摘要： Heterostructures of dissimilar crystalline materials are key in the development of photoelectronic devices. Such structures rely on matching lattice constants for efficient transport. Nevertheless, an amorphous material, amorphous Se is becoming important in high-energy photoelectronics. Thus there is a need to understand the heterostructures it forms with conventional crystalline materials. Since the transport properties of such heterostructures will be limited by lattice mismatches, methods to improve transport are necessary. We investigated the effect of electrolysis on the electronic properties of Se based multilayer films deposited on n-type silicon (Se/n-Si) and showed that conduction and photoresponse can be changed by electrolysis processing. The Se surface of the Se/n-Si samples was used as an anode in the electrolysis of NaCl solution. Afterwards, the samples were measured using current–voltage and capacitance–voltage variations in dark conditions and under illumination. Electrolysis processed samples showed higher conduction current and photocurrent, compared to samples not used in electrolysis. This is due to the introduction of Cl into the Se, which affects carrier lifetimes: increasing hole lifetime and reducing electron lifetime. We therefore suggest that electrolysis can be applied to modify the electronic properties of Se/n-Si heterostructures.