Hierarchical quantum master equation approach to electronic-vibrational coupling in nonequilibrium transport through nanosystems: Reservoir formulation and application to vibrational instabilities

TL;DR

This paper introduces a hierarchical quantum master equation method that accurately models nonequilibrium charge transport in nanosystems with strong electronic-vibrational interactions, especially under high vibrational excitation conditions.

Contribution

The novel HQME approach treats vibrational degrees of freedom in the reservoir subspace, enabling analysis of high excitation levels and vibrational instabilities in nanosystems.

Findings

Vibrational excitation follows a geometric distribution at weak coupling.

The method accurately captures vibrational instabilities and current-induced heating.

Results are valid across a broad range of transport regimes.

Abstract

We present a novel hierarchical quantum master equation (HQME) approach which provides a numerically exact description of nonequilibrium charge transport in nanosystems with electronic-vibrational coupling. In contrast to previous work [Phys. Rev. B $\bf{94}$, 201407 (2016)], the active vibrational degrees of freedom are treated in the reservoir subspace and are integrated out. This facilitates applications to systems with very high excitation levels, for example due to current-induced heating, while properties of the vibrational degrees of freedom, such as the excitation level and other moments of the vibrational distribution function, are still accessible. The method is applied to a generic model of a nanosystem, which comprises a single electronic level that is coupled to fermionic leads and a vibrational degree of freedom. Converged results are obtained in a broad spectrum of parameters, ranging from the nonadiabatic to the adiabatic transport regime. We specifically investigate the phenomenon of vibrational instability, that is, the increase of current-induced vibrational excitation for decreasing electronic-vibrational coupling. The novel HQME approach allows us to analyze the influence of level broadening due to both molecule-lead coupling and thermal effects. Results obtained for the first two moments suggest that the vibrational excitation is always described by a geometric distribution in the weak electronic-vibrational coupling limit.