Giant Tunability of Intersubband Transitions and Quantum Hall Quartets in Few-Layer InSe Quantum Wells.

A two-dimensional (2D) quantum electron system is characterized by quantized energy levels, or subbands, in the out-of-plane direction. Populating higher subbands and controlling the intersubband transitions have wide technological applications such as optical modulators and quantum cascade lasers. In conventional materials, however, the tunability of intersubband spacing is limited. Here we demonstrate electrostatic population and characterization of the second subband in few-layer InSe quantum wells, with giant tunability of its energy, population, and spin-orbit coupling strength, via the control of not only layer thickness but also the out-of-plane displacement field. A modulation of as much as 350% or over 250 meV is achievable, underscoring the promise of InSe for tunable infrared and THz sources, detectors, and modulators.

Thickness- and Twist-Angle-Dependent Interlayer Excitons in Metal Monochalcogenide Heterostructures.

Interlayer excitons, or bound electron-hole pairs whose constituent quasiparticles are located in distinct stacked semiconducting layers, are being intensively studied in heterobilayers of two-dimensional semiconductors. They owe their existence to an intrinsic type-II band alignment between both layers that convert these into p-n junctions. Here, we unveil a pronounced interlayer exciton (IX) in heterobilayers of metal monochalcogenides, namely, γ-InSe on ε-GaSe, whose pronounced emission is adjustable just by varying their thicknesses given their number of layers dependent direct band gaps. Time-dependent photoluminescense spectroscopy unveils considerably longer interlayer exciton lifetimes with respect to intralayer ones, thus confirming their nature. The linear Stark effect yields a bound electron-hole pair whose separation d is just (3.6 ± 0.1) Å with d being very close to dSe = 3.4 Å which is the calculated interfacial Se separation. The envelope of IX is twist-angle-dependent and describable by superimposed emissions that are nearly equally spaced in energy, as if quantized due to localization induced by the small moiré periodicity. These heterostacks are characterized by extremely flat interfacial valence bands making them prime candidates for the observation of magnetism or other correlated electronic phases upon carrier doping.

Light sources with bias tunable spectrum based on van der Waals interface transistors.

Light-emitting electronic devices are ubiquitous in key areas of current technology, such as data communications, solid-state lighting, displays, and optical interconnects. Controlling the spectrum of the emitted light electrically, by simply acting on the device bias conditions, is an important goal with potential technological repercussions. However, identifying a material platform enabling broad electrical tuning of the spectrum of electroluminescent devices remains challenging. Here, we propose light-emitting field-effect transistors based on van der Waals interfaces of atomically thin semiconductors as a promising class of devices to achieve this goal. We demonstrate that large spectral changes in room-temperature electroluminescence can be controlled both at the device assembly stage -by suitably selecting the material forming the interfaces- and on-chip, by changing the bias to modify the device operation point. Even though the precise relation between device bias and kinetics of the radiative transitions remains to be understood, our experiments show that the physical mechanism responsible for light emission is robust, making these devices compatible with simple large areas device production methods.

Layer- and gate-tunable spin-orbit coupling in a high-mobility few-layer semiconductor.

Spin-orbit coupling (SOC) is a relativistic effect, where an electron moving in an electric field experiences an effective magnetic field in its rest frame. In crystals without inversion symmetry, it lifts the spin degeneracy and leads to many magnetic, spintronic, and topological phenomena and applications. In bulk materials, SOC strength is a constant. Here, we demonstrate SOC and intrinsic spin splitting in atomically thin InSe, which can be modified over a broad range. From quantum oscillations, we establish that the SOC parameter α is thickness dependent; it can be continuously modulated by an out-of-plane electric field, achieving intrinsic spin splitting tunable between 0 and 20 meV. Unexpectedly, α could be enhanced by an order of magnitude in some devices, suggesting that SOC can be further manipulated. Our work highlights the extraordinary tunability of SOC in 2D materials, which can be harnessed for in operando spintronic and topological devices and applications.

