Guo Zhendong, Yuan Man, Chen Gaoyuan, Liu Feng, Lu Ruifeng, Yin Wan-Jian
Department of Applied Physics, Nanjing University of Science and Technology, Nanjing, 210094, China.
College of Energy, Soochow Institute for Energy and Materials InnovationS (SIEMIS) and Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow University, Suzhou, 215006, China.
Adv Sci (Weinh). 2024 May;11(20):e2305799. doi: 10.1002/advs.202305799. Epub 2024 Mar 19.
Lead halide perovskites with superior optoelectrical properties are emerging as a class of excellent materials for applications in solar cells and light-emitting devices. However, perovskite films often exhibit abundant intrinsic defects, which can limit the efficiency of perovskite-based optoelectronic devices by acting as carrier recombination centers. Thus, an understanding of defect chemistry in lead halide perovskites assumes a prominent role in further advancing the exploitation of perovskites, which, to a large extent, is performed by relying on first-principles calculations. However, the complex defect structure, strong anharmonicity, and soft lattice of lead halide perovskites pose challenges to defect studies. In this perspective, on the basis of briefly reviewing the current knowledge concerning computational studies on defects, this work concentrates on addressing the unsolved problems and proposing possible research directions in future. This perspective particularly emphasizes the indispensability of developing advanced approaches for deeply understanding the nature of defects and conducting data-driven defect research for designing reasonable strategies to further improve the performance of perovskite applications. Finally, this work highlights that theoretical studies should pay more attention to establishing close and clear links with experimental investigations to provide useful insights to the scientific and industrial communities.
具有优异光电性能的卤化铅钙钛矿正成为一类用于太阳能电池和发光器件的优秀材料。然而，钙钛矿薄膜通常表现出大量的本征缺陷，这些缺陷可作为载流子复合中心，从而限制基于钙钛矿的光电器件的效率。因此，了解卤化铅钙钛矿中的缺陷化学在进一步推进钙钛矿的开发中起着重要作用，这在很大程度上是通过依靠第一性原理计算来实现的。然而，卤化铅钙钛矿复杂的缺陷结构、强烈的非谐性和柔软的晶格给缺陷研究带来了挑战。从这个角度出发，在简要回顾当前关于缺陷计算研究的知识的基础上，这项工作专注于解决未解决的问题并提出未来可能的研究方向。这一观点特别强调了开发先进方法以深入理解缺陷本质以及进行数据驱动的缺陷研究以设计合理策略来进一步提高钙钛矿应用性能的必要性。最后，这项工作强调理论研究应更加注重与实验研究建立紧密而明确的联系，以便为科学界和工业界提供有用的见解。
