\ql \li956\sb0\sl-207\slmult0 \par\pard\ql \li1314\sb6\sl-207\slmult0\
tx3406 \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf13\f14\fs18 human chromosome
\up0 \expndtw-2\charscalex100 4\tab \up0 \expndtw0\charscalex101 mediated by
triple-helix\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100
formation.\ul0\nosupersub\cf14\f15\fs18 Science,\ul0\nosupersub\cf19\f20\fs18
254\ul0\nosupersub\cf13\f14\fs18 , 1639-1642.\par\pard\ql \li2288\sb0\sl-199\
slmult0 \up0 \expndtw-1\charscalex100 `ne, C. (1993). Oligonucleotide-directed\
par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 triple-helix
formation.\ul0\nosupersub\cf14\f15\fs18 Curr. Opin. Struct. Biol. \up0 \
expndtw-2\charscalex100 \ul0\nosupersub\cf19\f20\fs18 3\ul0\nosupersub\cf13\f14\
fs18 ,\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 345-
356.\par\pard\ql \li956\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex105 Wang, E.,
Malek, S. & Feigon, J. (1992). Structure of a\par\pard\ql \li1314\sb1\sl-199\
slmult0 \up0 \expndtw0\charscalex101 G�T�A triplet in an intramolecular DNA
triplex.\par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 \ul0\
nosupersub\cf14\f15\fs18 Biochemistry,\ul0\nosupersub\cf19\f20\fs18 31\ul0\
nosupersub\cf13\f14\fs18 , 4838-4846.\par\pard\ql \li956\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex100 Wells, R. D., Collier, D. A., Hanvey, J. C., Shimizu, M. &\
par\pard\ql \li1314\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 Wohlrab, F.
(1988). The chemistry and biology of\par\pard\ql \li1314\sb0\sl-199\slmult0 \
up0 \expndtw-1\charscalex100 unusual DNA structures adopted by oligopurine\
par\pard\ql \li1314\sb1\sl-199\slmult0 \up0 \expndtw-2\charscalex100 and
oligopyrimidine sequences.\ul0\nosupersub\cf14\f15\fs18 FASEB J.\ul0\
nosupersub\cf19\f20\fs18 2\ul0\nosupersub\cf13\f14\fs18 , 2939-\par\pard\ql \
li1314\sb0\sl-199\slmult0 \up0 \expndtw-2\charscalex100 2949.\par\pard\column \ql \
li5856\sb0\sl-207\slmult0 \par\pard\ql \li5856\sb0\sl-207\slmult0 \par\pard\ql \
li20\sb6\sl-207\slmult0 \up0 \expndtw-3\charscalex100 Yip, P. & Case, D. A. (1989).
A new method for refinement\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex103 of macromolecular structures based on nuclear\par\pard\ql \
li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex100 Overhauser effect
spectra.\ul0\nosupersub\cf14\f15\fs18 J. Magn. Reson. \up0 \expndtw-2\
charscalex100 \ul0\nosupersub\cf19\f20\fs18 83\ul0\nosupersub\cf13\f14\fs18 ,\par\
pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 643-648.\par\pard\ql
\li20\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 Yoon, K., Hobbs, C. A., Koch,
J., Sardaro, M., Kutny, R.\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw0\
charscalex103 & Weis, A. L. (1992). Elucidation of the sequence-\par\pard\ql \
li379\sb1\sl-199\slmult0 \up0 \expndtw-1\charscalex100 specific third strand
recognition of four Watson-\par\pard\ql \li379\sb0\sl-199\slmult0 \up0 \
expndtw0\charscalex102 Crick base-pairs in a pyrimidine triple-helix motif:\par\
pard\ql \li379\sb0\sl-199\slmult0 \up0 \expndtw-3\charscalex100 T�AT, C�GC, T�CG
and G�TA.\ul0\nosupersub\cf14\f15\fs18 Proc. Natl Acad. Sci.\par\pard\ql \
li379\sb0\sl-199\slmult0 \up0 \expndtw0\charscalex102 USA,\ul0\nosupersub\cf19\f20\
fs18 89\ul0\nosupersub\cf13\f14\fs18 , 3840-3844.\par\pard\ql \li20\sb0\sl-199\
slmult0 \up0 \expndtw-1\charscalex100 Zhu, L., Reid, B. R., Kennedy, M. & Drobny,
G. P. (1994).\par\pard\ql \li379\sb1\sl-199\slmult0 \up0 \expndtw-4\charscalex100
Modulation of J couplings by cross relaxation in DNA\par\pard\ql \li379\sb0\sl-199\
slmult0 \up0 \expndtw0\charscalex103 sugars.\ul0\nosupersub\cf14\f15\fs18 J. Magn.
Res. ser. A,\ul0\nosupersub\cf19\f20\fs18 111\ul0\nosupersub\cf13\f14\fs18 , 195-
202.\par\pard\ql \li8355\sb0\sl-230\slmult0 \par\pard\ql \li2519\sb44\sl-230\
slmult0 \up0 \expndtw0\charscalex100 \ul0\nosupersub\cf31\f32\fs20 Edited by P. E.
Wright \par\pard\sect\sectd\sbknone \ql \li2071\sb0\sl-230\slmult0 \par\pard\ql\
li2071\sb0\sl-230\slmult0 \par\pard\ql\li2071\sb4\sl-230\slmult0 \up0 \expndtw0\
charscalex103 \ul0\nosupersub\cf9\f10\fs20 (Received 21 November 1995; received in
revised form 17 January 1996; accepted 22 January 1996)

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