Properties of Bi2Te3Sb2Te3 Alloys

Mac J. Smith, R. J. Knight, and C. W. Spencer

Citation: J. Appl. Phys. 33, 2186 (1962); doi: 10.1063/1.1728925

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21R6 S. MENDELSON

"Joffe effect." This leads to greater multiplication on
neighboring slip planes and more homogeneous flow at
low stresses. Greater stn:ngth is then attributed to the
resulting higher dislocation density. This also suggests a
mechanism to account for the brittle nature of these
crystals (i.e., when cross-slip is easy the material is
ductile and vice versa) and might explain the sensitivity
of these crystals to deformation rate.
When a screw dislocation intersects the surface at an
oblique angle it can cross-slip under the image force
until it is normal to the surface. This force is usually
very small and cannot in itself account for the observed
cross-slip. Cross-slip is opposed by the lattice resistance
and to some extent by the energy required to form the
surface step after the screw cross-slips.n It is aided, on
17 J. J. Gilman, Phil. Mag. 6, 159 (1961).
the other hand, by the resulting reduction in dislocation
length and quite signiflCantly by the repulsive stresses
from other screws in the slip plane. It is not clear how
water manifests itself in assisting cross-slip. It might
enhance the glide of edges, lying below the surface, out
of the crystal and thus leave the ends of screws free to
cross-slip.
ACKNOWLEDGMENTS
The author wishes to thank Dr. E. S. Machlin of
Columbia University for helpful advise given during
this study. Gratitude is also expressed to Dr. A. S.
Nowick of the IBM Research Center, Yorktown
Heights, New York, and Dr. W. G. Johnston of the
General Electric Research Laboratories, Schenectady,
New York, for their advice and interest in this work.

JOURNAL OF APPLIED PHYSICS VOLUME 33, N1TMBER 7 JPLY 1962

MAC J. SMITH,· R. J. KNIGHT,t AND C. W. SPENCER

School of Chemical and Metallurgical Engineering, Cornell University, Ithaca, New York
(Received January 22, 1962)

The phase diagram for the Bi,Tea-Sb,Tea pseudo-binary system is of the solid-solution type, where the
distribution coefficient k is equal to unity at 33.3 and 66.7 mole % Sb,Tea. The c lattice parameter remains
essentially constant across the diagram at 30.49 A for both slowly crystallized and quenched alloys. For
quenched alloys the a lattice parameter decreases almost linearly, from a value of 4.487 A, for pure Bi,Tea,
to a value of 4.275 A, for pure Sb,Tea; however, a significant contraction from linear variation is found in
slowly crystallized materials. EG diminishes in an essentially linear fashion from 0.16 eV, for pure Bi,Tea,
to 0.12 eVat 24.2 mole % Sb,Tea in both slowly crystallized and quenched materials. EG remains approxi-
mately constant from 24.2 to 66.7 mole % Sb,Tea for slowly crystallized materials but continues to drop
for quenched materials.

