High-Throughput Screening of Flux Materials for Single Crystal Growth by Combinatorial Pulsed Laser Deposition
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High-Throughput Screening of Flux Materials for Single Crystal Growth by Combinatorial Pulsed Laser Deposition R. Takahashi1), T. Tanigawa1), Y. Yamamoto2), Y. Yonezawa1), 3), Y. Matsumoto4), H. Koinuma1), 2), 5) 1) Materials and Structures Laboratory, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan 2) National Institute of Materials Science, 1-1 Namiki, Tsukuba, Ibaragi, 305-0044, Japan 3) Fuji Electric Corporate Research and Development, Ltd, 2-2-1, Nagasaka, Yokohama-city 240-0194, Japan 4) Frontier Collaborative Research Center, Tokyo Institute of Technology, Yokohama 226-8503, Japan 5) CREST, Japan Science and Technology Corporation, Japan
Abstract We propose a new concept and method for high throughput screening of flux materials used in the bulk single crystal growth. The concept of our tri-phase epitaxy has been generalized as the flux-mediated epitaxy with the aid of quick optimization of flux materials in the combinatorial thin-film technology. Here, we report on the successful discovery of a new flux composition of Bi-Ti-Cu-O for the growth of high-quality Bi4Ti3O12 bulk crystal and thin film. 1. Introduction Flux is a material frequently used to assist the growth of single crystals which melt at high temperatures or incongruently. It is also used in thin film growths by vapor-liquid-solid (VLS) [1] and tri-phase epitaxies (TPE) [2]. In the latter process, a single crystal film was grown from a liquid flux film dissolving pulsed-laser ablation species in the gas phase. The appropriate flux compositions and reaction conditions can be predetermined from the relevant thermodynamic phase diagram. The gas species laser-ablated from the target dissolve into a liquid flux layer placed on the film/substrate surface, penetrate to reach the liquid-solid interface, and are condensed into the solid phase under quasi-equilibrium state. The resulting film crystallinity was as high as the corresponding bulk single crystal, as we verified in the fabrication of single crystalline films of high Tc superconducting NdBa2Cu3O7-δ (NBCO) by the TPE process [2]. In view of its principle, TPE can further be
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extended to a variety of materials in general whose single crystals can be grown from the liquid phase. Here we propose this generalized film fabrication process denoted as flux-mediated epitaxy (FME). The key-point of this FME is the appropriate selection, i.e. screening of flux material. A typical example is the Ba-Cu-O self-flux in TPE of NBCO film [2, 3]. Only in a few cases, however, we have detailed phase diagrams which we can use to predict candidate flux materials. Therefore, the first step towards the FME is the experimental screening of flux materials matched well with the single crystals to grow [4]. Here, we report on the verification of combinatorial pulsed laser deposition method for quick optimization of flux composition in the single crystalline Bi4Ti3O12 (BIT) film growth. 2. Experimental Figure. 1 illustrates the typically procedure for FME of BIT film
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