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Title: The Symmetrical Quasi-Classical Model for Electronically Non-Adiabatic Processes Applied to Energy Transfer Dynamics in Site-Exciton Models of Light-Harvesting Complexes

Journal Article · · Journal of Chemical Theory and Computation
 [1];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
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In a recent series of papers, it has been illustrated that a symmetrical quasi-classical (SQC) windowing model applied to the Meyer–Miller (MM) classical vibronic Hamiltonian provides an excellent description of a variety of electronically non-adiabatic benchmark model systems for which exact quantum results are available for comparison. In this study, the SQC/MM approach is used to treat energy transfer dynamics in site-exciton models of light-harvesting complexes, and in particular, the well-known 7-state Fenna–Mathews–Olson (FMO) complex. Again, numerically “exact” results are available for comparison, here via the hierarchical equation of motion (HEOM) approach of Ishizaki and Fleming, and it is seen that the simple SQC/MM approach provides very reasonable agreement with the previous HEOM results. Finally, it is noted, however, that unlike most (if not all) simple approaches for treating these systems, because the SQC/MM approach presents a fully atomistic simulation based on classical trajectory simulation, it places no restrictions on the characteristics of the thermal baths coupled to each two-level site, e.g., bath spectral densities (SD) of any analytic functional form may be employed as well as discrete SD determined experimentally or from MD simulation (nor is there any restriction that the baths be harmonic), opening up the possibility of simulating more realistic variations on the basic site-exciton framework for describing the non-adiabatic dynamics of photosynthetic pigment complexes.

Research Organization:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
AC02-05CH11231; CHE-1464647
OSTI ID:
1379141
Journal Information:
Journal of Chemical Theory and Computation, Vol. 12, Issue 3; ISSN 1549-9618
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 76 works
Citation information provided by
Web of Science

References (14)

A classical analog for electronic degrees of freedom in nonadiabatic collision processes journal April 1979
Symmetrical Windowing for Quantum States in Quasi-Classical Trajectory Simulations journal March 2013
Symmetrical windowing for quantum states in quasi-classical trajectory simulations: Application to electronically non-adiabatic processes journal December 2013
On the Theory of Oxidation‐Reduction Reactions Involving Electron Transfer. I journal May 1956
Symmetrical windowing for quantum states in quasi-classical trajectory simulations: Application to electron transfer journal August 2014
Communication: Note on detailed balance in symmetrical quasi-classical models for electronically non-adiabatic dynamics journal April 2015
A Symmetrical Quasi-Classical Spin-Mapping Model for the Electronic Degrees of Freedom in Non-Adiabatic Processes journal August 2015
Unified treatment of quantum coherent and incoherent hopping dynamics in electronic energy transfer: Reduced hierarchy equation approach journal June 2009
Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature journal October 2009
Semiclassical Description of Nonadiabatic Quantum Dynamics journal January 1997
Classical S Matrix: Numerical Application to Inelastic Collisions journal November 1970
Exchange Reactions with Activation Energy. I. Simple Barrier Potential for (H, H 2 ) journal November 1965
Why Quantum Coherence Is Not Important in the Fenna–Matthews–Olsen Complex journal June 2015
Electronically Nonadiabatic Dynamics in Singlet Fission: A Quasi-Classical Trajectory Simulation journal July 2014

Cited By (21)

Communication: Wigner functions in action-angle variables, Bohr-Sommerfeld quantization, the Heisenberg correspondence principle, and a symmetrical quasi-classical approach to the full electronic density matrix journal August 2016
Multi-level description of the vibronic dynamics of open quantum systems journal October 2019
Initial sampling in symmetrical quasiclassical dynamics based on Li–Miller mapping Hamiltonian journal January 2019
A walk through the approximations of ab initio multiple spawning journal April 2018
A symmetrical quasi-classical windowing model for the molecular dynamics treatment of non-adiabatic processes involving many electronic states journal March 2019
A new symmetrical quasi-classical model for electronically non-adiabatic processes: Application to the case of weak non-adiabatic coupling journal October 2016
Improved population operators for multi-state nonadiabatic dynamics with the mixed quantum-classical mapping approach journal January 2020
An assessment of mean-field mixed semiclassical approaches: Equilibrium populations and algorithm stability journal April 2016
A modified approach for simulating electronically nonadiabatic dynamics via the generalized quantum master equation journal January 2019
Combining the mapping Hamiltonian linearized semiclassical approach with the generalized quantum master equation to simulate electronically nonadiabatic molecular dynamics journal August 2019
Communication: Symmetrical quasi-classical analysis of linear optical spectroscopy journal May 2018
The symmetrical quasi-classical approach to electronically nonadiabatic dynamics applied to ultrafast exciton migration processes in semiconducting polymers journal July 2018
On the adiabatic representation of Meyer-Miller electronic-nuclear dynamics journal August 2017
A new perspective for nonadiabatic dynamics with phase space mapping models journal July 2019
Classical molecular dynamics simulation of electronically non-adiabatic processes journal January 2016
Performance evaluation of the symmetrical quasi-classical dynamics method based on Meyer-Miller mapping Hamiltonian in the treatment of site-exciton models journal November 2018
Combining Meyer–Miller Hamiltonian with electronic structure methods for on-the-fly nonadiabatic dynamics simulations: implementation and application journal January 2019
Improved population operators for multi-state nonadiabatic dynamics with the mixed quantum-classical mapping approach text January 2020
Delocalized excitons in natural light harvesting complexes text January 2018
Performance Evaluation of the Symmetrical Quasi-Classical Dynamics Method based on Meyer-Miller Mapping Hamiltonian in the Treatment of Site-Exciton Models text January 2018
Initial Sampling in Symmetrical Quasiclassical Dynamics Based on Li-Miller Mapping Hamiltonian text January 2018

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY