Many-body screening effects in liquid water
Abstract The screening arising from many-body excitations is a crucial quantity for describing absorption 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 in...
| Main Authors: | , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-38420-w |
| _version_ | 1797827479938793472 |
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| author | Igor Reshetnyak Arnaud Lorin Alfredo Pasquarello |
| author_facet | Igor Reshetnyak Arnaud Lorin Alfredo Pasquarello |
| author_sort | Igor Reshetnyak |
| collection | DOAJ |
| description | Abstract The screening arising from many-body excitations is a crucial quantity for describing absorption 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. |
| first_indexed | 2024-04-09T12:48:59Z |
| format | Article |
| id | doaj.art-f376ff2aead146598be57f99fb5a3ab6 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-04-09T12:48:59Z |
| publishDate | 2023-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-f376ff2aead146598be57f99fb5a3ab62023-05-14T11:21:04ZengNature PortfolioNature Communications2041-17232023-05-011411710.1038/s41467-023-38420-wMany-body screening effects in liquid waterIgor Reshetnyak0Arnaud Lorin1Alfredo Pasquarello2Chaire de Simulation à l’Echelle Atomique (CSEA), Ecole Polytechnique Fédérale de Lausanne (EPFL)Chaire de Simulation à l’Echelle Atomique (CSEA), Ecole Polytechnique Fédérale de Lausanne (EPFL)Chaire de Simulation à l’Echelle Atomique (CSEA), Ecole Polytechnique Fédérale de Lausanne (EPFL)Abstract The screening arising from many-body excitations is a crucial quantity for describing absorption 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.https://doi.org/10.1038/s41467-023-38420-w |
| spellingShingle | Igor Reshetnyak Arnaud Lorin Alfredo Pasquarello Many-body screening effects in liquid water Nature Communications |
| title | Many-body screening effects in liquid water |
| title_full | Many-body screening effects in liquid water |
| title_fullStr | Many-body screening effects in liquid water |
| title_full_unstemmed | Many-body screening effects in liquid water |
| title_short | Many-body screening effects in liquid water |
| title_sort | many body screening effects in liquid water |
| url | https://doi.org/10.1038/s41467-023-38420-w |
| work_keys_str_mv | AT igorreshetnyak manybodyscreeningeffectsinliquidwater AT arnaudlorin manybodyscreeningeffectsinliquidwater AT alfredopasquarello manybodyscreeningeffectsinliquidwater |