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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
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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
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
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
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 ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 3
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. 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.
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 ∎ (∎∎∎∎) ∎∎∎–∎∎∎ 5
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
Acknowledgments
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 ∎ (∎∎∎∎) ∎∎∎–∎∎∎
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