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Effects of the hot zone design during the growth of large size multi-crystalline
silicon ingots by the seeded directional solidification process

Article  in  Journal of Crystal Growth · January 2016


DOI: 10.1016/j.jcrysgro.2015.12.045

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Journal of Crystal Growth


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

Effects of the hot zone design during the growth of large size
multi-crystalline silicon ingots by the seeded directional
solidification process
Thi Hoai Thu Nguyen a, Szu-Han Liao a, Jyh-Chen Chen a,n, Chun-Hung Chen b,
Yen-Hao Huang b, Cheng-Jui Yang b, Huang-Wei Lin b, Huy Bich Nguyen c
a
Department of Mechanical Engineering, National Central University, Jhongli 320, Taiwan, ROC
b
Sino-American Silicon Products Inc., Taiwan, ROC
c
Faculty of Engineering and Technology, Nong Lam University, Ho Chi Minh City, Vietnam

art ic l e i nf o a b s t r a c t

Article history: In this study, the installation of insulation blocks in the hot zone is utilized to assist in the growth of
Received 30 September 2015 multi-crystalline silicon ingots with 800 kg of silicon charge using the seeded directional solidification
Received in revised form method. A transient global numerical simulation is carried out to investigate the heat and mass transport
8 December 2015
during growth process. At a higher solidification fraction, lower concavity of the crystal–melt interface
Accepted 24 December 2015
near the crucible wall can be obtained as compared to the standard model. The lowest concavity and
highest energy saving is achieved when insulation blocks are added to the side of a directional solidi-
Keywords: fication block and to the low part of the side insulation. The simulation results for this design also show a
A1. Computer simulation reduction of the melt velocity. The average oxygen concentration is slightly higher along the crystal–melt
A1. Directional solidification
interface, compared to the standard one.
A2. Seed crystals
& 2016 Elsevier B.V. All rights reserved.
B3. Solar cells

1. Introduction significantly affects the conversion efficiency of the solar cells. It is


well-known that the crystal–melt (c–m) interface has a great
Multi-crystalline silicon (mc-Si) solar cells have the highest influence on the orientation of the grain size and thermal stress
market share in the photovoltaics (PV) market. To accomplish the during the growth process. A flat or slightly convex c–m interface
goal of grid parity, the production cost of silicon solar cells must be is beneficial for an outward grain direction and lower thermal
reduced further and their efficiency has to be improved which is stress in the ingot. To obtain this favored interface, it is very imp-
strongly dependent on wafer production and quality. Recently the ortant to reduce heat loss throughout crucible system, especially
growth of large size mc-Si ingots with high quality has become the to control the radial heat flux. Different designs of insulation
main direction of development in wafer production. As the ingot partitions for optimization of the DS process have been studied
weight goes up, however, the rate of increase in the height of the [2–6]. The modeling and experimental results have shown that
ingot becomes less than the rate of increase in the area. Martinuzzi using a partition block can reduce the total heat consumption and
et al. [1] has suggested that the height of large size mc-Si ingots improve the shape of the solidification interface during the growth
produced from the casting process should not exceed 20 cm in process. This design also has a significant effect on the tempera-
ture distribution and thermal stress in the silicon ingots. There is
order to avoid the production of extended defects, the expense of
an optimal increase in velocity with a partition block which allows
crucible use and the production of upgraded silicon waste. Seeded
the fabrication of high quality wafers for high conversion effi-
directional solidification (DS) systems have been developed cap-
ciency mc-Si solar cells. Ding et al. [7] added an insulated crucible
able of obtaining high quality large size mc-Si crystals. In this
susceptor to the DS furnace to preserve seed crystals to produce a
technology, the bottom of the quartz crucible is paved with crys-
consistently flat or slightly convex seed–melt interface during the
talline silicon seed crystals which need to be preserved during the
melting process, while Chen et al. [8] showed that large energy
solidification process in order to prevent nucleation from the
saving can be achieved with the current DS furnace design with
bottom crucible wall. Grain orientation is important because it only minor geometric modifications achieved by adding solid
blocks to the lower corner of the side insulation. “Pivot surfaces”
n
Corresponding author. which were introduced to explain the decrease of total power, act
E-mail address: jcchen@cc.ncu.edu.tw (J.-C. Chen). by redirecting the radiation of the heat flux from the hot zone to

http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045
0022-0248/& 2016 Elsevier B.V. All rights reserved.

