Current-induced bond rupture in single-molecule junctions

TL;DR

This paper investigates how electronic-vibrational interactions can cause bond rupture in single-molecule junctions under current, using advanced simulation methods to analyze the effects of bias voltage and coupling strength on stability.

Contribution

It introduces a combined HQME and Ehrenfest simulation approach to study current-induced bond rupture, revealing conditions that can both destabilize and stabilize molecular junctions.

Findings

Bias voltage can induce bond dissociation.

Certain conditions increase molecular stability.

The method captures key mechanisms of bond rupture.

Abstract

Electronic-vibrational coupling in single-molecule junctions may result in current-induced bond rupture and is thus an important mechanism for the stability of molecular junctions. We use the hierarchical quantum master equation (HQME) method in combination with the quasi-classical Ehrenfest approach for the nuclear degrees of freedom to simulate current-induced bond rupture in single-molecule junctions. Employing generic models for molecular junctions with dissociative nuclear potentials, we analyze the underlying mechanisms. In particular, we investigate the dependence of the dissociation probability on the applied bias voltage and the molecule-lead coupling strength. The results show that an applied bias voltage can not only lead to dissociation of the molecular junction, but under certain conditions can also increase the stability of the molecule.