Interfacial Engineering of MoS2 Thin Films for Wettability-Dependent Resistive Switching and Neuromorphic Behaviors

Recent years have witnessed a surge in the research of memristors as fundamental building blocks for neuromorphic computing, owing to their exceptional ability to emulate the plastic behavior of biological synapses in a high-density, low-power hardware format. These devices are increasingly recognized as the key to achieving efficient artificial neural networks. Two-dimensional (2D) molybdenum disulfide (MoS2) is a premier candidate for artificial synapses due to its atomic scale and tunable electronic properties. However, achieving wafer-scale MoS2 thin films for integrated memristor systems remains a significant challenge. In this work, a scalable strategy combining cetyltrimethylammonium bromide (CTAB)-assisted electrochemical intercalation and oil–water interface self-assembly was developed to fabricate large-area 2H-phase MoS2 thin films. Leveraging the amphiphilic nature of CTAB-functionalized MoS2 nanosheets, continuous Janus-structured MoS2 films with asymmetric wetting properties (hydrophilic vs. hydrophobic) were successfully prepared. Vertical-structured Ag/Janus-structured MoS2/ITO memristors demonstrated robust non-volatile switching with high endurance and long-term retention. The devices successfully emulated biological synaptic behaviors, including short-term and long-term plasticity. Furthermore, the memristors exhibited distinct optoelectronic synergistic modulation under 405 nm illumination, enabling light-sensitive synaptic functions. This work offers a versatile interface engineering route for low-power integrated sensing–memory–computing hardware.