Please cite this article as: T.H.T. Nguyen, et al., Journal of Crystal Growth (2016), http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045i
2 T.H.T. Nguyen et al. / Journal of Crystal Growth ∎ (∎∎∎∎) ∎∎∎–∎∎∎

the bottom of the heat exchanger block in the cold zone. The effect incompressible flow. Moreover, all of the solid surfaces are
of the addition of insulation blocks on the impurity distribution assumed to be gray surfaces.
and the melt velocity, however, was not investigated in these The differential equations governing the fluid flow and heat
studies. This modification of the DS furnace changes the tem- transfer are given below.
perature field near the crucible wall and affects convection in the In the fluid flow:
silicon melt. The bottom corner of the crucible is the position ∂ρi  
!
where the heat flux becomes highest, therefore it is necessary to þ ∇ U ρi u i ¼ 0 ð1Þ
∂t
add insulation blocks in this region to reduce the heat loss. Teng
!
et al. [9,10] added an insulation block to prevent heat loss from the ∂ρi ui -  -  -
þ ui U∇ ρi ui ¼ ∇pi þ ∇ U τi þ ρi  ρi;0 U g ð2Þ
heat exchanger block to the gap of the insulation cage, which ∂t
resulted in an interface shape with lower deviation between the  
∂ρi C p;i T i !
crystal edge and the center. They also investigated the thermal þ ∇ U C p;i ρi ui T i ¼ ∇ Uðki ∇T i Þ ð3Þ
∂t
flow field and distribution of oxygen and carbon concentration in
  
the silicon melt. A gas flow guidance device installed in a mc-Si ∂ ρi C p;j !
crystal growth furnace enhanced the motion of argon gas flow þ ∇ U ρi ui C j ¼ ∇ UðDj ∇C j Þ ð4Þ
∂t
near the free surface [11,12]. As a result, a greater amount of SiO
gas is carried out of the furnace by the argon gas. po M
ρg ¼ ; ð5Þ
In this study, a series of transient global numerical simulation RT
are performed with 800 kg of total silicon charge. The effects of where ρ, ρ0, Cp, u, τ, g, T, k, C, D, p0, M and R are density, reference
the addition of insulation blocks to the side of the DS block and/or density, specific heat, velocity, stress tensor, gravitational accel-
to the low part of the side insulation, on the thermal field, the flow eration, temperature, thermal conductivity, concentration, diffu-
field and impurity transport during the growth process are sivity, pressure, molecular weight and universal gas constant,
investigated. Moreover, the enhancement of energy saving by respectively. Subscript i represents argon gas (g) or liquid silicon
these modifications is also discussed. (l), while subscript j stands for silicon monoxide (SiO) in the argon
gas region or oxygen (O) in the melt.
In the heater:
2. Mathematical model _
∇ðkh ∇T h Þ ¼ q; ð6Þ
where q: is the heat generation from the heater.
A schematic illustration of the structure of the seeded indus-
The thermal conditions on the interface between two opaque
trial DS furnace used to grow 800 kg mc-Si ingots is shown in
surfaces are
Fig. 1. The standard furnace is modified by the addition of insu-    
lation block A to the side of the DS block and insulation block B to ∂T ∂T
k ¼ k ; ð7Þ
the low part of the side insulation. During the growth process, the ∂n 1 ∂n 2
temperature at the furnace wall is kept constant at 300 K by a
water-cooling system. The side insulation with block B moves T 1 ¼ T 2: ð8Þ
upward independently. The melting process is controlled in the The radiative heat transfer along the interface between the
studied DS system, so as to preserve the 18mm high seed crystals opaque surface and gas is as follows:
at the crucible bottom. To save simulation time, the real config-    
∂T ∂T
uration of a DS furnace with its square crucible is replaced by a 2D k ¼ k þ σ s εT 4  qin ; ð9Þ
∂n opaque ∂n gas
axially-symmetric model which is cylindrical in shape. This sim-
plification has been widely used in the literature [2–12] and has where σs is the Stefan–Boltzmann constant, ε is the thermal
been validated by experiments [2,5,7]. The silicon melt is con- emissivity and qin is the incoming radiative heat flux.
sidered to be a Newtonian fluid and the deformation of the free The heat fluxes at the c–m interface should satisfy the Stefan
surface is neglected. Argon gas is regarded as an ideal gas with an condition, and the temperature at this interface should be equal to

