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Title: Dissociation products and structures of solid H 2 S at strong compression

Abstract

Hydrogen sulfides have recently received a great deal of interest due to the record high superconducting temperatures of up to 203 K observed on strong compression of dihydrogen sulfide ( H 2 S ). A joint theoretical and experimental study is presented in this paper in which decomposition products and structures of compressed H 2 S are characterized, and their superconducting properties are calculated. In addition to the experimentally known H 2 S and H 3 S phases, our first-principles structure searches have identified several energetically competitive stoichiometries that have not been reported previously: H 2 S 3 , H 3 S 2 , HS 2 , and H 4 S 3 . In particular, H 4 S 3 is predicted to be thermodynamically stable within a large pressure range of 25–113 GPa. High-pressure x-ray diffraction measurements confirm the presence of H 3 S and H 4 S 3 through decomposition of H 2 S that emerges at 27 GPa and coexists with residual H 2 S , at least up to the highest pressure of 140 GPa studied in our experiments. Electron-phonon coupling calculations show that H 4 S 3 has a small T c of below 2 K, and that H 2 S is mainly responsible for the observed superconductivity of samples prepared at low temperature ( < 100 K).

Authors:
 [1];  [2];  [3];  [4];  [1];  [5];  [6];  [6];  [7];  [7];  [8];  [9];  [9];  [4]
  1. Jiangsu Normal Univ., Xuzhou (China)
  2. Center for High Pressure Science and Technology Advanced Research, Shanghai (China); Jilin Univ., Changchun (China). State Key Lab. of Superhard Materials
  3. Jilin Univ., Changchun (China). State Key Lab. of Superhard Materials; Carnegie Inst. of Washington, Washington D.C. (United States)
  4. Jilin Univ., Changchun (China). State Key Lab. of Superhard Materials
  5. Univ. of Cambridge (United Kingdom)
  6. Cavendish Lab., Cambridge (United Kingdom)
  7. Center for High Pressure Science and Technology Advanced Research, Shanghai (China)
  8. Donostia International Physics Center (DIPC), Gipuzkoa (Spain); Univ. of the Basque Country, Donostia (Spain)
  9. Sorbonne Univ., Paris (France)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research in Extreme Environments (EFree)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); National Natural Science Foundation of China (NNSFC); Engineering and Physical Sciences Research Council (EPSRC); Spanish Ministry of Economy and Competitiveness; Agence nationale de la recherche (ANR); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1387308
Alternate Identifier(s):
OSTI ID: 1234300
Grant/Contract Number:  
SC0001057; 11204111; 11404148; 11274136; 11534003; EP/J017639/1; FIS2013-48286-C2-2-P; ANR-13-IS10-0003-01; NA-0002006; SC-0001057
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 93; Journal Issue: 2; Related Information: EFree partners with Carnegie Institution of Washington (lead); California Institute of Technology; Colorado School of Mines; Cornell University; Lehigh University; Pennsylvania State University; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; catalysis (heterogeneous); solar (photovoltaic); phonons; thermoelectric; energy storage (including batteries and capacitors); hydrogen and fuel cells; superconductivity; charge transport; mesostructured materials; materials and chemistry by design; synthesis (novel materials)

Citation Formats

Li, Yinwei, Wang, Lin, Liu, Hanyu, Zhang, Yunwei, Hao, Jian, Pickard, Chris J., Nelson, Joseph R., Needs, Richard J., Li, Wentao, Huang, Yanwei, Errea, Ion, Calandra, Matteo, Mauri, Francesco, and Ma, Yanming. Dissociation products and structures of solid H2S at strong compression. United States: N. p., 2016. Web. doi:10.1103/PhysRevB.93.020103.
Li, Yinwei, Wang, Lin, Liu, Hanyu, Zhang, Yunwei, Hao, Jian, Pickard, Chris J., Nelson, Joseph R., Needs, Richard J., Li, Wentao, Huang, Yanwei, Errea, Ion, Calandra, Matteo, Mauri, Francesco, & Ma, Yanming. Dissociation products and structures of solid H2S at strong compression. United States. doi:10.1103/PhysRevB.93.020103.
Li, Yinwei, Wang, Lin, Liu, Hanyu, Zhang, Yunwei, Hao, Jian, Pickard, Chris J., Nelson, Joseph R., Needs, Richard J., Li, Wentao, Huang, Yanwei, Errea, Ion, Calandra, Matteo, Mauri, Francesco, and Ma, Yanming. Mon . "Dissociation products and structures of solid H2S at strong compression". United States. doi:10.1103/PhysRevB.93.020103. https://www.osti.gov/servlets/purl/1387308.
@article{osti_1387308,
title = {Dissociation products and structures of solid H2S at strong compression},
author = {Li, Yinwei and Wang, Lin and Liu, Hanyu and Zhang, Yunwei and Hao, Jian and Pickard, Chris J. and Nelson, Joseph R. and Needs, Richard J. and Li, Wentao and Huang, Yanwei and Errea, Ion and Calandra, Matteo and Mauri, Francesco and Ma, Yanming},
abstractNote = {Hydrogen sulfides have recently received a great deal of interest due to the record high superconducting temperatures of up to 203 K observed on strong compression of dihydrogen sulfide (H2S). A joint theoretical and experimental study is presented in this paper in which decomposition products and structures of compressed H2S are characterized, and their superconducting properties are calculated. In addition to the experimentally known H2S and H3S phases, our first-principles structure searches have identified several energetically competitive stoichiometries that have not been reported previously: H2S3, H3S2, HS2, and H4S3. In particular, H4S3 is predicted to be thermodynamically stable within a large pressure range of 25–113 GPa. High-pressure x-ray diffraction measurements confirm the presence of H3S and H4S3 through decomposition of H2S that emerges at 27 GPa and coexists with residual H2S, at least up to the highest pressure of 140 GPa studied in our experiments. Electron-phonon coupling calculations show that H4S3 has a small Tc of below 2 K, and that H2S is mainly responsible for the observed superconductivity of samples prepared at low temperature (<100 K).},
doi = {10.1103/PhysRevB.93.020103},
journal = {Physical Review B},
number = 2,
volume = 93,
place = {United States},
year = {2016},
month = {1}
}

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