ISSN 10274510, Journal of Surface Investigation. Xray, Synchrotron and Neutron Techniques, 2012, Vol. 6, No. 3, pp. 494497.

Pleiades Publishing, Ltd., 2012.

Original Russian Text Yu.N. Drozdov, A.V. Novikov, D.V. Yurasov, P.A. Yunin, 2012, published in Poverkhnost. Rentgenovskie, Sinkhrotronnye i Neitronnye Issledovaniya, 2012, No. 6,
pp. 3639.

New Approach to the XRay Diffraction Analysis of Test Structures

during Flow Calibration in Epitaxial Growth Reactors
Yu. N. Drozdov, A. V. Novikov, D. V. Yurasov, and P. A. Yunin
Institute for Physics of Microstructures, Russian Academy of Sciences, Nizhni Novgorod, 603950 Russia
email: drozdyu@ipmras.ru
Received September 24, 2011

AbstractThe highresolution Xray diffractometry (HRXRD) technique is known as a powerful tool for
analyzing epitaxial heterostructures. However, standard analysis procedures do not allow the layer growth
time to be used as a fixed parameter during HRXRD spectra analysis. The growth time in modern facilities is
measured with a high degree of accuracy, which increases the reliability of HRXRD analysis particularly in
the case of spectra with reduced quality or complex heterostructures consisting of a large number of individual
homogeneous layers. A new algorithm is based on using flow rates of deposited components as variable
parameters, while the layer growth times are taken as fixed parameters. A particular feature of this new
approach is associated with the fact that the known growth time for each heterostructure layer is directly
included into the algorithm for adjustment of the calculated spectrum to the experimental Xray diffraction
spectrum (HRXRD). The flows of deposited layers are variable parameters and, thus, the algorithm turned
out to be very efficient for calibrating flow controllers in epitaxial growth reactors. The algorithm allows for
reliable estimation of the flow even in the case of poorly informative HRXRD spectra.
DOI: 10.1134/S1027451012060080

INTRODUCTION
The study is aimed at developing and testing a new
approach for determining the parameters of test struc
tures, which were grown for calibrating the flows of
deposited substances in molecularbeam and gas
phase epitaxy reactors. At present, this is performed
using highresolution Xray diffraction analysis
(HRXRD), where the thickness and composition of a
solid solution in test layers are determined. However,
universal algorithms used for it do not take into
account the known growth time of individual layers
[1, 2]. In modern growth setups, the flows are main
tained constant due to different feedback circuits, and
the growth time which is calculated with a high degree
of accuracy is specified. Accounting for this additional
information increases the reliability and accuracy of
estimates. The problem originated from the practice of
test structure analysis during the calibration of flows
of Ge and Si atoms embedded into a GexSi1x layer in
a Riber SIVA21 system for molecularbeam epitaxy.
The standard procedure of specifying the thickness
and the composition of the layers by adjusting the cal
culated Xray diffraction spectrum to the experimen
tally obtained one turned out to be insufficient in some
cases since conversion into flows of deposited sub
stances, with the growth time of each layer taken into
account, yielded some disagreement with the growth
conditions and the required additional analysis cycles.
A distinctive feature of the new approach is the
direct inclusion of the known growth time of each

layer into the algorithm for adjusting the calculated

spectrum to the experimental HRXRD one. The flows
of deposited substances are variable parameters.
DESCRIPTION OF THE ALGORITHM
The algorithm for calculating the spectrum, i.e.,
the diffraction reflection curve (DRC), is based on the
known recursion formula for dynamical Xray diffrac
tion [1, 2]. The DRC is calculated for a case when one
extra layer, homogeneous in its thickness, is added to
the structure. The following parameters of this layer
are specified: thickness, type of crystalline structure,
elemental composition, concentration of the solid
solution (if it is a solution), and elastic deformation of
the layer coherently conjugated with a substrate. The
proposed algorithm is a certain superstructure over
the standard scheme. The focus of the analysis shifts
from the structure to the growing process. The flows of
deposited substances (that are varied) and the growth
times of layers (that are fixed) are considered as
parameters of the growth process. These parameters
are used for calculating the thickness and composition
of the layers, and after that the standard algorithm
starts to work. We used the software described earlier in
[3]; its source code that makes modification of the
software possible is available.
Let us describe in more detail the elementary
example of an n [Si/GeSi] periodic structure, where
the flow fSi remains constant, while the flow fGe is
blocked by a shutter during Si layer growth. The flows

