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Journal of Crystal Growth 360 (2012) 76–80

Contents lists available at SciVerse ScienceDirect

Journal of Crystal Growth


journal homepage: www.elsevier.com/locate/jcrysgro

Numerical studies on a type of mechanical stirring in directional


solidification method of multicrystalline silicon for photovoltaic applications
S. Dumitrica a, D. Vizman a,n, J.-P. Garandet b, A. Popescu a
a
Physics Faculty, West University of Timisoara, Bd. V. Parvan 4, 300223 Timisoara, Romania
b
CEA, LITEN, Institut National de l’Energie Solaire, 50 Avenue du Lac Léman, 73377 Le Bourget du Lac Cedex, France

a r t i c l e i n f o a b s t r a c t

Available online 18 January 2012 With the increase of the dimensions of multicrystalline silicon ingots obtained by directional solidification,
Keywords: it is necessary to propose new methods allowing to tailor the convection within the melt adapted for large
A1. Computer simulation scale crucibles. Melt stirring is widely used to influence the melt flow and the shape of the solid–liquid
A1. Fluid flow interface in crystal growth processes.
A1. Stirring Therefore, the objective of this paper is to study by numerical methods the forced convection induced
A2. Ingot casting method by an idealized stirrer on the melt flow and interface shape in a directional solidification furnace in order to
B2. Multicrystalline silicon see the potential of such a device.
Numerical simulations were carried out for a pilot scale furnace configuration (38  38  40 cm3). The
computational domain used for the 3D-simulations consists of silicon melt and crystal. Time-dependent
computations were carried out with the software STHAMAS3D.
It was obtained that, the stirrer’s rotation leads to a strong increase of both the melt convection and the
S–L interface deflection.
& 2012 Elsevier B.V. All rights reserved.

1. Introduction raising again the question of whether turbulent flows take


place during solidification. An increased convection may also
According to a study [1] made by European Association of have an impact on the cohesion of the crucible coatings: the
Photovoltaic industry, the solar energy could cover till 2020, up to release of particles within the melt should be avoided since
12% of needs of electric energy of European Union. Crystalline they may act as sites favoring the nucleation of spurious grains
silicon, either mono- or multi-crystalline, currently represents ahead of the solidification front and causes severe mechanical
almost 90% of the photovoltaic energy production. Directional stresses if they are engulfed in the growing crystal [2–4];
solidification is the technique with highest market share in the – with the use of feedstock of lesser purity, the achievement of a
production of crystalline silicon for photovoltaic applications. total mixing regime in the melt allowing for an optimal segrega-
In the frame of the race towards cost reduction, two major trends tion of the impurities at the end of the ingot while keeping a high
will shape the developments of the field in the years to come: growth rate for productivity reasons will require careful adjust-
ments [5,6].
– ever increasing sizes: today’s research is on 800 kg ingots and
1  1 m2 crucible sizes, but there is no reason to think that this Due to skin depth issues, electromagnetic control of melt flow
represents an ultimate limit;
can have a limited effect on heat and mass transfer in the center
– use of silicon feedstock of lesser purity than standard electro- region of large scale Si ingots grown from melt [7,8]. It is therefore
nic grade material.
necessary to analyze new methods allowing the tailoring of the
In this frame, a number of issues that had been tackled empiri- convection within the melt adapted for large scale silicon ingots.
cally in the past will need to be addressed using a scientific approach. One option could be mechanical stirring using a stirrer made of the
Among them, the control of convection will become a major issue: same material as the crucible. Some studies have investigated the
effect of mechanical stirring upon the properties of different alloys
– with the advent of large scale crucibles, the implementation (Al–Si and Mg alloy), during various casting processes [9–12].
of an unidirectional heat flux will be increasingly difficult, In order to analyze the potential of mechanical stirring on the
resulting in a detrimental curvature of the solid–liquid interface, melt control in directional solidification of multicrystalline silicon
numerical simulations are carried on in the present contribution.
n
Corresponding author. Tel./fax: þ 40 256 592 250. It is well established that numerical simulation can play an
E-mail address: vizman@physics.uvt.ro (D. Vizman). important role in the design and optimization of crystal growth

