Li Wei, Long Run, Tang Jianfeng, Prezhdo Oleg V
College of Science , Hunan Agricultural University , Changsha 410128 , People's Republic of China.
College of Chemistry, Key Laboratory of Theoretical & Computational Photochemistry of Ministry of Education , Beijing Normal University , Beijing 100875 , People's Republic of China.
J Phys Chem Lett. 2019 Jul 5;10(13):3788-3804. doi: 10.1021/acs.jpclett.9b00641. Epub 2019 Jun 25.
This Perspective summarizes recent research into the excited-state dynamics in lead halide perovskites that are of paramount importance for photovoltaic and photocatalytic applications. Nonadiabatic molecular dynamics combined with time-domain ab initio density functional theory allows one to mimic time-resolved spectroscopy experiments at the atomistic level of detail. The focus is placed on realistic aspects of perovskite materials, including point defects, surfaces, grain boundaries, mixed stoichiometries, dopants, and interfaces. The atomistic description of the quantum dynamics of electron and hole trapping and recombination, provided by the time-domain ab initio simulations, generates important insights into the mechanisms of charge and energy losses and guides the development of high-performance perovskite solar cell devices.
本视角总结了近期对卤化铅钙钛矿中激发态动力学的研究，这对于光伏和光催化应用至关重要。非绝热分子动力学与时域从头算密度泛函理论相结合，能够在原子层面的细节上模拟时间分辨光谱实验。重点关注钙钛矿材料的实际方面，包括点缺陷、表面、晶界、混合化学计量比、掺杂剂和界面。时域从头算模拟提供的电子和空穴俘获与复合量子动力学的原子描述，为电荷和能量损失机制提供了重要见解，并指导高性能钙钛矿太阳能电池器件的开发。
