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Zone-center optical phonon linewidth is a key parameter for infrared andRaman spectra as well as the Lorenz oscillator model. While three-phononscattering was often assumed to be the leading contribution, in this work wefind, surprisingly, that higher-order phonon scattering universally plays asignificant or even dominant role over three-phonon scattering at roomtemperature, and more so at elevated temperatures, for a wide range ofmaterials including diamond, Si, Ge, boron arsenide (BAs), cubic siliconcarbide (3C-SiC), and $\alpha$-quartz. This is enabled by the large fourphononscattering phase space of zone-center optical phonons, and distinct from heatconduction where at room temperature four-phonon scattering is still secondaryto three-phonon scattering. Moreover, our results imply that five-phonon andeven higher-order scattering may be significant for some large band-gapmaterials, e.g., BAs. Our predicted infrared optical properties through theLorenz oscillator model, after including four-phonon scattering, show muchbetter agreement with experimental measurements than those three-phonon basedpredictions. This work will raise broad interest of studying high-orderscattering in various areas beyond heat conduction.

Role of higher-order phonon scattering in the zone-center optical phonon linewidth and the Lorenz oscillator model