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Computational Approach for Epitaxial Polymorph Stabilization through Substrate Selection

机译:通过衬底选择来稳定外延多晶型物的计算方法

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摘要

With the ultimate goal of finding new polymorphs through targeted synthesis conditions and techniques, we outline a computational framework to select optimal substrates for epitaxial growth using first principle calculations of formation energies, elastic strain energy, and topological information. To demonstrate the approach, we study the stabilization of metastable VO2 compounds which provides a rich chemical and structural polymorph space. We find that common polymorph statistics, lattice matching, and energy above hull considerations recommends homostructural growth on TiO2 substrates, where the VO2 brookite phase would be preferentially grown on the a-c TiO2 brookite plane while the columbite and anatase structures favor the a-b plane on the respective TiO2 phases. Overall, we find that a model which incorporates a geometric unit cell area matching between the substrate and the target film as well as the resulting strain energy density of the film provide qualitative agreement with experimental observations for the heterostructural growth of known VO2 polymorphs: rutile, A and B phases. The minimal interfacial geometry matching and estimated strain energy criteria provide several suggestions for substrates and substrate film orientations for the heterostructural growth of the hitherto hypothetical anatase, brookite, and columbite polymorphs. These criteria serve as a preliminary guidance for the experimental efforts stabilizing new materials and/or polymorphs through epitaxy. The current screening algorithm is being integrated within the Materials Project online framework and data and hence publicly available.
机译:为了通过有针对性的合成条件和技术找到新的多晶型物,我们概述了一个计算框架,该方法使用地层能,弹性应变能和拓扑信息的第一原理计算为外延生长选择最佳衬底。为了证明这一方法,我们研究了亚稳态VO2化合物的稳定性,该化合物提供了丰富的化学和结构多晶型物空间。我们发现常见的多晶型统计量,晶格匹配和考虑船体的能量建议在TiO2基底上进行同构生长,其中VO2板钛矿相将优先生长在ac TiO2板钛矿平面上,而co石和锐钛矿结构则有利于相应的ab平面TiO2相。总体而言,我们发现,该模型结合了基材和目标薄膜之间的几何晶胞面积匹配,以及薄膜的应变能密度,与已知VO2多晶型物的金红石异质生长的实验观察结果在质量上吻合。 A和B阶段。最小的界面几何匹配和估计的应变能标准为迄今假设的锐钛矿,板钛矿和钴矿多晶型物的异质结构生长提供了一些关于基质和基质膜取向的建议。这些标准为通过外延稳定新材料和/或多晶型物的实验工作提供了初步指导。当前的筛选算法已集成到材料项目在线框架和数据中,因此可以公开获得。

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