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Progress in Chemistry 2012, Vol. 24 Issue (06): 1105-1119 Previous Articles   Next Articles

• Special Issue of Quantum Chemistry •

Approximate Theoretical Methods for Nonadiabatic Dynamics of Polyatomic Molecules

Lan Zhenggang1, Jiushu Shao2   

  1. 1. Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China;
    2. Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, China
  • Received: Revised: Online: Published:
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Nonadiabatic dynamics is ubiquitous in photo-physical and photo-chemical processes. The description of nonadiabatic transitions requires the treatment of coupled electron-nuclei motions. Exact quantum dynamical calculations, due to the insurmountable computational scaling with the size of the system, are only applicable to small molecular systems. In recent years, several approximat methods based on the quantum-classical dynamics were proposed to describe the nonadiabatic dynamics of polyatomic molecular systems. This article provides a concise review of different versions of quantum-classical dynamics approaches including the classical Ehrenfest method, the surface-hopping technique, and the mixed-quantum-classical dynamics in terms of the Winger representation. The pros and cons of the on-the-fly numerical implementation of these schemes combining the ab initio electronic structure calculations are discussed and perspectives on further development of quantum-classical treatment of nonadiabatic dynamics are given. Contents
1 Introduction
2 Hamiltonian and nonadiabatic dynamics
3 Classical Ehrenfest dynamics and surface-hopping dynamics
3.1 Mean-field (or classical Ehrenfest) dynamics
3.2 Surface-hopping dynamics
4 Mixed-quantum-classical dynamics based on wigner representation
5 Conclusions and outlook
Key words: nonadiabatic dynamics, quantum-classical dynamics, on-the-fly dynamics

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