Full Temperature-Dependent Potential and Anharmonicity in Metallic Hydrogen: Colossal NQE and the Consequences

Abstract

The temperature-dependent effective potential (TDEP) method for anharmonic phonon dispersion is generalized to the full potential case by combining with path integral formalism. This extension naturally resolves the intrinsic difficulty in the original TDEP at low temperature. The new method is applied to solid metallic hydrogen at high pressure. A colossal nuclear quantum effect (NQE) and subsequent anharmonicity are discovered, which not only leads to unexpectedly large drift of protons, but also slows down the convergence rate substantially when computing the phonon dispersions. By employing direct ab initio path integral molecular dynamics simulations as the benchmark, a possible breakdown of phonon picture in metallic hydrogen due to colossal NQE is indicated, implying novel lattice dynamical phenomena might exist. Inspired by this observation, a general theoretical formalism for quantum lattice dynamics beyond phonon is sketched, with the main features being discussed.

arXiv comment35 pages, 9 figures, 1 table, with Supporting Information

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• General linear correction method for DFT+X energy: application to U-M (M=Al, Ga, In) alloys under high pressure