Mode-decomposition based on crystallographic symmetry in the band-unfolding method

TL;DR

This paper introduces a group-theoretic method to decompose unfolded phonon band structures into symmetry-based modes and chemical element contributions, enabling detailed analysis of disordered systems.

Contribution

It develops a novel procedure using projection operators for small representations and chemical elements to analyze unfolded band structures based on crystallographic symmetry.

Findings

Identified discontinuous and split branches in disordered Cu-Au phonon bands.

Demonstrated the method's ability to distinguish contributions from different chemical elements.

Revealed how chemical disorder affects phonon band structures.

Abstract

The band-unfolding method is widely used to calculate the effective band structures of a disordered system from its supercell model. The unfolded band structures show the crystallographic symmetry of the underlying structure, where the difference of chemical components and the local atomic relaxation are ignored. It has been, however, still difficult to decompose the unfolded band structures into the modes based on the crystallographic symmetry of the underlying structure, and therefore detailed analyses of the unfolded band structures have been restricted. In this study, we develop a procedure to decompose the unfolded band structures according to the small representations (SRs) of the little groups. For this purpose, we derive the projection operators for SRs based on the group representation theory. We also introduce another type of projection operators for chemical elements, which enables us to decompose the unfolded band structures into the contributions of different combinations of chemical elements. Using the current method, we investigate the phonon band structure of disordered face-centered cubic Cu0.75Au0.25, which has large variations of atomic masses and force constants among the atomic sites due to the chemical disorder. We find several peculiar behaviors such as discontinuous and split branches in the unfolded phonon band structure. They are found to occur because different combinations of the chemical elements contribute to different regions of frequency.