3D monolithic integration of logic and memory has been the most sought after solution to surpass the Von Neumann bottleneck, for which a low-temperature processed material system becomes inevitable. Two-dimensional materials, with their excellent electrical properties and low thermal budget are potential candidates. Here, we demonstrate a low-temperature hybrid co-integration of one-transistor-one-resistor memory cell, comprising a surface functionalized 2D WSe2 p-FET, with a solution-processed WSe2 Resistive Random Access Memory. The employed plasma oxidation technique results in a low Schottky barrier height of 25 meV with a mobility of 230 cm2 V−1 s−1, leading to a 100x performance enhanced WSe2 p-FET, while the defective WSe2 Resistive Random Access Memory exhibits a switching energy of 2.6 pJ per bit. Furthermore, guided by our device-circuit modelling, we propose vertically stacked channel FETs for high-density sub-0.01 μm2 memory cells, offering a new beyond-Si solution to enable 3-D embedded memories for future computing systems.

Realization of high-density and reliable resistive random access memories based on two-dimensional semiconductors is crucial toward their development in next-generation information storage and neuromorphic computing. Here, wafer-scale integration of solution-processed two-dimensional MoS2 memristor arrays are reported. The MoS2 memristors achieve excellent endurance, long memory retention, low device variations, and high analog on/off ratio with linear conductance update characteristics. The two-dimensional nanosheets appear to enable a unique way to modulate switching characteristics through the inter-flake sulfur vacancies diffusion, which can be controlled by the flake size distribution. Furthermore, the MNIST handwritten digits recognition shows that the MoS2 memristors can operate with a high accuracy of >98.02%, which demonstrates its feasibility for future analog memory applications. Finally, a monolithic three-dimensional memory cube has been demonstrated by stacking the two-dimensional MoS2 layers, paving the way for the implementation of two memristor into high-density neuromorphic computing system.

We clarify that the chemisorption of oxygen atoms at the edges is a key contributor to the frequently observed edge enhancement and spatial non-uniformities of photoluminescence (PL) in WS2 monolayers. Here we have investigated with momentum- and real-space nanoimaging of the chemical and electronic density inhomogeneity of WS2 flakes. Our finding from a large panoply of techniques together with density functional theory calculation confirms that the oxygen chemisorption leads to the electron accumulation at the edges. This facilitates the trion dominance of PL at the edges of WS2 flakes. Our results highlight and unravel the significance of chemisorbed oxygen at the edges in the PL emission and electronic structure of WS2, providing a viable path to enhance the performance of transition-metal-dichalcogenide-based devices.

Defects are commonly found in two-dimensional (2D) transition-metal dichalcogenide (TMD) materials. Such defects usually dictate the optical and electrical properties of TMDs. It is thus important to develop techniques to characterize the defects directly with good spatial resolution, specificity, and throughput. Herein, we demonstrate that Kelvin probe force microscopy (KPFM) is a versatile technique for this task. It is able to unveil defect heterogeneity of 2D materials with a spatial resolution of 10 nm and energy sensitivity better than 10 meV. KPFM mappings of monolayer WS2 exhibit interesting work function variances that are associated with defects distribution. This finding is verified by aberration-corrected scanning transmission electron microscopy and density functional theory calculations. In particular, a strong correlation among the work function, electrical and optical responses to the defects is revealed. Our findings demonstrate the potential of KPFM as an effective tool for exploring the intrinsic defects in TMDs.

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