High-Performance 2D Ambipolar MoTe2 Lateral Memristors by Mild Oxidation.

2D transition metal dichalcogenides (TMDCs) have been intensively explored in memristors for brain-inspired computing. Oxidation, which is usually unavoidable and harmful in 2D TMDCs, could also be used to enhance their memristive performances. However, it is still unclear how oxidation affects the resistive switching behaviors of 2D ambipolar TMDCs. In this work, a mild oxidation strategy is developed to greatly enhance the resistive switching ratio of ambipolar 2H-MoTe2 lateral memristors by more than 10 times. Such an enhancement results from the amplified doping due to O2 and H2O adsorption and the optimization of effective gate voltage distribution by mild oxidation. Moreover, the ambipolarity of 2H-MoTe2 also enables a change of resistive switching direction, which is uncommon in 2D memristors. Consequently, as an artificial synapse, the MoTe2 device exhibits a large dynamic range (≈200) and a good linearity (1.01) in long-term potentiation and depression, as well as a high-accuracy handwritten digit recognition (>96%). This work not only provides a feasible and effective way to enhance the memristive performance of 2D ambipolar materials, but also deepens the understanding of hidden mechanisms for RS behaviors in oxidized 2D materials.

Dual-Limit Growth of Large-Area Monolayer Transition Metal Dichalcogenides.

The large-scale growth of monolayer transition metal dichalcogenide (TMDC) films is a determinant for the implementation of two-dimensional materials in industrial applications. However, the simultaneous realization of uniform monolayer thickness and large-area coverage is still a challenge, because it requires precise control of reaction kinetics in both space and time dimensions. Herein, we achieve a variety of large-area monolayer TMDCs films by a dual-limit growth (DLG) that is realized through nanoporous carbon nanotube (CNT) films. In the DLG, a precursor-loaded CNT film placed face-to-face with a substrate provides a space-limited environment facilitating the monolayer growth, while the byproducts formed in the CNT film timely limits the supply of precursors released from nanopores of the CNT film, inhibiting the growth of multilayer TMDCs on the substrate. Consequently, large-area monolayer TMDC films are grown in a wide range of reaction times and show good homogeneity in thickness, optical properties, and device performance over the entire substrate. The DLG strategy is widely applicable for the growth of a variety of TMDC films including WSe2, MoS2, MoSe2, WS2, and ReS2. Our work provides a universal strategy to attain large-area monolayer TMDC films that can be used in practical applications of integrated circuits.

Water nanolayer facilitated solitary-wave-like blisters in MoS2 thin films.

Solitary waves are unique in nonlinear systems, but their formation and propagation in the nonlinear fluid-structure interactions have yet to be further explored. As a typical nonlinear system, the buckling of solid thin films is fundamentally related to the film-substrate interface that is further vulnerable to environments, especially when fluids exist. In this work, we report an anomalous, solitary-wave-like blister (SWLB) mode of MoS2 thin films in a humid environment. Unlike the most common telephone-cord and web buckling deformation, the SWLB propagates forward like solitary waves that usually appear in fluids and exhibits three-dimensional expansions of the profiles during propagation. In situ mechanical, optical, and topology measurements verify the existence of an interfacial water nanolayer, which facilitates a delamination of films at the front side of the SWLB and a readhesion at the tail side owing to the water nanolayer-induced fluid-structure interaction. Furthermore, the expansion morphologies and process of the SWLB are predicted by our theoretical model based on the energy change of buckle propagation. Our work not only demonstrates the emerging SWLB mode in a solid material but also sheds light on the significance of interfacial water nanolayers to structural deformation and functional applications of thin films.

Perforated Carbon Nanotube Film Assisted Growth of Uniform Monolayer MoS2.

Scaling up the chemical vapor deposition (CVD) of monolayer transition metal dichalcogenides (TMDCs) is in high demand for practical applications. However, for CVD-grown TMDCs on a large scale, there are many existing factors that result in their poor uniformity. In particular, gas flow, which usually leads to inhomogeneous distributions of precursor concentrations, has yet to be well controlled. In this work, the growth of uniform monolayer MoS2 on a large scale by the delicate control of gas flows of precursors, which is realized by vertically aligning a well-designed perforated carbon nanotube (p-CNT) film face-to-face with the substrate in a horizontal tube furnace, is achieved. The p-CNT film releases gaseous Mo precursor from the solid part and allows S vapor to pass through the hollow part, resulting in uniform distributions of both gas flow rate and precursor concentrations near the substrate. Simulation results further verify that the well-designed p-CNT film guarantees a steady gas flow and a uniform spatial distribution of precursors. Consequently, the as-grown monolayer MoS2 shows quite good uniformity in geometry, density, structure, and electrical properties. This work provides a universal pathway for the synthesis of large-scale uniform monolayer TMDCs, and will advance their applications in high-performance electronic devices.

Liquid Precursor-Guided Phase Engineering of Single-Crystal VO2 Beams.

