Strong anharmonic and quantum effects in Pm(3)over-barn AIH3 under high pressure: A first-principles study

Motivated by the absence of experimental superconductivity in the metallic Pm (3) over barn phase of A1H(3) despite the predictions, we reanalyze its vibrational and superconducting properties at pressures P >= 99 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 lambda makes T-c 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.