Li-F polarity-driven stabilization of −VII oxidation state of gold at high pressure

The exploration of unconventional oxidation states is pivotal for expanding fundamental bonding paradigms and accessing exotic matter. Achieving highly negative oxidation states in transition metals remains a significant challenge. Here, we propose a dual-driven strategy combining a strong reductant (Li) and oxidant (F) under high pressure, stabilizing the oxidation state -VII of gold (Au) in a ternary electride Li₁₀AuF. This insulating phase hosts paired interstitial anionic electrons and features an Au center nominally isoelectronic with the noble gas radon, governed by F-enhanced charge polarization, pressure-induced orbital reshuffling, and p-d hybridization that lowers the energy of Au 6p orbitals. Replacing F with I or P progressively reduces Au charge and interstitial electron localization, transforming semiconducting Li₁₀AuF into semimetallic Li₁₀AuI and ultimately superconducting Li₁₀AuP. These results demonstrate how chemically polarized element combinations under compression can unlock unexpected oxidation states and charge distributions, guiding the design of quantum materials with emergent functionalities.