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Title: Dilute carbon in H3S under pressure

Abstract

Recently, room temperature superconductivity was measured in a carbonaceous sulfur hydride material whose identity remains unknown. Herein, first-principles calculations are performed to provide a chemical basis for structural candidates derived by doping H3S with low levels of carbon. Pressure stabilizes unusual bonding configurations about the carbon atoms, which can be six-fold coordinated as CH6 entities within the cubic H3S framework, or four-fold coordinated as methane intercalated into the H-S lattice, with or without an additional hydrogen in the framework. The doping breaks degenerate bands, lowering the density of states at the Fermi level ($$N_\text{F}$$), and localizing electrons in C-H bonds. Low levels of CH4 doping do not increase $$N_\text{F}$$ to values as high as those calculated for $$Im3\bar{m}$$-H3S, but they can yield a larger logarithmic average phonon frequency, and an electron–phonon coupling parameter comparable to that of $$\textit{R}\text{3}\textit{m}$$-H3S. Finally, the implications of carbon doping on the superconducting properties are discussed.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. State Univ. of New York (SUNY), Buffalo, NY (United States)
  2. Univ. of Illinois, Chicago, IL (United States)
Publication Date:
Research Org.:
Univ. of Illinois, Chicago, IL (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation; National Science Foundation (NSF); USDOE Office of Science (SC), Fusion Energy Sciences (FES)
OSTI Identifier:
1865212
Alternate Identifier(s):
OSTI ID: 1865713
Grant/Contract Number:  
NA0003975; SC0020340
Resource Type:
Published Article
Journal Name:
npj Computational Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2057-3960
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electronic structure; Structure of solids and liquids; Superconducting properties and materials; Superconductors; Theoretical chemistry

Citation Formats

Wang, Xiaoyu, Bi, Tiange, Hilleke, Katerina P., Lamichhane, Anmol, Hemley, Russell J., and Zurek, Eva. Dilute carbon in H3S under pressure. United States: N. p., 2022. Web. doi:10.1038/s41524-022-00769-9.
Wang, Xiaoyu, Bi, Tiange, Hilleke, Katerina P., Lamichhane, Anmol, Hemley, Russell J., & Zurek, Eva. Dilute carbon in H3S under pressure. United States. https://doi.org/10.1038/s41524-022-00769-9
Wang, Xiaoyu, Bi, Tiange, Hilleke, Katerina P., Lamichhane, Anmol, Hemley, Russell J., and Zurek, Eva. Wed . "Dilute carbon in H3S under pressure". United States. https://doi.org/10.1038/s41524-022-00769-9.
@article{osti_1865212,
title = {Dilute carbon in H3S under pressure},
author = {Wang, Xiaoyu and Bi, Tiange and Hilleke, Katerina P. and Lamichhane, Anmol and Hemley, Russell J. and Zurek, Eva},
abstractNote = {Recently, room temperature superconductivity was measured in a carbonaceous sulfur hydride material whose identity remains unknown. Herein, first-principles calculations are performed to provide a chemical basis for structural candidates derived by doping H3S with low levels of carbon. Pressure stabilizes unusual bonding configurations about the carbon atoms, which can be six-fold coordinated as CH6 entities within the cubic H3S framework, or four-fold coordinated as methane intercalated into the H-S lattice, with or without an additional hydrogen in the framework. The doping breaks degenerate bands, lowering the density of states at the Fermi level ($N_\text{F}$), and localizing electrons in C-H bonds. Low levels of CH4 doping do not increase $N_\text{F}$ to values as high as those calculated for $Im3\bar{m}$-H3S, but they can yield a larger logarithmic average phonon frequency, and an electron–phonon coupling parameter comparable to that of $\textit{R}\text{3}\textit{m}$-H3S. Finally, the implications of carbon doping on the superconducting properties are discussed.},
doi = {10.1038/s41524-022-00769-9},
journal = {npj Computational Materials},
number = 1,
volume = 8,
place = {United States},
year = {2022},
month = {4}
}

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