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THE EFFECT OF VIBRATIONAL


CONVECTION DURING DIRECTIONAL
SOLIDIFICATION UNDER MICROGRAVITY
0. Fedorov 1, V. Demcenko 2
1

Space Research Institute of NAS and SSA of Ukraine (SRI NAS U-SSAU)
2 Paton Electric Welding Institute of NAS of Ukraine

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Space materials science is one of the priorities of


different national and international space programs,
in particular, in the research on the International
Space Station. So, great interest is connected with
obtaining materials in space conditions using melt
solidification methods. However, the development of
space technologies of practical importance meet serious difficulties associated with a lack of understanding of the hydrodynamic processes in weightlessness,
which determines the complex physical and chemical properties of crystalline materials.
Numerous studies of solidification in space conditions showed that in contrast to terrestrial conditions, the relative contribution of surface and bulk
processes significantly changes [1-3]. The physical
processes of heat and mass transfer in microgravity
(including the role of g-jitter) is far from complete
clarity, especially for important practical technology
for producing crystals from the melt. Some authors
consider that this factor is responsible for the difficulty of obtaining crystals with the desired structure
and properties [2]. At the same time insignificant influence of residual heat and mass transfer processes
on the microgravity environment established in other
research, [4]. The idea of the impact on crystallizing
melt by low friquency vibration includes not only the
possibility to suppress unwanted microaccelerations
(g-jitter), but also to actively influence the structure
of the crystallization front. This approach is one of
the most effective ways to influence the quality of
materials produced in flight conditions. Note that
the interest in the problem is not limited to space applications. Fundamentally important to ascertain the
conditions of effective use of vibration exposure as
solidification process control technology.
The subject of this work is the effect of vibrations
on the thermal and hydrodynamic processes during crystal growth using Bridgman and floating zone
techniques, which have the greatest prospect of practical application in space. In the present approach
we consider the gravitational convection, Marangoni

convection (essential with a free surface [5]), as well


as the vibrational effect on the melt for some special
cases. The results of simulation were compared with
some experimental data obtained by the authors using a transparent model substance - succinonitrile
(Bridgman method), and silicon (floating zone
method). Substances used, process parameters and
characteristics of the experimental units correspond
the equipment developed for onboard research and
serve as a basis for selecting optimum conditions vibration exposure as a factor affecting the solidification pattern. The direction of imposing vibrations
coincide with the axis of the crystal, the frequency
are presented by the harmonic Jaw, and the force of
gravity was varied by changing its absolute value.
Schemes of relevant processes are shown in Fig. I.
In the first method (Fig. 1, a), molten zone is
formed in the initial sample (I) using a heater (2).
The melt (3) which is moving along with the heater
provides the workpiece melting and subsequent melt
crystallization. In the Bridgeman method (Fig. I, b),
melting and crystallization were carried out using the
unit, which consists of heater (5), refrigerator (8) and
the heat-insulating layer (7). The unit was moved at a
predetermined speed v along the outer surface of the
ampoule 4, in which the sample is placed.
Mathematical model considered axisymmetric approximation of joint convective-conductive energy
transfer in the system crystal - melt. In the Bridgman scheme only the heat transfer through the gas
gap (6) was taken into account. Heat transfer coefficient was calculated as the reciprocal of the thermal
resistance of the gas gap; on the border with the insulator, it was assumed zero. Zone melting process was
carried out in a vacuum chamber, and surface tension
forces maintained the molten zone; electron-beam
heater as a source of energy was used (experimental
studies of heat flux distribution discussed in [61). The
heat exchange with the environmental the end surfaces of the sample was neglected. At the crystallization and melting fronts perfect contact between the

