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Lattice Parameter Local Determination for Trigonal, Hexagonal, and Tetragonal Crystal
Systems Using Several Coplanar X-Ray Reflections
Article in Crystallography Reports · November 2010
DOI: 10.1134/S106377451006026X

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ISSN 1063 7745, Crystallography Reports, 2010, Vol. 55, No. 6, pp. 1074–1078. © Pleiades Publishing, Inc., 2010.
Original Russian Text © A.E. Blagov, M.V. Dekapoltsev, M.V. Kovalchuk, V.V. Lider, Yu.V. Pisarevsky, P.A. Prosekov, 2010, published in Kristallografiya, 2010, Vol. 55, No. 6,
pp. 1133–1138.

STRUCTURAL
STUDIES

Dedicated to the memory of B.N. Grechushnikov

Lattice Parameter Local Determination for Trigonal,

Hexagonal, and Tetragonal Crystal Systems Using Several
Coplanar X Ray Reflections
A. E. Blagov, M. V. Dekapoltsev, M. V. Kovalchuk, V. V. Lider,
Yu. V. Pisarevsky, and P. A. Prosekov
Shubnikov Institute of Crystallography, Russian Academy of Sciences, Leninskiі pr. 59, Moscow, 119333 Russia e mail:
blagov@ns.crys.ras.ru
Received July 1, 2010

Abstract—The method for determining the local lattice parameters using quasi multiple X ray diffraction
(which was proposed and used only for crystals of the cubic system) has been expanded to measure the local
crystal lattice parameters for the trigonal, hexagonal, and tetragonal systems. Local variations in the lattice
parameters in the tetragonal paratellurite (TeO 2) and trigonal lanthanum–gallium tantalate
(La3Ga5.5Ta0.5O14) crystals have been investigated. Reflections necessary for implementing the quasi multi
ple X ray diffraction scheme are found for these crystals. The pairs of reflections that were found were used
to complete quasi multiple X ray diffraction schemes on a laboratory X ray source and determine the varia
–
tion in the lattice parameter a along the surface of these crystals. The relative measurement error was 4 × 10
6
at a spatial resolution of 140 μm. The accuracy of the method and the parameters determining this
characteristic were analyzed based on the results. The locality of the method and the limits of the spatial
resolution of an X ray diffraction measurement of lattice parameters are estimated.
DOI: 10.1134/S106377451006026X

INTRODUCTION reflections that satisfy (at least approximately) the

The experimental determination of lattice param
eters is one of the conventional problems solved by X
ray diffractometry. To study the real crystal struc ture,
i.e., obtain information about defects, the vari ation of
the composition throughout the crystal, the
distribution and concentrations of impurity atoms and
inclusions of other phases, etc., one needs meth ods
for determining the local lattice parameters and their
variations [1–3]. Recently, great interest has been
shown in superstructural nanoaggregates, which often
impart crystals with new qualities. Thus, accurately
–5
(with an error of ~10 ) measuring local parameters
with a high spatial resolution has become particularly
urgent.
Some well known methods for accurately deter
mining lattice parameters (the Kossel method [4], the
method of highly divergent beam [5], and the Bond
method [6]) allow one to determine lattice parameters
with a high accuracy (reaching 10 –4–10–5). However,
these techniques are either invalid or require a special
technique for local measurements.
There is an efficient and convenient method for
accurately determining lattice parameters which is
based on measuring the angular distance between two
condition of coplanar multiple X ray diffraction. One
significant advantage of this method is the possibility
of determining local variations in lattice parameters
with a high spatial resolution (to a few tens of a
micrometer) using a laboratory source. In view of the
aforementioned features, quasi multiple X ray dif
fraction is of interest for a number of technical prob
lems related to crystal growth technology and an anal
ysis of the defect crystal structure. This method was
proposed in [1] and then successfully developed in [2,
3] for measuring the parameters of cubic crystals. At
the same time, the restriction of this method to cubic
crystals significantly narrowed the range of its applica
tion.
In this paper we report the results of studying the
features of this method and developing it for the trigo
nal, hexagonal, and tetragonal crystal systems. We
experimentally investigated the local variations in the
lattice parameter in tetragonal paratellurite (TeO 2)
and trigonal lanthanum–gallium tantalate
(La3Ga5.5Ta0.5O14; langatate, LGT) crystals.

