Strong correlation between ionic bonding strength and superconductivity in compressed hydrides

Abstract

Understanding the superconductivity in relation to chemical bonding is essential for the development of superconductors. We propose that pressure-reduced ionic bonding strength is beneficial for improving superconductivity in hydrides (negative correlation between bonding strength and critical temperature). We model ionic hydrides using a prototypical ionic lattice (CsCl-type) with simple-valence metal Li/Rb and hydrogen and control the bonding strength via external pressure. First-principles calculations reveal that the ionic bonding strength in LiH increases with pressure while its critical temperature ($T_{\mathrm{c}}$) simultaneously decreases. A higher $T_{\mathrm{c}}$ at lower pressures is attributed to stronger electron-phonon coupling (EPC) induced by weaker ionic bonds and significant EPC contributions from mid-frequency phonons. RbH's pressure dependences of bonding strength and $T_{\mathrm{c}}$ are the reverse of those of LiH, and the EPC primarily results from high-frequency phonons. The distinct interorbital electron transition mechanism and amounts of charge transfer are responsible for the opposite trend of changes in bonding strength and superconductivity in LiH and RbH. The proposed correlation is further validated by the other six ionic hydrides. Substantial $T_{\mathrm{c}}$ change (e.g., 126.2 K at 100 GPa and 5.7 K at 300 GPa in LiH) in response to bonding strength variation reveals a key factor for designing new superconductors.