Novel $J_{\mathrm{eff}}$=3/2 Metallic Phase and Unconventional Superconductivity in GaTa${}_4$Se${}_8$

Abstract

By means of density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations and resonant inelastic x-ray scattering (RIXS) experiments, we investigate the high-pressure phases of the spin-orbit-coupled $J_{\mathrm{eff}}=3/2$ insulator GaTa${}_4$Se${}_8$. Its metallic phase, derived from the Mott state by applying pressure, is found to carry $J_{\mathrm{eff}}=3/2$ moments. The characteristic excitation peak in the RIXS spectrum maintains its destructive quantum interference of $J_{\mathrm{eff}}$ at the Ta $L_2$-edge up to 10.4 GPa. Our exact diagonalization based DFT+DMFT calculations including spin-orbit coupling also reveal that the $J_{\mathrm{eff}}=3/2$ character can be clearly identified under high pressure. These results establish the intriguing nature of the correlated metallic magnetic phase, which represents the first confirmed example of $J_{\mathrm{eff}}$=3/2 moments residing in a metal. They also indicate that the pressure-induced superconductivity is likely unconventional and influenced by these $J_{\mathrm{eff}}=3/2$ moments. Based on a self-energy analysis, we furthermore propose the possibility of doping-induced superconductivity related to a spin-freezing crossover.

7 pages, 5 figures (additional 4 pages and 6 figures for supplemental materials)