Communication: Note on detailed balance in symmetrical quasi-classical models for electronically non-adiabatic dynamics

doi:10.1063/1.4916945

Title: Communication: Note on detailed balance in symmetrical quasi-classical models for electronically non-adiabatic dynamics

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Abstract

It is noted that the recently developed symmetrical quasi-classical (SQC) treatment of the Meyer-Miller (MM) model for the simulation of electronically non-adiabatic dynamics provides a good description of detailed balance, even though the dynamics which results from the classical MM Hamiltonian is “Ehrenfest dynamics” (i.e., the force on the nuclei is an instantaneous coherent average over all electronic states). This is seen to be a consequence of the SQC windowing methodology for “processing” the results of the trajectory calculation. For a particularly simple model discussed here, this is shown to be true regardless of the choice of windowing function employed in the SQC model, and for a more realistic full classical molecular dynamics simulation, it is seen to be maintained correctly for very long time.

Authors:

Miller, William H., E-mail: millerwh@berkeley.edu; Cotton, Stephen J., E-mail: StephenJCotton47@gmail.com ^[1]

Department of Chemistry and Kenneth S. Pitzer Center for Theoretical Chemistry, University of California and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 (United States)

Publication Date:: Tue Apr 07 00:00:00 EDT 2015

OSTI Identifier:: 22415593

Resource Type:: Journal Article

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 142; Journal Issue: 13; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606

Country of Publication:: United States

Language:: English

Subject:: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; COMPUTERIZED SIMULATION; DETAILED BALANCE PRINCIPLE; ELECTRONIC STRUCTURE; HAMILTONIANS; MATHEMATICAL MODELS; MOLECULAR DYNAMICS METHOD; PROCESSING; TRAJECTORIES

Citation Formats


                    Miller, William H., E-mail: millerwh@berkeley.edu, and Cotton, Stephen J., E-mail: StephenJCotton47@gmail.com. Communication: Note on detailed balance in symmetrical quasi-classical models for electronically non-adiabatic dynamics.  United States: N. p., 2015. 
        Web.  doi:10.1063/1.4916945.

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                    Miller, William H., E-mail: millerwh@berkeley.edu, & Cotton, Stephen J., E-mail: StephenJCotton47@gmail.com. Communication: Note on detailed balance in symmetrical quasi-classical models for electronically non-adiabatic dynamics.  United States.  https://doi.org/10.1063/1.4916945

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                    Miller, William H., E-mail: millerwh@berkeley.edu, and Cotton, Stephen J., E-mail: StephenJCotton47@gmail.com. 2015.  
        "Communication: Note on detailed balance in symmetrical quasi-classical models for electronically non-adiabatic dynamics".  United States.  https://doi.org/10.1063/1.4916945.

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@article{osti_22415593,

  title        = {Communication: Note on detailed balance in symmetrical quasi-classical models for electronically non-adiabatic dynamics},

  author       = {Miller, William H., E-mail: millerwh@berkeley.edu and Cotton, Stephen J., E-mail: StephenJCotton47@gmail.com},

  abstractNote = {It is noted that the recently developed symmetrical quasi-classical (SQC) treatment of the Meyer-Miller (MM) model for the simulation of electronically non-adiabatic dynamics provides a good description of detailed balance, even though the dynamics which results from the classical MM Hamiltonian is “Ehrenfest dynamics” (i.e., the force on the nuclei is an instantaneous coherent average over all electronic states). This is seen to be a consequence of the SQC windowing methodology for “processing” the results of the trajectory calculation. For a particularly simple model discussed here, this is shown to be true regardless of the choice of windowing function employed in the SQC model, and for a more realistic full classical molecular dynamics simulation, it is seen to be maintained correctly for very long time.},

  doi          = {10.1063/1.4916945},

  url          = {https://www.osti.gov/biblio/22415593},
  journal      = {Journal of Chemical Physics},

  issn         = {0021-9606},

  number       = 13,

  volume       = 142,

  place        = {United States},

  year         = {Tue Apr 07 00:00:00 EDT 2015},

  month        = {Tue Apr 07 00:00:00 EDT 2015}

}

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