Bilayer Lateral Heterostructures of Transition-Metal Dichalcogenides and Their Optoelectronic Response.

Two-dimensional lateral heterojunctions based on monolayer transition-metal dichalcogenides (TMDs) have received increasing attention given that their direct band gap makes them very attractive for optoelectronic applications. Although bilayer TMDs present an indirect band gap, their electrical properties are expected to be less susceptible to ambient conditions, with higher mobilities and density of states when compared to monolayers. Bilayers and few-layers single domain devices have already demonstrated higher performance in radio frequency and photosensing applications. Despite these advantages, lateral heterostructures based on bilayer domains have been less explored. Here, we report the controlled synthesis of multi-junction bilayer lateral heterostructures based on MoS2-WS2 and MoSe2-WSe2 monodomains. The heterojunctions are created via sequential lateral edge-epitaxy that happens simultaneously in both the first and the second layers. A phenomenological mechanism is proposed to explain the growth mode with self-limited thickness that happens within a certain window of growth conditions. With respect to their as-grown monolayer counterparts, bilayer lateral heterostructures yield nearly 1 order of magnitude higher rectification currents. They also display a clear photovoltaic response, with short circuit currents ∼103 times larger than those extracted from the as-grown monolayers, in addition to room-temperature electroluminescence. The improved performance of bilayer heterostructures significantly expands the potential of two-dimensional materials for optoelectronics.

Phase Modulators Based on High Mobility Ambipolar ReSe2 Field-Effect Transistors.

We fabricated ambipolar field-effect transistors (FETs) from multi-layered triclinic ReSe2, mechanically exfoliated onto a SiO2 layer grown on p-doped Si. In contrast to previous reports on thin layers (~2 to 3 layers), we extract field-effect carrier mobilities in excess of 102 cm2/Vs at room temperature in crystals with nearly ~10 atomic layers. These thicker FETs also show nearly zero threshold gate voltage for conduction and high ON to OFF current ratios when compared to the FETs built from thinner layers. We also demonstrate that it is possible to utilize this ambipolarity to fabricate logical elements or digital synthesizers. For instance, we demonstrate that one can produce simple, gate-voltage tunable phase modulators with the ability to shift the phase of the input signal by either 90° or nearly 180°. Given that it is possible to engineer these same elements with improved architectures, for example on h-BN in order to decrease the threshold gate voltage and increase the carrier mobilities, it is possible to improve their characteristics in order to engineer ultra-thin layered logic elements based on ReSe2.

One-pot growth of two-dimensional lateral heterostructures via sequential edge-epitaxy.

Two-dimensional heterojunctions of transition-metal dichalcogenides have great potential for application in low-power, high-performance and flexible electro-optical devices, such as tunnelling transistors, light-emitting diodes, photodetectors and photovoltaic cells. Although complex heterostructures have been fabricated via the van der Waals stacking of different two-dimensional materials, the in situ fabrication of high-quality lateral heterostructures with multiple junctions remains a challenge. Transition-metal-dichalcogenide lateral heterostructures have been synthesized via single-step, two-step or multi-step growth processes. However, these methods lack the flexibility to control, in situ, the growth of individual domains. In situ synthesis of multi-junction lateral heterostructures does not require multiple exchanges of sources or reactors, a limitation in previous approaches as it exposes the edges to ambient contamination, compromises the homogeneity of domain size in periodic structures, and results in long processing times. Here we report a one-pot synthetic approach, using a single heterogeneous solid source, for the continuous fabrication of lateral multi-junction heterostructures consisting of monolayers of transition-metal dichalcogenides. The sequential formation of heterojunctions is achieved solely by changing the composition of the reactive gas environment in the presence of water vapour. This enables selective control of the water-induced oxidation and volatilization of each transition-metal precursor, as well as its nucleation on the substrate, leading to sequential edge-epitaxy of distinct transition-metal dichalcogenides. Photoluminescence maps confirm the sequential spatial modulation of the bandgap, and atomic-resolution images reveal defect-free lateral connectivity between the different transition-metal-dichalcogenide domains within a single crystal structure. Electrical transport measurements revealed diode-like responses across the junctions. Our new approach offers greater flexibility and control than previous methods for continuous growth of transition-metal-dichalcogenide-based multi-junction lateral heterostructures. These findings could be extended to other families of two-dimensional materials, and establish a foundation for the development of complex and atomically thin in-plane superlattices, devices and integrated circuits.

