Homogeneous and inhomogeneous contributions to the luminescence linewidth of point defects in amorphous solids: Quantitative assessment based on time-resolved emission spectroscopy

TL;DR

This study introduces an experimental and theoretical approach to distinguish homogeneous and inhomogeneous linewidths of point defect luminescence in amorphous solids, validated through time-resolved emission spectroscopy on silica and lithium fluoride.

Contribution

It develops a quantitative model linking structural disorder to luminescence linewidths and provides a method to estimate homogeneous and inhomogeneous contributions separately.

Findings

Inhomogeneous broadening dominates the linewidth of ODC(II) in amorphous silica.

The model accurately describes the energy dependence of decay lifetimes.

Experimental validation confirms the theoretical predictions.

Abstract

The article describes an experimental method that allows to estimate the inhomogeneous and homogeneous linewidths of the photoluminescence band of a point defect in an amorphous solid. We performed low temperature time-resolved luminescence measurements on two defects chosen as model systems for our analysis: extrinsic Oxygen Deficient Centers (ODC(II)) in amorphous silica and F+ 3 centers in crystalline Lithium Fluoride. Measurements evidence that only defects embedded in the amorphous matrix feature a dependence of the radiative decay lifetime on the emission energy and a time dependence of the first moment of the emission band. A theoretical model is developed to link these properties to the structural disorder typical of amorphous solids. Specifically, the observations on ODC(II) are interpreted by introducing a gaussian statistical distribution of the zero phonon line energy position. Comparison with the results obtained on F+ 3 crystalline defects strongly confirms the validity of the model. By analyzing experimental data within this frame, we obtain separate estimations of the homogenous and inhomogeneous contributions to the measured total linewidth of ODC(II), which results to be mostly inhomogeneous.