Electrolyte-Controlled Photoelectrochemical Photocurrent Switching Effect in High-Performance Self-Powered Broadband Photoelectrochemical-Type Photodetectors Based on MnPS Nanosheets.

Photoelectric devices are extensively applied in optical logic systems, light communication, optical imaging, and so on. However, traditional photoelectric devices can only generate unidirectional photocurrent, which hinders the simplification and multifunctionality of devices. Recently, it has become a new research focus to achieve controllable reversal of the output photocurrent direction (bipolar current) in a photoelectric system. Considering that the device with bipolar current adds a reverse current operating state compared to traditional devices, the former is more suitable for developing new multifunctional photoelectric devices. Due to the existence of electrolytes, photoelectrochemical (PEC) systems contain chemical processes such as ion diffusion and migration and electrochemical reactions, which are unable to occur in solid-state transistor devices, and the effect of electrolyte pH on the performance of PEC systems is usually ignored. We prepared a MnPS-based PEC-type photodetector and reversed photocurrents by adjusting the pH of electrolytes, i.e., the electrolyte-controlled photoelectrochemical photocurrent switching (PEPS) effect. We clarified the effect of pH values on the direction of photocurrent from the perspectives of electrolyte energy level rearrangement splitting and the kinetic theory of the semiconductor electrode. This work not only contributes to a deeper understanding of carrier transport in PEC processes but also inspires the development of advanced multifunctional photoelectric devices.