crystals

Communication
Numerical Analysis of the Combined Influence of
Accelerated Crucible Rotation and Dynamic Crucible
Translation on Liquid Phase Diffusion Growth of SiGe
Mandeep Sekhon 1, *, Brian Lent 1 and Yanbao Ma 2
1 Crystal Growth Laboratory, University of Victoria, Victoria, BC V8W3P6, Canada; [email protected]
2 Water and Energy Laboratory, University of California at Merced, Merced, CA 95343, USA;
[email protected]
* Correspondence: [email protected]; Tel.: +1-209-7359599

Academic Editor: Bing Gao

Received: 25 July 2016; Accepted: 6 September 2016; Published: 13 September 2016

Abstract: The effects of accelerated crucible rotation technique (ACRT) and dynamic translation on
liquid phase diffusion (LPD) growth of Six Ge1−x single crystals have been separately investigated
numerically in earlier works and were found to have a very positive impact on the LPD growth
process. Building upon these findings, in this paper, we study the consequences of imposing both
ACRT and dynamic translation on this growth technique. Time-dependent, axisymmetric numerical
simulations using moving grid approach have been carried out using finite volume code Ansys Fluent.
Crucible translation effect is simulated using dynamic thermal boundary condition. Results are
compared to the case in which this growth system is subjected to ACRT only. It is predicted that by
combining ACRT with dynamic pulling, excellent axial compositional uniformity can be achieved
and growth rate can be improved substantially without significantly compromising on the benefits
of employing ACRT. The results show that it is advantageous to utilize the combination of ACRT
and dynamic translation during LPD growth rather than using them independently for producing
relatively uniform composition Six Ge1−x single crystals in a shorter span of time.

Keywords: liquid phase diffusion; simulation; germanium-silicon alloys; accelerated crucible rotation
technique; dynamic translation; modeling; solution growth; numerical study

1. Introduction

Six Ge1−x is an upcoming alloy semiconductor material that is gaining prominence because its
properties can be adjusted as per the needs of a particular application [1]. This is due to the fact
that this alloy system displays a complete solid and liquid state miscibility. On the downside, this
system also exhibits a wide gap between the solidus and liquidus lines making it difficult to grow
uniform composition Six Ge1−x crystals using the well-known melt growth techniques [2]. Some of the
applications of this material include photodetectors, high-performance discrete devices, heterodevices,
solar cells, and substrate for epitaxial growth [1,3].
Liquid phase diffusion (LPD) is a solution growth technique that has been used to grow axially
graded composition single crystals of Six Ge1−x [4]. The complete details of the LPD growth process
can be found in [4].
In order to produce an axially uniform composition crystal, the growth interface should be
maintained at a constant temperature. To accomplish this, the crucible should be pulled downwards
at a rate equal to the growth rate. The effect of crucible translation with the objective of growing
uniform Six Ge1−x crystals has been investigated in the literature [5–7]. In the work [7], an automatic

Crystals 2016, 6, 116; doi:10.3390/cryst6090116 www.mdpi.com/journal/crystals

Crystals 2016, 6, 116 2 of 8

feedback control system was developed with dynamic pull correction after every minute and resulted
in a 23 mm long crystal with uniform composition.
The effect of constant and dynamic pull rate on the LPD growth was studied in [8]. Numerical
simulation results showed that by translating the crucible in a dynamic fashion the interface
temperature could be maintained at a nearly constant value and consequently uniform axial crystal
composition could be achieved. Furthermore, the results also indicated that the growth time could be
reduced considerably by employing dynamic translation.
In the accelerated crucible rotation technique (ACRT) developed in [9], the crucible undergoes
acceleration and deceleration cyclically and is used to generate flow in the melt/solution crystal
growth techniques. In the spin up and spin down period of the ACRT, Ekman layer flow is produced at
the solid surface creating a radial flow and fluid also experiences spiral shearing [10]. A large body of
work exists in the literature studying the effects of ACRT experimentally and numerically on the melt
and solution growth techniques (see for instance [11–21]), and it has been found in many studies that
the application of ACRT leads to an improvement in the melt mixing, growth rate, radial compositional
uniformity, and solid/liquid interface flattening.
In the numerical work [22] on the LPD growth process, it was found that the growth interface
was concave in shape for a large fraction of the simulated growth period. To achieve uniformity in
the radial crystal composition along the growth interface, the shape of the interface should be flat.
In a recent work on this growth system [23], the effect of imposing ACRT on the LPD growth was
examined numerically. It was predicted that by utilizing the ACRT cycle at 12 rpm, the growth interface
could be made nearly flat which in turn helped in substantially improving the uniformity in radial
composition along the growth interface.
Motivated by the positive effects of dynamic translation and ACRT on the LPD growth, in this
work, we have investigated the impact of the combination of ACRT and dynamic pulling numerically.
The simulation results reveal that by superimposing dynamic translation on ACRT, the uniform axial
composition can be achieved with a significant improvement in the growth rate while retaining the
key advantages of using ACRT.

