Protonation induced high-Tc phases in iron-based superconductors evidenced by NMR and magnetization measurements

Chemical substitution during growth is a well-established method to manipulate electronic states of quantum materials, and leads to rich spectra of phase diagrams in cuprate and iron-based superconductors. Here we report a novel and generic strategy to achieve nonvolatile electron doping in series of (i.e. 11 and 122 structures) Fe-based superconductors by ionic liquid gating induced protonation at room temperature. Accumulation of protons in bulk compounds induces superconductivity in the parent compounds, and enhances the Tc largely in some superconducting ones. Furthermore, the existence of proton in the lattice enables the first proton nuclear magnetic resonance (NMR) study to probe directly superconductivity. Using FeS as a model system, our NMR study reveals an emergent high-Tc phase with no coherence peak which is hard to measure by NMR with other isotopes. This novel electric-field-induced proton evolution opens up an avenue for manipulation of competing electronic states (e.g. Mott insulators), and may provide an innovative way for a broad perspective of NMR measurements with greatly enhanced detecting resolution.