Quantum structural fluxion in superconducting lanthanum polyhydride.

The discovery of 250-kelvin superconducting lanthanum polyhydride under high pressure marked a significant advance toward the realization of a room‐temperature superconductor. X-ray diffraction (XRD) studies reveal a nonstoichiometric LaH_9.6 or LaH_10±δ polyhydride responsible for the superconductivity, which in the literature is commonly treated as LaH₁₀ without accounting for stoichiometric defects. Here, we discover significant nuclear quantum effects (NQE) in this polyhydride, and demonstrate that a minor amount of stoichiometric defects will cause quantum proton diffusion in the otherwise rigid lanthanum lattice in the ground state. The diffusion coefficient reaches ~10⁻⁷ cm²/s in LaH_9.63 at 150 gigapascals and 240 kelvin, approaching the upper bound value of interstitial hydrides at comparable temperatures. A puzzling phenomenon observed in previous experiments, the positive pressure dependence of the superconducting critical temperature T_c below 150 gigapascals, is explained by a modulation of the electronic structure due to a premature distortion of the hydrogen lattice in this quantum fluxional structure upon decompression, and resulting changes of the electron-phonon coupling. This finding suggests the coexistence of the quantum proton fluxion and hydrogen-induced superconductivity in this lanthanum polyhydride, and leads to an understanding of the structural nature and superconductivity of nonstoichiomectric hydrogen-rich materials. The role of stoichiometric defects in the superconducting polyhydride LaH_10±δ has received little attention so far. Here, the authors use molecular-dynamics simulations to show that a small amount of stoichiometric defects will cause quantum proton diffusion in the otherwise rigid lanthanum lattice. [ABSTRACT FROM AUTHOR]