期刊
JOURNAL OF CHEMICAL PHYSICS
卷 143, 期 10, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4930012
关键词
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资金
- Ministry of Science and Technology of China [MOST-2014CB921203]
- National Natural Science Foundation of China [NSFC-21173185]
- Research Fund for the Doctoral Program of Higher Education of China
For a general two-cluster network, a new methodology of the cluster-based generalized quantum kinetic expansion (GQKE) is developed in the matrix formalism under two initial conditions: the local cluster equilibrium and system-bath factorized states. For each initial condition, the site population evolution follows exactly a distinct closed equation, where all the four terms involved are systematically expanded over inter-cluster couplings. For the system-bath factorized initial state, the numerical investigation of the two models, a biased (2, 1)-site system and an unbiased (2, 2)-site system, verifies the reliability of the GQKE and the relevance of higher-order corrections. The time-integrated site-to-site rates and the time evolution of site population reveal the time scale separation between intra-cluster and inter-cluster kinetics. The population evolution of aggregated clusters can be quantitatively described by the approximate cluster Markovian kinetics. (C) 2015 AIP Publishing LLC.
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