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:
-
[1];
[2];
[3];
[2]
- 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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Works referenced in this record:
Short range order and Ag diffusion threshold in Ag x (Ge 0.25 Se 0.75 ) 100− x glasses
journal, August 2012
- Piarristeguy, A. A.; Cuello, G. J.; Fernández-Martínez, A.
- physica status solidi (b), Vol. 249, Issue 10
Transparent conductors as solar energy materials: A panoramic review
journal, October 2007
- Granqvist, Claes G.
- Solar Energy Materials and Solar Cells, Vol. 91, Issue 17
Past achievements and future challenges in the development of optically transparent electrodes
journal, November 2012
- Ellmer, Klaus
- Nature Photonics, Vol. 6, Issue 12
Flexible transparent conductive materials based on silver nanowire networks: a review
journal, October 2013
- Langley, Daniel; Giusti, Gaël; Mayousse, Céline
- Nanotechnology, Vol. 24, Issue 45
Metal Nanowire Networks: The Next Generation of Transparent Conductors
journal, September 2014
- Ye, Shengrong; Rathmell, Aaron R.; Chen, Zuofeng
- Advanced Materials, Vol. 26, Issue 39
Nanomaterial-Enabled Stretchable Conductors: Strategies, Materials and Devices
journal, January 2015
- Yao, Shanshan; Zhu, Yong
- Advanced Materials, Vol. 27, Issue 9
Metallic Nanowire-Based Transparent Electrodes for Next Generation Flexible Devices: a Review
journal, October 2016
- Sannicolo, Thomas; Lagrange, Mélanie; Cabos, Anthony
- Small, Vol. 12, Issue 44
High performance transparent multi-touch sensors based on silver nanowires
journal, June 2016
- Cann, Maria; Large, Matthew J.; Henley, Simon J.
- Materials Today Communications, Vol. 7
The Synthesis and Coating of Long, Thin Copper Nanowires to Make Flexible, Transparent Conducting Films on Plastic Substrates
journal, September 2011
- Rathmell, Aaron R.; Wiley, Benjamin J.
- Advanced Materials, Vol. 23, Issue 41
Silver Nanowire Networks as Flexible, Transparent, Conducting Films: Extremely High DC to Optical Conductivity Ratios
journal, June 2009
- De, Sukanta; Higgins, Thomas M.; Lyons, Philip E.
- ACS Nano, Vol. 3, Issue 7
Highly Efficient and Bendable Organic Solar Cells with Solution-Processed Silver Nanowire Electrodes
journal, April 2013
- Song, Myungkwan; You, Dae Sung; Lim, Kyounga
- Advanced Functional Materials, Vol. 23, Issue 34
In Vitro Dermal Safety Assessment of Silver Nanowires after Acute Exposure: Tissue vs. Cell Models
journal, April 2018
- Lehmann, Sylvia; Gilbert, Benjamin; Maffeis, Thierry
- Nanomaterials, Vol. 8, Issue 4
Silver Nanowire Exposure Results in Internalization and Toxicity to Daphnia magna
journal, November 2013
- Scanlan, Leona D.; Reed, Robert B.; Loguinov, Alexandre V.
- ACS Nano, Vol. 7, Issue 12
Short versus long silver nanowires: a comparison of in vivo pulmonary effects post instillation
journal, October 2014
- Silva, Rona M.; Xu, Jingyi; Saiki, Clare
- Particle and Fibre Toxicology, Vol. 11, Issue 1
Crumpling of silver nanowires by endolysosomes strongly reduces toxicity
journal, July 2019
- Lehmann, Sylvia G.; Toybou, Djadidi; Pradas del Real, Ana-Elena
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 30
Shape matters: effects of silver nanospheres and wires on human alveolar epithelial cells
journal, January 2011
- Stoehr, Linda C.; Gonzalez, Edgar; Stampfl, Andreas
- Particle and Fibre Toxicology, Vol. 8, Issue 1
Use of back-scatter electron signals to visualise cell/nanowires interactions in vitro and in vivo; frustrated phagocytosis of long fibres in macrophages and compartmentalisation in mesothelial cells in vivo
journal, January 2012
- Schinwald, Anja; Donaldson, Ken
- Particle and Fibre Toxicology, Vol. 9, Issue 1
Autophagy induction by silver nanowires: A new aspect in the biocompatibility assessment of nanocomposite thin films
journal, November 2012
- Verma, Navin K.; Conroy, Jennifer; Lyons, Philip E.