2. Numerical Simulation
From a numerical point of view, LPD comes under the category of the moving boundary problem.
In order to draw a valid comparison with the earlier work [23], we have followed the same dynamic
grid approach to handle the moving boundary. The simulations have been carried out using the finite
volume based software Ansys Fluent (ANSYS, Inc., Canonsburg, PA, USA) by developing special user
defined functions to move the mesh nodes. Triangular ACRT cycle (at 12 rpm) was used to carry out
the computation.
It is important to highlight that the governing equations in the case of a moving grid approach
involve additional terms to account for the grid motion. The grid flux in the discretized equations
must be computed from space conservation law or else there is a possibility of the creation of artificial
mass sources [24]. In Ansys Fluent, the problem of the artificial mass source is avoided as the space
conservation law is used while computing grid flux [25]. The position of the initial growth interface
was determined based on the isotherm corresponding to the melting point of germanium. The mesh is
comprised of 4674, 1518, 656, 1002 quadrilateral elements in the melt, seed, source, and quartz regions,
respectively. Further refining of the mesh did not result in any significant change in the solution.
Pressure-velocity coupling was dealt with using the PISO algorithm [26] and a time step size of 0.1 s
was adopted. A smaller time step did not change the solution while a larger time step resulted in
convergence problems. The absolute convergence criterion [27] was used to judge convergence and
the solution was considered converged when residuals had fallen below 10−4 for continuity, radial and
axial momentum equations and below 10−6 for concentration and energy equations. The domain of
the problem is comprised of silicon source at the top, the Si-Ge melt in the middle, the Ge-seed below,
and the vertical wall of the quartz ampoule (see Figure 1). It must be noted that some of the results
Crystals 2016, 6, 116 3 of 8

presented in this paper were obtained by writing special user defined functions in Ansys Fluent as
they were
Crystals 2016,not directly available from the GUI of Ansys Fluent.
6, 116 3 of 8

(a) (b)
Figure 1. Initial computational mesh used for numerical simulation in the (a) Liquid subdomain (b)
Figure 1. Initial computational mesh used for numerical simulation in the (a) Liquid subdomain
Solid subdomains.
(b) Solid subdomains.

