Lead halide perovskites (LHPs) have attracted considerable attention as promising materials for photovoltaic and optoelectronic applications. Intrinsic point defects play an important role in determining the performance of semiconductor devices. LHPs exhibit strong ionic character and unique electronic structure; thus, their defect properties are quite different from conventional covalent bond semiconductors. Understanding the defect science is crucial to the performance optimization of LHP-based devices. State-of-the-art first-principles calculation methods enable one to explore atomistic mechanisms of various defect-related processes, and tremendous efforts from theoretical simulations have provided invaluable insights to the defect physics and defect control of LHPs. In this review, we summarize recent progress, made with the help of theoretical modeling, on atomic-scale understanding about intrinsic point defects and related processes in LHPs. The fundamental properties of intrinsic point defects in LHPs are first introduced, including defect formation energy, charge transition level, and defect tolerance and its origin. A particular emphasis is given to the effects of band edge position on calculated defect properties. The impact of these defects on structural properties, carrier dynamics, and photoluminescence of LHPs is then presented. Advanced strategies to engineer the defects in LHPs are also reviewed, such as growth condition, defect passivation, and doping. Finally, we discuss open issues and outline directions toward a better understanding of defects of LHPs from a theoretical perspective. The goal of the review is to provide a comprehensive summary of atomic-scale understanding of intrinsic point defects in LHPs and to help further related research in the perovskite community.

中文翻译：

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对卤化铅钙钛矿本征点缺陷物理和控制的原子尺度理解

卤化铅钙钛矿（LHPs）作为光伏和光电应用的有前途的材料引起了相当多的关注。本征点缺陷在决定半导体器件的性能方面起着重要作用。LHPs 具有很强的离子特性和独特的电子结构；因此，它们的缺陷特性与传统的共价键半导体有很大不同。了解缺陷科学对于基于 LHP 的设备的性能优化至关重要。最先进的第一性原理计算方法使人们能够探索各种缺陷相关过程的原子机制，理论模拟的巨大努力为 LHP 的缺陷物理和缺陷控制提供了宝贵的见解。在这次审查中，我们总结了最近的进展，在理论建模的帮助下，对 LHP 中的固有点缺陷和相关过程进行原子级理解。首先介绍了 LHP 中本征点缺陷的基本性质，包括缺陷形成能、电荷跃迁能级、缺陷耐受性及其起源。特别强调了带边缘位置对计算缺陷特性的影响。然后介绍了这些缺陷对 LHP 的结构特性、载流子动力学和光致发光的影响。还回顾了设计 LHP 缺陷的高级策略，例如生长条件、缺陷钝化和掺杂。最后，我们讨论了未解决的问题并概述了从理论角度更好地理解 LHP 缺陷的方向。