凝聚态体系中激发态载流子动力学研究  

Investigation of ab initio nonadiabatic molecular dynamics of excited carriers in condensed matter systems

作　　者：郑镇法 蒋翔 褚维斌 张丽丽[1] 郭宏礼 赵传寓 王亚南 王傲雷 郑奇靖 赵瑾[1,2] Zheng Zhen-Fa;Jiang Xiang;Chu Wei-Bin;Zhang Li-Li;Guo Hong-Li;Zhao Chuan-Yu;Wang Ya-Nan;Wang Ao-Lei;Zheng Qi-Jing;Zhao Jin(Key Laboratory of Strongly-Coupled Quantum Matter Physics,Chinese Academy of Sciences,ICQD/Hefei National Laboratory for Physical Sciences at Microscale,Department of Physics,University of Science and Technology of China,Hefei 230026,China;Department of Physics and Astronomy,University of Pittsburgh,Pittsburgh 15260,America)

机构地区：[1]中国科学技术大学物理系,合肥微尺度物质科学国家研究中心国际功能材料量子设计中心,中科院强耦合量子材料物理重点实验室,合肥230026 [2]匹兹堡大学物理与天文系,匹兹堡15260

出　　处：《物理学报》2021年第17期184-215,共32页Acta Physica Sinica

基　　金：国家自然科学基金(批准号:11974322,11620101003);国家重点研发计划(批准号:2017YFA0204904)资助的课题.

摘　　要：激发态动力学是凝聚态物理中至关重要且富有挑战的科学问题,不仅需要从时间、空间、能量和动量等多个维度来描述,同时还需要考虑各种准粒子的相互作用以及多体效应.本文聚焦凝聚态体系激发态动力学的理论和应用研究,结合含时密度泛函、GW-BSE与面跳跃方法,发展了激发态动力学第一性原理计算软件Hefei-NAMD,构建了可以同时从时间、空间、动量、能量、自旋等多个维度研究凝聚态体系激发态动力学的理论和程序框架,并实现了自旋分辨的GW+real-time BSE(GW+rtBSE)激子动力学.利用这套方法,研究了凝聚态体系激发态动力学的许多问题,包括界面电荷转移动力学、电子空穴复合动力学以及二维TMD材料的谷激子动力学等.这些研究从第一性原理计算的角度,模拟激发态载流子在实空间、能量空间和动量空间的含时演化,为凝聚态体系的激发态动力学及准粒子耦合过程提供了深刻细致的理解.The excited state dynamics is always an important and challenging problem in condensed matter physics.The dynamics of excited carriers can have different relaxation channels,in which the complicated interactions between different quasi-particles come into play collectively.To understand such ultrafast processes,the ab initio investigations are essential.Combining the real-time time-dependent density functional theory with fewest switches surface hopping scheme,we develop time-dependent ab initio nonadiabatic molecular dynamics(NAMD)code Hefei-NAMD to simulate the excited carrier dynamics in condensed matter systems.Using this method,we investigate the interfacial charge transfer dynamics,the electron–hole recombination dynamics,and the excited spin-polarized hole dynamics in different condensed matter systems.Moreover,we combine ab initio nonadiabatic molecular dynamics with GW plus real-time Bethe-Salpeter equation for the spin-resolved exciton dynamics.We use it to study the spin-valley exciton dynamics in MoS_(2).It provides a powerful tool for exciton dynamics in solid systems.The state-of-the-art NAMD studies provide a unique insight into a understanding of the ultrafast dynamics of the excited carriers in different condensed matter systems on an atomic scale.

关 键 词：激发态动力学 Hefei-NAMD 非绝热分子动力学 GW+real-time BSE 

分 类 号：O469[理学—凝聚态物理]