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Nature of the Superionic Phase Transition of Lithium Nitride from Machine Learning Force Fields
Imperial Coll London, England.
Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering. Imperial Coll London, England.
Imperial Coll London, England; Imperial Coll London, England.
Trinity Coll Dublin, Ireland; Trinity Coll Dublin, Ireland.
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2023 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 35, no 15, p. 6133-6140Article in journal (Refereed) Published
Abstract [en]

Superionic conductors have great potential as solid-stateelectrolytes,but the physics of type-II superionic transitions remains elusive.In this study, we employed molecular dynamics simulations, using machinelearning force fields, to investigate the type-II superionic phasetransition in & alpha;-Li3N. We characterized Li3N above and below the superionic phase transition by calculatingthe heat capacity, Li+ ion self-diffusion coefficient,and Li defect concentrations as functions of temperature. Our findingsindicate that both the Li+ self-diffusion coefficient andLi vacancy concentration follow distinct Arrhenius relationships inthe normal and superionic regimes. The activation energies for self-diffusionand Li vacancy formation decrease by a similar proportion across thesuperionic phase transition. This result suggests that the superionictransition may be driven by a decrease in defect formation energeticsrather than changes in Li transport mechanism. This insight may haveimplications for other type-II superionic materials.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2023. Vol. 35, no 15, p. 6133-6140
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-196652DOI: 10.1021/acs.chemmater.3c01271ISI: 001032191100001OAI: oai:DiVA.org:liu-196652DiVA, id: diva2:1788938
Note

Funding Agencies|Faraday Institution [EP/S003053/1, FIRG025]; Swedish Research Council (VR) program [2021-00486]; Eric and Wendy Schmidt AI in Science Postdoctoral Fellowship; Schmidt Futures program; Irish Research Council; Irish Research Council Advanced Laureate Award [IRCLA/2019/127]; Royal Society [UF130329, URF/R/191006]; EPSRC [EP/P020194/1]

Available from: 2023-08-17 Created: 2023-08-17 Last updated: 2023-08-17

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