0022-0248/$ - see front matter & 2012 Elsevier B.V. All rights reserved.
doi:10.1016/j.jcrysgro.2012.01.011
S. Dumitrica et al. / Journal of Crystal Growth 360 (2012) 76–80 77

processes because of their low cost and high flexibility in model- In the present work, where the objective is on the understanding
ing various experimental configurations [13,14]. of the stirrer influence on melt flow and interface shape, the
Our aim is to study by numerical methods the forced convec- following assumptions have been made:
tion induced by an idealized stirrer on the melt flow and interface
shape in directional solidification method of multicrystalline a) the form of the stirring device was considered to be cylindrical, of
silicon in order to see the potential of such a device. diameter D¼8 cm, centered on the domain axis and immersed in
Numerical simulations were carried out for a pilot scale the melt to a depth of 15 cm. It can be rotated at different
furnace configuration, that correspond to the standard G2 (second angular velocities during the crystal growth process (Fig. 1);
generation) of the photovoltaic industry. State of the art industrial b) the stirring device is not considered as being ‘‘physically’’ in
practice now focuses on G5 and G6 (5th and 6th generations) the melt, but the effect of its rotation has been considered
crucibles, but the G2 size is still used in pilot scale furnaces as by imposing an azimuthal volume force in each point of the
representative of the industrial conditions [15]. In addition to region where the stirrer is located. The force has the following
crystal growth issues, the G2 size also has potential for applica- form:
tions in the purification of upgraded metallurgical grade silicon ! ! !
by directional solidification (38  38  40 cm3). f rot ¼ ðroo Þ  r ð6Þ
!
where o is the angular velocity corresponding to the stirrer
2. Numerical model !
rotation. Defining r ¼ 9 r 9 as the distance of that point to the
stirrer’s axis, as shown in Fig. 2, the module of the stirring
Numerical simulation has been made for a pilot scale furnace
force can be expressed as:
with crucible dimensions of 38 cm  38 cm  40 cm. The compu-
Therefore:
tational domain used for the local 3D-simulations consists of (
silicon melt and crystal and is shown in Fig. 1. Time-dependent ! rro2 , r rD=2
computations were carried out with the software STHAMAS3D. j f rot j ¼ ,
0, r 4 D=2
The melt flow is described by the three-dimensional equations
for mass, momentum and heat transfer, taking into account the were D is the stirrer diameter.
Boussinesq approximation for a Newtonian incompressible fluid:
The heat transfer in the solid is governed by conduction, and at
r! u ¼0 ð1Þ
the liquid–solid interface latent heat production has been con-
! sidered for the given crystallization velocity:
@u ! ! ! !  
r þ rð u rÞ u mr2 u ¼ rp f ð2Þ
@t kS rT S kLrT L ¼ vg rS DH ð7Þ
 
@T ! 2 where kS and kL are the thermal conductivities of solid and melt,
rC p þð u rÞT kr T ¼ 0 ð3Þ vg is the pulling rate set to 10 mm/h for our simulations and DH is
@t
the latent heat.
!
where r is the fluid density, u is the flow velocity, p the pressure, The temperature has been considered fixed at the crucible walls,
!
C p the heat capacity, k the thermal conductivity, f is source term corresponding to a temperature gradient of 10 K/cm in the crystal
for the momentum. The source term can be written as: and 3 K/cm in the melt. At the free surface of the melt a radiative
! ! ! heat exchange with the environment was taken into account. The
f ¼ f nat þ f rot ð4Þ reference temperature for radiation was set to 1785 K.
The time dependent calculations have been made using STHA-
with:
MAS3D software which was developed at the Crystal Growth
Laboratory in Erlangen and it was already used for convection
! ! simulations in Czochralski [14] and directional solidification config-
f nat ¼ rðT ref Þ g bðTT ref Þ ð5Þ
urations [13]. STHAMAS3D’s numerical procedure is based on the
– corresponding to the component of natural convection, and finite volume method, and the implicit Euler method is used for
! calculating the time integrals. No turbulence models are considered
f rot , corresponding to the component of forced convection
produced by the stirrer. in our numerical scheme.

Melt
H Vt

Crystal
B
L
! ! ! !
Fig. 2. Azimuthal volume force: f rot ¼ ðroo Þ  r , where o is the angular velocity
Fig. 1. Schematic view of the crucible and the stirrer. !
and r is the radius.
78 S. Dumitrica et al. / Journal of Crystal Growth 360 (2012) 76–80