1074
 LATTICE PARAMETER LOCAL DETERMINATION
(а)
(h2k2l2)
(h1k1l1)
Ψ0
Fig. 1. Schematic diagram of coplanar diffraction for the reflection pair: (a) XS–X ray source Ψ0 is the angular distance between the
(h1k1l1) and (h2k2l2) reflection peaks; (b) О 1О2 = ϕ, А1А2 = Ψ0, θ1 and θ2—Bragg angles corresponding to (h1k1l1) and (h2k2l2)
reflections.
SPECIFIC FEATURES OF MEASURING LOCAL
LATTICE PARAMETERS OF CRYSTALS
BELONGING TO THE TRIGONAL,
HEXAGONAL, AND TETRAGONAL SYSTEMS
USING QUASI MULTIPLE X RAY
DIFFRACTION
The method under consideration is based on mea
suring the angle between two diffraction peaks corre
sponding to two previously chosen reflections satisfy
ing conditions similar to multiple X ray diffraction
(the so called quasi multiple X ray diffraction) in the
coplanar geometry.
In the case of the coplanar geometry of quasi mul
tiple X ray diffraction (Fig. 1), the angle between the
crystal orientations at which the (h1k1l1) and (h2k2l2)
reflection peaks can be observed obeys the relation
Ψ0 = ϕ – |θ1 – θ2|, (1)
where θ1 and θ2 are the Bragg angles corresponding to
the (h1k1l1) and (h2k2l2) crystallographic planes and
ϕ is the angle between these planes.
When recording the rocking curves in the vicinity
of ∼Ψ0, one can detect (h1k1l1) and (h2k2l2) diffraction
reflections with a high angular resolution and thus
accurately measure the desired angle Ψ0 between the
corresponding diffraction peaks. The error in deter
–5
mining the lattice parameter can be as small as 10 –
10–6, as was demonstrated in [2] for cubic crystals.
Note that crystal rotation by a small angle Ψ0 during
measurements barely affects the method locality, due
to which measurements can be performed with a spa
tial resolution equal to the width of the beam projec
tion on the sample.
This method is generally accurate and convenient
to use at Ψ0 < 300–500″. For much larger angles, the
instrumental error and measurement time increase.
In the diffraction geometry under consideration
(Fig. 1), Ψ0 is a function of the unit cell parameters of
the crystal analyzed: a, b, с, α, β, and γ; the indices hkl
CRYSTALLOGRAPHY REPORTS Vol. 55 No. 6
1075
(b) h1k1l1
XS 90°– θ1
A1 A2
O1 O2
90°– θ2
h2k2l2
of the reflection pair used; and the X ray wavelength λ.
For the crystals belonging to the trigonal, hexagonal,
and tetragonal systems, the search for reflections is
reduced to a cyclic enumeration of the h1k1l1 and h2k2l2
indices and a calculation of Ψ0 at a specified wave
length λ and reference values of a and с. The reflection
pairs for which Ψ0 does not exceed 500″ are assumed
to be suitable for further analysis.
For arbitrary pairs of reflections, the angular dis
tance Ψ0 makes it possible to study the ratio of the
parameters c and a along the sample surface. In some
cases this is sufficient to analyze crystal homogeneity.
Under the condition l1 = l2 = 0, the parameter с is
excluded from calculations. In this case, pairs of
coplanar reflections of the (h k 0) and (h k 0) type
1 1 2 2
make it possible to unambiguously determine the lat
tice parameter а and study its change along the sur
face. A similar situation can be implemented by
choosing a pair of reflections for which the angular
distance between the diffraction peaks is sensitive to a
change in one of the parameters and is not very sensi
tive to a change in the other one.
The relative error of the method is given by the for
mula δа/а = εδΨ, where δΨ is the experimental error
–1
in determining Ψ0 and ε = tan θ1 – tan θ2 is a coef
ficient characterizing the sensitivity of Ψ0 for the cho
sen pair of reflections to small changes in the lattice
parameter [1, 2]. Thus, pairs of reflections with a max
imum difference in the tangents of Bragg angles ensure
the highest measurement accuracy.
SAMPLES FOR STUDY
The objects of this study were paratellurite (TeO ) 2
and lanthanum–gallium tantalate (La3Ga5.5Ta0.5O14)
crystals. Langatate crystals belong to the trigonal sys
tem, group 32. They are widely used in various piezo
electric devices based on surface and bulk acoustic
2010
1076 BLAGOV et al.
Calculated reflection pairs for LGT and TeO2 crystals, λ[MoKα1]

