Phonon-polariton mediated thermal radiation and heat transfer among molecules and macroscopic bodies: nonlocal electromagnetic response at mesoscopic scales

TL;DR

This paper develops a mesoscopic framework combining atomistic and continuum models to study phonon-polariton effects on thermal radiation and heat transfer at nanometric scales, revealing significant deviations from traditional local models.

Contribution

It introduces a novel mesoscopic approach that integrates ab-initio electronic and vibrational fluctuations with electromagnetic scattering, capturing nonlocal effects at mesoscopic scales.

Findings

Phonon-polariton effects can alter heat transfer by orders of magnitude.

Nonlocal electromagnetic responses significantly impact thermal emission.

Elongated molecular systems exhibit qualitatively different thermal behaviors.

Abstract

Thermal radiative phenomena can be strongly influenced by the coupling of phonons and long-range electromagnetic fields at infrared frequencies. Typically employed macroscopic descriptions of thermal fluctuations tend to ignore atomistic effects that become relevant at nanometric scales, whereas purely microscopic treatments ignore long-range, geometry-dependent electromagnetic effects. We describe a mesoscopic framework for modeling thermal fluctuation phenomena among molecules in the vicinity of macroscopic bodies, conjoining atomistic treatments of electronic and vibrational fluctuations obtained from ab-initio density functional theory in the former with continuum descriptions of electromagnetic scattering in the latter. The interplay of these effects becomes particularly important at mesoscopic scales, where phonon polaritons can be strongly influenced by the finite sizes, shapes, and non-local/many-body response of the bodies to electromagnetic fluctuations. We show that even in small but especially in elongated low-dimensional molecular systems, such effects can modify thermal emission and heat transfer by orders of magnitude and produce qualitatively different behavior compared to predictions based on local, dipolar, or pairwise approximations valid only in dilute media.