INTRODUCTION these alloys, report a maximum in hole mobilities in the

T HERE is considerable evidence to indicate that
several of the properties of Bi2Tea-Sb2Tea alloys
vary in an irregular manner across the alloy system. 1- 10
Kokosh and Sinani,l in a study of sintered specimens of
* Presently with Oak Ridge National Laboratory, Oak Ridge,
Tennessee.
t Presently with Ronson Metals Corporation, Newark, New
Jersey.
1 G. V. Kokosh and S. S. Sinani, Soviet Phys.-Solid State 2
1012 (1960).
'U. Berkholtz, Z. Naturforsch. 13a, 780 (1958).
a 1. R. Testardi and J. R. Wiese, Trans. Met. Soc. AIME 221,
647 (1961).
4 J. R. Wies.e and Richard Pyle, J. Metals 12, 715-754 (1960),
the Fall Meetmg of the Metallurgical Society.
5 F. D. Rosi, B. Abeles, and R. V. Jengen, J. Phys. Chern. Solids
10, 191 (1959).
• S. V. Airapetiants and B. A. Efimova, Zhur. Tekh. Fiz. 28
1768 (1958).
7 G. E. Smith and R. Wolfe, Bull. Am. Phys. Soc. 6, 137 (1961).
8 D. A. Wright, Nature 181, 834 (1958).
91. Terarnoto and S. Takayanagi, J. Phys. Chern. Solids 19
124 (1961).
10 G. J. Cosgrove, J. P. McHugh, and W. A. Tiller, J. Appl.
Phys. 32, 621 (1961).
vicinity of both 33.3 and 66.7 mole % Sb 2Tea. As a con-
sequence, these authors suggest that ordering occurs at
these two compositions in the system. Birkholtz2 inves-
tigated properties of single crystals of the alloys which
had been grown in a Bridgman furnace at a rate of
1 mm min-I, and reported a maximum of mobility
values near 33.3 mole % Sb 2Tea and a minimum in these
values near 66.7 mole % Sb 2Tea.
Testardi and Wiese,a in a study of the densities of
' zone-leveled crystals and of quenched ingots, find a
gentle peaking of densities at compositions in the vicin-
ity of 33.3 and 66.7 mole % Sb2Tea for the zone-leveled
material, but not for the quenched material. Cosgrove
et al.l° report that as the growth rate increases for
BiSbTea, doped with 0.56 wt % Se, the resistivity
increases, the Seebeck effect decreases, and the lattice
'
thermal conductivity increases. These effects are pri-
marily attributed to the variation in the degree of
microsegregation produced in the crystals as a function
'
of freezing conditions. Wiese and Pyle4 report that the
pseudo-binary phase diagram for the system is of the

