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Comprehensive Study of Sub-Grain Boundaries in Si Bulk Multicrystals

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Comprehensive Study of Sub-Grain Boundaries in Si Bulk Multicrystals 3FTFBSDI Comprehensive Study of Sub-grain Boundaries in Si Bulk Multicrystals A new approach, combination of defects characterization (a) (b) technique using x-ray diffraction and model crystal growth n S o u i 5 t experiments, was applied to investigate the physics of Si b c - e 4 G r i B bulk multicrystals. This provides fundamental knowledge of m 30 d m d / 3 h e t sub-grain boundaries, which is of crucial importance to y n , s w n 20 2 i o t o y r improve crystal quality of Si bulk multicrystals applicable to i t , i G 1 d s / high efficiency solar cells. o m P 10 0 m y - -1 1 Over the past decade, Si bulk multicrystal has emerged 0 as the substrate material for commercial solar cells. To x 0 10 20 Position, x/mm No data accelerate the adoption of solar cells to the world, ongoing 10mm research targets further reductions in energy costs by Fig.2. (a) Cross-section of the sample, (b) distribution of sub- improving material performance, while reducing manufacturing GBs density analyzed by spatially-resolved x-ray diffraction. costs and raw material costs. We approached this issue from deep understanding of crystal physics of Si multicrystals, namely formation mechanism of multicrystalline structure study gave common recognition of sub-GBs as dominant and generation mechanism and properties of defects. The defects of the solar cells. former study lead us to proposal of the dendritic casting Although we were able to investigate structure, distribution method [1]. This article presents the latter study. and electrical properties of sub-GBs in the practical growth Among the defects in the Si bulk multicrystals, we focused method, it is difficult to clarify the generation mechanisms on sub-grain boundaries (sub-GBs) because they are known due to the random and complicated multicrystalline structures. to perform as serious carrier recombination sites for solar We therefore developed model crystal growth using multi cells. To improve the crystal quality of Si multicrystals, we seed crystals with controlled configurations, which provide must comprehensively clarify the physics of sub-GBs, i.e. simplification and systematical control of multicrystalline 1) electrical properties, 2) interaction with impurities and structure. strain, 3) generation, propagation and vanishing mechanisms We found that sub-GBs are generated from grain and 4) influence of grain boundary structure and crystal boundaries and their amount depends on the grain boundary orientations, as illustrated in Fig.1. structure. Furthermore, finite element stress analysis We firstly applied spatially-resolved x-ray diffraction to modeling the experimented multicrystalline structure revealed defects characterization of Si bulk multicrystals to precisely that local shear stress around the grain boundary is the key analyze structure and distribution of sub-GBs. Coordinating driving force of the sub-GBs generation. This research insist their high angular resolution with crystallographic that controlling the grain boundary structure in the practical multicrystalline structure, we succeeded in detecting the sub- growth method is a reliable way to suppress the sub-GBs GBs with small angle difference, as shown in Fig.2. We found generation. that sub-GBs distribute locally and tend to propagate to the These fundamental knowledge of sub-GBs should be growth direction of the ingot across some grain boundaries. applicable to improve the material performance of Si Following the structural characterization, we revealed their multicrystals and promise high efficiency solar cells, although electrical properties they are significantly electrically active and interaction with impurities and vanishing mechanism of sub- work as current leakage sites for solar cells. This fundamental GBs remain to be investigated. References Crucible [1] K. Fujiwara, W. Pan, N. Usami, K. Sawada, M. Tokairin, Electrical properties Y. Nose, A. Nomura, T. Shishido and K. Nakajima, Acta Si melt Mater., 54, 3191 (2006). Directional growth Interaction with impurities [2] N. Usami, K. Kutsukake, K. Fujiwara, and K. Nakajima, J. and strain Appl. Phys., 102, 103504 (2007). [3] K. Kutsukake, N. Usami, K. Fujiwara, Y. Nose, and K. Generation, propagation Nakajima, Mater. Trans., 48, 143 (2007). and vanishing mechanisms Influence of GB structure Contact to GBs and crystal orientation Kazuo Nakajima (Crystal Physics Division) e-mail: [email protected] Fig.1. Research topics of sub-GBs in Si bulk multicrystals. KINKEN Research Highlights 2008 IMR Future Energy / Environmental Materials 27 3FTFBSDI Do Si Single Crystal Balls Save the World from the Global Energy Crisis? Spherical Si single crystals for solar cell substrates have were initially fabricated by jet-dropping method controlling been grown successfully with a yield of almost 100% by temperature of the furnace and pressure of atmosphere in optimizing the supercooling for the recrystallization