131


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Fig. 1. Crystal growth using floating zone (a) and Bridgman (b) techniques. 1 - crystal, 2 - heater, 3 - melt, 4 - ampoule, 5 - heater, 6 - gaseous gap, 7 - insulator,
8 - refrigerator, 9 - melt

liquid and solid phases is supposed (the latent heat


was neglected).
Hydrodynamic processes in the melt are described
by the Navier-Stokes equations in the Boussinesq
approximation. The vibration of surface considered
harmonic oscillations ( g (t) =A sin (2mut), w - frequency, A - amplitude of vibrational acceleration);
the vibration and background gravity was considered
operating along the axis of the crystal.
1

The results of numerical experiments


Roating zone method
Thermal and hydrodynamic processes under zone
melting studied for the silicon sample (R = 10 mm
and L = 100 mm) and pulling velocity of broach
annular electron beam heater in the range of 110 m/s. The distribution of the heat flux density
on the surface of the sample was set in accordance
with the experimental data [7] obtained by the split
anode. Numerical study found that the height of
melted zone determined by the power of electronbeam heating and practically does not depend on the
pulling velocity. This fact might be explained by small
values of the thermal Peclet number. The calculated
height of the melt zone on the lateral surface of the
sample is 10 mm, which is within 5 % with the value
measured experimentally. Fig. 2 and 3 show the temperature field and velocity pattern of the melt in qua-

si-stationary state for silicon single crystal grown by


floating-zone method in terrestrial conditions and in
reduced gravity. Motion of the melt is formed mainly
under the influence of buoyancy force: on the free
surface there is the ascending stream which unfolds
in radial direction near the front of melting, forming
a toroidal vortex (shown schematically by large arrows), with the center shifted to the front of melting.
The highest flow rate (3 cm/sec) was observed on the
free surface in the area of maximum heat flow, and at
the axial portions of the melt (because of the sample
cylindricity).
The flow of liquid silicon under reduced gravity is
governed by competitive interaction of thermo-gravitational and thermo-capillary forces, resulting in
secondary vortex formation in the molten zone near
the crystallization front.
At reduced gravity the speed of the melt flow decreases by two orders of magnitude, the height of the
molten zone reduced by 5 % and a convex crystallization front formed.
We considered two specific cases: 1) the resulting acceleration g(t) (superposition of background
acceleration of gravity and vibration acceleration)
in one period of vibration possess the same sign as
the background acceleration; 2) g(t) changes the
sign(vibration of high intensity). It is reasonable to
introduce the constant of the hydrodynamic process

132

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3. Thermal state of the sample (a) and melt flow pattern

floating-zone method for single crystal grown in terrestrial


conditions

(b) for growing a silicon crystal under low gravity

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streamlines (b) near the crystallization front (ampoule radius of
7.5 mm, Bridgeman method, succinonitrile)

---- -------

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- -.>

- - -- -- . -~

-"

-...

..________.,,,,...

-;

'g' which mean the time required for adjustment of


flow from one steady state to another. For numerical evaluation of the value ofTg the acceleration pulse
from g0 = I I 0-3 cm/c 2 up to g0 = 5 I o-3 cm/c 2 was
introduced. Calculations for floating zone give the
value of the constant about one second. In the case of
vibration with the period of one cycle comparable to
'g' vibration disturbances lead to a significant change
in hydrodynamic flow in the molten zone. As the result, the direction of melt circulation of the vortex
flow is reversed during one period of vibration. The
increase in amplitude does not change the structure
of streams. In contrast, at high frequency vibration
( > I 0 Hz) bipolar vibration acceleration averaged,
so that the structure and intensity of convective flows
saved almost the same as in the absence of vibration.

Bridgman Technique

Bridgman method scheme (Fig. I, b) corresponds to the laboratory ground installation, which
is under development for flight experiment. Gravitational convection in the melt is due to the radial
temperature gradient [8]. The attention was primarily paid to the melt streams near the crystallization
front because they determine morphological stability.
For precise description of flow pattern of the liquid
phase, we extracted the certain melt fragment near
crystallization front (Fig. I). Under buoyancy forces
in the liquid phase, global vortex is formed; near the
wall of heater the melt rises to the top of the ampoule
and in the axial part of the ampoule formed descending flow directed to the crystallization front (Fig. 4,