The governing equations are the Continuity, Momentum Balance, Energy Balance and Mass
Transportgoverning
The equations.equations
The completeare the Continuity,
set of governingMomentum Balance,
equations can found Energy Balance paper
in the previous and Mass[23]
Transport
and are notequations.
repeated The
here.complete set ofthat
It is assumed governing
the same equations can found
temperature in the
gradient previous
exists belowpaper [23]
the initial
and are not
position repeated
of the here.
crucible It ison
based assumed that the same
the experimental temperature
observations. gradient list
A complete exists below the initial
of assumptions can
position of the crucible based on the experimental observations. A complete list of assumptions
be found in earlier work [28]. As mentioned before, to simulate the effects of crucible translation can be
found
dynamicin earlier
thermal work [28]. Asconditions
boundary mentionedwerebefore, to simulate
prescribed andthe
theeffects
detailsofcan
crucible translation
be found dynamic
in the work [8].
thermal boundary conditions were prescribed and the details can be found in the work
For the boundary and initial conditions for the concentration and velocity fields, the reader is referred [8]. For the
boundary and
to the paper initial
[23]. Theconditions for the concentration
details regarding and velocity
the implementation of the fields,
dynamicthe grid
reader is referred
approach to the
in Ansys
paper [23]. The details regarding the implementation
Fluent for the LPD growth process can be found elsewhere [28]. of the dynamic grid approach in Ansys Fluent
for the LPD growth process can be found elsewhere [28].
3. Results and Discussions
3. Results and Discussions
While carrying out the numerical simulations, the crucible subjected to accelerated crucible
While carrying out the numerical simulations, the crucible subjected to accelerated crucible
rotation (triangular cycle at 12 rpm) was pulled dynamically after 5 h of growth time. The pull rate
rotation (triangular cycle at 12 rpm) was pulled dynamically after 5 h of growth time. The pull rate was
was adjusted after completion of one or more ACRT cycles in order to maintain a nearly uniform
adjusted after completion of one or more ACRT cycles in order to maintain a nearly uniform crystal
crystal composition along the centerline. A comparison is made with the previously examined case
composition along the centerline. A comparison is made with the previously examined case in which
in which only ACRT is applied to the ampoule [23].
only ACRT is applied to the ampoule [23].
It is important to note that after early hours of growth, LPD becomes a diffusion dominated
It is important to note that after early hours of growth, LPD becomes a diffusion dominated
process [22] and consequently in the later hours of growth the flow is mainly generated due to the
process [22] and consequently in the later hours of growth the flow is mainly generated due to the
application of ACRT [23]. The ACRT induced flow structure does not alter much with the addition
application of ACRT [23]. The ACRT induced flow structure does not alter much with the addition of
of dynamic translation and it can be observed from Figure 2 that there is a minor drop in the
dynamic translation and it can be observed from Figure 2 that there is a minor drop in the maximum
maximum radial velocity near the growth interface with the incorporation of dynamic pulling.
radial velocity near the growth interface with the incorporation of dynamic pulling.
Crystals 2016, 6, 116 4 of 8
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Crystals 2016, 6, 116 4 of 8

Figure
Figure 2.2. Maximum
Maximum outward
outward and
and inward
inward radial
radial velocities
velocities in
in the
the vicinity
vicinity of
of the
the growth
growth interface
interface after
after
66Figure
h of growth
h of growth time.
2. Maximum
time. outward and inward radial velocities in the vicinity of the growth interface after
Figure 2. Maximum
6 h of growth time. outward and inward radial velocities in the vicinity of the growth interface after
As
6 h ofshown in time.
growth Figure 3, the concentration difference along the growth interface increases slightly
As shown in Figure 3, the concentration difference along the growth interface increases slightly as
as dynamic
As shown pulling
in Figureis superimposed on ACRT.
3, the concentration Thisalong
difference can the
be attributed to theincreases
growth interface increaseslightly
in the
dynamic pulling
As shown inisFigure
superimposed
3, the the on ACRT. This
concentration can be along
difference attributed
the to the increase
growth interface in the temperature
temperature
as dynamic difference
pulling is along
superimposed growthon interface
ACRT. in the
This cancase
be of combined
attributed theincreases
to ACRT slightly
and dynamic
increase in the
difference
as dynamicalong the growth
pulling is interface in the
superimposed oncase of combined
ACRT. This canACRT
be and dynamic
attributed to pulling
the (see Figure
increase in 4).
the
pulling (see Figure
temperature 4). It along
difference can bethe readily observed
growth from
interface inFigure
the case5 that
of the interface
combined temperature
ACRT at the
and dynamic
It can be readily
temperature observed
difference from Figure 5 that the interface temperature at the centerline becomes nearly
centerline
pulling (seebecomes
Figure 4). It along
nearly can bethe
constant growth
readily theinterface
withobserved from inFigure
application the case
of dynamicof combined
5 that translation.
the interfaceACRT
This, and dynamic
in turn,
temperature leads
at the
constant
pulling withFigure
(see the application
4). It can of dynamic
be readily translation.
observed fromThis, in turn,
Figure 5 leads
that the tointerface
a nearly temperature
constant centerline
at the
to a nearlybecomes
centerline constant nearly
centerline crystal
constant composition
with in the axial
the application direction
of dynamic as shownThis,
translation. in Figure 6. leads
in turn,
crystal composition nearly
centerline in the axial direction as
theshown in Figuredynamic
6.
to a nearlybecomes
constant centerline constant with
crystal application
composition in the of
axial directiontranslation.
as shownThis, in turn,
in Figure 6. leads
to a nearly constant centerline crystal composition in the axial direction as shown in Figure 6.

