Excited Carrier Dynamics in Condensed Matter Systems Investigated by ab initio Nonadiabatic Molecular Dynamics

Abstract

The excited carrier dynamics generally exist in different physical and chemical processes in condensed matter systems, and it plays crucial role in different research areas such as solar energy conversion and optoelectronics. In the recent 20 years, ab initio nonadiabatic molecular dynamics (NAMD) methods for the condensed matter systems have been developed. This chapter reviews recent theoretical works from J. Zhao’s group of excited carrier dynamics in condensed matter systems using ab initio time-dependent NAMD simulation, including charge transfer dynamics at interfaces, e-h recombination in semiconductors, and spin-valley exciton dynamics in 2D transition metal dichalcogenide material. It introduces the method combining time-dependent Kohn-Sham equation with the surface hopping based on classical-path approximation. From the ab initio NAMD simulation, one can see that the major factor affects the nonradiative e-h recombination is the e-ph coupling. Therefore, different schemes were proposed to tune the e-h recombination rate by changing the e-ph coupling.