Generalization of Kirchhoff's Law of Thermal Radiation: The Inherent Relations Between Quantum Efficiency and Emissivity

TL;DR

This paper establishes a fundamental relation between emissivity, absorptivity, and quantum efficiency in thermal radiation, extending Kirchhoff's law out of equilibrium and providing insights for energy device development.

Contribution

It introduces a new theoretical and experimental relation, psilon = lpha(1-QE), linking these properties beyond equilibrium conditions.

Findings

The relation psilon = lpha(1-QE) is experimentally validated.

At equilibrium, the relation reduces to Kirchhoff's law.

The work advances understanding of non-thermal emission evolution with temperature.

Abstract

Planck's law of thermal radiation depends on the temperature, $T$, and the emissivity, $\epsilon$, of a body, where emissivity is the coupling of heat to radiation that depends on both phonon-electron nonradiative interactions and electron-photon radiative interactions. Another property of a body is absorptivity, $\alpha$, which only depends on the electron-photon radiative interactions. At thermodynamic equilibrium, nonradiative interactions are balanced, resulting in Kirchhoff's law of thermal radiation that equals these two properties, i.e., $\epsilon = \alpha$. For non-equilibrium, quantum efficiency ($QE$) describes the statistics of photon emission, which like emissivity depends on both radiative and nonradiative interactions. Past generalized Planck's equation extends Kirchhoff's law out of equilibrium by scaling the emissivity with the pump-dependent chemical-potential $\mu$, obscuring the relations between the body properties. Here we theoretically and experimentally demonstrate a prime equation relating these properties in the form of $\epsilon = \alpha(1-QE)$, which is in agreement with a recent universal modal radiation law for all thermal emitters. At equilibrium, these relations are reduced to Kirchhoff's law. Our work lays out the fundamental evolution of non-thermal emission with temperature, which is critical for the development of lighting and energy devices.