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 PROPERTIES OF
solid-solution type, where the liquidus and solidus
curves across the system are nearly congruent. How-
ever, Rosi et al. S find a change in sign of the distribution
coefficient k in the interior of the phase diagram for
materials grown at a rate of 6 mm h-1 and attribute
this phenomenon to a minimum in the solid solubility
curve in the vicinity of 30% Sb 2Te3.
Rosi et al. s have inferred that the energy bandgap
decreases as Sb 2Te3 is alloyed into Bi2Te3, since the
intrinsic resistivity decreases with increasing Sb 2Te3
content. Testardi and Wiese3 have observed minima in
values of thermal energy gaps at 33.3 and 66.7%
Sb 2Te3 and attribute this to a tighter packing of atoms
in ordered alloys. Airapetiants and Efimova 6 postulate
an overlap of the conduction and valence band in
Sb2Te3, resulting in an apparent bandgap of zero for the
terminal compound. Their postulation, however, does
not agree with the values of the optical energy gap
0.30 eV reported by Black et al.H for Sb 2Te3.
The purpose of this paper is to report the results of a
study of the phase equilibrium and crystallographic
relationships in the pseudo-binary alloy system,
Bi2Te3-Sb2Te3, and to report and discuss certain
electrical properties of this system. A comparison is
made between the properties of alloys in the system and
those of the Bi 2Te3 - Bi 2Se3 system.
PREPARATION OF SPECIMENS
Alloys were prepared from 99.999% pure antimony,
bismuth, and tellurium obtained from the American
Smelting and Refining Company. Thirty gram samples
of the correct composition ratios were weighed to an
accuracy of ± 1 X 10-4 g. Individual alloys were sealed
in 9-mm i.d. Vycor tubes while under a vacuum of
approximately 10-5 mm Hg. Capsules containing the
alloys were held above their melting point in a Bridgman
furnace for 24 h in order to provide thorough mixing
of the liquid. Three methods of specimen preparation
were used: (1) capsules were withdrawn from the fur-
nace and water-quenched; (2) capsules were dropped at
a rate of 1.4 mm h-1; (3) capsules were dropped at a
rate of 0.25 mm h-1. Single-crystal specimens were
usually obtained in the latter two instances, although
frequently the ends of the ingot were polycrystalline.
EXPERIMENTAL TECHNIQUES
Chemical composition of specimens and distribution
coefficients k for the system were obtained using the
x-ray fluorescence technique. 12- 14 The distribution co-
efficient k is defined as the ratio of composition of the
Ii J. Black, E. Conwell, L. Seigle, and C. W. Spencer, J. Phys.
Chem. Solids 2, 240 (1957).
12 W. G. Pfann, Zone Melting (John Wiley & Sons, Inc., New
York, 1958).
13 L. Von Hamos, Arikiv Matematik, Astronomi, Ock Fysik
31a, No. 25 (1945).
14 L. S. Birks, X -ray Spectrochemical Analysis (Interscience
Publishers, Inc., New York, 1959).
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Bi2Tea-Sh2Te3 ALLOYS 21~i
solid to composition of the liquid. Standard alloy com-
positions were prepared for x-ray fluorescence analysis
by weighing out mixtures of the constituent elements at
intervals of 10 mole % Sb 2Te:l. These mixtures were
then melted, quenched, and powdered.
Inverse heating rates and specific heats were obtained
by constant-input calorimetric techniques. ls Lattice
parameters and relative line intensities were measured
on quenched and slowly crystallized specimens across
the pseudo-binary diagram by the Debye-Scherrer
powder method.!" Resistivity, number of extrinsic cur-
rent carriers, and hole mobility were determined
parallel to the cleavage planes as a function of tempera-
ture by standard techniques. Thermal energy gaps for
the system were calculated from the resistivity vs tem-
perature data. In order to obtain electrical measure-
ments up to the melting point of the materials, the
specimen and associated electrical leads were enclosed
in a N onex glass container under a vacuum of approxi-
mately 10-5 mm HgP Lattice thermal conductivity
was determined for 33.3 and 66.7% Sb2Te3 alloys by
employing the method of Pinnow et al. 18 This method
makes use of the thermoelectric effect to obtain thermal
diffusivity, from which thermal conductivity is sepa-
rated by an independent determination of specific heat
and density. Since all alloys are essentially degenerate,
lattice thermal conductivity can then be approximated
by subtracting the electronic contribution from the
value of total thermal conductivity.s The Wiedemann-
Franz law was used to approximate the electronic con-
tribution to thermal conductivity.
EXPERIMENTAL RESULTS
Phase Diagram
A phase diagram for the Bi2Te3-Sb2Te3 pseudo-
binary system has been determined using thermal
analysis to establish the temperatures of the liquidus
and solidus curves and x-ray fluorescence to establish
distribution coefficients. That the system is in fact
pseudo-binary has been confirmed, since the mole frac-
tion of tellurium remains constant at all compositions.
When ingot crystallization rates (drop rates) are
0.25 mm h-1 or less, alloys containing 33.3 and 66.7
mole % Sb 2Te3 exhibit distribution coefficients equal to
unity. Furthermore, thermal analysis indicates that the
liquidus and solidus temperatures coincide for these
alloys. All distribution coefficients in the composition
range of 0 to 33.3, 33.3 to 66.7, and 66.7 to 100 mole %
Sb 2Te3 are found to be greater than unity for alloys
crystallized at a rate of 0.25 mm h- I . Table I lists com-
,. c. S. Smith, "Metals Technology," AIME Tech. Pub.
No. 1100.
16 B. D. Cullitz, X-ray Diffraction (Addison-Wesley Publishing
Company, Inc., Reading, Massachusetts, 1956).
17 M. J. Smith, E. S. Kirk, and C. W. Spencer, J. Appl. Phys.
31. 1504 (1960).
18 D. Pinnow, C. Y. Li, and C. W. Spencer, Rev. Sci. Instr. 32,
1417 (1961).
2188 SMITH, KNIGHT, AND SPENCER

TABLE I. Distribution coefficients, liquidus temperatures, and

solidus temperatures for alloys crystallized at a rate of 0.25 mm
h- I .
- -
- ~----~. _._.- --- ".------

Liquid Solid
composition composition J)istribution Solidus Liquidus
in mole % in mole % coefficient k temperature temperature
Sb,Tea Sb,Te. (C,(CI) in °C in °C

