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High-Pressure Hydrogen Sulfide from First Principles: A Strongly Anharmonic Phonon-Mediated Superconductor
Open accessAbstract
We use first-principles calculations to study structural, vibrational, and superconducting properties of H_{2}S at pressures P≥200 GPa. The inclusion of zero-point energy leads to two different possible dissociations of H2S, namely 3H2S→2H3S+S and 5H2S→3H3S+HS2, where both H3S and HS2 are metallic. For H3S, we perform nonperturbative calculations of anharmonic effects within the self-consistent harmonic approximation and show that the harmonic approximation strongly overestimates the electron-phonon interaction (λ≈2.64 at 200 GPa) and Tc. Anharmonicity hardens H─S bond-stretching modes and softens H─S bond-bending modes. As a result, the electron-phonon coupling is suppressed by 30% (λ≈1.84 at 200 GPa). Moreover, while at the harmonic level Tc decreases with increasing pressure, the inclusion of anharmonicity leads to a Tc that is almost independent of pressure. High-pressure hydrogen sulfide is a strongly anharmonic superconductor.
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Cites
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
Kresse, G., & Furthmüller, J. (1996) · Physical Review B · doi:10.1103/physrevb.54.11169 · Cited by 123,652
Possible highT c superconductivity in the Ba?La?Cu?O system
Bednorz, J. G., & M�ller, K. A. (1986) · Zeitschrift f�r Physik B Condensed Matter · doi:10.1007/bf01303701 · Cited by 14,319
Cited by
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Peng, F., Sun, Y., Pickard, C. J., Needs, R. J., Wu, Q., & Ma, Y. (2017) · Physical Review Letters · doi:10.1103/physrevlett.119.107001 · Cited by 955
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Oganov, A. R., Pickard, C. J., Zhu, Q., & Needs, R. J. (2019) · Nature Reviews Materials · doi:10.1038/s41578-019-0101-8 · Cited by 717
Self-citationTadano, T., & Tsuneyuki, S. (2015) · Physical Review B · doi:10.1103/physrevb.92.054301 · Cited by 640
Quantum hydrogen-bond symmetrization in the superconducting hydrogen sulfide system
Errea, I., Calandra, M., Pickard, C. J., Nelson, J. R., Needs, R. J., Li, Y., Liu, H., Zhang, Y., Ma, Y., & Mauri, F. (2016) · Nature · doi:10.1038/nature17175 · Cited by 331
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Metadata
- Authors
- Errea, I., Calandra, M., Pickard, C. J., Nelson, J., Needs, R. J., Li, Y., Liu, H., Zhang, Y., Ma, Y., & Mauri, F.
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2015-04-16
- Volume
- 114
- Issue
- 15
- Pages
- 157004-157004
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W2138890585
- Cited by
- 488
- References
- 2
- FWCI
- 55.72
- Type
- journal article
- Language
- en
- Open access
- green
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- Errea, I., Calandra, M., Pickard, C. J., Nelson, J., Needs, R. J., Li, Y., Liu, H., Zhang, Y., Ma, Y., & Mauri, F. (2015). High-Pressure Hydrogen Sulfide from First Principles: A Strongly Anharmonic Phonon-Mediated Superconductor. Physical Review Letters. https://doi.org/10.1103/physrevlett.114.157004
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