Figure 3. Difference between crystal composition at the wall and at the centerline along the growth interface.
Figure Difference
Figure 3.3.Difference between
between crystalcrystal composition
composition atand
at the wall theatwall and at the
the centerline centerline
along the growthalong the
interface.
growth3.interface.
Figure Difference between crystal composition at the wall and at the centerline along the growth interface.

Figure 4. Difference between temperature at the wall and at the centerline along the growth interface.
Figure 4. Difference between temperature at the wall and at the centerline along the growth interface.
Figure
Figure 4. 4.Difference
Differencebetween
betweentemperature
temperatureat
at the
the wall and at
at the
thecenterline
centerlinealong
alongthe
thegrowth
growthinterface.
interface.
Crystals 2016, 6, 116
116 5 of 8
Crystals 2016, 6, 116 5 of 8
Crystals 2016, 6, 116 5 of 8

Figure
Figure 5. Variation
5. Variation ofthe
Variation of
of theinterface
the interfacetemperature
interface temperatureatat
temperature atthe
thecenterline
the centerlinewith
centerline with
with growth
growth
growth time
time after
after
time the
thethe
after initiation
initiation of
initiation
Figure
of
dynamic5. translation
dynamicVariation of(tthe
translation (t
= 5=interface
5
h).h). temperature at the centerline with growth time after the initiation
of dynamic translation (t = 5 h).
of dynamic translation (t = 5 h).

Figure 6. Variation of the axial crystal

crystal composition at the centerline after the initiation of dynamic
Figure 6. Variation of the axial crystal composition at the centerline after the initiation of dynamic
translation (t = 5 h). of the axial crystal composition at the centerline after the initiation of dynamic
Figure 6. Variation
translation (t = 5 h).
translation (t = 5 h).
A dramatic
A dramatic increase
increase in
in both
both instantaneous
instantaneous and and time
time averaged
averaged growth
growth velocity
velocity with
with the
the inclusion
inclusion
of A dramatic
dynamic
of dynamic increase
translation in
can both
be instantaneous
clearly seen in and time
Figure 7 averaged
and Table growth
1, velocity
respectively. with
This the inclusion
explains the
dynamictranslation
translationcan
canbebe
clearly seen
clearly in Figure
seen 7 and
in Figure 7 Table 1, respectively.
and Table This explains
1, respectively. the greater
This explains the
of dynamic translation
greater interface
interface can be
displacement clearly
after seen in Figure 7 and Table 1, respectively. This explains the
interface
greater displacement after 7 h of
displacement 77 h
growth
after h time
of growth
of growth
observedtime observed
in Figure
time observed in Figure
8 when
in Figure 88 when
using the when using the
combination
using of
greater
ACRT interface
combination of
and dynamic displacement
ACRT and dynamic
pulling after 7 h
pulling
instead pulling
of ACRT of growth
instead of time
ACRT observed
alone.ofMoreover,alone. in Figure
Moreover,
it can it 8
can
also be inferred when
also be
from using the
inferred
combination of ACRT and dynamic instead ACRT alone. Moreover, it can also be Figure
inferred8
combination
from
that Figure
dynamic 8of ACRT
that
pulling andnot
dynamic
does dynamic
pulling
have pulling
does
any not instead
have
significant of significant
any ACRT alone.
detrimental Moreover,
detrimental
impact on the it can also
impact
interface on beinterface
the inferred
flattening effect
from Figure 8 that dynamic pulling does not have any significant detrimental impact on the interface
from Figure
flattening
of ACRT. 8 that
effect of dynamic
ACRT. pulling does not have any significant detrimental impact on the interface
flattening effect of ACRT.
flattening effect of ACRT.

Figure 7.
Figure 7. Growth
Growth velocity
velocity variation
variation at
at the
the centerline
centerline during
during aa single
single ACRT
ACRT cycle
cycle at
at tt == 77 h.
h.
Figure 7. Growth velocity variation at the centerline during a single ACRT
ACRT cycle
cycle at
at tt == 7 h.
Crystals 2016, 6, 116 6 of 8
Crystals 2016, 6, 116 6 of 8

Table 1.1. Variation

Table Variation of
ofthe
thetime
time averaged
averaged growth
growth velocity
velocity at
at the
the centerline
centerline with
with growth
growth time
time after
after the
the
initiation of dynamic
dynamic translation
translation (t
(t == 5 h).

