Superconductivity in Honeycomb Antiferromagnet CrPSe3 via Irreversible Pressure-Mediated Interlayer Sliding

Interlayer engineering offers a compelling strategy for tailoring emergent quantum states in van der Waals materials. The latest discoveries of nickel-based superconducting materials have once again ignited extensive interest in exploring transition-metal-based high-temperature superconductors. Two-dimensional metal-centered geometry, subtle valence regulation, and interactions dominated by interlayer stacking are key to achieving the superconducting state. Here, we present that pressure-mediated interlayer sliding in the antiferromagnetic honeycomb lattice CrPSe3 triggers a cascade of electronic transitions, including an insulator-to-metal crossover, the emergence of a density-wave-like order, and possible superconductivity. The resulting phase diagram reveals a maximum transition temperature of 5.8 K concomitant with complete suppression of the density-wave-like order at 30.1 GPa. Comprehensive structural analyses uncover successive interlayer sliding accompanied by aberrant compressibility and pronounced volume collapse. Atomic-resolution imaging corroborates the irreversible sliding process, leading to a distinct metastable electronic state upon decompression. These insights underscore interlayer sliding as a powerful tool for manipulating quantum states in van der Waals materials.