Pressure‐Induced Re‐Entrant Superconductivity in Transition Metal Dichalcogenide TiSe2

Abstract Transition metal dichalcogenide TiSe 2 exhibits a superconducting dome within a low pressure range of 2–4 GPa, which peaks with the maximal transition temperature T c of ≈1.8 K. Here it is reported that applying high pressure induces a new superconducting state in TiSe 2 , which starts at ≈16 GPa with a substantially higher T c that reaches 5.6 K at ≈21.5 GPa with no sign of decline. Combining high‐throughput first‐principles structure search, X‐ray diffraction, and Raman spectroscopy measurements up to 30 GPa, It is found that TiSe 2 undergoes a first‐order structural transition from the 1 T phase under ambient pressure to a new 4 O phase under high pressure. Comparative ab initio calculations reveal that while the conventional phonon‐mediated pairing mechanism may account for the superconductivity observed in 1 T ‐TiSe 2 under low pressure, the electron‐phonon coupling of 4 O ‐TiSe 2 is too weak to induce a superconducting state whose transition temperature is as high as 5.6 K under high pressure. The new superconducting state found in pressurized TiSe 2 requires further study on its underlying mechanism.