We report ambipolar charge transport in α-molybdenum ditelluride (MoTe2 ) flakes, whereby the temperature dependence of the electrical characteristics was systematically analyzed. The ambipolarity of the charge transport originated from the formation of Schottky barriers at the metal/MoTe2 contacts. The Schottky barrier heights as well as the current on/off ratio could be modified by modulating the electrostatic fields of the back-gate voltage (Vbg) and drain-source voltage (Vds). Using these ambipolar MoTe2 transistors we fabricated complementary inverters and amplifiers, demonstrating their feasibility for future digital and analog circuit applications.

The controlled synthesis of large-area, atomically thin molybdenum ditelluride (MoTe2) crystals is crucial for its various applications based on the attractive properties of this emerging material. In this work, we developed a chemical vapor deposition synthesis to produce large-area, uniform, and highly crystalline few-layer 2H and 1T' MoTe2 films. It was found that these two different phases of MoTe2 can be grown depending on the choice of Mo precursor. Because of the highly crystalline structure, the as-grown few-layer 2H MoTe2 films display electronic properties that are comparable to those of mechanically exfoliated MoTe2 flakes. Our growth method paves the way for the large-scale application of MoTe2 in high-performance nanoelectronics and optoelectronics.

Two-dimensional layered crystals could show phonon properties that are markedly distinct from those of their bulk counterparts, because of the loss of periodicities along the c-axis directions. Here we investigate the phonon properties of bulk and atomically thin α-MoTe2 using Raman spectroscopy. The Raman spectrum of α-MoTe2 shows a prominent peak of the in-plane E(1)2g mode, with its frequency upshifting with decreasing thickness down to the atomic scale, similar to other dichalcogenides. Furthermore, we find large enhancement of the Raman scattering from the out-of-plane B(1)2g mode in the atomically thin layers. The B(1)2g mode is Raman inactive in the bulk, but is observed to become active in the few-layer films. The intensity ratio of the B(1)2g to E(1)2g peaks evolves significantly with decreasing thickness, in contrast with other dichalcogenides. Our observations point to strong effects of dimensionality on the phonon properties of MoTe2.

Growth of a uniform oxide film with a tunable thickness on two-dimensional transition metal dichalcogenides is of great importance for electronic and optoelectronic applications. Here we demonstrate homogeneous surface oxidation of atomically thin WSe2 with a self-limiting thickness from single- to trilayers. Exposure to ozone (O3) below 100 °C leads to the lateral growth of tungsten oxide selectively along selenium zigzag-edge orientations on WSe2. With further O3 exposure, the oxide regions coalesce and oxidation terminates leaving a uniform thickness oxide film on top of unoxidized WSe2. At higher temperatures, oxidation evolves in the layer-by-layer regime up to trilayers. The oxide films formed on WSe2 are nearly atomically flat. Using photoluminescence and Raman spectroscopy, we find that the underlying single-layer WSe2 is decoupled from the top oxide but hole-doped. Our findings offer a new strategy for creating atomically thin heterostructures of semiconductors and insulating oxides with potential for applications in electronic devices.

Transition metal oxides show much promise as effective p-type contacts and dopants in electronics based on transition metal dichalcogenides. Here we report that atomically thin films of under-stoichiometric tungsten oxides (WOx with x < 3) grown on tungsten diselenide (WSe2) can be used as both controlled charge transfer dopants and low-barrier contacts for p-type WSe2 transistors. Exposure of atomically thin WSe2 transistors to ozone (O3) at 100 °C results in self-limiting oxidation of the WSe2 surfaces to conducting WOx films. WOx-covered WSe2 is highly hole-doped due to surface electron transfer from the underlying WSe2 to the high electron affinity WOx. The dopant concentration can be reduced by suppressing the electron affinity of WOx by air exposure, but exposure to O3 at room temperature leads to the recovery of the electron affinity. Hence, surface transfer doping with WOx is virtually controllable. Transistors based on WSe2 covered with WOx show only p-type conductions with orders of magnitude better on-current, on/off current ratio, and carrier mobility than without WOx, suggesting that the surface WOx serves as a p-type contact with a low hole Schottky barrier. Our findings point to a simple and effective strategy for creating p-type devices based on two-dimensional transition metal dichalcogenides with controlled dopant concentrations.