Developing a nanoscale, integrable, and electrically pumped single mode light source is an essential step toward on-chip optical information technologies and sensors. Here, we demonstrate nanocavity enhanced electroluminescence in van der Waals heterostructures (vdWhs) at room temperature. The vertically assembled light-emitting device uses graphene/boron nitride as top and bottom tunneling contacts and monolayer WSe2 as an active light emitter. By integrating a photonic crystal cavity on top of the vdWh, we observe the electroluminescence is locally enhanced (>4 times) by the nanocavity. The emission at the cavity resonance is single mode and highly linearly polarized (84%) along the cavity mode. By applying voltage pulses, we demonstrate direct modulation of this single mode electroluminescence at a speed of ∼1 MHz, which is faster than most of the planar optoelectronics based on transition metal chalcogenides (TMDCs). Our work shows that cavity integrated vdWhs present a promising nanoscale optoelectronic platform.Keywords: Electroluminescence; optoelectronics; photonic crystal cavity; transition metal dichalcogenides; van der Waals heterostructure;

Semiconductor heterostructures are backbones for solid-state-based optoelectronic devices. Recent advances in assembly techniques for van der Waals heterostructures have enabled the band engineering of semiconductor heterojunctions for atomically thin optoelectronic devices. In two-dimensional heterostructures with type II band alignment, interlayer excitons, where Coulomb bound electrons and holes are confined to opposite layers, have shown promising properties for novel excitonic devices, including a large binding energy, micron-scale in-plane drift-diffusion, and a long population and valley polarization lifetime. Here, we demonstrate interlayer exciton optoelectronics based on electrostatically defined lateral p–n junctions in a MoSe2–WSe2 heterobilayer. Applying a forward bias enables the first observation of electroluminescence from interlayer excitons. At zero bias, the p–n junction functions as a highly sensitive photodetector, where the wavelength-dependent photocurrent measurement allows the direct observation of resonant optical excitation of the interlayer exciton. The resulting photocurrent amplitude from the interlayer exciton is about 200 times smaller than the resonant excitation of intralayer exciton. This implies that the interlayer exciton oscillator strength is 2 orders of magnitude smaller than that of the intralayer exciton due to the spatial separation of electron and hole to the opposite layers. These results lay the foundation for exploiting the interlayer exciton in future 2D heterostructure optoelectronic devices.Keywords: interlayer exciton; optoelectronics; p−n junction; transition metal dichalcogenides; van der Waals heterostructure;

Raman scattering is a ubiquitous phenomenon in light–matter interactions, which reveals a material’s electronic, structural, and thermal properties. Controlling this process would enable new ways of studying and manipulating fundamental material properties. Here, we report a novel Raman scattering process at the interface between different van der Waals (vdW) materials as well as between a monolayer semiconductor and 3D crystalline substrates. We find that interfacing a WSe2 monolayer with materials such as SiO2, sapphire, and hexagonal boron nitride (hBN) enables Raman transitions with phonons that are either traditionally inactive or weak. This Raman scattering can be amplified by nearly 2 orders of magnitude when a foreign phonon mode is resonantly coupled to the A exciton in WSe2 directly or via an A1′ optical phonon from WSe2. We further showed that the interfacial Raman scattering is distinct between hBN-encapsulated and hBN-sandwiched WSe2 sample geometries. This cross-platform electron–phonon coupling, as well as the sensitivity of 2D excitons to their phononic environments, will prove important in the understanding and engineering of optoelectronic devices based on vdW heterostructures.Keywords: exciton−phonon interaction; hexagonal boron nitride; van der Waals interface; WSe2;

Single defects in monolayer WSe2 have been shown to be a new class of single photon emitters and have potential applications in quantum technologies. Whereas previous work relied on optical excitation of single defects in isolated WSe2 monolayers, in this work we demonstrate electrically driven single defect light emission by using both vertical and lateral van der Waals heterostructure devices. In both device geometries, we use few layer graphene as the source and drain and hexagonal boron nitride as the dielectric spacer layers for engineered tunneling contacts. In addition, the lateral devices utilize a split back gate design to realize an electrostatically defined p–i–n junction. At low current densities and low temperatures (∼5 K), we observe narrow spectral lines in the electroluminescence (EL) whose properties are consistent with optically excited defect bound excitons. We show that the emission originates from spatially localized regions of the sample, and the EL spectrum from single defects has a doublet with the characteristic exchange splitting and linearly polarized selection rules. All are consistent with previously reported single photon-emitters in optical measurements. Our results pave the way for on-chip and electrically driven single photon sources in two-dimensional semiconductors for quantum technology applications.

Monolayers of transition metal dichalcogenides (TMDCs) are atomically thin direct-gap semiconductors with potential applications in nanoelectronics, optoelectronics, and electrochemical sensing. Recent theoretical and experimental efforts suggest that they are ideal systems for exploiting the valley degrees of freedom of Bloch electrons. For example, Dirac valley polarization has been demonstrated in mechanically exfoliated monolayer MoS2 samples by polarization-resolved photoluminescence, although polarization has rarely been seen at room temperature. Here we report a new method for synthesizing high optical quality monolayer MoS2 single crystals up to 25 μm in size on a variety of standard insulating substrates (SiO2, sapphire, and glass) using a catalyst-free vapor–solid growth mechanism. The technique is simple and reliable, and the optical quality of the crystals is extremely high, as demonstrated by the fact that the valley polarization approaches unity at 30 K and persists at 35% even at room temperature, suggesting a virtual absence of defects. This will allow greatly improved optoelectronic TMDC monolayer devices to be fabricated and studied routinely.Keywords: molybdenum disulfide; monolayer; photoluminescence; valley polarization; valleytronics; vapor−solid growth

Second order optical nonlinear processes involve the coherent mixing of two electromagnetic waves to generate a new optical frequency, which plays a central role in a variety of applications, such as ultrafast laser systems, rectifiers, modulators, and optical imaging. However, progress is limited in the mid-infrared (MIR) region due to the lack of suitable nonlinear materials. It is desirable to develop a robust system with a strong, electrically tunable second order optical nonlinearity. Here, we demonstrate theoretically that AB-stacked bilayer graphene (BLG) can exhibit a giant and tunable second order nonlinear susceptibility χ(2) once an in-plane electric field is applied. χ(2) can be electrically tuned from 0 to ∼105 pm/V, 3 orders of magnitude larger than the widely used nonlinear crystal AgGaSe2. We show that the unusually large χ(2) arise from two different quantum enhanced two-photon processes thanks to the unique electronic spectrum of BLG. The tunable electronic bandgap of BLG adds additional tunability on the resonance of χ(2), which corresponds to a tunable wavelength ranging from ∼2.6 to ∼3.1 μm for the up-converted photon. Combined with the high electron mobility and optical transparency of the atomically thin BLG, our scheme suggests a new regime of nonlinear photonics based on BLG.