Enhancing superconducting transition temperature of lanthanum superhydride by increasing hydrogen vacancy concentration

Abstract: Various clathrate superhydride superconductors have been found to possess hydrogen deficiency in experimental samples, while their impacts on superconductivity are often neglected. In this study, we investigate the superconductivity of lanthanum superhydride with hydrogen deficiency (LaH$_{10-\delta}$) from first principles using path-integral approaches. Under the effects of thermal and quantum fluctuations, hydrogen vacancies are found to diffuse within the system, leading to modifications in ion vibrations, electronic structure and electron-phonon coupling. These changes result in a non-monotonic dependence of superconducting transition temperature ($T_c$) on the vacancy concentration ($\delta$). By comparing the experimental and theoretical equations of state, we suggest that $\delta$ varies across samples under different pressures. This explains the positive pressure dependence of $T_c$ in experiments below 150 GPa. Remarkably, within this pressure range, we find that $T_c$ could be further raised by increasing $\delta$.