Spin-mapping approach for nonadiabatic molecular dynamics

The Journal of Chemical Physics
Johan E Runeson, Jeremy O Richardson

Abstract

We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-12 coherent state, we use the Stratonovich-Weyl transform to construct a classical phase space of a spin vector constrained to a spherical surface whose radius is consistent with the quantum magnitude of the spin. In contrast with the singly excited harmonic oscillator basis used in Meyer-Miller-Stock-Thoss (MMST) mapping, the theory requires no additional projection operators onto the space of physical states. When treated under a quasiclassical approximation, we show that the resulting dynamics are equivalent to those generated by the MMST Hamiltonian. What differs is the value of the zero-point energy parameter as well as the initial distribution and the measurement operators used in constructing correlation functions. For various spin-boson models, the results of the method are seen to be a significant improvement compared to both standard Ehrenfest dynamics and linearized semiclassical MMST mapping, without adding any computational complexity.

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Feb 24, 2019·The Journal of Chemical Physics·Maximilian A C SallerJeremy O Richardson

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Citations

Nov 30, 2019·Physical Chemistry Chemical Physics : PCCP·Jie ZhengZhenggang Lan
Jan 24, 2020·The Journal of Chemical Physics·Eric R Heller, Jeremy O Richardson
Mar 3, 2020·The Journal of Chemical Physics·Johan E Runeson, Jeremy O Richardson
Nov 22, 2020·The Journal of Chemical Physics·Jonathan R Mannouch, Jeremy O Richardson
Nov 22, 2020·The Journal of Chemical Physics·Jonathan R Mannouch, Jeremy O Richardson
Mar 6, 2021·The Journal of Physical Chemistry Letters·Xin HeJian Liu
Mar 24, 2021·The Journal of Physical Chemistry Letters·Maximilian A C SallerEitan Geva
Apr 4, 2021·The Journal of Chemical Physics·Sutirtha N Chowdhury, Pengfei Huo
Jul 10, 2021·The Journal of Chemical Physics·Duncan BossionPengfei Huo
Jul 17, 2021·The Journal of Chemical Physics·Haifeng LangPhilipp Hauke
Aug 3, 2021·The Journal of Physical Chemistry. a·Xin HeJian Liu

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