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Accurate Determination of Phonon Lifetimes from the Spectral Domain

Milos Dubajic1,*, Andreas Pusch2, Michael P. Nielsen2, and Samuel D. Stranks1,3,†

  • *Contact author: milos.dubajic@hotmail.com
  • †Contact author: sds65@cam.ac.uk
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PRX Energy 4, 033020 – Published 25 September, 2025

DOI: https://doi.org/10.1103/vklp-9bvg

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 modeling. We outline the origin of this ambiguity, provide historical context on how this error has 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.

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Popular Summary

The performance of energy technologies such as solar cells, thermoelectrics, and solid-state batteries depends strongly on phonons. Phonon lifetimes are critical for predicting heat flow, charge transport, and ion motion. Surprisingly, many widely used formulas for extracting phonon lifetimes from spectroscopic data are incorrect, leading to systematic errors in reported values. These errors, often by factors of two or more, originated decades ago from a misinterpretation in the literature and have since propagated across the community, especially in the study of energy materials. This work traces the historical source of this confusion, clarifies the distinction between different types of phonon relaxation, and derives the correct expressions. By resolving these ambiguities, the authors provide a reliable foundation for interpreting experimental spectra and for guiding the design of next-generation materials for clean energy applications.

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PRX Energy 4, 033020– Published 25 September, 2025
  • Received 11 March 2025
  • Accepted 21 August 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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