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Open quantum systems with nonlinear environmental backactions: Extended dissipaton theory vs core-system hierarchy
Zi-Hao Chen1, Yao Wang1, Rui-Xue Xu1
1Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
The Journal of Chemical Physics
|February 22, 2023
Summary
This study details quantum dissipation theories using hierarchical quantum master equations and the extended dissipaton equation of motion (DEOM) formalism for accurate thermodynamic predictions.
Area of Science:
- Quantum Chemistry
- Theoretical Chemistry
- Chemical Physics
Background:
- Quantum dissipation describes how quantum systems lose energy to their environment.
- Quadratic environment couplings are common in condensed-phase quantum dynamics.
- Hierarchical quantum master equations offer a framework for studying open quantum systems.
Purpose of the Study:
- To present a comprehensive theory of quantum dissipation with quadratic environment couplings.
- To develop and verify the extended dissipaton equation of motion (DEOM) formalism.
- To apply these theories to equilibrium and nonequilibrium thermodynamics.
Main Methods:
- Brownian solvation mode embedded hierarchical quantum master equations.
- Core-system hierarchy construction for DEOM verification.
- Quadratic imaginary-time DEOM for equilibrium calculations.
- Lambda(t)-DEOM for nonequilibrium thermodynamics.
Main Results:
- The extended DEOM formalism was rigorously verified.
- Accurate reproduction of the Jarzynski equality and Crooks relation.
- Demonstration of numerical efficiency for the extended DEOM.
- Highlighting the utility of core-system hierarchy for visualizing solvation dynamics.
Conclusions:
- The developed extended DEOM theories provide a rigorous and efficient framework for quantum dissipation.
- These methods accurately capture thermodynamic properties in both equilibrium and nonequilibrium regimes.
- The choice between extended DEOM and core-system hierarchy depends on the specific research needs, balancing efficiency and interpretability.
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