Phase Transition and Liquid-like Superionic Conduction in Ag2S
Abstract
Superionic conductivity in certain polymorphs of Ag2S has inspired numerous concepts for materials applications, but the relationship between the structure and the mobility of silver ions remains poorly explored. In this paper, we report ab initio molecular dynamics simulations for low- (acanthite) and high-temperature (argentite) Ag2S polymorphs that reveal the dynamical processes, giving rise to the superionic behavior in the latter. Similarities between their sulfur sublattices enable simulations of silver ion diffusivities and pathways on essentially an equal footing. For the higher temperature polymorph, calculated temperature-dependent mean square displacements and activation energies by the nudged elastic band method show good correspondence with expectations from the experiment. In the superionic state, silver atoms diffuse in a liquid-like behavior with no preferred diffusion pathways, within the relatively stable body-centered cubic sulfur framework. Conversely, conduction in acanthite appears to depend more on the mobilities of electronic charge carriers.
- Authors:
-
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. Grenoble Alpes, Univ. of Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre, Grenoble (France)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. Grenoble Alpes, Univ. of Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre, Grenoble (France)
- Publication Date:
- Research Org.:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1639035
- Report Number(s):
- PNNL-SA-152823
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 124; Journal Issue: 18; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Transport properties; sulfur; diffusion; electrical conductivity; ions
Citation Formats
Simonnin, Pauline, Sassi, Michel, Gilbert, Benjamin, Charlet, Laurent, and Rosso, Kevin M. Phase Transition and Liquid-like Superionic Conduction in Ag2S. United States: N. p., 2020.
Web. doi:10.1021/acs.jpcc.0c00260.
Simonnin, Pauline, Sassi, Michel, Gilbert, Benjamin, Charlet, Laurent, & Rosso, Kevin M. Phase Transition and Liquid-like Superionic Conduction in Ag2S. United States. https://doi.org/10.1021/acs.jpcc.0c00260
Simonnin, Pauline, Sassi, Michel, Gilbert, Benjamin, Charlet, Laurent, and Rosso, Kevin M. Tue .
"Phase Transition and Liquid-like Superionic Conduction in Ag2S". United States. https://doi.org/10.1021/acs.jpcc.0c00260. https://www.osti.gov/servlets/purl/1639035.
@article{osti_1639035,
title = {Phase Transition and Liquid-like Superionic Conduction in Ag2S},
author = {Simonnin, Pauline and Sassi, Michel and Gilbert, Benjamin and Charlet, Laurent and Rosso, Kevin M.},
abstractNote = {Superionic conductivity in certain polymorphs of Ag2S has inspired numerous concepts for materials applications, but the relationship between the structure and the mobility of silver ions remains poorly explored. In this paper, we report ab initio molecular dynamics simulations for low- (acanthite) and high-temperature (argentite) Ag2S polymorphs that reveal the dynamical processes, giving rise to the superionic behavior in the latter. Similarities between their sulfur sublattices enable simulations of silver ion diffusivities and pathways on essentially an equal footing. For the higher temperature polymorph, calculated temperature-dependent mean square displacements and activation energies by the nudged elastic band method show good correspondence with expectations from the experiment. In the superionic state, silver atoms diffuse in a liquid-like behavior with no preferred diffusion pathways, within the relatively stable body-centered cubic sulfur framework. Conversely, conduction in acanthite appears to depend more on the mobilities of electronic charge carriers.},
doi = {10.1021/acs.jpcc.0c00260},
journal = {Journal of Physical Chemistry. C},
number = 18,
volume = 124,
place = {United States},
year = {2020},
month = {4}
}
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