Waiting time between charging and discharging processes in molecular junctions

TL;DR

This paper develops a theoretical framework based on Markovian master equations to analyze the statistical distribution of charging and discharging times in molecular junctions, providing insights into electron tunneling dynamics.

Contribution

It introduces a general formula for the distribution of dwelling times in molecular junctions using quantum jump operators derived from the Liouvillian of the master equation.

Findings

Derived a formula for dwelling time distribution in molecular junctions.

Identified quantum jump operators corresponding to charging and discharging events.

Analyzed the statistical properties of charge residence times.

Abstract

When electric current flows through a molecular junction, the molecule constantly charges and discharges by tunnelling electrons. These charging and discharging events occur at specific but random times and separated by stochastic time intervals. These time intervals can be associated with dwelling time for a charge (electron or hole) to reside on the molecule. In this paper, the statistical properties of these time intervals are studied and general formula for their distribution is derived. The theory is based on the Markovian master equation which takes into account transitions between vibrational states of charged and neutral molecule in the junction. Two quantum jump operators are identified from the Liouvillian of the master equation - one corresponds to charging of the molecule and the other discharges the molecule back to neutral state. The quantum jump operators define the conditional probability that given that the molecule was charged by a tunneling electron at time $t$, the molecule becomes neutral at later time $t+\tau$ discharging the electron to the drain electrode. Statistical properties of these time intervals $\tau$ are studied with the use of this distribution.