Fig. 1. Schematic diagram of the seeded industrial DSS furnace.

Please cite this article as: T.H.T. Nguyen, et al., Journal of Crystal Growth (2016), http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045i
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the melting temperature: 3. Results and discussion


   
∂T ∂T
ρcryst un ΔH ¼ k þ k ; ð10Þ In this study, a transient global model is used to investigate the
∂n melt ∂n cryst effects of different modifications of the furnace structure on the
thermal field, the flow field and the distribution of impurity
T ¼ T melt ; ð11Þ during seeded DS process. As can be seen from Figs. 3 and 4, the
simulated heating power consumption and the variation of TC2
where ρcryst is the crystal density, un is the local crystalline rate agree with the experimental results. This good consistency
normal to the c–m interface and ΔH is the latent heat. The normal demonstrates the applicability of the model for the simulation
velocity component at the solid walls and along the free surface of the thermal conditions in a DS furnace. It is clear that the
are set to be zero while the tangential velocity component is equal total heater power increases while TC2 is reduced with the
to the solid wall velocity. In addition, the velocity in the tangential growth time.
direction must satisfy the shear–stress condition: A “W” shaped c–m interface always occurs during the DS
growth process. The severe concavity of the c–m interface near the
∂uτl ∂uτg ∂σ
μl ¼ μg þ ∇τ T; ð12Þ silica crucible wall causes a reduction of the yield and quality of
∂n ∂n ∂T the ingot. During growth, the side insulation moves up and the
where μ is the dynamic viscosity; n and τ are the normal and melt is solidified by heat extraction from the bottom and side wall
tangential directions to the free surface, respectively; σ is the of the crucible support. The occurrence of a concave c–m interface
surface tension of the silicon melt. is due to heat removal from the side wall of the crucible support. It
The boundary condition for oxygen is the same as presented in is obvious that to reduce the concavity of the c–m interface near
our previous study [10]. The temperature at the crystallization the silica crucible wall, the heat flux in the positive radial direction
front is considered to be the silicon melting temperature, 1685 K. It at the c–m interface near the silica crucible wall should be
is assumed that sub-cooling does not occur at the c–m interface in reduced. To achieve this goal, three cases are considered in the
present study. In Case 1, an insulation block (block A) is added to
this work.
the side of the DS block. This block may have a significant effect on
The governing equations for the heat and mass transport dur-
reducing the heat loss in the early stages. With a higher solidifi-
ing seeded DS silicon crystal growth are solved numerically using
cation fraction, however, it is difficult to control the heat flux using
the CGSim (Crystal Growth software) program package of STR
this design because the position of the c–m interface is far away
based on the Finite Volume Method (FVM). The computational
from block A. Thus, heat loss through the crucible side wall
grid for a DS furnace for growing mc-Si ingots is shown in Fig. 2. It
becomes more significant, which leads to the addition of another
is found that the Rayleigh number of the silicon melt, based on the
insulation block to control radial heat flux at the later stages. In
crucible radius, is about O(108). Obviously, the melt flow is in the Case 2, therefore, block B is added at the low part of the side
transient regime because the order of the critical Rayleigh number insulation. The reduction effect of heat extraction in the positive
is O(107) [13]. The Reynolds-averaged Navier-Stoke (RANS) equa- radial direction from this installation can be expected to become
tions with one equation model are used to calculate the transient more significant as the side insulation moves further up (higher
regime in the melt flow that is owed to buoyancy. The Wolfshtein solidification fraction of silicon ingot). Finally, the effect of com-
model is applied to catch the proper increase in the dissipation bining blocks A and B are investigated in Case 3.
rate near the wall given the buoyancy flow in the transient regime. Fig. 5 shows a comparison of the interface shape between the
In the formulation of the turbulent kinetic viscosity, the constant modified cases (Cases 1, 2, 3) and standard case. A “W” shaped c–
Cμ is set to 0.09. The view factors used to determine the total m interface is obtained during the process in all cases. The large
radiative flux coming into a given surface are re-computed when size of the ingot and the growth conditions may result in this
the side insulation and the added solid block move upward. interface shape. As can be seen, these designs can produce sig-
Thermocouple 1 (TC1) is positioned near the top heater while nificant improvement of the concavity of the c–m interface during
thermocouple 2 (TC2) is at the center of the bottom of the crucible the growth process. The best interface shape is obtained in the last
support. TC1 is used as the target function for the unsteady case, combining block A and B. To clearly analyze the effect of
computation to control the heater power output. During the pro- these modifications, the shape of the c–m interface for one half
cess, the power will be adjusted using the well-known PID algo-
rithm to reach the target temperature. The physical properties of
the materials used in the present study are detailed in our pre-
vious papers [10,12]. The added solid blocks have the same ther-
mal properties as the insulation.

