Solution-processed black phosphorus nanoflakes for integrating nonvolatile resistive random access memory and the mechanism unveiled

In this study, we demonstrated the integration of black phosphorus (BP) nanoflakes in a resistive random access memory (RRAM) with a facile and complementary metal-oxide-semiconductor-compatible process. The solution-processed BP nanoflakes embedded in polystyrene (PS) as an active layer were sandwiched between aluminum electrodes (Al/BP:PS/Al). The device shows a figure of merit with typical bipolar behavior and forming-free characteristics as well as excellent memory performances such as nonvolatile, low operation voltage (1.75 V) and high ON/OFF ratio (>10²) as well as the long retention time (>1500 s). The improved device performances were attributed to the formation of effective trap sites from the hybrid structure of the active layer (BP:PS), especially the BP nanoflakes and the partly oxidized species (P _x O _y ). Moreover, the extrinsic aluminum oxide layer was observed after the device operation. The mechanism of switching behavior was further unveiled through the carrier transport models, which confirms the conductive mechanisms of space-charge-limited current and Ohmic conductance at high resistance state (HRS) and low resistance state, respectively. Additionally, in the high electric field at HRS, the transfer curve was well fitted with the Poole-Frenkel emission model, which could be attributed to the formation of the aluminum oxide layer. Accordingly, both the trapping/de-trapping of carriers and the formation/rupture of conductive filaments were introduced as transport mechanisms in our devices. Although the partial P _x O _y species on BP were inevitable during the liquid phase exfoliation process, which was regarded as the disadvantages for various applications, it turns to a key point for improving performances in memory devices. The proposed approach to integrating BP nanoflakes in the active layer of the RRAM device could pave the way for next-generation memory devices.