Nonadiabatic Dynamics in Atomistic Environments: Harnessing Quantum-Classical Theory with Generalized Quantum Master...

Area of Science:

• Quantum dynamics
• Computational chemistry
• Materials science

Background:

• Accurately simulating nonadiabatic dynamics in quantum systems coupled to atomistic environments is crucial for understanding processes like exciton transport and catalysis.
• Existing methods face challenges in efficiency and accuracy when dealing with complex, fully atomistic environments.

Purpose of the Study:

• To introduce and validate the MF-GQME approach for treating nonadiabatic dynamics.
• To demonstrate its quantitative accuracy and computational efficiency across various charge-transfer regimes.

Main Methods:

• The MF-GQME approach combines Ehrenfest mean field theory with the generalized quantum master equation framework.
• The method was applied to fully atomistic environments to model quantum systems.

Main Results:

• The MF-GQME approach achieves quantitative accuracy in simulating nonadiabatic dynamics.
• Significant computational speed-ups, up to 3 orders of magnitude, were observed compared to direct Ehrenfest theory.
• The method successfully handles diverse charge-transfer regimes within atomistic environments.

Conclusions:

• The MF-GQME approach provides an efficient and accurate tool for studying nonadiabatic quantum relaxation processes.
• This advancement enables detailed investigation of atomistic effects in complex quantum systems where such studies were previously intractable.