General Framework for Quantifying Dissipation Pathways in Open Quantum Systems. I. Theoretical Formulation

Abstract: We present a general and practical theoretical framework to investigate how energy is dissipated in open quantum system dynamics. This is done by quantifying the contributions of individual bath components to the overall dissipation of the system. The framework is based on the Nakajima-Zwanzig projection operator technique which allows us to express the rate of energy dissipation into a specific bath degree of freedom by using traces of operator products. The approach captures system-bath interactions to all orders, but is based on second-order perturbation theory on the off-diagonal subsystem's couplings and a Markovian description of the bath. The usefulness of our theory is demonstrated by applying it to various models of open quantum systems involving harmonic oscillator or spin baths, and connecting the outcomes to existing results such as our previously reported formula derived for locally coupled harmonic bath [J. Chem. Phys. 154, 084109 (2021)]. We also prove that the dissipation calculated by our theory rigorously satisfies thermodynamic principles such as energy conservation and detailed balance. Overall, the strategy can be used to develop the theory and simulation of dissipation pathways to interpret and engineer the dynamics of open quantum systems.