Nature of the Superionic Phase Transition of Lithium Nitride from Machine Learning Force FieldsShow others and affiliations
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]
2023-08-172023-08-172023-08-17