Emergent superconductivity in an iron-based honeycomb lattice initiated by pressure-driven spin-crossover

The discovery of iron-based superconductors (FeSCs), with the highest transition temperature (T_c) up to 55 K, has attracted worldwide research efforts over the past ten years. So far, all these FeSCs structurally adopt FeSe-type layers with a square iron lattice and superconductivity can be generated by either chemical doping or external pressure. Herein, we report the observation of superconductivity in an iron-based honeycomb lattice via pressure-driven spin-crossover. Under compression, the layered FePX₃ (X = S, Se) simultaneously undergo large in-plane lattice collapses, abrupt spin-crossovers, and insulator-metal transitions. Superconductivity emerges in FePSe₃ along with the structural transition and vanishing of magnetic moment with a starting T_c ~ 2.5 K at 9.0 GPa and the maximum T_c ~ 5.5 K around 30 GPa. The discovery of superconductivity in iron-based honeycomb lattice provides a demonstration for the pursuit of transition-metal-based superconductors via pressure-driven spin-crossover.