- Toxicology and Applied Pharmacology, Vol. 264, Issue 3
Silver Nanowire Particle Reactivity with Human Monocyte-Derived Macrophage Cells: Intracellular Availability of Silver Governs Their Cytotoxicity
journal, September 2017
- Theodorou, Ioannis G.; Müller, Karin H.; Chen, Shu
- ACS Biomaterials Science & Engineering, Vol. 3, Issue 10
Environmental Transformations of Silver Nanoparticles: Impact on Stability and Toxicity
journal, February 2012
- Levard, Clément; Hotze, E. Matt; Lowry, Gregory V.
- Environmental Science & Technology, Vol. 46, Issue 13
Formation of Nanosilver from Silver Sulfide Nanoparticles in Natural Waters by Photoinduced Fe(II, III) Redox Cycling
journal, November 2016
- Li, Lingxiangyu; Zhou, Qunfang; Geng, Fanglan
- Environmental Science & Technology, Vol. 50, Issue 24
Corrosion Mechanisms for Silver Exposed to the Atmosphere
journal, January 1992
- Graedel, T. E.
- Journal of The Electrochemical Society, Vol. 139, Issue 7
Tarnishing of Silver by Organic Sulfur Vapors: Rates and Film Characteristics
journal, January 1982
- Sinclair, J. D.
- Journal of The Electrochemical Society, Vol. 129, Issue 1
Corrosion at the Nanoscale: The Case of Silver Nanowires and Nanoparticles
journal, November 2005
- Elechiguerra, Jose Luis; Larios-Lopez, Leticia; Liu, Cui
- Chemistry of Materials, Vol. 17, Issue 24
Über die kubischen Hochtemperaturmodifikationen der Sulfide, Selenide und Telluride des Silbers und des einwertigen Kupfers
journal, January 1936
- Rahlfs, Paul
- Zeitschrift für Physikalische Chemie, Vol. 31B, Issue 1
The Crystallography of Silver Sulfide, Ag 2 S
journal, January 1958
- Frueh, Alfred J.
- Zeitschrift für Kristallographie, Vol. 110, Issue 1-6
Single-crystal neutron diffraction study of the fast-ion conductor β-Ag2S between 186 and 325°C
journal, January 1980
- Cava, R. J.; Reidinger, F.; Wuensch, B. J.
- Journal of Solid State Chemistry, Vol. 31, Issue 1
Diffusion mechanism in the superionic conductor Li4PS4I studied by first-principles calculations
journal, June 2018
- Sicolo, Sabrina; Kalcher, Constanze; Sedlmaier, Stefan J.
- Solid State Ionics, Vol. 319
Structural, electronic and optical properties of copper, silver and gold sulfide: a DFT study
journal, February 2016
- Suárez, Javier Amaya; Plata, José J.; Márquez, Antonio M.
- Theoretical Chemistry Accounts, Vol. 135, Issue 3
Metal-non-metal transition in silver chalcogenides
journal, October 1977
- Junod, P.; Hediger, H.; Kilchör, B.
- Philosophical Magazine, Vol. 36, Issue 4
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Assessing the performance of recent density functionals for bulk solids
journal, April 2009
- Csonka, Gábor I.; Perdew, John P.; Ruzsinszky, Adrienn
- Physical Review B, Vol. 79, Issue 15
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
A unified formulation of the constant temperature molecular dynamics methods
journal, July 1984
- Nosé, Shuichi
- The Journal of Chemical Physics, Vol. 81, Issue 1
Constant Temperature Molecular Dynamics Methods
journal, January 1991
- Nosé, Shuichi
- Progress of Theoretical Physics Supplement, Vol. 103
Canonical dynamics: Equilibrium phase-space distributions
journal, March 1985
- Hoover, William G.
- Physical Review A, Vol. 31, Issue 3
Reversible work transition state theory: application to dissociative adsorption of hydrogen
journal, February 1995
- Mills, Gregory; Jónsson, Hannes; Schenter, Gregory K.
- Surface Science, Vol. 324, Issue 2-3
A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
- Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
Error estimates on averages of correlated data
journal, July 1989
- Flyvbjerg, H.; Petersen, H. G.
- The Journal of Chemical Physics, Vol. 91, Issue 1
Some tracer correlation factors in the f.c.c. lattice†
journal, January 1984
- Murch, G. E.
- Journal of Physics and Chemistry of Solids, Vol. 45, Issue 4