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Semiclassical approaches to perturbative time-convolution and time-convolutionless quantum master equations for
Xiang Sun1,2,3, Zengkui Liu1,2,3
1Division of Arts and Sciences, NYU Shanghai, 567 West Yangsi Road, Shanghai 200124, China.
The Journal of Chemical Physics
|May 15, 2024
Summary
This study compares time-convolution (TC) and time-convolutionless (TCL) quantum master equations (QMEs) for modeling photoinduced dynamics. TC QMEs generally offer higher accuracy than TCL QMEs, particularly for excitation energy transfer (EET) in complex systems.
Area of Science:
- * Theoretical chemistry and condensed-phase physics.
- * Quantum dynamics and energy transfer mechanisms.
Background:
- * Understanding photoinduced processes is key for developing new energy materials.
- * Nonadiabatic dynamics in complex systems require accurate theoretical models.
Purpose of the Study:
- * To investigate nonadiabatic dynamics using time-convolution (TC) and time-convolutionless (TCL) quantum master equations (QMEs).
- * To evaluate the accuracy of TC and TCL QMEs against exact quantum mechanics and semiclassical methods.
- * To provide guidance for applying these QME approaches to condensed-phase systems.
Main Methods:
- * Employing multistate harmonic (MSH) models with Hamiltonians mapped from all-atom simulations.
- * Treating electronic couplings as a perturbation within the MSH framework.
- * Applying TC and TCL QMEs to study charge transfer in organic photovoltaics and excitation energy transfer (EET) in photosynthetic complexes.
Main Results:
- * TC QMEs generally provide more accurate results than TCL QMEs, especially for EET dynamics.
- * Both TC and TCL QMEs are versatile and adaptable to various systems.
- * Semiclassical approximations show a trade-off between accuracy and computational cost.
Conclusions:
- * TC and TCL QMEs, within the MSH model, are effective for studying photoinduced dynamics.
- * The study offers valuable insights into the performance of these QME approaches for atomistic condensed-phase systems.
- * Findings guide the selection and application of theoretical methods for energy conversion material research.
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