We investigated applications of the hierarchical equation of motion (HEOM) method to perform high order perturbation calculations of reduced quantum dynamics for a harmonic bath with arbitrary spectral densities. Three different schemes are used to decompose the bath spectral density into analytical forms that are suitable to the HEOM treatment: (1) The multiple Lorentzian mode model that can be obtained by numerically fitting the model spectral density. (2) The combined Debye and oscillatory Debye modes model that can be constructed by fitting the corresponding classical bath correlation function. (3) A new method that uses undamped harmonic oscillator modes explicitly in the HEOM formalism. Methods to extract system-bath correlations were investigated for the above bath decomposition schemes. We also show that HEOM in the undamped harmonic oscillator modes can give detailed information on the partial Wigner transform of the total density operator. Theoretical analysis and numerical simulations of the spin-Boson dynamics and the absorption line shape of molecular dimers show that the HEOM formalism for high order perturbations can serve as an important tool in studying the quantum dissipative dynamics in the intermediate coupling regime.
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7 April 2014
Research Article|
April 04 2014
Reduced quantum dynamics with arbitrary bath spectral densities: Hierarchical equations of motion based on several different bath decomposition schemes
Hao Liu;
Hao Liu
Beijing National Laboratory for Molecular Sciences
, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun, Beijing 100190, China
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Lili Zhu;
Lili Zhu
Beijing National Laboratory for Molecular Sciences
, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun, Beijing 100190, China
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Shuming Bai;
Shuming Bai
Beijing National Laboratory for Molecular Sciences
, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun, Beijing 100190, China
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J. Chem. Phys. 140, 134106 (2014)
Article history
Received:
November 05 2013
Accepted:
March 18 2014
Citation
Hao Liu, Lili Zhu, Shuming Bai, Qiang Shi; Reduced quantum dynamics with arbitrary bath spectral densities: Hierarchical equations of motion based on several different bath decomposition schemes. J. Chem. Phys. 7 April 2014; 140 (13): 134106. https://doi.org/10.1063/1.4870035
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