Enhanced Coulomb pseudopotentials in high-pressure hydrides from first principles

Abstract

In the Eliashberg theory of superconductivity, Coulomb interactions oppose the phonon-mediated attraction and suppress the superconducting critical temperature $T_{\mathrm{c}}$. However, most first-principles predictions continue to treat this repulsion with an empirical Coulomb pseudopotential $μ^*_{\text{ME}}$ in the range 0.1-0.15. Here we present first-principles calculations of the Coulomb parameter $μ$ and pseudopotential $μ^*_{\text{ME}}$ in superconducting hydrides across a range of pressures. The screened Coulomb interaction is evaluated at the random phase approximation level with the Mantel code. We demonstrate that several hydride systems, including H$_3$S, YSbH$_6$ and Mg$_2$IrH$_6$, have strong Coulomb repulsions driven by a large density of states at the Fermi energy, $N_{\mathrm{F}}$. For Mg$_2$IrH$_6$ we obtain $μ=0.62$ and $μ^*_{\text{ME}}\approx0.39$, leading to a 40 K suppression in $T_{\mathrm{c}}$ relative to a standard $μ^*_{\text{ME}}=0.16$. Our obtained $μ^*_{\text{ME}}$ is far above the conventional range and, accounting for the energy dependence of the density of states, resolves the factor-of-two discrepancy between $T_{\mathrm{c}}$ estimates of previous studies. Across all systems and pressures studied, we find that $μ$ closely tracks $N_{\mathrm{F}}$, suggesting that commonly used $μ^*_{\text{ME}}$ values lead to overestimated $T_{\mathrm{c}}$ in materials where the density of states at the Fermi energy is large.