(h1k1l1) (h2k2l2) ΘB1 , deg ΘB2, deg | Ψ0 |, '' ε Beam projection, μm

(for a 100 μm slit)
Langatate
(260) (110) 21.03 4.95 54.7 3.4 1160
(260) (770) 21.03 37.11 68.4 2.7 170
(699) (440) 64.3 20.17 81.8 0.6 290
(442) (880) 21.81 43.6 340.5 1.8 150
(521) (770) 18.57 37.11 364.9 2.4 160
Paratellurite
(220) (370) 12.04 34.16 1164.8 2.1 270
(770) (250) 46.88 23.40 1032.1 1.6 250
(440) (585) 24.65 47.19 170.3 1.6 260
(220) (464) 12.04 34.29 63.1 2.1 260
(220) (371) 12.04 34.30 100.9 2.1 260

waves. Paratellurite crystals belong to the tetragonal
system, group 422. They are most widely used in vari
ous acousto optic devices: modulators, filters, deflec
tors, etc. Modern technology makes it possible to
grow both LGT and TeO2 crystals that are large in size
and high quality. We used LGT samples in the form of
plates with a normal oriented in the 1 1 2 0 direction
and TeO2 samples in the form of plates normally ori
ented in the [110] direction (this cut is characterized
by a bright reflection (220)).
The table contains the reflection pairs for both
crystals, the calculated angular distances between the
reflections, the sensitivity coefficients of the pairs
found to changes in the lattice parameter, and the sizes
of the beam projection on the sample.
For the langatate crystal we could find several pairs
satisfying the condition l1 = l2 = 0, Ψ0 < 300″. We chose
the pair (260–770) because it provided the min imum
spatial resolution. For the paratellurite crystal, the found
pairs with l1 = l2 = 0 had an angular distance Ψ0
significantly exceeding 300″. The reflection pairs (220–
464) and (220–371) turned out to be the most
appropriate. The pairs with l1 ≠ l2 ≠ 0 make it possible to
study only the ratio of the parameters а and с, but for the
reflections (220–371) the angular distance Ψ0 is barely
sensitive to changes in the parameter с.
System for signal processing θ
and recording rocking curves 80 μm slit
Detector 1
Si (440)
Sample Monochromator
Detector 2
Fig. 2. X ray optical scheme of the experiment.
A change in Ψ0 by one arcsec (ΔΨ0 = 1″) corre
sponds to the following relative changes in the lattice
–4 5
parameters c and a: c/c = 4 × 10 and a/a = 10 . In
–5
other words, with a relative change a/a = 10 in the
lattice parameter a, the angular distance between the
reflections (220–371) changes by one arcsec (ΔΨ0 =
1″), while the same change in the parameter с ( с/с =
–5
10 ) corresponds to the change ΔΨ0 = 0.025″. Thus,
one can neglect the contribution of the variation in с
and use this pair to study the variation in only а. The
calculations for the pair (220–464) show that the sen
sitivity to variation in а is comparable with the sen
sitivity to variation in с, and this pair cannot be used
to study the variation in the parameter а inde pendent
of с.
In [7] the reflection pair (220–371) was chosen to
investigate the features of multiple X ray diffraction in
TeO2 crystals. We used these reflections to analyze the
variation in the lattice parameter а along the sample
surface.
EXPERIMENTAL SETUP
AND MEASUREMENT RESULTS
Experiments were performed on a standard TRS K
X ray spectrometer (Fig. 2) within the double crystal
МоКα source nonparallel geometry. The radiation source was an X
ray tube with a molybdenum anode. An X ray beam,
which was formed based on single symmetric
reflection from a Si(440) monochromator, was limited
0.1 mm slit by a slit installed before the sample; this allowed us to
use the MoKα1 line in the experiments. The reflection
intensity was measured by two scintillation NaI detec
tors with independent counting channels.

