Coupled-Trajectory Quantum-Classical Approach to Electronic Decoherence in Nonadiabatic Processes

被引:125
|
作者
Min, Seung Kyu [1 ,2 ]
Agostini, Federica [1 ]
Gross, E. K. U. [1 ]
机构
[1] Max Planck Inst Mikrostrukturphys, D-06120 Halle, Germany
[2] Ulsan Natl Inst Sci & Technol, Sch Nat Sci, Dept Chem, Ulsan 689798, South Korea
关键词
MOLECULAR-DYNAMICS; PROTON-TRANSFER; MODEL; PHOTOISOMERIZATION; PHOTODISSOCIATION; INSIGHTS; EVENT;
D O I
10.1103/PhysRevLett.115.073001
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
We present a novel quantum-classical approach to nonadiabatic dynamics, deduced from the coupled electronic and nuclear equations in the framework of the exact factorization of the electron-nuclear wave function. The method is based on the quasiclassical interpretation of the nuclear wave function, whose phase is related to the classical momentum and whose density is represented in terms of classical trajectories. In this approximation, electronic decoherence is naturally induced as an effect of the coupling to the nuclei and correctly reproduces the expected quantum behavior. Moreover, the splitting of the nuclear wave packet is captured as a consequence of the correct approximation of the time-dependent potential of the theory. This new approach offers a clear improvement over Ehrenfest-like dynamics. The theoretical derivation presented in this Letter is supported by numerical results that are compared to quantum mechanical calculations.
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页数:5
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