Higher-order kinetic expansion of quantum dissipative dynamics: Mapping quantum networks to kinetic networks
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Cao_Higher-order kinetic.pdf
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1.15 MB
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Adobe PDF
Checksum (MD5)
cbc367f8c336ba82751c62b987934bf6
Author(s)
Wu, Jianlan
Cao, Jianshu
Date Issued
July 2013
Journal
The Journal of Chemical Physics
Publisher
American Institute of Physics (AIP)
Citation
Wu, Jianlan, and Jianshu Cao. “Higher-order kinetic expansion of quantum dissipative dynamics: Mapping quantum networks to kinetic networks.” The Journal of Chemical Physics 139, no. 4 (2013): 044102. © 2013 AIP Publishing LLC
Version
Final published version
Abstract
We apply a new formalism to derive the higher-order quantum kinetic expansion (QKE) for studying dissipative dynamics in a general quantum network coupled with an arbitrary thermal bath. The dynamics of system population is described by a time-convoluted kinetic equation, where the time-nonlocal rate kernel is systematically expanded of the order of off-diagonal elements of the system Hamiltonian. In the second order, the rate kernel recovers the expression of the noninteracting-blip approximation method. The higher-order corrections in the rate kernel account for the effects of the multi-site quantum coherence and the bath relaxation. In a quantum harmonic bath, the rate kernels of different orders are analytically derived. As demonstrated by four examples, the higher-order QKE can reliably predict quantum dissipative dynamics, comparing well with the hierarchic equation approach. More importantly, the higher-order rate kernels can distinguish and quantify distinct nontrivial quantum coherent effects, such as long-range energy transfer from quantum tunneling and quantum interference arising from the phase accumulation of interactions.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1063/1.4812781
