On the accurate determination of phonon lifetimes from the spectral domain

Abstract

Concerningly, numerous incorrect expressions for extracting phonon lifetimes from spectroscopic linewidths remain prevalent in the literature, resulting in misinterpretation of experimental data. This has significant consequences in the broader energy materials field, where erroneous lifetimes risk misinforming materials design and device modelling. We outline the origin of this ambiguity, provide historical context on how this error propagated, and present the correct formula. In addition, we highlight a frequently overlooked source of error, the contribution of phase relaxation to spectral broadening. A unified approach enables fair comparison of values obtained from different spectroscopic methods, accurate benchmarking against first-principles calculations, and, most importantly, precise determination of macroscopic physical properties derived from phonon lifetime measurements.