CRYSTALLOGRAPHY REPORTS Vol. 55 No. 6 2010

 LATTICE PARAMETER LOCAL DETERMINATION 1077
Ψ ,′′ a/a × 10
–5

0
150 3
100

50 2

0
1
– 50

– 100 0

– 150

– 200 0 0.5 1.0 1.5 2.0 2.5 3.0

X, mm
–2 –1 0 1 2
Azimuthal angle φ, deg
Fig. 4. Change in the lattice parameter a measured in the
Fig. 3. Experimental dependence of the angular distance Y(10 10 ) direction in the langatate
Ψ0 between the (260)–(770) reflections on the azimuthal crystal plate of the
position of the crystal (angle ϕ). 11 20 Х cut using the (260)–(770) reflection pair. The scan
step is 140 μm and the scanned area size is 3 mm.

Measurements of Langatate Lattice Local Parameters
It can be seen in Fig. 1b that the angular distance
Ψ0 reaches a maximum when the reflection diffraction
vectors and the vectors of the incident and diffracted
waves are in an exact coplanar position. To satisfy the
experimental conditions, the reflection diffraction
vectors must lie in the diffraction plane set by the
monochromator. The crystal position corresponding to
the aligned coplanar scheme and the corresponding
Ψ0 value (the position of the peak in the curve in Fig.
3) were determined by measuring a series of rock ing
curves of the reflections at azimuthal crystal scan ning
(rotation) within ±2° with a step of 5'. The scheme
was additionally aligned after each azimuthal rotation
step (crystal inclination). This additional alignment
compensated for the deviation of the dif fraction
vector of symmetric reflection from the scat tering
plane, which occurred at azimuthal crystal rota tion,
when the rotation axis of the crystal did not exactly
coincide with the diffraction vector of sym metric
reflection.
The aligned coplanar scheme makes it possible to
determine the lattice parameter magnitude. The mea
surement error, provided that the coplanar scheme is
exactly aligned, is determined by the error in measur
ing Ψ0 and the instrumental error. Ways to introduce
corrections for the error in aligning the crystal sample
were considered in detail in [8]. Along with the correc
tions for the alignment error, one must also take into
account the effect of temperature, the refraction
induced change in the Bragg angles, etc.
The relative change in the lattice parameter a along
the (1 1 2 0 ) face of the sample in the ( 1 0 1 0) direction
is shown in Figs. 4 and 5. When detecting Ψ0, rocking
curves were recorded at the width of the X ray beam
projection on the sample of 140 μm (slit size 80 μm).
Series of rocking curves were measured with X ray
beam scanning over the sample. In Fig. 4 the scan step
was 140 μm and the scanned area was 3 mm. In Fig. 5
the corresponding values were 660 μm and 13 mm,
respectively. Under the measurement conditions used,
the relative error in determining the lattice parameter
–6
a was δa/а ~ 4 × 10 .
Measurements of Paratellurite Lattice Local Parameters
As was shown above, the angular distance between
the (220–371) reflection peaks of paratellurite is
almost insensitive to small variations in the parameter
с; its relative changes, up to 10–4, do not exceed the
error in determining Ψ0.
–5
a/a × 10
5
Step 660 μm
4 Step 140 μm
3
2
1
0
–1
0 2 4 6 8 10 12
X, mm
Fig. 5. Change in the lattice parameter а measured in the
Y(10 10 ) direction in the langatate crystal plate of the
11 20 Х cut using the (260)–(770) reflection pair. The scan
step is 660 μm and the scanned area size is 13 mm.