0 0 587 587
20 24.2 1.21
25 28.9 1.15
33.3 33.3 1.00 598
45 52.5 1.16
48 55.0 1.14
50 53.9 1.07 601 603
60 602 602
66.7 66.7 1.00 609
70 610 613
80 82.8 1.03
90 90.5 1.00
100 100 1 617 617
FIG. 2. Lattice parameters for quenched and powdered poly-
crystalline alloys and for powdered, single-crystal material grown
at a rate of 0.25 mm h- I .
positions, distribution coefficients, and melting points
for several slowly crystallized alloys. A phase diagram A small heat effect is observed at 419°±2°C in all
that agrees with this information is presented in rapidly solidified alloys. The effect is observed on both
Fig. l. heating and cooling and is largest near the center of the
Crystallization rate significantly influences the appar- diagram. It is not observed in the terminal components
ent positions of the liquidus and solidus curves in the and disappears in all the alloys when the crystallization
composition range of 33.3 to 66.7 mole % Sb 2Teg, and rate is less than 0.1 mm h-1. A reappearance of the heat
in some instances the results are in marked disagree- effect, however, is noted when a once slowly crystallized
ment with the phase diagram shown in Fig. 1. For material is melted and allowed to resolidify rapidly.
example, thermal analysis indicates that at fast growth
rates a temperature difference tlT appears between the X-Ray Diffraction
liquidus and solidus of the 66.7 mole % Sb 2Teg alloy and
that the magnitude of this temperature difference is Values for the a and c lattice parameters for alloys
directly related to the crystallization rate. At crystalli- across the pseudo-binary diagram were determined
zation rates of approximately 5 mm h-1 and 0.25 using the Debye-Scherrer powder method16 and are
mm h-t, the solid that initially crystallizes from a recorded in Fig. 2. Alloys were indexed in the manner
liquid composition of 50.0 mole % Sb 2Teg contains 53.9 described by Francombe/9 where a hexagonal unit cell
mole % Sb 2Teg, indicating a distribution coefficient was used to represent the structure. The basal lattice
greater than one. However, at an intermediate crystalli- parameter c remains unchanged under all conditions
zation rate of 1 mm h-1, the same alloy yields an initial studied. The axial lattice parameter a, however, de-
solid of 47.0 mole % Sb 2Teg, indicating a distribution creases in dimension from Bi2Teg to Sb 2Teg. Lattice
coefficient less than one. It is presumed that distribution parameters of quenched materials vary linearly from 0
coefficient data obtained from ingots solidified at 1 mm to 80% Sb 2Teg. The a parameter for single crystals,
h-1 would indicate a phase diagram, probably meta- grown at the rate of 0.25 mm h-t, exhibits disconti-
stable, with a local congruent minimum at approxi- nuities in slope near 33.3 and 66.7 mole % Sb2Tea, but
mately 596°C and 60 mole % Sb2Tea. varies approximately linearly over composition ranges
between these points. Qualitatively, these results show
the same trends as those of Birkholtz,2 although there
620
(617)
are significant differences in absolute values between the
615
two sets of data. The lattice parameters of the terminal
compound BhTea agree very closely with the values
610 determined by Francombe,19 and values for Sb 2Teg are
in fair agreement with those reported by Donges et al. 20
~605
For poth the quenched and slowly crystallized
.a.. 60
.!:
materials, additional lines appear over those observed
~ in the pure components Bi2Tea and Sb 2Te3. In one
~595 instance an additional peak appeared in the diffractom-
~ eter recording of a Debye-Scherrer x-ray diffraction
590
pattern of a slowly crystallized 66.7% Sb 2Te3 alloy,
10 20 30 '10 50 60 70 80 90 100
which did not appear in this alloy in the quenched con-
Mole Percent 5b 2 Te 3
19 M. H. Francombe, Brit. J. App!. Phys. 9, 145 (1958).
FIG. 1. Bi.Tea-Sb.Te3 pseudo-binary phase diagram. 20 E. Donges, Z. anorg. u. allgem. Chern. 265, 56 (1951).

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 2189

dition. This line wastentatively indexed as correspond-

ing to the (106) plane in the hexagonal lattice.