133


g (t)

jHmmnnmnn I

5s

10 s

15 s

20 s

Fig. 5. Temperature fields in the melt under intense vibration


succinonitrile (t = 0 corresponds to the steady state after 6000
s exposure without vibration)

a). As the result of flow braking near the front weak


intensive unsteady vortices appeared. (Fig. 4, b).
Identified in simulation processes unsteady secondary vortices mentioned above were directly observed in the experimental Bridgman setup [6]. To do
this, markers (Lycopodium spores) inserted to melt
succinonitrile, whose motion was fixed and recordered. Observed thus markers can be divided into two
groups. In the first, the trajectories of particle motion
consistent with the circulation of the melt in the global vortex. The second group of markers that localized
near crystallization front oscillates, that may indicate
the existence of secondary vortices predicted by numerical simulation. Simplified experimental scheme
does not allow to get quantitative data on flow rates,
but the nature of the particle motion in front qualitatively indicates unsteady nature of the melt near the
front and the existence of several circulation circuits
near the crystallization front.
Consider the effects of vibration on the hydrodynamics of the melt in the Bridgman scheme at terrestrial conditions A< go- In the presence of vibration
the melt flow localized near the wall of the ampoule
and flow rate in the axial zone significantly weakened. With this circumstance apparently connected
disappearance of oscillating secondary vortices near
the crystallization front, which arise in the absence

of vibration. This effect is observed in the frequency


range cu= 10-50 Hz.
The other situation occurs when the low-frequency vibration oflarge amplitude accelerations (A >g0).
Under these conditions Rayleigh-Taylor instability of
melt flow appears, which is a consequence of alternating of total acceleration.
As illustration the results of numerical calculations Fig. 5 shows the temperature fields (almost correspond to the lines of current) under the following
conditions of vibration g(t) = Asign(2rrwt), A = 9.8
m/s 2 , = 0.05.
The results of calculations show that the sensitivity of hydrodynamic processes to vibration are essentially different for the two characteristic bands:
1) the total acceleration g(t) is of constant sign (A <
< g0); 2) g(t) changes sign for one period of vibration
(A> go).
In the first range of amplitudes numerical experiment demonstrates the effect of suppressing the unsteady vortices for both methods of crystal growth. In
Bridgman installation in the absence of vibration unsteady secondary vortices arises near the crystallization front. Qualitatively, the same result is discussed
in [9] to the same experimental conditions and using the same system succinonitrile -acetone. The
authors obtained a local vortex rotating in the direction counter to the direction of rotation of the global
vortex. Imposition of torsion vibrations led to the
partition of the vortex into two to equalize the concentration in homogeneity along the crystallization
front. In our case, the imposition of axial vibrations
of small amplitude contributed to the disappearance
of secondary vortices in the scheme of Bridgman. A
similar effect is found in the numerical experiment
for the floating zone method when under vibration
exposure additional vortex near the crystallization
(melting) front suppressed, Fig. 4. This effect is observed in both schemes experiment despite the different relative positioning of the axis of symmetry and
the global flow direction of vibration.
In the second case, when the vibration amplitude
exceeds the amplitude of the background effects of
acceleration (A > g 0 ), the pattern changes significantly. Differences in the melt flow pattern for the
techniques under consideration (both in the presence
of vibration impact and without them) are associated
with different thermal conditions in the liquid phase.
In the scheme of Bridgman the melt temperature
increases monotonically along the axial coordinate
from the crystallization temperature to the temperature of the heater, keeping unchanged the sign of the
temperature gradient. In the floating zone method,
the thermal center of the melt is symmetric with
respect to melting and solidification fronts. Conse-

