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Dilute carbon in H3S under pressure

Xiaoyu Wang, Tiange Bi, Katerina P. Hilleke, Anmol Lamichhane, Russell J. Hemley, Eva Zurek

2022npj Computational Materials24 citationsDOIOpen Access PDF

Abstract

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 H 3 S with low levels of carbon. Pressure stabilizes unusual bonding configurations about the carbon atoms, which can be six-fold coordinated as CH 6 entities within the cubic H 3 S 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 F ), and localizing electrons in C-H bonds. Low levels of CH 4 doping do not increase N F to values as high as those calculated for $$Im\bar{3}m$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>I</mml:mi> <mml:mi>m</mml:mi> <mml:mover> <mml:mrow> <mml:mn>3</mml:mn> </mml:mrow> <mml:mo>¯</mml:mo> </mml:mover> <mml:mi>m</mml:mi> </mml:mrow> </mml:math> -H 3 S, but they can yield a larger logarithmic average phonon frequency, and an electron–phonon coupling parameter comparable to that of R 3 m -H 3 S. The implications of carbon doping on the superconducting properties are discussed.

Topics & Concepts

DopingMaterials scienceHydrogenChemistryOrganic chemistryOptoelectronicsOrganic and Molecular Conductors ResearchHigh-pressure geophysics and materialsInorganic Fluorides and Related Compounds
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