Electrical Properties
Resistivity vs temperature data taken on single
crystals of several alloys solidified at 1.4 and 0.25
mm h-1 are shown in Figs. 3(a) and 3(b), respectively.
Thermal energy gaps, which have a value of 0.10 eV or
greater, as determined from the slope of the intrinsic
E
(,)
portions of these curves, are plotted in Fig. 4 as a func-
I tion of composition. Introduction of Sb 2Te3 into Bi2Te3
oS was found to diminish the thermal energy gap, in
III
o qualitative agreement with earlier statements by Rosi
Xg
et al. 5 and Testardi and Wiese. 3The curve for the rapidly
>. crystallized alloys is approximately linear and extra-
=i 8 polates to a value of approximately zero for pure Sb 2Te3.
:;7 I/)
It is interesting to note that apparent energy gaps,
taken from the slopes of intrinsic portions of the resis-
CI)
a:6 tivity curves, for the more rapidly crystallized alloys
containing 41.40, 54.75, and 66.7 mole % Sb 2Te3 fall
5. very close to this straight line extrapolation. These
points are not plotted as they do not have precise
quantitative significance; usual approximate solutions
1.4 1.8 3.0 3.4 to Fermi-Dirac statistics are not applicable for these
(a)
small energy gaps.
Several physical and electrical properties of alloys
containing 33.3 and 66.7 mole % Sb2Te3 are compared
3 ,- . --..... with those of the terminal compounds in Table II. The
. ....~
/
mobility temperature variation of both alloys ap-
,,( .",a_a'D~
proaches a T-2 law in the temperature range from room

I'
. ~/'r;,r--...;;.. ,-...... .~
..
.. a,riD
I._.~ a
temperature to the onset of intrinsic conduction.

:o.-..~/;!\ ""'\\ ~.
2
DISCUSSION
......
E ~~ . ~ Rapid solidification causes the formation of meta-
(,)

c:
I
. ' \ stable alloys in the BhTe3-Sb2Te3 pseudo-binary alloy
III
system. This phenomenon is evident from the significant
0 increase in the a lattice parameter for quenched alloys,
X

->.
.:; I .wr------------------------------------e
-I/)

I/)
CI)
9

8 ~,
28
.26
.24

a: 22
-;:
7 ,!!20
g- .18
Il)
6 ,.. .16
• .14

K ~ .12
5 ;;
\. ~ .10

1.0 1.4 1.8 2.2 2.6 30 ':.08

I- .os
IOOO/oK .04
(b)
.02
FIG. 3. (a) Electrical resistivity vs lOOOj"K for single-crystal o ~ ro ~ ~ M ~ ro ~ ~ ~
samples grown at a rate of 1.4 mm h~' in a Bridgman furnace. Mole Percent Sb 2 Te3
A-13.8 mole 'Y<! Sh;rc", B-33.5 mole % Sh;re" C-41.4 mole
'Ii., Sb,Te" D- 54.75 mole '/') Sh;re", E~-66.7 mole % Sb,Te3, FIG. 4. Thermal energy gap vs composition for single-crystal
]<'-73.3 mole 'Y<, Sh;re". (h) Electrical resistivity vs t(XJOj"K for specimens crystallized at 0.25 and 1.4 mm Ie'. (Note: H" value
single-crystal samples grown at a rate of 0.25 mm h ' in a shown for pure Slllre" was not an experimentally ohserved datum
Bridgman furnace. G-S7.25 mole % Sh;re3, H--14.S mole % point hut was posl1dated in reference 6.) 0 = crystallized at 0.25
Sbirea, 1-24.2 mole % Shire" J-33.3 mole % Shire" K-66.7 mm h~l, 6 = crystallized at 1.4 mm h~l, O=Li et al.,25 .=Hlack
mole % Sb 2Te3. et al.,ll and. = Airapetiants et al."

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2190 SMITH, KNIGHT, AND SPENCER

TABLE II. Physical and electrical parameters for Bi 2Tea, Sb2Tea, and alloys containing 33.3 and 66.7 mole % Sb 2Tea.

Electronic Lattice Resistivity

Thermal Thermal Specific Thermal thermal thermal Power of at which
energy dif'fusivity heat Cp Density conductivity conductivity conductivity temperature thermal con-
Mole % bandgap (cm'/sec) (cal/g OK) (g/cm') (W/cm OK) (W/cm OK) (W/cm OK) dependence of ductivity was
Sb,Te. (eV) at 300 0 K at 300 0 K at 300 0 K at 300 0 K at 300 0 K at 300 0 K hole mobility determined
0
Bi,Tea 0.16- 0.0194' 0.0374d 7.803' 0.029' 0.016' 0.013' 1.98< 4.5 XI0- 4f
33.3 0.13 0.0196 0.042 7.39 0.Q25 0.016 0.009 1.96 4.5 X 10-'
66.7 0.1 0.0202 0.047 7.07 0.028 0.022 0.006 1.77 3.4 XIO-'
100 0.30b 6.440' 0.047' 0.034' 0.011' I_ 2.1 XlO-'(

a See reference 25.

