Temperature correction to dichotomic fluctuation models for open quantum system dynamics

Abstract We investigate the dynamics of an asymmetric two‐level system (TLS) subject to stochastic energy fluctuations described by a dichotomic Markov process, which is a powerful model applicable to excitonic transport in molecular aggregates, decoherence in qubits, and spectral fluctuations in single‐molecule spectroscopy. While the standard dichotomic noise model offers exact solutions that capture non‐Markovian dynamics, it violates detailed balance and fails to ensure thermal equilibrium. To overcome this, we introduce a temperature‐corrected version by adding a counterterm to the exact equations of motion, thereby restoring the correct equilibrium behavior. Furthermore, we explore the TLS dynamics under varying initial conditions and parameter regimes. The results demonstrate that the model reproduces both short‐time coherent evolution and long‐time thermal populations and captures single‐system behavior relevant to experiments on isolated quantum systems. This work provides a powerful framework for studying non‐Markovian dynamics in open quantum systems.

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Publication Details

Journal
Journal of the Chinese Chemical Society
Published
2025-08-14
DOI
https://doi.org/10.1002/jccs.70061
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
Field-Weighted Citation Impact
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article

Temperature correction to dichotomic fluctuation models for open quantum system dynamics

Kai‐Cheng Liu, Yuan‐Chung Cheng, T. Wang, Chiao‐Yuan Hung
Journal of the Chinese Chemical Society
Spectroscopy and Quantum Chemical Studies
article

Temperature correction to dichotomic fluctuation models for open quantum system dynamics

Kai‐Cheng Liu, Yuan‐Chung Cheng, T. Wang, Chiao‐Yuan Hung
article en

Abstract

Abstract We investigate the dynamics of an asymmetric two‐level system (TLS) subject to stochastic energy fluctuations described by a dichotomic Markov process, which is a powerful model applicable to excitonic transport in molecular aggregates, decoherence in qubits, and spectral fluctuations in single‐molecule spectroscopy. While the standard dichotomic noise model offers exact solutions that capture non‐Markovian dynamics, it violates detailed balance and fails to ensure thermal equilibrium. To overcome this, we introduce a temperature‐corrected version by adding a counterterm to the exact equations of motion, thereby restoring the correct equilibrium behavior. Furthermore, we explore the TLS dynamics under varying initial conditions and parameter regimes. The results demonstrate that the model reproduces both short‐time coherent evolution and long‐time thermal populations and captures single‐system behavior relevant to experiments on isolated quantum systems. This work provides a powerful framework for studying non‐Markovian dynamics in open quantum systems.

Journal of the Chinese Chemical SocietyVol. 72(9)
National Taiwan University of Science and Technology (TW), National Taiwan University (TW), National Center for Theoretical Sciences (TW), National Center for Theoretical Sciences, Physics Division
Openalex Percentile: Top 77%
Spectroscopy and Quantum Chemical Studies
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