Wang Yi-Siang, Nijjar Parmeet, Zhou Xin, Bondar Denys I, Prezhdo Oleg V
Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States.
College of Environment and Chemical Engineering, Dalian University, Dalian 116622, P. R. China.
J Phys Chem B. 2020 May 28;124(21):4326-4337. doi: 10.1021/acs.jpcb.0c03030. Epub 2020 May 15.
Motivated by the need to study nonequilibrium evolutions of many-electron systems at the atomistic ab initio level, as they occur in modern devices and applications, we developed a quantum dynamics approach bridging master equations and surface hopping (SH). The Lindblad master equation (LME) allows us to propagate efficiently ensembles of particles, while SH provides nonperturbative evaluation of transition rates that evolve in time and depend explicitly on nuclear geometry. We implemented the LME-SH technique within real-time time-dependent density functional theory using global flux SH, and we demonstrated its efficiency and utility by modeling metallic films, in which charge-phonon dynamics was studied experimentally and showed an unexpectedly strong dependence on adhesion layers. The LME-SH approach provides a general framework for modeling efficiently quantum dynamics in a broad range of complex many-electron condensed-matter and nanoscale systems.
受研究多电子系统在原子从头算水平上的非平衡演化的需求所驱动，这种演化出现在现代器件和应用中，我们开发了一种连接主方程和表面跳跃（SH）的量子动力学方法。林德布拉德主方程（LME）使我们能够有效地传播粒子系综，而表面跳跃则提供了对随时间演化且明确依赖于核几何结构的跃迁速率的非微扰评估。我们使用全局通量表面跳跃在实时含时密度泛函理论中实现了LME-SH技术，并通过对金属膜进行建模展示了其效率和实用性，在金属膜中电荷-声子动力学已通过实验进行了研究，且显示出对粘附层出乎意料的强烈依赖性。LME-SH方法为在广泛的复杂多电子凝聚态物质和纳米尺度系统中高效模拟量子动力学提供了一个通用框架。
