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A multi-state mapping approach to surface hopping.

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This study introduces an enhanced mapping approach for surface hopping, improving accuracy for quantum-classical systems. The new method accurately models electronic populations and coherences in complex systems.

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Area of Science:

  • Quantum Chemistry
  • Theoretical Chemistry
  • Chemical Physics

Background:

  • Surface hopping methods are crucial for simulating non-adiabatic dynamics in molecular systems.
  • Existing methods like fewest switches surface hopping (FSSH) have limitations in accurately describing electronic coherences and populations.
  • The mapping approach to surface hopping (MASH) offers a promising alternative for semiclassical simulations.

Purpose of the Study:

  • To develop and validate a multiple electronic state adaptation of the Mannouch-Richardson mapping approach.
  • To improve the accuracy of semiclassical simulations for electronically non-adiabatic processes.
  • To provide a more robust method for calculating electronic populations and coherences.

Main Methods:

  • Adaptation of the Mannouch-Richardson mapping approach to handle multiple electronic states.
  • Treatment of electronic populations and coherences on an equal footing.
  • Comparison with exact benchmark results for three- and seven-state models of the Fenna-Matthews-Olson (FMO) complex.
  • Benchmarking against fewest switches surface hopping (FSSH) and other semiclassical methods.

Main Results:

  • The adapted mapping approach yields significantly more accurate electronic populations and coherences compared to FSSH.
  • The method demonstrates accuracy comparable to or exceeding existing semiclassical techniques for FMO models.
  • Comparison with the original Mannouch-Richardson method shows comparable accuracy, with the new method excelling in multi-state systems.

Conclusions:

  • The developed multiple electronic state mapping approach provides a highly accurate and versatile tool for simulating non-adiabatic dynamics.
  • This method overcomes limitations of FSSH and offers a reliable alternative for complex quantum-classical systems.
  • The approach is applicable to a broader range of electronically non-adiabatic systems, including those with multiple excited states.