Quantum Path Interference through Incoherent Motions in Multilevel Quantum Systems

TL;DR

This paper develops a unified Ehrenfest-based model to study quantum path interference in multilevel dissipative systems, avoiding common approximations and providing insights into the effects of incoherent interactions with phonons and light.

Contribution

It extends the Ehrenfest scheme to simultaneously model system-light and system-phonon interactions, offering a more realistic approach to quantum path interference analysis.

Findings

Quantum path interference affects steady state populations.

Ehrenfest scheme can be derived from stochastic Schrödinger equation.

Model avoids assumptions about spectral densities and correlation functions.

Abstract

Quantum path interferences or resonances in multilevel dissipative quantum systems play an important and intriguing role in the transport processes of nanoscale systems. Many previous minimalistic models used to describe the quantum path interference driven by incoherent fields are based on the approximations including the second order perturbation for the weak coupling limit, the ad-hoc choices of two-time correlation functions and $\it{etc}$. On the other hand, the similar model to study the non-adiabatic molecular electronic excitation have been extensively developed and many efficient quantum molecular dynamics simulation schemes, such as the Ehrenfest scheme, have been proposed. In this paper, I aim to propose an unified model, extend the Ehrenfest scheme to study the interactions of system-light and system-phonon simultaneously and gain insight into and principles of the roles of quantum path interferences in the realistic molecular systems. I discuss how to derive the time-dependent stochastic Schr$\ddot{o}$dinger equation from the Ehrenfest scheme as a foundation to discuss the detailed balance for the weak coupling limit and therefore the quantum correction in the Ehrenfest scheme. Different from the master equation technique, the Ehrenfest scheme doesn't need any specific assumptions about spectral densities and two time correlation functions. With simple open two-level and three-level quantum systems, I show the effect of the quantum path interference on the steady state populations. Currently I only focus on the role of the phonon thermal reservoir. The electromagnetic field (solar light) will be modeled as a thermal reservoir and discussed in detail in the future paper.