Three-dimensional to layered halide perovskites: a parameter-free hybrid functional method for predicting electronic band gaps

This study employed density functional theory with doubly screened dielectric-dependent hybrid (DSH) functional to predict the band gaps of Pb- and Sn-based inorganic and hybrid 3D halide perovskites, as well as layered hybrid perovskites. The DSH functional employs material-dependent mixing parameters derived from macroscopic electronic dielectric constant, and accurately predicts band gaps for 3D perovskites only if structural local disorder is taken into account. For layered hybrid perovskites, we propose using the calculated dielectric constant of the respective 3D perovskites to define the DSH screening. This dataset contains input and output files of all DFT and DSH calculations applied to Pb- and Sn-based layered halide perovskites with various organic spacers and multilayered structures, such as BA series with n =1, 2, 3. The computational framework introduced here provides an efficient parameter-free ab initio methodology suitable for predicting the electronic properties of 3D, layered halide perovskites and their heterostructures, towards modelling materials for advanced optoelectronic devices.

本研究采用密度泛函理论（density functional theory, DFT）结合双屏蔽介电依赖杂化（doubly screened dielectric-dependent hybrid, DSH）泛函，预测铅基和锡基无机及杂化三维卤化物钙钛矿（3D halide perovskites）以及层状杂化钙钛矿的带隙。DSH泛函采用源自宏观电子介电常数的材料依赖混合参数，且仅当考虑结构局部无序时，才能准确预测三维钙钛矿的带隙。对于层状杂化钙钛矿，我们建议使用相应三维钙钛矿的计算介电常数来定义DSH屏蔽。本数据集包含所有DFT和DSH计算的输入与输出文件，这些计算应用于具有不同有机间隔层和多层结构的铅基及锡基层状卤化物钙钛矿，例如n=1、2、3的BA系列。本文介绍的计算框架提供了一种高效、无参数的从头算（ab initio）方法，适用于预测三维及层状卤化物钙钛矿及其异质结构的电子性质，旨在为先进光电器件的材料建模提供支持。