化学动力学中的非绝热过程及其理论研究
摘要
Electronic transitions induced by nuclear motions are called nonadiabatic processes. In recent years, numerous experimental studies showed ultrafast nonadiabatic processes widely exist in molecular systems. The theoretical treatment of nonadiabatic dynamics is extremely challenging, because electron-nuclei coupled motions induce the breakdown of the Born-Oppenheimer approximation. We try to summarize the state-of-art theoretical understanding of nonadiabatic dynamics in recent years. Particularly, we wish to briefly discuss the development of theoretical methods (nonadiabatic dynamics approaches and electronic-structure methods) and review the theoretical understanding of nonadiabatic dynamics of various typical systems (photostability of biological molecules, photoisomerization, intersystem crossing, excited-state energy and electron transfers). Although the great progress has been achieved in the theoretical treatment of nonadiabatic dynamics, it is still very challenging to investigate complex systems with large number of degrees of freedom. In the future, the further development in this field should largely rely on the joint progress of dynamics theory, quantum chemistry and computer technology.