CRYSTALLOGRAPHY REPORTS Vol. 55 No. 6 2010

1078
96.2
96.0
95.8
Ψ , ′′
095.6
95.4
95.2
95.0
94.8
0 0.25 0.50 0.75 1.00 1.25 1.50
X, mm
Fig. 6. Experimental dependence of the angular distance
Ψ0 between the (220)–(371) reflections of paratellurite
(left ordinate axis) and the relative change in the lattice
parameter a (right ordinate axis) at X ray beam scanning
over the (110) face.
Figure 6 shows the results of measuring the angular
distance between the (220–371) reflections of paratel
lurite (left ordinate axis) and the corresponding rela
tive change in the lattice parameter a (right ordinate
axis) at an X ray beam displacement over the (220)
surface in the [100] direction with a step of 150 μm.
The X ray beam projection on the sample surface was
150 μm and the scanned area size was 1.5 mm.
The angular positions of the peaks in the experi
mental rocking curves were determined using the
Lorentzian approximation. The error in determining
the peak position using the analytical approximation
of experimental rocking curves did not exceed 0.1″.
The most important factors for the measurement
accuracy were the collection time at a point, the angu
lar scan step, and the diffracted beam intensity. Multi
ple measurements of a series of rocking curves of
reflections at the same point were performed for sev
eral hours to determine the instrumental error in mea
suring the angular distance Ψ0. The error in measuring
Ψ0 did not exceed 0.4″. The changes in temperature
during measurements were insignificant ~0.5°, and no
temperature corrections were introduced.
DISCUSSION AND CONCLUSIONS
The results obtained indicate that the method for
measuring local lattice parameters, which is based on
quasi multiple X ray diffraction and was previously
developed for studying cubic crystals, can be used to
analyze crystals of trigonal, hexagonal, and tetragonal
systems. The accuracy, locality, and informativeness of
this method depend on the choice of reflection pairs.
Bragg reflections were calculated for paratellurite
and langatate crystals (representatives of tetragonal
and trigonal systems) and reflection pairs were chosen
for them to implement schemes of quasi multiple X
ray diffraction in experiments and perform local
accurate measurements of lattice parameters. It was
View publication stats
BLAGOV et al.
1.2 shown that only one lattice parameter can be indepen
1.0 dently measured using one pair of reflections.
All measurements were performed on a standard
0.8 double crystal spectrometer. Schemes of quasi multi
ple X ray diffraction were implemented using the
–5
0.610 (260–770) and (220–371) reflection pairs for lan
gatate and paratellurite crystals, respectively. The rela
×
0.4
tive error in measuring the variation in the lattice
a/
a
0.2 parameter a along the sample surface was δa/а ~ 4 ×
–6
0 10 . A spatial resolution of 140 μm was reached at a
– 0.2 slit width of 80 μm. The intensities of diffracted X ray
beams indicate that the spatial resolution can be
improved several times. The increase in resolution is
limited by the relatively low intensity of laboratory
X ray sources (according to our estimates, the limiting
resolution for a laboratory source is 10–20 μm). These
limitations can be partially removed using brighter
sources, especially synchronization radiation beams.
For bright sources the spatial resolution is limited by
the diffraction divergence, which is significant at sub
micron beam sizes.
The approach discussed in this study can also be
used to measure local inhomogeneities in crystals of
lower order systems, which have a larger number of
independent unit cell parameters. In the simplest case
of an orthorhombic system with three independent
parameters, it is sufficient to choose three pairs of
quasi multiple X ray reflections and develop algo
rithms for numerical calculations of the lattice param
eters from the measured angular distances between the
positions of reflection peaks.
ACKNOWLEDGMENTS
This study was supported by the Ministry of Educa
tion and Science of the Russian Federation (GK
16.740.11.0095), and grant MK 156.2010.2 of the
President of the Russian Federation.
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Translated by Yu. Sin’kov
CRYSTALLOGRAPHY REPORTS Vol. 55 No. 6 2010