Paolo Pegolo^1*, Stefano Baroni^1,2*, Federico Grasselli^3*

1 SISSA—Scuola Internazionale Superiore di Studi Avanzati, 34136 Trieste, Italy

2 CNR—Istituto Officina dei Materiali, SISSA, 34136 Trieste, Italy

3 COSMO—Laboratory of Computational Science and Modelling, IMX, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland

* Corresponding authors emails: ppegolo@sissa.it, baroni@sissa.it, federico.grasselli@epfl.ch

DOI10.24435/materialscloud:8f-d7 [version v1]

Publication date: Aug 15, 2023

How to cite this record

Paolo Pegolo, Stefano Baroni, Federico Grasselli, Self-interaction and transport of solvated electrons in molten salts, Materials Cloud Archive 2023.126 (2023), doi: 10.24435/materialscloud:8f-d7.

Description

The dynamics of (few) electrons dissolved in an ionic fluid—as when a small amount of metal is added to a solution while upholding its electronic insulation—manifests interesting properties that can be ascribed to nontrivial topological features of particle transport (e.g., Thouless' pumps). In the adiabatic regime, the charge distribution and the dynamics of these dissolved electrons are uniquely determined by the nuclear configuration. Yet, their localization into effective potential wells and their diffusivity are dictated by how the self-interaction is modeled. In this article, we investigate the role of self-interaction in the description of localization and transport properties of dissolved electrons in non-stoichiometric molten salts. Although the account for the exact (Fock) exchange strongly localizes the dissolved electrons, decreasing their tunneling probability and diffusivity, we show that the dynamics of the ions and of the dissolved electrons are largely uncorrelated, irrespective of the degree to which the electron self-interaction is treated, and in accordance with topological arguments. This record contains input and analysis scripts to reproduce the findings of this article.

Materials Cloud sections using this data

Files

File name	Size	Description
README.md MD5md5:5a362f688ecaf3c800c7fa75d5697e20	1.4 KiB	Detailed description of the repository.
analysis.ipynb MD5md5:fd6c9dc358121b917f2a7529b0a25a61	22.5 KiB	Jupyter notebook to reproduce the figures
AIP.mplstyle MD5md5:a9cb2012d7addf1b24c96039d09e4049	1.2 KiB	Matplotlib style used in the notebook
trajectories.zip MD5md5:4e299f47b9025f3be7ef53d0ca253c2b	72.3 MiB	Folder with the MD trajectories
fluxes.zip MD5md5:67fa0656c69af08e73af4151a0dd4b6f	33.9 MiB	Folder with the charge fluxes
RPDF.zip MD5md5:cc681982f59832dda18f446df59e1142	68.3 KiB	Folder with the radial pair distribution functions
cp2k_inputs.zip MD5md5:7e1873e358f100184b84113a67bfca04	14.9 KiB	Folder with CP2K inputs

License

Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.

External references

Keywords

transport ionic transport molten salts topological materials MaX Marie Curie Fellowship