Growth Growth Velocity (mm/h) at the Growth Velocity (mm/h) at the Centerline
Time (h)
Growth Velocity (mm/h) at the
Centerline (ACRT) (Data from [23])
Growth Velocity (mm/h) at the Centerline
(ACRT with Dynamic Translation)
Growth Time (h)
Centerline (ACRT) (Data from [23]) (ACRT with Dynamic Translation)
5.5 0.760 1.328
5.5 6 0.760
0.763 1.613 1.328
6 6.5 0.760
0.763 2.025 1.613
6.5 7 0.755
0.760 2.599 2.025
7 0.755 2.599

(a) (b)

Figure 8. Interface displacement in 7 h of growth time (a) ACRT, (b) ACRT with dynamic translation.
Figure 8. Interface displacement in 7 h of growth time (a) ACRT, (b) ACRT with dynamic translation.

The dynamic pull profile shown in Figure 9 was obtained by running the simulation in an
The dynamic
intermittent manner. pull profile
After shown in of
the completion Figure
each 9ACRTwas cycle
obtained(120 by running
s), the the simulation
simulation was stopped in
an
andintermittent
the crystal manner. Afteralong
composition the completion
the growthofinterface
each ACRT cycle
at the (120 s), the
centerline wassimulation
checked. Thewas pull
stopped
rate
and the crystal composition along the growth interface at the centerline
was adjusted if the crystal composition value was found to be changing significantly. The simulationwas checked. The pull rate
was adjusted
process was thenif thecontinued
crystal composition
with this new value was
pull found
rate to for
value be changing
another cycle. significantly.
The whole Theprocess
simulation
was
process was then continued with this new pull rate value for another
then repeated to obtain a nearly constant crystal composition along the growth interface at the cycle. The whole process
was then repeated
centerline. The pulltorateobtain a nearly
values and theconstant crystal composition
corresponding time intervals alongforthe growth
which interface
it was at the
maintained,
centerline. The pull rate values and the corresponding time intervals
were recorded throughout the simulation process and are depicted in Figure 9. It should be noted for which it was maintained,
were recorded
that due throughout
to numerical the simulation
difficulties relatedprocess
to mesh andquality
are depicted in Figure 9.could
the simulations It should be accurately
not be noted that
due to numerical difficulties related to mesh quality the simulations could
carried out further. Nevertheless, the simulation results clearly bring out the potential benefits not be accurately carried
of
out further. Nevertheless, the simulation results clearly bring
using the combination of ACRT and dynamic translation for the LPD growth system. out the potential benefits of using the
combination
It can beofobserved
ACRT and dynamic
from Figuretranslation
9 that the for the LPD
dynamic growth
pull profilesystem.
shows an upward trend and is
It can be observed from Figure 9 that the dynamic
about to reach its maximum value. This can be explained on the basis pull profile shows
of the anunderlying
upward trend and of
physics is
about
the LPD to reach
growth itsprocess.
maximum LPD value. This cangrowth
is a solution be explained
technique on the
andbasis
works of the underlying
on the principlephysics of the
of saturation
LPD growth process. LPD is a solution growth technique and works on
and precipitation. The difference in the liquidus equilibrium composition (solubility limit) and the the principle of saturation
and precipitation.
actual concentration Thenear
difference in theinterface
the growth liquidus is equilibrium
the driving composition
force for this (solubility
growthlimit) and The
process. the
actual concentration near the growth interface is the driving force for this
liquidus equilibrium composition near the growth interface is a function of the melt temperature. growth process. The liquidus
equilibrium
During the early composition
hours of near the growth
growth, the meltinterface is a function
temperature of the melt
is relatively hightemperature.
and hence the During the
liquidus
early hours of
equilibrium growth, theis melt
composition also temperature
high. Moreover, is relatively
the actual high and hence
amount the dissolved
of silicon liquidus equilibrium
in the melt
composition is also high. Moreover, the actual amount of silicon
near the growth interface is quite small. Hence, the driving potential for growth dissolved in the melt near and
is high the growth
results
interface
in the increase of the growth velocity. As mentioned earlier, in order to grow axially increase
is quite small. Hence, the driving potential for growth is high and results in the uniform
composition crystal, pull rate should match the growth velocity. Consequently, an upward trend in
the dynamic pull profile is observed in Figure 9. As the growth process continues, dynamic pulling
Crystals 2016, 6, 116 7 of 8

