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Title: Finite-temperature time-dependent variation with multiple Davydov states
Authors: Wang, Lu
Fujihashi, Yuta
Chen, Lipeng
Zhao, Yang
Keywords: Coherent states
Wave functions
Issue Date: 2017
Source: Wang, L., Fujihashi, Y., Chen, L., & Zhao, Y. (2017). Finite-temperature time-dependent variation with multiple Davydov states. The Journal of Chemical Physics, 146(12), 124127-.
Series/Report no.: The Journal of Chemical Physics
Abstract: The Dirac-Frenkel time-dependent variational approach with Davydov Ansätze is a sophisticated, yet efficient technique to obtain an accurate solution to many-body Schrödinger equations for energy and charge transfer dynamics in molecular aggregates and light-harvesting complexes. We extend this variational approach to finite temperature dynamics of the spin-boson model by adopting a Monte Carlo importance sampling method. In order to demonstrate the applicability of this approach, we compare calculated real-time quantum dynamics of the spin-boson model with that from numerically exact iterative quasiadiabatic propagator path integral (QUAPI) technique. The comparison shows that our variational approach with the single Davydov Ansätze is in excellent agreement with the QUAPI method at high temperatures, while the two differ at low temperatures. Accuracy in dynamics calculations employing a multitude of Davydov trial states is found to improve substantially over the single Davydov Ansatz, especially at low temperatures. At a moderate computational cost, our variational approach with the multiple Davydov Ansatz is shown to provide accurate spin-boson dynamics over a wide range of temperatures and bath spectral densities.
ISSN: 0021-9606
DOI: 10.1063/1.4979017
Schools: School of Materials Science & Engineering 
Rights: © 2017 American Institute of Physics (AIP). This paper was published in The Journal of Chemical Physics and is made available as an electronic reprint (preprint) with permission of American Institute of Physics (AIP). The published version is available at: []. One print or electronic copy may be made for personal use only. Systematic or multiple reproduction, distribution to multiple locations via electronic or other means, duplication of any material in this paper for a fee or for commercial purposes, or modification of the content of the paper is prohibited and is subject to penalties under law.
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:MSE Journal Articles

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