论文标题
有机无机杂化卤化物钙钛矿的二阶非线性光学特性的第一原理研究
First-Principles Studies of Second-Order Nonlinear Optical Properties of Organic-Inorganic Hybrid Halide Perovskites
论文作者
论文摘要
有机无机杂化卤化物钙钛矿引发了光伏应用的巨大兴趣。然而，尽管许多这些结构缺乏中心对称性和表现出铁电性，但尚未研究其非线性光学响应。在这项工作中，我们采用了开发的大规模平行，第一原理模拟工具（Archnlo）来探索典型的有机无机混合卤化卤化物钙钛矿家族的二阶非线性光学特性，CH3NH3MX3（M = GE，SN，PB; X = Cl; X = Cl，Br，I）。我们发现这些杂种钙壶表现出第二次谐波产生和线性电形效应。非线性光学效应受阳离子/阴离子和相应带隙的类型和位置的强烈影响。尤其是，CH3NH3SNI3的扭曲的立方相基本上是三斜晶期表现出明显的第二谐波产生和电磁效应，与广泛使用的材料（例如GAAS）相当。有机无机杂交卤化物钙钛矿及其低温，基于溶液的制造铺平的这些二阶光学性能为实现和实施低成本的非线性光学设备的道路铺平了道路。
Organic-inorganic hybrid halide perovskites have ignited tremendous interests for photovoltaic applications. However, their nonlinear optical response has not been studied although many of these structures lack the centrosymmetry and exhibit ferroelectricity. In this work, we employ our developed large-scale parallel, first-principles simulation tool (ArchNLO) to explore second-order nonlinear optical properties of a typical family of organic-inorganic hybrid halide perovskites, CH3NH3MX3 (M= Ge, Sn, Pb; X=Cl, Br, I). We find that these hybrid perovskites exhibit second harmonic generation and linear electro-optic effect. The nonlinear optical effects are strongly influenced by the types and positions of cations/anions and corresponding band gaps. Particularly, the distorted cubic phase, which is essentially triclinic, of CH3NH3SnI3 shows significant second harmonic generation and electro-optic effect, which are comparable with those widely used materials, such as GaAs. These second-order optical properties of organic-inorganic hybrid halide perovskites and their low-temperature, solution-based fabrication pave the way for achieving and implementing nonlinear optical devices with low cost.