of the growth velocity. As mentioned earlier, in order to grow axially uniform composition crystal,
Crystals
pull 2016,
rate 6, 116 match the growth velocity. Consequently, an upward trend in the dynamic 7pull
should of 8

profile is observed in Figure 9. As the growth process continues, dynamic pulling should result in
should result in an appreciable reduction of the melt temperature and hence the liquidus equilibrium
an appreciable reduction of the melt temperature and hence the liquidus equilibrium composition
composition near the growth interface should also decrease. Also, with the passage of time, the actual
near the growth interface should also decrease. Also, with the passage of time, the actual silicon
silicon concentration in the melt near the growth interface increases significantly. As a result, the
concentration in the melt near the growth interface increases significantly. As a result, the overall
overall driving potential for the growth process should reduce and lead to the reduction of the growth
driving potential for the growth process should reduce and lead to the reduction of the growth velocity.
velocity. Thus, it can be expected that dynamic pull rate should start decreasing after reaching its
Thus, it can be expected that dynamic pull rate should start decreasing after reaching its peak value.
peak value.

Figure 9. Dynamic pull profile between

between tt == 5 h and t = 7 h.

4. Conclusions
Conclusions
This paper
paperbuilds
buildsupon
uponthetheearlier
earlier works
works on on
the the
LPDLPD growth
growth process
process in which
in which the effects
the effects of ACRT of
ACRT and dynamic
and dynamic translation
translation were examined
were examined separatelyseparately
[8,23]. A [8,23]. A comparison
comparison is drawn is to drawn
the casetowhen
the case
the
when
crucibletheiscrucible is only to
only subjected subjected
ACRT. IttoisACRT.
found It is found
that that the combination
the combination of ACRT and of ACRT
dynamic and dynamic
translation
translation
does not alter does
the not
flowalter the flow
structure structureThe
significantly. significantly.
concentrationThedifference
concentration
alongdifference
the growthalong the
interface
growth
is foundinterface is found
to increase to with
slightly increase slightly with
the inclusion the inclusion
of dynamic of dynamic
translation. translation.
It is predicted thatIttemperature
is predicted
that temperature
and hence crystal and hence crystal
composition at the composition
centerline of atthethe centerline
growth of the
interface growth
becomes interface
nearly constantbecomes
with
nearly
the usage constant with pulling.
of dynamic the usage of dynamic
Furthermore, thispulling. Furthermore,
combination leads to this combination
a significant leads to in
improvement a
significant
instantaneous improvement in instantaneous
and time averaged and time
growth velocity averaged
without growth velocity
deteriorating without
the interface deteriorating
flattening effect
the interface
of ACRT. Thisflattening
study shows effect of ACRT.
promising This of
results study shows promising
the combined effects ofresults
ACRT and of the combined
dynamic effects
translation
of
onACRT
the LPD and dynamic
growth. Thetranslation
combined on the and
ACRT LPDdynamic
growth. translation
The combined ACRTneed
processes and dynamic translation
further optimization
processes
to find the need further
best LPD optimization
growth to findrequires
process, which the best LPD systematic
a more growth process, which requires
experimental study. a more
systematic experimental study.
Author Contributions: Mandeep Sekhon carried out the simulations and drafted the paper. Brian Lent conceived
Author
the ideaContributions: Mandeep
and significantly Sekhon
contributed carried
to the out theand
correction simulations and drafted
improvement the paper. Brian
of the manuscript. YanbaoLent
Maconceived
helped in
interpretation
the idea of results,
and significantly critically reviewed
contributed the paper,
to the correction andand made important
improvement of thesuggestions
manuscript.for its improvement.
Yanbao Ma helped
in the interpretation
Conflicts ofauthors
of Interest: The results,declare
critically reviewed
no conflict the paper, and made important suggestions for
of interest.
its improvement.
References
Conflicts of Interest: The authors declare no conflict of interest.
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