High-throughput screening of hybrid quaternary halide perovskites for optoelectronics

Abstract

Despite their high efficiency and low manufacturing costs, halide perovskite solar cells suffer from poor stability and lead toxicity, which inhibit their practical use on a large scale. To overcome these challenges, the development of stable and environmentally benign quaternary halide perovskites is a promising solution. Current efforts are mostly focused on inorganic halide double perovskites and are limited to the cubic phase structure. Here we show a high-throughput screening of lead-free hybrid quaternary halide compounds for potential photovoltaic and light-emitting applications. Based on four different structural templates of inorganic quaternary halide compounds, including but not limited to the traditional cubic double perovskite structure, we have built a comprehensive quantum materials repository containing more than 5000 hypothetical hybrid quaternary compounds using large-scale ab initio electronic structure calculation. By using automated decomposition enthalpy calculations and other related material descriptors, we have identified eight candidates as promising light absorbers and two candidates as light emitters. All these candidates exhibit robust material stability and desired optoelectronic properties and can be classified into two different crystal systems including the traditional cubic double perovskite phase and the tetragonal phase. This work demonstrates the necessity of considering all the possible quaternary prototype structures in the high-throughput computational materials design.