The computational block-structured non-orthogonal grid is in comparison with a cylindrical crucible configuration where
subdivided in two blocks with a local grid refinement at the walls they have a complete toroidal shape.
in order to resolve the boundary layers. The mesh in the melt Even at a low frequency of 5 rpm the effect of melt mixing near
consists typically of 350.000 control volumes, which is sufficient S–L interface can be seen (Fig. 3(b)) and the melt flow has a
to resolve the main features of the flow. In [13] the dependence of stronger azimuthal component. Increasing the stirrer rotation, the
z-component of the flow velocity along the central vertical line for mixing effect near the S–L interface increases as can be seen in
different grid size was analyzed. It was showed that at this grid Fig. 3(c) and (d).
refinement level there is almost no dependence of the solution on In a vertical section in the middle of the computational domain
the size of the control volume. (xOz section), when no stirrer rotation is present, there are two
To determine the solid–liquid interface position and form, use main convection zones: one near the S–L interface and one near
has been made of a phase tracking procedure, according to which the melt free surface (Fig. 4(a)). The driving forces in these
after every time step the grid is deformed in such way that the areas are generated by the lateral gradients at the S–L interface
boundary between melt and solid fits to the melting temperature. In (associated to the interface deflection) and at the free surface,
order to obtain a realistic solution starting from an arbitrary initial which are a consequence of the global heat transfer in the
solution at least 800 s real time should be computed with a time furnace.
step of 0.1 s. Therefore the 3D time dependent simulations have When the mixing device is rotated with a frequency of 5 rpm,
been made on a 20 nods HP-AND-Opteron 2.2 GHz cluster. the mixing in the vertical section is improved, but the melt flow
remains mostly stratified (Fig. 4(b)). Increasing the rotation
frequency, the asymmetry of melt flow in vertical section
3. Results and discussions increases and the melt mixing is much stronger (Fig. 4(c) and (d)),
with maximum velocity for 0 rpm: 0.7 cm/s; 5 rpm: 5 cm/s; 10 rpm:
Computations have been performed for the melt flow and for 10 cm/s; 30 rpm: 25.5 cm/s. This effect should be understood having
the rotation frequencies of the stirring device of 5, 10, 20, 30, in mind that the interface shape and deflection is changing with
40 rpm and a pulling velocity of 10 mm/h. stirrer rotation rate (see Fig. 6).
In Fig. 3, particle tracking plots are presented in a region Also it has to be noted that at rotation speeds which correspond
located 7 cm above the S–L interface. Paraview software was used to frequencies of 5, 10 and 20 rpm there is a direct proportionality
for visualization and a point seed in the center of the region was between the frequency and the maximum azimuthal velocity (Vmax)
considered. In the absence of stirrer rotation, as the crucible has a of the melt (Fig. 5). In order of magnitude terms, this is indicative of
squared form, it is expected to see this reflected in the melt flow a balance between the azimuthal force, producing the motion, and
symmetry. This appears clearly in Fig. 3(a). In this case, convec- the inertia:
tion rolls (cylindrically shaped), generated by the convexity of the
s-l interface, and characteristic of Bridgman or Vertical Gradient
Freeze methods, can be observed in the main part of the cavity. ! ! V 2max
ro2 D=2 ¼ r9ð V max rÞ V max 9  r ð8Þ
Near the corners, these convection rolls have a different behavior d

Fig. 3. Particle tracking at 7 cm above the S–L interface for different rotation rate of the stirrer: (a) 0 rpm, (b) 5 rpm, (c) 10 rpm and (d) 30 rpm.
S. Dumitrica et al. / Journal of Crystal Growth 360 (2012) 76–80 79

Fig. 4. Velocity field in xOz section for different rotation rate of the stirrer: (a) 0 rpm, (b) 5 rpm, (c) 10 rpm and (d) 30 rpm.

Fig. 6. Interface deflection for different rotation rates.


Fig. 5. Relation between Vmax and the rotation rate.

the simulation results, the predictions of Eq. (9) are reported in Fig. 5
where d is the length scale of primary inertial vortex. These yields: along with the experimental values. The agreement between the
two sets of data is excellent below 20 rpm, but some deviations with
V 2max  o2 ðdD=2Þ ð9Þ
the proportionality law are observed at frequencies of 30 and
40 rpm (Fig. 5). Also the axis of the main vortex is no more along
Assuming d is independent of o, the proportionality between the center axis of the crucible for higher rotation frequency
Vmax and o follows. Taking d¼D/2, a reasonable choice considering (430 rpm) (see Fig. 3). An explanation of this fact might be the
80 S. Dumitrica et al. / Journal of Crystal Growth 360 (2012) 76–80

counterbalance of the azimuthal force by natural convection, which Acknowledgments


becomes more intense as the interface deflection increases (Fig. 6),
or possibly by the fact that the modification of the flow structure Financial support under the grant CONSIL C1-02 in the frame of
impacts on the value of d. Nevertheless, the agreement with the the cooperation agreement between IFA-Romania and CEA-France.
predictions of the simple scaling law remains acceptable. This work was supported by the strategic grant POSDRU/
Let us now come back on the influence of stirring on the CPP107/DMI1.5/S/78421, Project ID78421 (2010), co-financed by
interface shape. If no stirrer rotation is present, the S–L interface the European Social Fund within the Sectorial Operational Pro-
is slightly convex toward the melt. With the increase of stirrer gram Human Resources Development 2007–2013.
rotation the interface deflection increases (Fig. 6). For 5 rpm the Dr. Jochen Friedrich and Prof. Dr. G. Mueller, Fraunhofer
increase of interface deflection is rather small but for 40 rpm Institute IISB, for the permanent support in the development of
the interface deflection is almost 6 cm. This behavior is due to the STHAMAS3D software.
stronger convection in the vertical section, generated by the
higher stirrer rotations, which facilitate the transport of hot melt
from upper parts to the S–L interface.
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