Temperature-dependent phonon lifetimes and thermal conductivity of silicon by inelastic neutron scattering and <i>ab initio</i> calculations

Abstract

Inelastic neutron scattering on a single crystal of silicon was performed at temperatures from 100 to 1500 K. These experimental data were reduced to obtain phonon spectral intensity at all wave vectors $\stackrel{P\vec}{Q}$ and frequencies $\ensuremath{\omega}$ in the first Brillouin zone. Thermal broadenings of the phonon peaks were obtained by fitting and by calculating with an iterative ab initio method that uses thermal atom displacements on an ensemble of superlattices. Agreement between the calculated and experimental broadenings was good, with possible discrepancies at the highest temperatures. Distributions of phonon widths versus phonon energy had similar shapes for computation and experiment. These distributions grew with temperature but maintained similar shapes. Parameters from the ab initio calculations were used to obtain the thermal conductivity from the Boltzmann transport equation, which was in good agreement with experimental data. Despite the high group velocities of longitudinal acoustic phonons, their shorter lifetimes reduced their contribution to the thermal conductivity, which was dominated by transverse acoustic modes.