Electron-vibration effects on the thermoelectric efficiency of molecular junctions

TL;DR

This study investigates how electron-vibration interactions influence the thermoelectric efficiency of molecular junctions, revealing that such coupling generally reduces efficiency but can still yield promising thermoelectric performance.

Contribution

It provides a self-consistent non-equilibrium adiabatic analysis of electron-vibration effects on thermoelectric properties in molecular junctions, including comparisons with exact low-density approaches.

Findings

Electron-vibration coupling increases thermal conductance.

Deviations from Wiedemann-Franz law decrease with interaction.

Thermoelectric figure of merit peaks around unity for realistic parameters.

Abstract

The thermoelectric properties of a molecular junction model, appropriate for large molecules such as fullerenes, are studied within a non-equilibrium adiabatic approach in the linear regime at room temperature. A self-consistent calculation is implemented for electron and phonon thermal conductance showing that both increase with the inclusion of the electron-vibration coupling. Moreover, we show that the deviations from the Wiedemann-Franz law are progressively reduced upon increasing the interaction between electronic and vibrational degrees of freedom. Consequently, the junction thermoelectric efficiency is substantially reduced by the electron-vibration coupling. Even so, for realistic parameters values, the thermoelectric figure of merit can still have peaks of the order of unity. Finally, in the off-resonant electronic regime, our results are compared with those of an approach which is exact for low molecular electron densities. We give evidence that in this case additional quantum effects, not included in the first part of this work, do not affect significantly the junction thermoelectric properties in any temperature regime.