Published July 20, 2022 | Version v1
Dataset Open

Temperature dependent properties of the aqueous electron

  • 1. Chaire de simulation à l'échelle atomique, École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland
  • 2. HQS Quantum Simulations GmbH, Haid-und-Neu-Straße 7, D-76131 Karlsruhe, Germany

* Contact person

Description

The temperature-dependent properties of the aqueous electron have been extensively studied using mixed quantum-classical simulations in a wide range of thermodynamic conditions based on one-electron pseudopotentials. While the cavity model appears to explain most of the physical properties of the aqueous electron, only a non-cavity model has so far been successful in accounting for the temperature dependence of the absorption spectrum. Here, we present an accurate and efficient description of the aqueous electron under various thermodynamic conditions by combining hybrid functional-based molecular dynamics, machine learning techniques, and multiple time-step methods. Our advanced simulations accurately describe the temperature dependence of the absorption maximum in the presence of cavity formation. Specifically, our work reveals that the red shift of the absorption maximum results from an increasing gyration radius with temperature, rather than from global density variations as previously suggested.

Files

File preview

files_description.md

All files

Files (416.4 MiB)

Name Size
md5:6d688183faa8cccf5a92db34d5911af5
293 Bytes Preview Download
md5:9f733582475b42ca15db5ce642ed0950
416.4 MiB Download

References

Journal reference
J.Lan, V.Rybkin, A. Pasquarello, Angewandte Chemie International Edition, doi: 10.1002/anie.202209398

Journal reference
J.Lan, V.Rybkin, A. Pasquarello, Angewandte Chemie International Edition