Towards a first principles description of phonons in Ni$_{50}$Pt$_{50}$ disordered alloys: the role of relaxation

TL;DR

This study combines density-functional perturbation theory and the itinerant coherent potential approximation to analyze how atomic relaxation influences phonon properties and neutron scattering in disordered Ni50Pt50 alloys, highlighting relaxation's significant impact.

Contribution

It introduces a first-principles approach to account for atomic relaxation effects on phonons in disordered alloys, improving upon previous empirical methods.

Findings

Relaxation significantly alters force constants and scattering cross sections.

The effect of relaxation is more pronounced in disordered alloys than in ordered ones.

First-principles calculations better match experimental observations.

Abstract

Using a combination of density-functional perturbation theory and the itinerant coherent potential approximation, we study the effects of atomic relaxation on the inelastic incoherent neutron scattering cross sections of disordered Ni$_{50}$Pt$_{50}$ alloys. We build on previous work, where empirical force constants were adjusted {\it ad hoc} to agree with experiment. After first relaxing all structural parameters within the local-density approximation for ordered NiPt compounds, density-functional perturbation theory is then used to compute phonon spectra, densities of states, and the force constants. The resulting nearest-neighbor force constants are first compared to those of other ordered structures of different stoichiometry, and then used to generate the inelastic scattering cross sections within the itinerant coherent potential approximation. We find that structural relaxation substantially affects the computed force constants and resulting inelastic cross sections, and that the effect is much more pronounced in random alloys than in ordered alloys.