Role of Dispersive Interactions in Determining Structural Properties of Organic-Inorganic Halide Perovskites: Insights from First-Principles Calculations
Role of Dispersive Interactions in Determining Structural Properties of Organic-Inorganic Halide Perovskites: Insights from First-Principles Calculations
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DOI：
10.1021/jz5012934
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发表时间：
2014-08-07
影响因子：
5.7
通讯作者：
Kronik, Leeor
中科院分区：
文献类型：
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作者：
Egger, David A.;Kronik, Leeor
有机-无机钙钛矿的结构和键合的微观图像对于理解其显着的半导体和光伏特性至关重要。在密度泛函理论处理的基础上，包括自旋-轨道耦合和色散相互作用，我们提供了详细的洞察到铅卤化物钙钛矿的晶体结合和量化的结构特性上的不同类型的相互作用的效果。我们的分析表明，在这些材料中的凝聚力的特点是由各种相互作用，其中包括重要的贡献，从货车范德华相互作用之间的卤素原子和氢键。我们还评估了自旋轨道耦合的作用，并表明它会导致轻微的铅卤化物键合的变化，不显着影响晶格参数。我们的研究结果表明，色散效应的考虑是必不可少的理解一般的有机-无机钙钛矿的结构和键合，特别是提供可靠的理论预测的结构参数。
A microscopic picture of structure and bonding in organic-inorganic perovskites is imperative to understanding their remarkable semiconducting and photovoltaic properties. On the basis of a density functional theory treatment that includes both spin-orbit coupling and dispersive interactions, we provide detailed insight into the crystal binding of lead-halide perovskites and quantify the effect of different types of interactions on the structural properties. Our analysis reveals that cohesion in these materials is characterized by a variety of interactions that includes important contributions from both van der Waals interactions among the halide atoms and hydrogen bonding. We also assess the role of spin-orbit coupling and show that it causes slight changes in lead-halide bonding that do not significantly affect the lattice parameters. Our results establish that consideration of dispersive effects is essential for understanding the structure and bonding in organic-inorganic perovskites in general and for providing reliable theoretical predictions of structural parameters in particular.