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research article

Self-interaction and transport of solvated electrons in molten salts

Pegolo, Paolo
•
Baroni, Stefano
•
Grasselli, Federico  
September 7, 2023
Journal Of Chemical Physics

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 the 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.

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Type
research article
DOI
10.1063/5.0169474
Web of Science ID

WOS:001146183600001

Author(s)
Pegolo, Paolo
Baroni, Stefano
Grasselli, Federico  
Date Issued

2023-09-07

Publisher

Aip Publishing

Published in
Journal Of Chemical Physics
Volume

159

Issue

9

Article Number

094116

Subjects

Physical Sciences

•

Charge-Transport

•

Liquid Metals

•

Miscibility

•

Localization

•

Quantization

•

Polarization

•

Diffusion

•

Polarons

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
FunderGrant Number

European Commission through the MAX Center of Excellence for supercomputing applications

101093374

Italian MUR through the PRIN project FERMAT

2017KFY7XF

Italian National Center from HPC, Big Data, and Quantum Computing

CN00000013

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Available on Infoscience
February 23, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/205321
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