Resonant Electron Transport in Single-Molecule Junctions: Vibrational Excitation, Rectification, Negative Differential Resistance and Local Cooling

TL;DR

This paper investigates vibronic effects in resonant electron transport through single-molecule junctions, revealing phenomena like vibrational excitation, rectification, NDR, and local cooling, with detailed mechanisms including electron-hole pair creation.

Contribution

It extends previous models by incorporating electron-hole pair creation processes and analyzing vibronic effects in systems with multiple electronic states.

Findings

Vibrational excitation and rectification observed in models.

Negative differential resistance identified under certain conditions.

Local cooling effects demonstrated in molecular junctions.

Abstract

Vibronic effects in resonant electron transport through single-molecule junctions are analyzed. The study is based on generic models for molecular junctions, which include electronic states on the molecular bridge that are vibrationally coupled and exhibit Coulomb interaction. The transport calculations employ a master equation approach. The results, obtained for a series of models with increasing complexity, show a multitude of interesting transport phenomena, including vibrational excitation, rectification, negative differential resistance (NDR) as well as local cooling. While some of these phenomena have been observed or proposed before, the present analysis extends previous studies and allows a more detailed understanding of the underlying transport mechanisms. In particular, it is shown that many of the observed phenomena can only be explained if electron-hole pair creation processes at the molecule-lead interface are taken into account. Furthermore, vibronic effects in sytems with multiple electronic states and their role for the stability of molecular junctions are analyzed.