of Si the system. droplets that were once fabricated by the jet-dropping The as-jetted spherical Si multicrystals were then method. annealed at 1000°C for 2-5 hours in a mixed atmosphere of oxygen and nitrogen to form oxide films (SiO2) on their Among solar cells based on various materials, crystalline surface. Then the spherical Si multicrystals were melted to Si wafer-based photovoltaic modules, i.e., single- and multi- droplets on a silica plate in an atmosphere of oxygen, and the crystalline-Si solar cells, are running ahead, dominating Si droplets were recrystallized to be single crystals at almost 90% of the world’s photovoltaic (PV) production. supercooling of a certain range (Fig. 1). It was found that the Although Si whose Clarke number is 25.8 is the second most recrystallization process occurred unidirectionally in each Si abundant element in the earth crust, a Si-based solar cell is droplet and recrystallized spherical Si single crystals free of not an exception that has to be on the track of the cost defects (dislocations and oxidation induced stacking faults, reduction to expand the market besides aiming at the high OSF) was obtained at a supercooling in the range of 12-42°C conversion efficiency. Spherical Si solar cells attract (Fig. 2). Under this condition, spherical Si single crystals for considerable attention because of the expected feature of solar cell substrates have been grown successfully with a low-waste and low cost fabrication. The advantage of yield of almost 100%. While the crystal growth showed a spherical Si crystals fabricated using dropping method is that dendritic growth mode and only multicrystals was obtained the Si crystals can be fabricated directly from dropping molten when the supercooling was larger than 87°C. Si without any fabrication process that is always required in the production of the Si wafer-based devices. This results in References a great potential for low-waste and low cost fabrication of [1] T. Taishi, T. Hoshikawa, M. Yamatani, K. Shirasawa, X. solar cell substrates. Huang, S. Uda and K. Hoshikawa, J. Cryst. Growth, 306, 452 Increasing the energy conversion efficiency to the (2007). theoretical value has been a super tough challenge to Si [2] T. Hoshikawa, T. Taishi, X. Huang, S. Uda, M. Yamatani, wafer-based PV devices, either single crystalline or K. Shirasawa and K. Hoshikawa, J. Cryst. Growth, 307, 466 multicrystalline. 1 % increment has required bloody efforts of (2007). a number of people, a couple of decades and plenty of [3] X. Huang, S. Uda, H. Tanabe, N. Kitahara, H. Arimune money. Although the conversion efficiency of spherical Si- and K. Hoshikawa, J. Cryst. Growth, 307, 341 (2007). based solar cells is approximately 2-3 % lower than that made from Si wafer-based ones, the increment of the Contact to efficiency is remarkable these years. This is because we Satoshi Uda (Crystal Chemistry Division) have good understanding of degradation of lifetime associated e-mail: [email protected] with crystalline defects [1,2] and we have also found the optimum growth condition in terms of supercooling of a Si droplet for the completely crystalline Si sphere [3]. The recrystallization process of Si droplets was studied. Several hundreds spherical Si multicrystals per second with a diameter of approximately 400 μm in a teardrop shape Increase of supercooling Single crystal growth is possible Multicrystalline growth Approximate Unidirectional growth Almost unidirectional growth unidirectional growth Dendrite growth Melt Melt Melt Melt Crystal Crystal Crystal Crystal Silica Silica Silica Silica ∆T=25˚C ∆T=40˚C ∆T=60˚C ∆T=90˚C Fig. 1 Recrystallization processes in an isolated Si droplet on a silica plate at different Fig. 2 Cross-section of the recrystallized degree of supercooling. spherical single Si crystal obtained under the supercooling of 12 ˚C. 28 Future Energy / Environmental Materials IMR KINKEN Research Highlights 2008 3FTFBSDI Lithium Borohydride: A Light-Weight Hydride Showing “Lithium Super-ionic Conductvity” The electrical conductivity of lithium borohydride (LiBH4) Temperature (K) jumped by three orders of magnitude due to structural -1 423 373 323 10 ) 1 transition from orthorhombic to hexagonal phases at - ) . m -2 u c approximately 390 K. The hexagonal phase exhibited a high 10 . S a ( -3 -1 ( electrical conductivity of the order of 10 Scm . Furthermore, . C σ -3 o 10 S d 7 y t the conductivity obtained from Li-NMR was in good n i D E v i agreement with the measured electrical conductivity. It was t -4 c 10 u 360 380 400 concluded that the electrical conductivity in the hexagonal d n -5 o Temp. (K) phase is due to the Li super-ionic conduction. c 10 l a c i -6 r t 10 Heating Recently, we have reported that the microwave irradiation c e Cooling l E -7 process can be applied to the dehydriding (hydrogen release) 10 reaction of LiBH4, a light-weight hydride [1, 2]. The rate of 2.2 2.4 2.6 2.8 3.0 3.2 -1 the temperature increase in LiBH4 by the microwave 1000/T (K ) irradiation was drastically enhanced above 380 K, which resulted in a fast dehydriding reaction of LiBH4.
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