494

NEW APPROACH TO THE XRAY DIFFRACTION ANALYSIS OF TEST STRUCTURES

that are expressed in nm/s represent the deposition

rates of individual components. In the case where the
components of the GexSi1x solid solution are simulta
neously deposited and the Vegards law is fulfilled,
these rates are additively summed with a high degree of
accuracy [4]. We designate the values of fSi and fGe as
flows of deposited substances, since they are con
trolled in the reactor and maintained stable with the
help of several flow controllers, with the aim of cali
brating these controllers in growth rate units. As a rule,
the substrate temperatures in the reactor are not very
high and, thus, reevaporation flow can be neglected.
In the growth process, the growth times of the layers tSi
and tGeSi are specified. In this case, the thicknesses of
the layers are

hSi = f Sit Si,

(1)

hGeSi = ( fSi + f Ge ) t GeSi;

(2)

The concentration of the solid solution is

x = f Ge ( fSi + f Ge ) ;

(3)

The period of the superlattice structure is

D = hSi + hGeSi;
The mean over the entire lattice is

(4)

x = f Get GeSi D.

(5)

A solution is sought by successive iterations; the

initial values of the flows are specified based on antic
ipated values; the flows are varied. The new parame
ters of the layers, according to which the spectrum is
calculated, correspond to modified flows. Minimiza
tion of the functional of discrepancies between the
experimental and calculated spectrum makes it possi
ble to estimate the flows with the information con
tained in the experimental spectrum and in the speci
fied layer growth times taken into account.
RESULTS AND DISCUSSION
The test structures are specially designed so that the
layer thickness and composition can be unambigu
ously determined based on the HRXRD spectrum. A
peak corresponding, in terms of its position and width,
to a single GeSi layer must be present on the satellite
envelope. If the structure is strictly periodic, the layers
are planar and unrelaxed, and the spectrum is not dis
torted by the diffusion background and contains the
entire set of interference maxima, a standard analysis
algorithm yields a correct and exact solution. In this
case, a new algorithm results in the same solution and
does not yield any noticeable advantages. It becomes
useful only if the spectrums informativ is insufficient.
This insufficiency may be as a result of the following:
Poisson noise related to an insufficient Xray beam
intensity, structural flaws intensifying the diffusion
background, or features of the structure yielding low
intensity of the maxima.

495

An insufficient informative value of the spectrum is

often attributed to either the heterosystems structure
or to an insufficient beam intensity. Structures charac
terized by distortion in the planarity of thin layers at
the heterojunctions can serve as examples of the first
type [5]. Periodic structures with weak composition
modulation can exemplify the second type. Let us
consider such an example in greater detail. Figure 1
gives the experimental spectrum of an R214 lattice.
The succession and parameters of the layers are speci
fied during growing: 50 [Ge0.04Si0.96 hGeSi = 3 nm,
tGeSi = 30 s / Si hSi = 10 nm, tSi = 104 s]. The thickness
of the GeSi layer is small and the Ge concentration is
low; therefore, the satellite maxima are weak and very
noisy. It is only possible to reliably determine the
period D (based on the intersatellite distance) and the
mean composition x (based on the position of the
superlattice zero peak 0SL). Refinement of the struc
tural parameters with the help of the standard algo
rithm yields a strong correlation between the compo
sition and the thickness of the GeSi layer. This can be
clearly seen in Fig. 1 where both calculated spectra
(2 and 3) are very close, while the model parameters
drastically differ. The reason for this is quite obvious.
Agreement between the calculated and the experi
mentally obtained spectra is generally reached by
superposing the series of sharp peaks (1;0SL;+1).
However, the solution in this case is ambiguous. An
increase in the thickness of the GeSi layer can be com
pensated by decreasing the thickness of the Si layer
(for D to be preserved) and by decreasing x (for the
mean x to remain constant). The positions of all
maxima remain the same, The intensity slightly differs
(see the inset in Fig. 1), but the accuracy of analysis
using the standard algorithm drastically decreases
when the experimental spectrum is distorted by noise
and the diffusion background. If the parameter corre
lation is not taken into account, this can yield overes
timation of the accuracy of analysis. It is demonstrated
in Fig. 2 which shows two cross sections of the discrep
ancy functional R as a function of the GeSi layer thick
ness. The functional characterizes the deviation of the
calculated spectrum from the experimental one:
R = [log(kIc) logIe]2/(logIe)2,
where Ic are the calculated intensities, Ie are the exper
imental intensities (see Fig. 1a), and k is the common
scale factor. A logarithm of intensity is used with the
aim of increasing the role of weak peaks [5]. Line 1 was
obtained when hGeSi was varied, all other parameters
remaining unchanged. It has a sharp minimum with a
~0.1 nm downward excursion. Line 2 was obtained
when hGeSi was varied with simultaneous adjustment of
other parameters for x and D to be preserved. It can
be seen that this line is much wider and the real error
of the standard algorithm in this case is much larger
than 0.1 nm. Correlation of the parameters manifests
itself as an extension of the area of the minimum R in

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DROZDOV et al.
()
Si 400

104
0SL

Intensity, arb.units

103
102
101

1
+1

100
101
68.0
105

Intensity, arb.units

104

68.5

69.0
2, deg
(b)

