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Single layered molybdenum disulfide with a direct bandgap is a promising twodimensional material that goes beyond graphene for next generation nanoelectronics. Here, we report the controlled vapor phase synthesis of molybdenum disulfide atomic layers and elucidate a fundamental mechanism for the nucleation, growth, and grain boundary formation in its crystalline monolayers. Atomic layered graphene has shown many fascinating properties as a supplement to silicon-based semiconductor technologies [1][2][3][4] . Consequently, great effort has been devoted to the development and understanding of its synthetic processes [5][6][7][8] . However, graphene with its high leaking current, due to its zero bandgap energy, is not suitable for many applications in electronics and optics 9, 10 . Recent developments in two different classes of materials -transition metal oxides and sulfides -have shown many promises to fill the existing gaps [10][11][12] . For example, the successful demonstration of molybdenum disulfide (MoS 2 )-based field-effect transistors (FET) 11 , has prompted an intense exploration of the physical properties of few-layered MoS 2 films [13][14][15][16][17] .MoS 2 is a layered semiconductor with a bandgap in the range of 1.2-1.8 eV, whose physical properties are significantly thickness-dependent 13,14 . For instance, a considerable enhancement in the photoluminescence of MoS 2 has been observed as the thickness of the material decreases 14 . The lack of inversion symmetry in single-layer Initially, small triangular domains were nucleated at random locations on the bare substrate (Fig. 1a). Then, the nucleation sites continued to grow and formed boundaries when two or more domains met (Figs. 1b and 1c), resulting in a partially continuous film.This process can eventually extend into large-area single-layered MoS 2 continuous films if sufficient precursor supply and denser nucleation sites are provided (Fig. 1d) In the quest for feasible strategies to control the nucleation process, we take advantage of some of our common experimental observations. Our experiments show that the MoS 2 triangular domains and films are commonly nucleated and formed in the vicinity of the substrates' edges, scratches, dust particles, or rough surfaces (supplementary Fig. S4).We utilized this phenomenon to control the nucleation by strategically creating step edges on substrates using conventional lithography processes (Fig. 1e). The patterned substrates with uniform distribution of rectangular SiO 2 pillars (40×40 μm 2 in size, 40 μm apart, and ~40 nm thick) were directly used in the CVD process for MoS 2 growth ( The inherent dependence of this approach on the edge-based nucleation resembles some of the observations and theoretical predictions in the growth other layered materials [29][30] .Theoretical studies have revealed a significant reduction in the energy barrier of graphene nucleation close to the step edges, as compared to flat surfaces of transition metal substrates 30 . We propose that similar edge-based catalytic pr...

Graphene and hexagonal boron nitride (h-BN) have similar crystal structures with a lattice constant difference of only 2%. However, graphene is a zero-bandgap semiconductor with remarkably high carrier mobility at room temperature, whereas an atomically thin layer of h-BN is a dielectric with a wide bandgap of ∼5.9 eV. Accordingly, if precise two-dimensional domains of graphene and h-BN can be seamlessly stitched together, hybrid atomic layers with interesting electronic applications could be created. Here, we show that planar graphene/h-BN heterostructures can be formed by growing graphene in lithographically patterned h-BN atomic layers. Our approach can create periodic arrangements of domains with size ranging from tens of nanometres to millimetres. The resulting graphene/h-BN atomic layers can be peeled off the growth substrate and transferred to various platforms including flexible substrates. We also show that the technique can be used to fabricate two-dimensional devices, such as a split closed-loop resonator that works as a bandpass filter.

Recently, two-dimensional layers of transition metal dichalcogenides, such as MoS2, WS2, MoSe2, and WSe2, have attracted much attention for their potential applications in electronic and optoelectronic devices. The selenide analogues of MoS2 and WS2 have smaller band gaps and higher electron mobilities, making them more appropriate for practical devices. However, reports on scalable growth of high quality transition metal diselenide layers and studies of their properties have been limited. Here, we demonstrate the chemical vapor deposition (CVD) growth of uniform MoSe2 monolayers under ambient pressure, resulting in large single crystalline islands. The photoluminescence intensity and peak position indicates a direct band gap of 1.5 eV for the MoSe2 monolayers. A back-gated field effect transistor based on MoSe2 monolayer shows n-type channel behavior with average mobility of 50 cm(2) V(-1) s(-1), a value much higher than the 4-20 cm(2) V(-1) s(-1) reported for vapor phase grown MoS2.

