Pressure‐Regulated Photovoltaic Response in Antimony Triiodide With Asymmetric Metal Contact

The effective modification of photovoltaic activities in photoelectric devices is significant for enhancing energy conversion efficiency. Here, the pressure‐tunable photovoltaic properties in the SbI 3 device with Au/Pt asymmetric electrodes are demonstrated. At initial pressure, the SbI 3 device exhibits an anticipated self‐driven photoresponse characteristic at zero external bias, and a significant enhancement in photocurrent response is observed with increasing bias to −0.2 V, nearly two orders of magnitude higher than the initial value. With increasing pressure, the SbI 3 device exhibits tunable photocurrent response, reaching a maximum value at ≈1.2 GPa, while the photovoltage response decreases monotonously during compression, which is closely associated with the dynamic evolution of the work function and bandgap of SbI 3 upon successive compression. These findings signify that SbI 3 is a promising candidate for future photoelectric devices, which opens a new window of opportunity for further exploration, regulation, and understanding of high‐performance photovoltaic devices under extreme conditions.