Fig. 2. Grid distribution in DS crucible system. Fig. 3. Comparison of simulation and experimental total heater power.

Please cite this article as: T.H.T. Nguyen, et al., Journal of Crystal Growth (2016), http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045i
4 T.H.T. Nguyen et al. / Journal of Crystal Growth ∎ (∎∎∎∎) ∎∎∎–∎∎∎

Fig. 4. Comparison of simulation and experimental TC2.


Fig. 7. Convexity at the central region vs. different solidification fractions for the
standard case and the modified cases.

Fig. 5. C–m interface shape at different solidification fractions for the standard case
and the modified cases. Fig. 8. Concavity near crucible wall vs. different solidification fractions for the
standard case and the modified cases.

Fig. 6. Definition of D_center and D_wall of the c–m interface shape.

side is separated into two parts as indicated in Fig. 6. It can be seen


that there is convexity in the central region and concavity near the
crucible wall, where D_center is defined as the difference between
the crystal center and the minimum point of the c–m interface,
and D_wall is the difference between the highest position (which
always appears at the side crucible wall) and the minimum point.
Figs. 7 and 8 present the variation in the convexity and con-
Fig. 9. Heat loss presented by comparison of TC2 for the standard case and the
cavity of the crystallization front with different solidification
modified cases.
fractions. When only block A (Case 1) is added to the side of the DS
block, lower convexity of the c–m interface near the central region region of DS block and the bottom of the graphite crucible support.
and concavity near the crucible wall are obtained. The addition of In the only block B case (Case 2), however, escape of the radial heat
block A can lead to a significant decrease in heat loss from the side flux from the side crucible wall is prevented. This means that there

