Quantum Many-Body Principles of Localized-State Ensemble Luminescence

TL;DR

This paper develops a quantum many-body theory for localized-state ensemble luminescence in solids, explaining temperature-dependent optical behaviors and deriving key empirical formulas.

Contribution

It introduces a novel quantum many-body framework that incorporates electron-phonon and electron-electron interactions for LSE luminescence analysis.

Findings

Quantitative interpretation of abnormal thermal luminescence behaviors

Elucidation of electron-phonon and electron-electron interaction roles

Derivation of Varshni's and Huang-Rhys formulas from the theory

Abstract

Localized electron states induced by various disorders,including defects and impurities,usually exist in solids.Their optical properties,especially their luminescence properties,are of both scientific and technological significance.But a microscopic theory has not yet been established for such localized-state ensemble (LSE) luminescence.In this Letter,we attempt to fill this void via developing a quantum many-body (MB) luminescence theory taking into account both electron-phonon (e-p) and electron-electron (e-e) interactions.By using the developed MB-LSE theory,abnormal thermal behaviors such as redshift and subsequent blueshift of peak position,narrowing and succeeding broadening of linewidth,decline in intensity,and variation in lifetime can be quantitatively interpreted.The roles of electron-phonon and electron-electron interactions in the variable-temperature LSE luminescence are thus elucidated. Within the framework of the MB-LSE theory, moreover, Varshni's empirical formula for bandgap temperature dependence and Huang-Rhys factor for e-p coupling are further derived and discussed.