Time-dependent density-functional theory for open electronic systems  

作　　者：ZHENG Xiao WANG RuLin 

机构地区：[1]Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China [2]Department of Physics, University of Science and Technology of China

出　　处：《Science China Chemistry》2014年第1期26-35,共10页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China(21103157,21233007,and 21322305);the Fundamental Research Funds for Central Universities(2340000034 and 2340000025);the Strategic Priority Research Program(B)of the CAS(XDB01020000)

摘　　要：Time-dependent density-functional theory(TDDFT)has been successfully applied to predict excited-state properties of isolated and periodic systems.However,it cannot address a system coupled to an environment or whose number of electrons is not conserved.To tackle these problems,TDDFT needs to be extended to accommodate open systems.This paper provides a comprehensive account of the recent developments of TDDFT for open systems(TDDFT-OS),including both theoretical and practical aspects.The practicality and accuracy of a latest TDDFT-OS method is demonstrated with two numerical examples:the time-dependent electron transport through a series of quasi-one-dimensional atomic chains,and the real-time electronic dynamics on a two-dimensional graphene surface.The advancement of TDDFT-OS may lead to promising applications in various fields of chemistry,including energy conversion and heterogeneous catalysis.Time-dependent density-functional theory（TDDFT）has been successfully applied to predict excited-state properties of isolated and periodic systems.However,it cannot address a system coupled to an environment or whose number of electrons is not conserved.To tackle these problems,TDDFT needs to be extended to accommodate open systems.This paper provides a comprehensive account of the recent developments of TDDFT for open systems（TDDFT-OS）,including both theoretical and practical aspects.The practicality and accuracy of a latest TDDFT-OS method is demonstrated with two numerical examples：the time-dependent electron transport through a series of quasi-one-dimensional atomic chains,and the real-time electronic dynamics on a two-dimensional graphene surface.The advancement of TDDFT-OS may lead to promising applications in various fields of chemistry,including energy conversion and heterogeneous catalysis.

关 键 词：TIME-DEPENDENT DENSITY FUNCTIONAL theory real-time electronic dynamics hierarchical EQUATIONS of motion 

分 类 号：O572.322[理学—粒子物理与原子核物理]