Microscopic modeling of the effect of phonons on the optical properties of solid-state emitters

TL;DR

This paper develops a first-principles microscopic model to understand how phonons influence the optical emission spectrum, including isotopic shifts, of solid-state emitters like silicon-vacancy centers in diamond.

Contribution

It introduces a novel microscopic approach combining the spin-boson model with molecular and force-constant descriptions to analyze phonon effects on optical properties.

Findings

Quantitative estimation of electron-phonon interactions.

Explanation of isotopic shifts in emission spectra.

Insight into symmetry breaking effects on optical lines.

Abstract

Understanding the effect of vibrations in optically active nano systems is crucial for successfully implementing applications in molecular-based electro-optical devices, quantum information communications, single photon sources, and fluorescent markers for biological measurements. Here, we present a first-principles microscopic description of the role of phonons on the isotopic shift presented in the optical emission spectrum associated to the negatively charged silicon-vacancy color center in diamond. We use the spin-boson model and estimate the electron-phonon interactions using a symmetrized molecular description of the electronic states and a force-constant model to describe molecular vibrations. Group theoretical arguments and dynamical symmetry breaking are presented in order to explain the optical properties of the zero-phonon line and the isotopic shift of the phonon sideband.