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research article

Seebeck Coefficient of Ionic Conductors from Bayesian Regression Analysis

Drigo, Enrico
•
Baroni, Stefano
•
Pegolo, Paolo  
June 10, 2024
Journal of Chemical Theory and Computation

We propose a novel approach to evaluating the ionic Seebeck coefficient in electrolytes from relatively short equilibrium molecular dynamics simulations, based on the Green-Kubo theory of linear response and Bayesian regression analysis. By exploiting the probability distribution of the off-diagonal elements of a Wishart matrix, we develop a consistent and unbiased estimator for the Seebeck coefficient, whose statistical uncertainty can be arbitrarily reduced in the long-time limit. We assess the efficacy of our method by benchmarking it against extensive equilibrium molecular dynamics simulations conducted on molten CsF using empirical force fields. We then employ this procedure to calculate the Seebeck coefficient of molten NaCl, KCl, and LiCl using neural network force fields trained on ab initio data over a range of pressure-temperature conditions.

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Type
research article
DOI
10.1021/acs.jctc.4c00124
Web of Science ID

WOS:001244008400001

Author(s)
Drigo, Enrico
Baroni, Stefano
Pegolo, Paolo  
Date Issued

2024-06-10

Publisher

Amer Chemical Soc

Published in
Journal of Chemical Theory and Computation
Subjects

Physical Sciences

•

Statistical-Mechanical Theory

•

Born Repulsive Parameters

•

Partial Molar Properties

•

Markov Random-Processes

•

Irreversible-Processes

•

Transport-Coefficients

•

Reciprocal Relations

•

Computer Calculation

•

Alkali Halides

•

Sizes

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
FunderGrant Number

HORIZON EUROPE European Innovation Council

101093374

European Commission

2022W2BPCK

Italian MUR through the PRIN project ARES

Available on Infoscience
July 3, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/209018
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