Memory kernel non-additivity in the generalized quantum master equation for a system coupled to multiple heat baths

The generalized quantum master equation provides an exact equation of motion for the reduced density operator of a quantum system coupled to one or more baths, with all bath-induced effects encoded in a memory kernel superoperator. In this paper, we investigate whether the memory kernel for a system coupled simultaneously to multiple independent baths can be written as a sum of memory kernels associated with the corresponding single-bath problems. We show that such additivity holds in the weak system-bath coupling limit, where the second-order memory kernel separates into independent bath contributions. Beyond this limit, however, the baths become dynamically correlated through their mutual coupling to the system, and the exact multi-bath memory kernel is no longer equal to the sum of exact single-bath memory kernels. We demonstrate this non-additivity for a two-level system linearly coupled to hot and cold harmonic baths, using the hierarchical equations of motion method to construct the memory kernels. The results show that non-additivity increases with system-bath coupling strength and is process-dependent: coherence damping remains comparatively well described by an additive kernel, whereas population-coherence and coherence-coherence transfer exhibit pronounced non-additive behavior. These findings clarify the limitations of additive multi-bath descriptions and highlight the ambiguity of decomposing heat flow into independent bath-resolved contributions beyond weak system-bath coupling.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2026-08-20
DOI
https://doi.org/10.1063/5.0346129
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
Field-Weighted Citation Impact
0.00

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article

Memory kernel non-additivity in the generalized quantum master equation for a system coupled to multiple heat baths

Eitan Geva, Xiaohan Dan, Víctor S. Batista, Callie Wilson
The Journal of Chemical Physics
Spectroscopy and Quantum Chemical Studies
article

Memory kernel non-additivity in the generalized quantum master equation for a system coupled to multiple heat baths

Eitan Geva, Xiaohan Dan, Víctor S. Batista, Callie Wilson
article en

Abstract

The generalized quantum master equation provides an exact equation of motion for the reduced density operator of a quantum system coupled to one or more baths, with all bath-induced effects encoded in a memory kernel superoperator. In this paper, we investigate whether the memory kernel for a system coupled simultaneously to multiple independent baths can be written as a sum of memory kernels associated with the corresponding single-bath problems. We show that such additivity holds in the weak system-bath coupling limit, where the second-order memory kernel separates into independent bath contributions. Beyond this limit, however, the baths become dynamically correlated through their mutual coupling to the system, and the exact multi-bath memory kernel is no longer equal to the sum of exact single-bath memory kernels. We demonstrate this non-additivity for a two-level system linearly coupled to hot and cold harmonic baths, using the hierarchical equations of motion method to construct the memory kernels. The results show that non-additivity increases with system-bath coupling strength and is process-dependent: coherence damping remains comparatively well described by an additive kernel, whereas population-coherence and coherence-coherence transfer exhibit pronounced non-additive behavior. These findings clarify the limitations of additive multi-bath descriptions and highlight the ambiguity of decomposing heat flow into independent bath-resolved contributions beyond weak system-bath coupling.

The Journal of Chemical PhysicsVol. 165(7)
University of Michigan (US), Yale University (US)
National Science Foundation
Openalex Percentile: Top 12%
Spectroscopy and Quantum Chemical Studies
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