Pronounced Photovoltaic Response from Multilayered Transition-Metal Dichalcogenides PN-Junctions.

Transition metal dichalcogenides (TMDs) are layered semiconductors with indirect band gaps comparable to Si. These compounds can be grown in large area, while their gap(s) can be tuned by changing their chemical composition or by applying a gate voltage. The experimental evidence collected so far points toward a strong interaction with light, which contrasts with the small photovoltaic efficiencies η ≤ 1% extracted from bulk crystals or exfoliated monolayers. Here, we evaluate the potential of these compounds by studying the photovoltaic response of electrostatically generated PN-junctions composed of approximately 10 atomic layers of MoSe2 stacked onto the dielectric h-BN. In addition to ideal diode-like response, we find that these junctions can yield, under AM-1.5 illumination, photovoltaic efficiencies η exceeding 14%, with fill factors of ~70%. Given the available strategies for increasing η such as gap tuning, improving the quality of the electrical contacts, or the fabrication of tandem cells, our study suggests a remarkable potential for photovoltaic applications based on TMDs.

Ambipolar molybdenum diselenide field-effect transistors: field-effect and Hall mobilities.

We report a room temperature study on the electrical response of field-effect transistors (FETs) based on few-layered MoSe2, grown by a chemical vapor transport technique, mechanically exfoliated onto SiO2. In contrast to previous reports on MoSe2 FETs electrically contacted with Ni, MoSe2 FETs electrically contacted with Ti display ambipolar behavior with current on to off ratios up to 10(6) for both hole and electron channels when applying a small excitation voltage. A rather small hysteresis is observed when sweeping the back-gate voltage between positive and negative values, indicating the near absence of charge "puddles". For both channels the Hall effect indicates Hall mobilities µH ≃ 250 cm(2)/(V s), which are comparable to the corresponding field-effect mobilities, i.e., µFE ∼ 150 to 200 cm(2)/(V s) evaluated through the conventional two-terminal field-effect configuration. Therefore, our results suggest that MoSe2 could be a good candidate for p-n junctions composed of a single atomic layer and for low-power, complementary logic applications.

Field-effect transistors based on few-layered α-MoTe(2).

Here we report the properties of field-effect transistors based on a few layers of chemical vapor transport grown α-MoTe2 crystals mechanically exfoliated onto SiO2. We performed field-effect and Hall mobility measurements, as well as Raman scattering and transmission electron microscopy. In contrast to both MoS2 and MoSe2, our MoTe2 field-effect transistors are observed to be hole-doped, displaying on/off ratios surpassing 10(6) and typical subthreshold swings of ∼140 mV per decade. Both field-effect and Hall mobilities indicate maximum values approaching or surpassing 10 cm(2)/(V s), which are comparable to figures previously reported for single or bilayered MoS2 and/or for MoSe2 exfoliated onto SiO2 at room temperature and without the use of dielectric engineering. Raman scattering reveals sharp modes in agreement with previous reports, whose frequencies are found to display little or no dependence on the number of layers. Given that MoS2 is electron-doped, the stacking of MoTe2 onto MoS2 could produce ambipolar field-effect transistors and a gap modulation. Although the overall electronic performance of MoTe2 is comparable to those of MoS2 and MoSe2, the heavier element Te leads to a stronger spin-orbit coupling and possibly to concomitantly longer decoherence times for exciton valley and spin indexes.