Strong anharmonic and quantum effects in Pm3¯n AlH3 under high pressure: A first-principles study

Pugeng Hou, Francesco Belli, Raffaello Bianco, and Ion Errea
Phys. Rev. B 103, 134305 – Published 29 April 2021

Abstract

Motivated by the absence of experimental superconductivity in the metallic Pm3¯n phase of AlH3 despite the predictions, we reanalyze its vibrational and superconducting properties at pressures P99 GPa making use of first-principles techniques. In our calculations based on the self-consistent harmonic approximation method that treats anharmonicity beyond perturbation theory, we predict a strong anharmonic correction to the phonon spectra and demonstrate that the superconducting critical temperatures predicted in previous calculations based on the harmonic approximation are strongly suppressed by anharmonicity. The electron-phonon coupling concentrates on the lowest-energy hydrogen-character optical modes at the X point of the Brillouin zone. As a consequence of the strong anharmonic enhancement of their frequency, the electron-phonon coupling is suppressed by at least 30%. The suppression in λ makes Tc smaller than 4.2 K above 120 GPa, which is well consistent with the experimental evidence. Our results underline that metal hydrides with hydrogen atoms in interstitial sites are subject to huge anharmonic effects.

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  • Received 29 January 2021
  • Revised 26 March 2021
  • Accepted 6 April 2021

DOI:https://doi.org/10.1103/PhysRevB.103.134305

©2021 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Pugeng Hou1, Francesco Belli2,3, Raffaello Bianco3, and Ion Errea2,3,4

  • 1College of Science, Northeast Electric Power University, Changchun Road 169, 132012 Jilin, People's Republic of China
  • 2Fisika Aplikatua Saila, Gipuzkoako Ingeniaritza Eskola, University of the Basque Country (UPV/EHU), Europa Plaza 1, 20018 Donostia/San Sebastián, Spain
  • 3Centro de Física de Materiales (CSIC-UPV/EHU), Manuel de Lardizabal Pasealekua 5, 20018 Donostia/San Sebastián, Spain
  • 4Donostia International Physics Center (DIPC), Manuel de Lardizabal Pasealekua 4, 20018 Donostia/San Sebastián, Spain

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Issue

Vol. 103, Iss. 13 — 1 April 2021

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