Phonon Coherence and New Set of Sidebands in Phonon-Assisted Photoluminescence

TL;DR

This paper explores excitonic polaron states involving phonons, deriving exact ground state expressions and revealing two sets of phonon sidebands in photoluminescence, including a new set caused by environmental phonon coupling.

Contribution

It introduces a comprehensive model for excitonic polarons with exact ground state solutions and identifies a novel set of phonon sidebands due to environmental mode mixing.

Findings

Derived exact ground state with multi-phonon components.

Identified two distinct sets of phonon sidebands in PL.

Predicted Fano lineshape indicating coherence effects.

Abstract

We investigate excitonic polaron states comprising a local exciton and phonons in the longitudinal optical (LO) mode by solving the Schr\"{o}dinger equation. We derive an exact expression for the ground state (GS), which includes multi-phonon components with coefficients satisfying the Huang-Rhys factors. The recombination of GS and excited polaron states gives one set of sidebands in photoluminescence (PL): the multi-phonon components in the GS produce the Stokes lines and the zero-phonon components in the excited states produce the anti-Stokes lines. By introducing the mixing of the LO mode and environal phonon modes, the exciton will also couple with the latter, and the resultant polaron states result in another set of phonon sidebands. This set has a zero-phonon line higher and wider than that of the first set due to the tremendous number of the environal modes. The energy spacing between the zero-phonon lines of the first and second sets is proved to be the binding energy of the GS state. The common exciton origin of these two sets can be further verified by a characteristic Fano lineshape induced by the coherence in the mixing of the LO and the environal modes.