Quadrupolar phase transition in superconducting lanthanum hydride

Abstract

Lanthanum hydride (LaH$_{10}$) has been widely studied for its high superconducting critical temperature of 250 K at about 170 GPa pressure. Although the structural ${R\bar{3}m}$-to-${Fm\bar{3}m}$ transition under pressure connected to the emergence of the superconducting phase in this material is broadly understood, the detailed characterization of its nature and its order parameter are still missing. By applying the cluster multipole moment analysis to the hydrogen sublattice, we reveal that this transition is triggered by a quadrupolar $T_{2g}$ order parameter, and we provide evidence for its weak first-order nature. By performing path integral molecular dynamics coupled to a message-passing atomic cluster expansion (MACE) neural network potential, trained on Perdew-Burke-Ernzerhof (PBE) density functional theory configurations, we show that the collapse of the order parameter at the transition is simultaneously associated with the discontinuous softening of the optical $T_{2g}$ phonons. Their symmetry lets them carry a non-negligible electron-phonon coupling in LaH$_{10}$, while the weak first-order nature of the transition makes them soft. The presence of structural instabilities with low-frequency quadrupolar distortions can be a key ingredient to enhance superconductivity in superhydrides and provides guidance for the discovery of new high-$T_c$ superconductors in hydrogen-rich compounds.