134

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quently, when (A > g 0) and low frequency vibration


occurs in the Bridgman scheme the Rayleigh-Taylor
instability of melt flow appeared, and the configuration and the dynamics of the global vortex is determined by vibration exposure.
Under the same conditions, the circulation of the
melt in the floating zone method of preserving stability and the impact of vibration perturbations limited
to changes the direction of rotation of the vortex.
Thus, in this range of vibration floating zone method
is less sensitive to vibration perturbations.
The experimental techniques under discussion
demonstrated the applicability of vibration to suppress irregular flow near the crystallization front.
These kinds of flows affect not only the macroscopic
distribution of impurities, and microsegregation
structure as well. It is known that the intentional
distribution of impurities before crystallization front
is a powerful way to control the structure and structure- sensitive properties of the crystalline material [ 1O]. Subsequent steps in this direction suggest
keeping variability direction of microgravity vector,
three-dimensional modeling and comparison, with
the actual pattern on the solidification of transparent
substances.

Conclusions
1. Vibration influence on the melt during directional solidification can be an effective means of controlling the solidification structure at different levels
of gravitational convection. If vibration is imposed
along the axis of growing, numerical simulation revealed significant features of the melt flow for Bridgman and floating zone techniques in two characteristic bands of vibration action.
2. Upon application of low-frequency oscillations
of small amplitude (A < g0 ) along the axis of growing
it was found the suppression of the secondary vortex
flows near the crystallization front in both methods
of obtaining crystals.
3. When alternating vibration exposure (A > g )
0
and low frequency vibration Rayleigh-Taylor instability in melt flow is occurred when using Bridgman
method.

4. The same conditions in the floating zone method


are characterized by steady melt flow and the effects
of vibration are reduced only to change the direction
of melt flow. Low sensitivity to the Rayleigh-Taylor
instability is due to the symmetry of the temperature
field of the melt along the axial coordinate.
REFERENCES

l. Ivanov l.l., Zemskov V.S., Kubasov V.N. et al. The melting, crystallization and phase formation in weightlessness. - Moscow: Nauka. - 1979. - 256 p. (in Russian).
2. Zemskov V.S., Rauhman M.R., Sha/imov V.P Influence of
microgravity on the homogeneity of semiconductor crystals grown on spacecraft by directional solidification
methods. Results and perspectives of research in IM ET
RAS 11 Surface. X-rays, synchrotrons and neutron research. - 2001. - No. 9. - P. 41-47 (in Russian).
3. Paton B.E., Asnis E.A., Zabo/otin S.P. et al. Processing of
advanced materials in space 11 Space science and technology. - 2002. - Y. 8. - No. 516. - P. 15-18 (in Russian).
4. Ma:aoni S., Shevtsova V., Mia/dun A. et al. Vibrating liquids in space 11 Europhysics news. - 20 I 0. - Y. 41. No. 6. - P. 14-16.
5. Fedyushkin A., Bourago N., Po/ezhaev V., Lharikov E. The
influence of vibration on hydrodynamics and heat-mass
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Growth. - 2005. - Y. 275. - P. 1557-1563.
6. Ovsiyenko D.E., Fedorov O.P., Temkin D.E., Chemerinsky
G.P. Interaction of solid particles with crystals growing
from the melt 11 Crystallography. - 1987. - V. 32. Issue 5. - P. 1246-1252 (in Russian).
7. Zharikov E. V., Avetisov l.H., Skorenko A. V. et al. Preparation of space experiment on growing crystals by directional solidification method under vibration impact on the
Russian segment of the International Space Station 11
Surface. X-rays, synchrotrons and neutron research. 200 I. - No. 9. - P. 56-62 (in Russian).
8. Gershuny G.Z., Zhukhovitskii E.M. Convective stability of
incompressible fluid. - Moskow: Nauka, 1972. - P. 296
(in Russian).
9. Yu WC., Chen Z.B., Hsu WT. et al. Reversing radial segregation and suppressing morphological instability during
Bridgman crystal growth by angular vibration 11 Journal
of Crystal Growth. - 2004. - Y. 271. - No. 3-4. -

P. 474-480.
IO. Fedorov O.P. Crystal growth processes: kinetics, growth
shapes, heterogeneity. - Kyiv: Naukova Dumka. 2010. - P. 207 (in Russian).

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