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is a reduction in the loss of radial heat at the c–m interface near near the crucible wall section is reduced more significantly in
the crucible wall in the positive direction. The c–m interface comparison with Case 1. It is clear that block A has greater influ-
becomes more convex in the central section and the concavity ence on the convexity while block B has greater influence on the
concavity of the c–m interface during the growth process. There is
not much difference of convexity in the central region but there is
a significant difference of concavity near the crucible wall in Case
3 as compared to Case 1. Moreover, a significant shift in the lowest
position of the interface is obtained between the modified and
standard model (Fig. 5). Fig. 9 shows a decrease in TC2 which
represents heat loss through the crucible bottom. Heat flux mov-
ing out of the crucible system is prevented by the addition of
insulation blocks so TC2 becomes lower in the modified models.
A comparison of heating power consumption, plotted in Fig.10,
is also made to estimate the energy saving of the modifications.
The average reduction in total heater power for Case 1, Case 2, and
Case 3 is 7.4%, 8.7%, and 13%, respectively, as compared to the
standard case. The prevention of heat loss by adding insulation
blocks to the side insulation or/and the side of a DS block lead to
the decrease in heating power consumption. The greatest energy
saving is obtained with the combination of block A and block B.
Saving energy is an important goal for the optimization of crystal
growth systems.
Fig. 10. Total heating power consumption vs. growth time for the standard case The distribution of the oxygen concentration with SiO con-
and the modified cases. centration and flow motion obtained with the standard model at

1500
1800
2100 1
2400
7.0 2 3
7.4
7.8
4
8.2
5
r

10%

z
200
500

800
2.0
2.4 4
2.8 2

r
50%
Fig. 11. Distribution of oxygen and SiO concentration (left, ΔCO ¼0.2 ppma, ΔCSiO ¼ 100 ppma) and flow pattern (right) for the standard model.

Please cite this article as: T.H.T. Nguyen, et al., Journal of Crystal Growth (2016), http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045i
6 T.H.T. Nguyen et al. / Journal of Crystal Growth ∎ (∎∎∎∎) ∎∎∎–∎∎∎

1800
2100
2400
2700

6.6
2+3
7.0
7.4
4
7.8
8.2
5 r

10%

200
500

800 6
2.0
2.8 2.4 2+3
4
3.2

50%
Fig. 12. Distribution of oxygen and SiO concentration (left, ΔCO ¼ 0.2 ppma, ΔCSiO ¼100 ppma) and flow pattern (right) for Case 3.

10% and 50% silicon solidification is presented in Fig. 11. Heat is distribution is strongly dependent on the flow pattern. Fig. 12
transferred to the melt through the crucible wall and radiated to displays the flow structure and the distribution of oxygen and SiO
the free melt surface. This results in the maximum temperature of concentration for Case 3. The temperature at the side crucible wall
the silicon melt appearing at the triple-junction point of the cru- is higher in Case 3 than that in the standard model because the
cible-melt–gas phase. When 10% of the silicon melt is solidified, addition of the insulation block prevents the loss of heat flux from
the flow pattern in the bulk silicon includes five vortexes. Since the side crucible wall. A higher wall temperature results in a
the temperature difference at the free surface near the center greater release of oxygen impurity from the silica crucible wall
region is very small, the shear effect induced by the flow motion of into the silicon melt. The effect of Maragoni convection becomes
the argon gas may be greater than the Marangoni effect in this larger in Case 3, suppressing the shear stress effect induced by the
region. Therefore, a very small clockwise vortex (1) appears near argon gas flow, so vortex (1) does not occur in the center region
the free surface in the center region. Along the free surface, the near the free surface. Since there is a significant reduction in the
temperature near the crucible side wall is higher than that near concavity of the c–m interface in Case 3, in comparison with the
the center. The anti-clockwise vortices (2) and (3) are generated by standard one, the strength of buoyancy vortex (4) becomes weaker
both the buoyancy and thermocapillary forces. In contrast, in the and vortices (2) and (3) get larger. This results in the merging of
bottom part of the melt region, the temperature near the crucible vortices (2) and (3), as shown in Fig. 12a. In Fig. 12b, a small vortex
wall is lower than that near the center, since the c–m interface (6) appears at the free surface near the crucible wall due to the
near the crucible wall is concave. Hence, vortex (4) induced by the enhancement of the thermocapillary force by the higher radial
buoyancy force is clockwise. The small cell (5) occurring near the temperature gradient. Fig. 13 presents a reduction in the melt
c–m interface is due to the large size of the crucible. When the velocity near the crucible side wall due to the decrease in the
solidification fraction reaches 50%, vortices (1), (3) and (5) dis- buoyancy force. The strength of the buoyancy cell is not enough to
appear. The decrease in the melt depth causes a significant carry the oxygen atoms in the lower region of the silicon melt
reduction in the strength and size of cell (2). It then moves towards the free surface for evaporation. The slower flow motion
downward to partially cover the c–m interface while the other one also increases the evaporation of the oxygen atoms that have
(4) covers the free surface, as well as the rest of the region of the remained in the upper region near the crucible wall. There is
solidification interface. As shown in Fig. 11, the oxygen impurity clearly a higher SiO concentration above the free surface and a