b See reference 11.
e See reference 18.
d P. V. Gultyaev and A. V. Petrov. Soviet Phys.-Solid State I. 330 (1959).
e See reference 3.
1 See reference 5.
_ N. B. Hannay. Semiconductors (Reinhold Publishing Corporation. New York. 1959). pp. 418-424.

and, in some alloys, by a decrease in Ea. The smaller a
lattice parameter in the more slowly crystallized
materials is probably associated with ordering of the
antimony and bismuth atoms in the basal plane of the
hexagonal structure. An ordered structure has been
proposed by Kokosh and Sinani1 and is further sub-
stantiated by the present observation of extra peaks in
the Debye-Scherrer diffractometer recordings. If the
ordered configuration is such that antimony and bis-
muth atoms have a minimum number of like nearest
neighbors, the most highly ordered structures will be
found in alloys containing 1: 3 and 2: 3 bismuth to
antimony ratios in the basal plane (viz., 33.3 and 66.7
mole % Sb2Te3)'
Near the center of the phase diagram, most properties
of the alloys show a marked dependence upon freezing
rate. Although microsegregation, as discussed by Cos-
grove et aUo for BiSbTe3 (doped with 0.56 wt % Se),
seems to be a reasonable postulate, this will not ade-
quately account for the substantial changes in physical
and electrical properties which are observed as a func-
tion of freezing rate. Therefore, until quantitative
information concerning the properties of the micro-
regions becomes available, nothing further can be said
about the magnitude of their effect relative to the
magnitude of other effects which depend upon growth
conditions, such as degree of crystallographic order and
chemical composition.
Mooser and Pearson21 have discussed empirical cor-
relations between Ea and several parameters, such as
lattice constant and heat of formations, for several
compound-semiconductor series. Although a theoretical
basis for these correlations is not available as yet, their
work performs a valuable service in that information is
systematized in such a manner that extrapolation and
interpolation are possible. Care must be exercised in the
use of such correlations, however, in instances where a
21 E. Mooser and W. B. Pearson, Progress in Semiconductors
(Heywood and Company, London, 1(0), Vol. S, p. 1m.
change in the position of band extrema is involved.
Through alloying and pressure studies of this series of
rhombohedral compounds and their alloys, it should be
possible to correlate the effects of change in bond length,
change in bond angle, and relative electronegativity of
the different atoms with the change in Ea for a particu-
lar band structure. When Bi 2Sea is alloyed with Bi 2Te3
the bond angle, as measured by c/ a, remains essentially
constant, although both c and a diminish. 22 At the same
time EG increases smoothly and reasonably rapidly in
the dilute range. 23 .24 In the present instance when
Sb 2Te3 is alloyed with BizTe3, Ea decreases smoothly in
the dilute range while c remains essentially constant and
a decreases. Increases in pressure upon Bi 2Tea cause a
smooth decrease in E G ,25 although the changes in lattice
parameter accompanying the process are unknown.
Since in all three instances Ea varies smoothly with the
alloy or pressure variable, it seems reasonably certain
that the same band structure is involved. However,
sufficient information is not available as yet to establish
correlations which identify the significant variables
affecting Ea in alloys of these substances.
ACKNOWLEDGMENTS
The authors are grateful to Dr. Che-Yu Li for his
suggestions and assistance in the research program, to
G. R. Miller for help in materials preparation, and to
J. T. Smith for taking many of the measurements. This
research was supported by the United States Air Force
under a contract monitored by the Air Force'Office of
Scientific Research at the Air Research and Develop-
ment Command.
22 J. R. Wiese and L. Muldawer, J. Phys. Chern. Solids 15, 13
(1960).
231. G. Austin and A. Sheard, J. Electronics and Control 3, 236
(1957). .
24 C. Y. Li and G. R. Miller, unpublished research at Cornell
University, Ithaca, New York.
25 C. Y. Li, A. L. Ruoff, and C. W. Spencer, J. Appl. Phys. 32,
1733 (1901).

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