Ternary two-dimensional dichalcogenide alloys exhibit compositionally modulated electronic structure, and hence, control of dopant concentration within each individual layer of these compounds provides a powerful tool to efficiently modify their physical and chemical properties. The main challenge arises when quantifying and locating the dopant atoms within each layer in order to better understand and fine-tune the desired properties. Here we report the synthesis of molybdenum disulfide substitutionally doped with a broad range of selenium concentrations, resulting in over 10% optical band gap modulations in atomic layers. Chemical analysis using Z-contrast imaging provides direct maps of the dopant atom distribution in individual MoS2 layers and hence a measure of the local optical band gaps. Furthermore, in a bilayer structure, the dopant distribution is imaged layer-by-layer. This work demonstrates that each layer in the bilayer system contains similar local Se concentrations, randomly distributed, providing new insights into the growth mechanism and alloying behavior in two-dimensional dichalcogenide atomic layers. The results show that growth of uniform, ternary, two-dimensional dichalcogenide alloy films with tunable electronic properties is feasible.

We report the direct growth of large, atomically thin GaSe single crystals on insulating substrates by vapor phase mass transport. A correlation is identified between the number of layers and a Raman shift and intensity change. We found obvious contrast of the resistance of the material in the dark and when illuminated with visible light. In the photoconductivity measurement we observed a low dark current. The on-off ratio measured with a 405 nm at 0.5 mW/mm(2) light source is in the order of 10(3); the photoresponsivity is 17 mA/W, and the quantum efficiency is 5.2%, suggesting possibility for photodetector and sensor applications. The photocurrent spectrum of few-layer GaSe shows an intense blue shift of the excitation edge and expanded band gap compared with bulk material.

Micrometer-sized electrochemical capacitors have recently attracted attention due to their possible applications in micro-electronic devices. Here, a new approach to large-scale fabrication of high-capacitance, two-dimensional MoS2 film-based micro-supercapacitors is demonstrated via simple and low-cost spray painting of MoS2 nanosheets on Si/SiO2 chip and subsequent laser patterning. The obtained micro-supercapacitors are well defined by ten interdigitated electrodes (five electrodes per polarity) with 4.5 mm length, 820 μm wide for each electrode, 200 μm spacing between two electrodes and the thickness of electrode is ∼0.45 μm. The optimum MoS2 -based micro-supercapacitor exhibits excellent electrochemical performance for energy storage with aqueous electrolytes, with a high area capacitance of 8 mF cm(-2) (volumetric capacitance of 178 F cm(-3) ) and excellent cyclic performance, superior to reported graphene-based micro-supercapacitors. This strategy could provide a good opportunity to develop various micro-/nanosized energy storage devices to satisfy the requirements of portable, flexible, and transparent micro-electronic devices.

Biological synapses store and process information simultaneously by tuning the connection between two neighboring neurons. Such functionality inspires the task of hardware implementation of neuromorphic computing systems. Ionic/electronic hybrid three-terminal memristive devices, in which the channel conductance can be modulated according to the history of applied voltage and current, provide a more promising way of emulating synapses by a substantial reduction in complexity and energy consumption. 2D van der Waals materials with single or few layers of crystal unit cells have been a widespread innovation in three-terminal electronic devices. However, less attention has been paid to 2D transition-metal oxides, which have good stability and technique compatibility. Here, nanoscale three-terminal memristive transistors based on quasi-2D α-phase molybdenum oxide (α-MoO ) to emulate biological synapses are presented. The essential synaptic behaviors, such as excitatory postsynaptic current, depression and potentiation of synaptic weight, and paired-pulse facilitation, as well as the transition of short-term plasticity to long-term potentiation, are demonstrated in the three-terminal devices. These results provide an insight into the potential application of 2D transition-metal oxides for synaptic devices with high scaling ability, low energy consumption, and high processing efficiency.