Tashiro Tomoya, Suzuki Hajime, Takahashi Keisuke
Department of Chemistry, Hokkaido University, North 10, West 8, Sapporo 060-0810, Japan.
Phys Chem Chem Phys. 2024 May 15;26(19):14440-14447. doi: 10.1039/d4cp00980k.
128 organic halide perovskites are systematically investigated using high-throughput first principles calculations where Ge and Sn-based materials are searched. The results revealed that all calculated materials exhibited exothermic reactions. Notably, a correlation between the heat of formation and X-site ions is identified. Six specific compounds, namely FA-Ge-I-I-I, FA-Sn-F-I-I, FA-Sn-Cl-I-I, FA-Sn-Br-Br-I, FA-Sn-Br-I-I, and FA-Sn-I-I-I, where FA stands for formamidinium, are found to have a bandgap ranging from 1.0 to 2.0 eV, characterized by a direct bandgap in their band structure. Electronic structure analysis indicated that the CBM (conduction band minimum) is influenced by the B-site p-orbital, while the VBM (valence band maximum) is influenced by the X-site p-orbitals. This study underscores the capability of high-throughput calculations to unveil hidden trends in perovskite materials, offering an effective approach for the exploration of promising perovskite materials.
利用高通量第一性原理计算系统地研究了128种有机卤化物钙钛矿，在此过程中搜索了基于锗和锡的材料。结果表明，所有计算出的材料都表现出放热反应。值得注意的是，确定了生成热与X位离子之间的相关性。发现六种特定化合物，即FA-Ge-I-I-I、FA-Sn-F-I-I、FA-Sn-Cl-I-I、FA-Sn-Br-Br-I、FA-Sn-Br-I-I和FA-Sn-I-I-I（其中FA代表甲脒）的带隙在1.0至2.0 eV之间，其能带结构的特征是直接带隙。电子结构分析表明，导带最小值（CBM）受B位p轨道影响，而价带最大值（VBM）受X位p轨道影响。这项研究强调了高通量计算揭示钙钛矿材料潜在趋势的能力，为探索有前景的钙钛矿材料提供了一种有效方法。