The study of VO2 flourishes due to its rich competing phases induced by slight stoichiometry variations. However, the vague mechanism of stoichiometry manipulation makes the precise phase engineering of VO2 still challenging. Here, stoichiometry manipulation of single-crystal VO2 beams in liquid-assisted growth is systematically studied. Contrary to previous experience, oxygen-rich VO2 phases are abnormally synthesized under a reduced oxygen concentration, revealing the important function of liquid V2 O5 precursor: It submerges VO2 crystals and stabilizes their stoichiometric phase (M1) by isolating them from the reactive atmosphere, while the uncovered crystals are oxidized by the growth atmosphere. By varying the thickness of liquid V2 O5 precursor and thus the exposure time of VO2 to the atmosphere, various VO2 phases (M1, T, and M2) can be selectively stabilized. Furthermore, this liquid precursor-guided growth can be used to spatially manages multiphase structures in single VO2 beams, enriching their deformation modes for actuation applications.

All-Transfer Electrode Interface Engineering Toward Harsh-Environment-Resistant MoS2 Field-Effect Transistors.

Nanoscale electronic devices that can work in harsh environments are in high demand for wearable, automotive, and aerospace electronics. Clean and defect-free interfaces are of vital importance for building nanoscale harsh-environment-resistant devices. However, current nanoscale devices are subject to failure in these environments, especially at defective electrode-channel interfaces. Here, harsh-environment-resistant MoS2 transistors are developed by engineering electrode-channel interfaces with an all-transfer of van der Waals electrodes. The delivered defect-free, graphene-buffered electrodes keep the electrode-channel interfaces intact and robust. As a result, the as-fabricated MoS2 devices have reduced Schottky barrier heights, leading to a very large on-state current and high carrier mobility. More importantly, the defect-free, hydrophobic graphene buffer layer prevents metal diffusion from the electrodes to MoS2 and the intercalation of water molecules at the electrode-MoS2 interfaces. This enables high resistances of MoS2 devices with all-transfer electrodes to various harsh environments, including humid, oxidizing, and high-temperature environments, surpassing the devices with other kinds of electrodes. The work deepens the understanding of the roles of electrode-channel interfaces in nanoscale devices and provides a promising interface engineering strategy to build nanoscale harsh-environment-resistant devices.

Humidity-Controlled Dynamic Engineering of Buckling Dimensionality in MoS2 Thin Films.

Dynamic engineering of buckling deformation is of vital importance as it provides multiphase modulation of thin film devices. In particular, dynamic switch of buckles between one-dimensional (1D) and two-dimensional (2D) configurations in a single film system on rigid substrates is intriguing but very challenging. The current approach to changing buckling configuration is mainly achieved by varying the built-in stress at the film-substrate interface, but it is difficult to realize dynamic engineering on rigid substrates. Herein, we report a dynamic engineering of buckling deformation in MoS2 thin films by humidity-tuned interfacial adhesion. With the change of humidity, the MoS2 thin films deform from 1D telephone-cord buckles to 2D web-like buckles due to the hydrophilic nature of both MoS2 and substrate. Such 1D-to-2D evolution of buckles is attributed to the weakened interfacial adhesion of mixed deformation modes induced by humidity, which is verified by finite-element modeling. These buckled films further find potential applications as patterned templates for liquid condensation and sensing units for tactile sensors. Our work not only demonstrates the humidity-controlled dimensionality engineering of buckles in MoS2 thin films but also sheds light on the functional applications of buckled films based on their profile features.

Monolayer MoS2 Synaptic Transistors for High-Temperature Neuromorphic Applications.

As essential units in an artificial neural network (ANN), artificial synapses have to adapt to various environments. In particular, the development of synaptic transistors that can work above 125 °C is desirable. However, it is challenging due to the failure of materials or mechanisms at high temperatures. Here, we report a synaptic transistor working at hundreds of degrees Celsius. It employs monolayer MoS2 as the channel and Na+-diffused SiO2 as the ionic gate medium. A large on/off ratio of 106 can be achieved at 350 °C, 5 orders of magnitude higher than that of a normal MoS2 transistor in the same range of gate voltage. The short-term plasticity has a synaptic transistor function as an excellent low-pass dynamic filter. Long-term potentiation/depression and spike-timing-dependent plasticity are demonstrated at 150 °C. An ANN can be simulated, with the recognition accuracy reaching 90%. Our work provides promising strategies for high-temperature neuromorphic applications.

Ultrafast, Kinetically Limited, Ambient Synthesis of Vanadium Dioxides through Laser Direct Writing on Ultrathin Chalcogenide Matrix.

Vanadium dioxide (VO2) is a strongly correlated electronic material and has attracted significant attention due to its metal-to-insulator transition and diverse smart applications. Traditional synthesis of VO2 usually requires minutes or hours of global heating and low oxygen partial pressure to achieve thermodynamic control of the valence state. Further patterning of VO2 through a series of lithography and etching processes may inevitably change its surface valence, which poses a great challenge for the assembly of micro- and nanoscale VO2-based heterojunction devices. Herein, we report an ultrafast method to simultaneously synthesize and pattern VO2 on the time scale of seconds under ambient conditions through laser direct writing on a V5S8 "canvas". The successful ambient synthesis of VO2 is attributed to the ultrafast local heating and cooling process, resulting in controlled freezing of the intermediate oxidation phase during the relatively long kinetic reaction. A Mott memristor based on a V5S8-VO2-V5S8 lateral heterostructure can be fabricated and integrated with a MoS2 channel, delivering a transistor with abrupt switching transfer characteristics. The other device with a VSxOy channel exhibits a large negative temperature coefficient of approximately 4.5%/K, which is highly desirable for microbolometers. The proposed approach enables fast and efficient integration of VO2-based heterojunction devices and is applicable to other intriguing intermediate phases of oxides.