Pressure‐Induced Enhancement and Retainability of Optoelectronic Properties in Layered Zirconium Disulfide

Abstract Transition metal dichalcogenides (TMDs) exhibit excellent electronic and photoelectric properties under pressure, prompting researchers to investigate their structural phase transitions, electrical transport, and photoelectric response upon compression. Herein, the structural and photoelectric properties of layered ZrS 2 under pressure using in situ high‐pressure photocurrent, Raman scattering spectroscopy, alternating current impedance spectroscopy, absorption spectroscopy, and theoretical calculations are studied. The experimental results show that the photocurrent of ZrS 2 continuously increases with increasing pressure. At 24.6 GPa, the photocurrent of high‐pressure phase P2 1 /m is three orders of magnitude greater than that of the initial phase at ambient pressure. The minimum synthesis pressure for pure high‐pressure phase P2 1 /m of ZrS 2 is 18.8 GPa, which exhibits a photocurrent that is two orders of magnitude higher than that of the initial phase and displays excellent stability. Additionally, it is discovered that the crystal structure, electrical transport properties and bandgap of layered ZrS 2 can also be regulated by pressure. This work offers researchers a new direction for synthesizing high‐performance TMDs photoelectric materials using high pressure, which is crucial for enhancing the performance of photoelectric devices in the future.