102

69.5

70.0

101
100

103 101

102

102
68.0

68.4
+1

101
100
101
68.0

68.5

69.0
2, deg

69.5

70.0

Fig. 1. Experimental (1) and calculated (2, 3) spectra for the 50[GeSi/Si]/Si(100) structure in the vicinity of the Si (400) maxi
mum. The calculated spectra correspond to the following models: (1) x = 0.039, hGeSi = 3.3 nm, hSi = 10.9 nm; (2) x = 0.026,
hGeSi =5.0 nm, hSi = 9.2 nm. The inset shows the 1 satellite area on the calculated spectra (1) and (2).

the direction inclined to the axes (as schematically

shown in the inset in Fig. 2).
On the contrary, the new algorithm taking into
account the time of layer growth yields an unambigu
ous solution (model of spectrum 2 in Fig. 1). Actually,
the solution in the given example does not require
spectral adjustment. Based on the measured D and x,
the flows are determined:
fGe = xD/tGeSi,
fSi = (D fGetGeSi)/(tSi + tGeSi),
Then the layer parameters are estimated based on
Eqs. (1)(3). The given example yielded as follows:

x = 0.009; D = 14.3 nm; fGe = 0.0043 nm/s; fSi =

0.105 nm/s.
Such a technique is useful, e.g., when analyzing
[AlxGa1xAs/GaAs] lattices with small x. Satellites are
recorded near the reflection GaAs (200); the 0SL
maximum is recorded near another reflection (GaAs
(400)). Application of the standard algorithm necessi
tates the simultaneous adjustment of both spectra.
Flow controllers in the elementary model
described above only stabilize the flows and com
pletely block the Ge flow during Si layer growth. In a
more general case, the controllers are calibrated, and
the flows for each (j) layer are set with the help of soft
ware by specifying the coefficient Kj: fj = f0Kj. The issue

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NEW APPROACH TO THE XRAY DIFFRACTION ANALYSIS OF TEST STRUCTURES

0.30
1

0.20
R

x(Ge)

0.25
1

0.15
2

0.10

h(GeSi)

0.05
1

4
5
h(GeSi), nm

Fig. 2. Cross sections of the discrepancy functional R in

the vicinity of the minimum in the direction of the axis of
the GeSi layer thickness parameter: (1) at all other
parameters fixed; (2) at D and x which were kept con
stant. The inset gives the schematic of the functional at the
(xGe, hGeSi) plane and cross section directions.

of HRXRD spectrum analysis with the help of the pro

posed algorithm does not become complicated as the
coefficients Kj are considered given (as well as the layer
growth times).
The new algorithm is attractive since the number of
varied parameters does not increase with an increase
in the number of layers in the structure, since the
growth time is specified for each new layer, and the
flows are clarified for the structure as a whole. Thjs
allows its application even for those structures that are
difficult for HRXRDanalysis, such as quantumcas
cade lasers.
On the other hand, it is necessary to touch upon the
limitations of the proposed algorithm. An increase in
its capabilities is based on a more rigid model, i.e.,
the layers grow homogeneous in their composition and
their thickness is proportional to the growth time.
However, it is unlikely to hold for very thin layers (see,
e.g., [7]) where a nonlinear correlation between the
growth time and thickness is possible. Application of
the model for solving the discussed problem is justified
by two facts. Firstly, the operation of the preset reactor
during both molecularbeam epitaxy [4] and metal
organic gas phase epitaxy [8] is based on this very
model. Any deviation from this model is a signal for
further adjustment of the reactor operation. Secondly,
from the standpoint of flow evaluation the HRXRD
spectrum contains excess information, but this
excess allows the deviation of the actual structure from

497

the used model to be diagnosed. The case of a relaxed

structure where the length of the lattice coherence is
smaller than the structure thickness belongs to general
limitations for all techniques of adjustment of the cal
culated spectrum to the experimentally obtained one.
Thus, the calculations based on the dynamic theory
become incorrect. In this case, other techniques of
spectrum analysis are used (see, e.g., [9]).
CONCLUSIONS
Thus, the algorithm for HRXRD analysis based on
data on the growth times of the heterostructure layers
turned out to be rather efficient. It is especially useful
for calibrating flow controllers in epitaxial growth
reactors since the varied parameters in the case of
adjustment of the calculated spectrum to the experi
mental one are the flows of deposited substances. The
algorithm allows for reliable flow determination even
in the case of poorly informative HRXRD spectra.
ACKNOWLEDGMENTS
The study was supported by the Programs of the
Presidium of the Russian Academy of Sciences and
the State Committee of the Russian Federation Min
istry of Education and Science no. 16.552.11.7007.
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4. M. A. Herman and H. Sitter, Molecular Beam Epitaxy,
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No. 3

2012