Environment dependent vibrational heat transport in molecular Junctions : Rectification, quantum effects, vibrational mismatch

TL;DR

This study investigates vibrational heat transport in molecular junctions using a quantum self-consistent reservoir model, revealing effects of environment, vibrational mismatch, and system parameters on thermal rectification and heat transfer.

Contribution

It introduces a versatile quantum model to analyze environment-dependent vibrational heat transport and rectification in molecular junctions, accounting for phonon scattering and spectral mismatch effects.

Findings

Thermal rectification depends on environment type and molecular grading.

Vibrational mismatch significantly influences heat transfer efficiency.

Heat current varies with chain length, temperature gradient, and phonon scattering rate.

Abstract

Vibrational heat transport in molecular junctions is a central issue in different contemporary research areas like Chemistry, material science, mechanical engineering, thermoelectrics and power generation. Our model system consists of a chain of molecules which sandwiched between two solids that are maintained at different temperatures. We employ quantum self-consistent reservoir model, which is built on generalized quantum Langevin equation, to investigate quantum effects and far from equilibrium conditions on thermal conduction at nanoscale. The present self-consistent reservoir model can easily mimic the phonon-phonon scattering mechanisms. Different thermal environments are modelled as (i) Ohmic, (ii) sub-Ohmic, and (iii) super-Ohmic environment and their effects are demonstrated for the thermal rectification properties of the system with spring graded or mass graded feature. The behavior of heat current across molecular junctions as a function of chain length, temperature gradient and phonon scattering rate are studied. Further, our analysis reveals the effects of vibrational mismatch between the solids phonon spectra on heat transfer characteristics in molecular junctions for different thermal environments.