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An efficient solution to the decoherence enhanced trivial crossing problem in surface hopping.

Xin Bai1, Jing Qiu1, Linjun Wang1

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A new restricted decoherence (RD) strategy enhances the self-consistent fewest switches surface hopping (SC-FSSH) algorithm. This improved SC-FSSH-RD method accelerates simulations for charge transport in molecules, enabling larger time intervals for accurate results.

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Area of Science:

  • Computational Chemistry
  • Quantum Dynamics
  • Materials Science

Background:

  • Tully's fewest switches surface hopping (FSSH) is a key algorithm for simulating quantum dynamics.
  • Trivial crossing and decoherence present challenges in FSSH accuracy and efficiency.
  • Existing decoherence strategies can exacerbate the trivial crossing problem.

Purpose of the Study:

  • To investigate time interval convergence in FSSH with decoherence corrections.
  • To address the limitations of current decoherence strategies in handling trivial crossings.
  • To develop an improved FSSH algorithm for efficient and accurate charge transport simulations.

Main Methods:

  • Incorporation of a novel restricted decoherence (RD) strategy into the self-consistent (SC) FSSH algorithm, creating SC-FSSH-RD.
  • Application of SC-FSSH-RD to general Hamiltonians with varying electronic and electron-phonon couplings.
  • Mimicking charge transport dynamics in molecular systems ranging from tens to hundreds of molecules.

Main Results:

  • SC-FSSH-RD achieves convergence with a significantly large time interval of 0.1 fs.
  • Simulation time is reduced by over an order of magnitude compared to standard methods.
  • Accurate capture of both band and hopping mechanisms in charge transport.
  • Demonstrated ability to perform surface hops in the adiabatic representation.

Conclusions:

  • SC-FSSH-RD effectively overcomes the trivial crossing problem enhanced by decoherence corrections.
  • The method significantly improves computational efficiency for simulating charge transport.
  • SC-FSSH-RD is versatile, applicable in diabatic and locally diabatic representations.
  • Potential for describing general nonadiabatic dynamics of electrons and excitons in various materials.