Published March 29, 2023 | Version v1
Dataset Open

Many-body screening effects in liquid water

  • 1. Chaire de Simulation à l'Echelle Atomique (CSEA), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

* Contact person

Description

The screening arising from many-body excitations is a crucial quantity for describing ab-sorption and inelastic X-ray scattering (IXS) of materials. Similarly, the electron screening plays a critical role in state-of-the-art approaches for determining the fundamental band gap. However, ab initio studies of the screening in liquid water have remained limited. Here, we use a combined analysis based on the Bethe-Salpeter equation and time-dependent density functional theory. We first show that absorption spectra at near-edge energies are insufficient to assess the accuracy by which the screening is described. Next, when the energy range under scrutiny is extended, we instead find that the IXS spectra are highly sensitive and allow for the selection of the optimal theoretical scheme. This leads to good agreement with experiment over a large range of transferred energies and momenta, and enables establishing the elusive fundamental band gap of liquid water at 9.3 eV.

Files

File preview

files_description.md

All files

Files (75.7 KiB)

Name Size
md5:662df978bf15a65322641ea4df81f97d
268 Bytes Preview Download
md5:371ebd3b8d229dc94e6c97860b7f3e33
42.2 KiB Preview Download
md5:6869980ee0e1bceba07db7fdb337f341
33.3 KiB Preview Download

References

Journal reference
I. Reshetnyak, A. Lorin, A. Pasquarello, Nat Commun 14, 2705 (2023)., doi: 10.1038/s41467-023-38420-w