Temperature-dependent Electronic Spectral Functions from Band-Structure Unfolding

TL;DR

This paper presents a method to compute temperature-dependent electronic spectral functions non-perturbatively by implementing band-structure unfolding in the FHI-aims software, improving accuracy at elevated temperatures.

Contribution

It introduces an implementation of band-structure unfolding in FHI-aims to accurately obtain spectral functions beyond perturbative approximations.

Findings

Implemented band-structure unfolding in FHI-aims

Enhanced the calculation of temperature-dependent spectral functions

Provided updates to the original unfolding technique

Abstract

The electronic band structure, describing the periodic dependence of electronic quantum states on lattice momentum in reciprocal space, is a fundamental concept in solid-state physics. However, it's only well-defined for static nuclei. To account for thermodynamic effects, this concept must be generalized by introducing the temperature-dependent spectral function, which characterizes the finite-width distributions of electronic quantum states at each reciprocal vector. Many-body perturbation theory can compute spectral functions and associated observables, but it approximates the dynamics of nuclei and its coupling to the electrons using the harmonic approximation and linear-order electron-phonon coupling elements, respectively. These approximations may fail at elevated temperatures or for mobile atoms. To avoid inaccuracies, the electronic spectral function can be obtained non-perturbatively, capturing higher-order couplings between electrons and vibrational degrees of freedom. This process involves recovering the representation of supercell bands in the first Brillouin zone of the primitive cell, a process known as unfolding. In this contribution, we describe the implementation of the band-structure unfolding technique in the electronic-structure theory package FHI-aims and the updates made since its original development.