Please cite this article as: T.H.T. Nguyen, et al., Journal of Crystal Growth (2016), http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045i
T.H.T. Nguyen et al. / Journal of Crystal Growth ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 7

Fig. 15. Vcr/Gc parameter with different interface positions for the standard case
and the modified cases.

higher oxygen level in the bulk melt for Case 3, as can be seen by
comparing the distribution of the SiO and oxygen concentration in
Fig. 11 and Fig. 12. Fig. 14 presents the average oxygen con-
centration along the c–m interface for the standard case and Case
3. The average oxygen content along the c–m interface decreases
when the solidification fraction gets higher. It gets higher for
Case 3.
The Voronkov ratios Vcr/Gc, defined as the ratio of the crystal-
lization rate to the crystal thermal gradient normal to the c–m
interface, for the standard and modified model, are shown in
Fig.15. It is well-known that the Vcr/Gc parameter stands for the
formation of defects in silicon ingots. As can be seen, this para-
meter is reduced in the modified model as compared to the
standard one. The lowest value is obtained for Case 3. For all
cases, the Vcr/Gc parameter is higher than the critical value (Vcr/
Gc ¼0.12 mm2/min/K [14]). This means that vacancies will occur in
the ingot but the formation of these defects is reduced in Case 1,
Case 2 and Case 3.
Fig. 13. Axial melt velocity at 10mm from the inner crucible wall immersed in the
silicon melt for the standard case and Case 3.

4. Conclusions

The hot zone inside a DS furnace used to grow mc-Si crystal


with 800 kg total charge has been modified by adding insulation
blocks to the side of the DS block or/and at the low part of the side
insulation. The simulation results show that the addition of both
insulation blocks can effectively improve the concavity of the c–m
interface at a higher solidification fraction due to the significant
decrease in heat loss through the side crucible wall. Moreover, this
combination can obtain the highest energy saving in total heating
power consumption. There is a slightly higher average oxygen
concentration along the c–m interface due to the higher wall
temperature and the lower melt velocity as compared to the
standard one. The decrease of Vcr/Gc parameter for the modified
models indicates the lower vacancy formation in the ingot.

Acknowledgments

The authors would like to thank the Ministry of Science and


Fig. 14. Comparison of average oxygen concentration with different solidification Technology of Taiwan, R.O.C, for their support for this study
fractions for the standard case and Case 3. through Grant no. NSC-103-2221-E-008 -038 -MY3.

Please cite this article as: T.H.T. Nguyen, et al., Journal of Crystal Growth (2016), http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045i
8 T.H.T. Nguyen et al. / Journal of Crystal Growth ∎ (∎∎∎∎) ∎∎∎–∎∎∎

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Please cite this article as: T.H.T. Nguyen, et al., Journal of Crystal Growth (2016), http://dx.doi.org/10.1016/j.jcrysgro.2015.12.045i

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