Generalized first-principles method to study near-field heat transfer mediated by Coulomb interaction

TL;DR

This paper introduces a comprehensive first-principles approach using nonequilibrium Green's functions to analyze Coulomb-mediated near-field heat transfer, revealing new insights into flux saturation and material effects at nanoscales.

Contribution

It develops a general microscopic method combining DFT and Green's functions to accurately model near-field heat transfer mediated by Coulomb interactions, surpassing traditional local response theories.

Findings

Heat flux saturates at extreme near fields, deviating from 1/d dependence.

Calculated heat flux can exceed black-body limit by up to 5×10^4 times.

Heat transfer shows a 1/d^2 dependence at large separations.

Abstract

We present a general microscopic first-principles method to study the Coulomb-interaction-mediated heat transfer in the near field. Using the nonequilibrium Green's function formalism, we derive Caroli formulas for heat transfers between materials with translational invariance. The central physical quantities are the screened Coulomb potential and the spectrum function of polarizability. Within the random phase approximation, we calculate the polarizability using the linear response density functional theory and obtain the screened Coulomb potential from a retarded Dyson equation. We show that the heat transfer mediated by the Coulomb interaction is consistent with that of the $p$-polarized evanescent waves which dominate the heat transfer in the near field. We adopt single-layer graphene as an example to calculate heat transfers between two parallel sheets separated by a vacuum gap $d$. Our results show a saturation of heat flux at the extreme near field which is different from the reported $1/d$ dependence for local response functions. The calculated heat flux is up to $5\times10^4$ times more than the black-body limit, and a $1/d^2$ dependence is shown at large separations. From the spectrum of energy current density, we infer that the near-field enhancement of heat transfer stems from electron transitions around the Fermi energy. With a uniform strain, the heat flux increases for most of the distances while a negative correlation is shown at the moderate field. Our method is valid for inhomogeneous materials in which the macroscopic response function used in conventional theory of fluctuational electrodynamics would fail at the subnanometer scale.