Partially polaron-transformed quantum master equation for exciton and charge transport dynamics
Seogjoo J. Jang, Queens College and The Graduate Center, CUNY
Polaron-transformed quantum master equation (PQME) [1-3] offers a unified framework to describe the dynamics of quantum systems in both limits of weak and strong couplings to environmental degrees of freedom. Thus, PQME serves as an efficient method to describe charge and exciton transfer/transport dynamics for a broad range of parameters in condensed or complex environments. However, in some cases, the polaron transformation (PT) being employed in the formulation invokes an over-relaxation of slow modes and results in premature suppression of important coherence terms. This talk presents a recent effort to develop a formal framework to address this issue by employing a partial PT that has smaller weights for low frequency bath modes. It is demonstrated that a closed form expression of a 2nd order time-local PQME including all the inhomogeneous terms can be derived for a general form of partial PT, although more complicated than that for the full PT. Applications to a model with two system states demonstrate the feasibility and utility of the present approach.
References
1. S. Jang, “Theory of multichromophoric coherent resonance energy transfer: A polaronic quantum master equation approach,” J. Chem. Phys. 135, 034105 (2011). https://arxiv.org/abs/2203.02812
2. L. Yang, M. Devi, and S. Jang, “Polaronic quantum master equation theory of inelastic and coherent resonance energy transfer for soft systems,” J. Chem. Phys. 137, 024101 (2012).
3. S. J. Jang, “Effects of Donor–Acceptor Quantum Coherence and Non-Markovian Bath on the Distance Dependence of Resonance Energy Transfer,” J. Phys. Chem. C 123 (9), 5767-5775 (2019)