Phonon broadening from supercell lattice dynamics: random and correlated disorder

TL;DR

This paper presents a supercell lattice dynamics method using band unfolding to analyze disorder-induced phonon broadening in crystalline materials, with insights into effects of mass and interaction disorder.

Contribution

It introduces a novel approach combining supercell calculations and band unfolding to quantify phonon broadening due to disorder, validated against virtual crystal approximation.

Findings

Disorder causes measurable phonon broadening in spectra.

Correlated disorder affects phonon dispersion and broadening.

Homoatomic neighbor disfavoring increases phonon broadening.

Abstract

We demonstrate how supercell implementations of conventional lattice dynamical calculations can be used to determine the extent and nature of disorder-induced broadening in the phonon dispersion spectrum of disordered crystalline materials. The approach taken relies on band unfolding, and is first benchmarked against virtual crystal approximation phonon calculations. The different effects of mass and interaction disorder on the phonon broadening are then presented, focussing on the example of a simple cubic binary alloy. For the mass disorder example, the effect of introducing correlated disorder is also explored by varying the fraction of homoatomic and heteroatomic neighbours. Systematic progression in the degree of phonon broadening, on the one hand, and the form of the phonon dispersion curves from primitive to face-centered cubic type, on the other hand, is observed as homoatomic neighbours are disfavoured. The implications for rationalising selection rule violations in disordered materials and for using inelastic neutron scattering measurements as a means of characterising disorder are discussed.