Theoretical optical and x-ray spectra of liquid and solid H_2O

TL;DR

This paper presents a theoretical approach using many-body perturbation theory to accurately compute optical and x-ray spectra of water and ice, highlighting the importance of excitonic effects and inelastic losses.

Contribution

It introduces a comprehensive ab initio method combining BSE with self-energy corrections for precise spectra of water and ice.

Findings

Many-body effects are essential for accurate spectra.

The approach improves upon independent-particle methods.

Quantitative agreement with experimental spectra is achieved.

Abstract

Theoretical optical and x-ray spectra of model structures of water and ice are calculated using a many-body perturbation theory, Bethe-Salpeter equation (BSE) approach implemented in the valence- and core-excitation codes AI2NBSE and OCEAN. These codes use ab initio density functional theory wave functions from a plane-wave, pseudopotential code, quasi-particle self energy corrections, and a BSE treatment of particle-hole interactions. The approach improves upon independent-particle methods through the inclusion of a complex, energy-dependent self energy and screened particle-hole interactions to account for inelastic losses and excitonic effects. These many-body effects are found to be crucial for quantitative calculations of ice and water spectra.