Perturbation theory and thermal transport in mass-disordered alloys: Insights from Green's function methods

Abstract

Lowest-order quantum perturbation theory (Fermi's golden rule) for phonon-disorder scattering has been used to predict thermal conductivities in several semiconducting alloys with surprising success given its underlying hypothesis of weak and dilute disorder. In this paper, we explain how this is possible by focusing on the case of maximally mass-disordered ${\mathrm{Mg}}_{2}{\mathrm{Si}}_{1\ensuremath{-}x}{\mathrm{Sn}}_{x}$. We use a Chebyshev polynomials Green's function method, which allows a full treatment of disorder on very large systems (tens of millions of atoms) to probe individual phonon linewidths and frequency-resolved thermal transport. We demonstrate that the success of perturbation theory originates from the specific form of mass disorder terms in the phonon Green's function and from the interplay between anharmonic and disorder scattering.