Vertical MoS2 Double-Layer Memristor with Electrochemical Metallization as an Atomic-Scale Synapse with Switching Thresholds Approaching 100 mV

Atomically thin two-dimensional (2D) materials—such as transition metal dichalcogenide (TMD) monolayers and hexagonal boron nitride (hBN)—and their van der Waals layered preparations have been actively researched to build electronic devices such as field-effect transistors, junction diodes, tunneling devices, and, more recently, memristors. Two-dimensional material memristors built in lateral form, with horizontal placement of electrodes and the 2D material layers, have provided an intriguing window into the motions of ions along the atomically thin layers. On the other hand, 2D material memristors built in vertical form with top and bottom electrodes sandwiching 2D material layers may provide opportunities to explore the extreme of the memristive performance with the atomic-scale interelectrode distance. In particular, they may help push the switching voltages to a lower limit, which is an important pursuit in memristor research in general, given their roles in neuromorphic computing. In fact, recently Akinwande et al. performed a pioneering work to demonstrate a vertical memristor that sandwiches a single MoS2 monolayer between two inert Au electrodes, but it could neither attain switching voltages below 1 V nor control the switching polarity, obtaining both unipolar and bipolar switching devices. Here, we report a vertical memristor that sandwiches two MoS2 monolayers between an active Cu top electrode and an inert Au bottom electrode. Cu ions diffuse through the MoS2 double layers to form atomic-scale filaments. The atomic-scale thickness, combined with the electrochemical metallization, lowers switching voltages down to 0.1–0.2 V, on par with the state of the art. Furthermore, our memristor achieves consistent bipolar and analogue switching, and thus exhibits the synapse-like learning behavior such as the spike-timing dependent plasticity (STDP), the very first STDP demonstration among all 2D-material-based vertical memristors. The demonstrated STDP with low switching voltages is promising not only for low-power neuromorphic computing, but also from the point of view that the voltage range approaches the biological action potentials, opening up a possibility for direct interfacing with mammalian neuronal networks.