Environment-dependent vibrational heat transport in molecular junctions: Rectification, quantum effects, vibrational mismatch.

Abstract

Vibrational heat transport in molecular junctions is a central issue in different contemporary research areas such as chemistry, materials science, mechanical engineering, thermoelectrics, and power generation. Our model system consists of a chain of molecules which are sandwiched between two solids that are maintained at different temperatures. We employ a quantum self-consistent reservoir model, which is built on a 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 modeled as (i) Ohmic, (ii) sub-Ohmic, and (iii) super-Ohmic environments, and their effects are demonstrated for the thermal rectification properties of the system with spring graded or mass graded features. The behavior of heat current across molecular junctions as a function of chain length, temperature gradient, and phonon scattering rates 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.