Interlayer Exciton Diode and Transistor.

Controlling the flow of charge neutral interlayer exciton (IX) quasiparticles can potentially lead to low loss excitonic circuits. Here, we report unidirectional transport of IXs along nanoscale electrostatically defined channels in an MoSe2-WSe2 heterostructure. These results are enabled by a lithographically defined triangular etch in a graphene gate to create a potential energy "slide". By performing spatially and temporally resolved photoluminescence measurements, we measure smoothly varying IX energy along the structure and high speed exciton flow with a drift velocity up to 2 × 106 cm/s, an order of magnitude larger than previous experiments. Furthermore, exciton flow can be controlled by saturating exciton population in the channel using a second laser pulse, demonstrating an optically gated excitonic transistor. Our work paves the way toward low loss excitonic circuits, the study of bosonic transport in one-dimensional channels, and custom potential energy landscapes for excitons in van der Waals heterostructures.

Nanoscale Trapping of Interlayer Excitons in a 2D Semiconductor Heterostructure.

For quantum technologies based on single excitons and spins, the deterministic placement and control of a single exciton is a longstanding goal. MoSe2-WSe2 heterostructures host spatially indirect interlayer excitons (IXs) that exhibit highly tunable energies and unique spin-valley physics, making them promising candidates for quantum information processing. Previous IX trapping approaches involving moiré superlattices and nanopillars do not meet the quantum technology requirements of deterministic placement and energy tunability. Here, we use a nanopatterned graphene gate to create a sharply varying electric field in close proximity to a MoSe2-WSe2 heterostructure. The dipole interaction between the IX and the electric field creates an ∼20 nm trap. The trapped IXs show the predicted electric-field-dependent energy, saturation at low excitation power, and increased lifetime, all signatures of strong spatial confinement. The demonstrated architecture is a crucial step toward the deterministic trapping of single IXs, which has broad applications to scalable quantum technologies.

Monolayer semiconductor nanocavity lasers with ultralow thresholds.

Engineering the electromagnetic environment of a nanometre-scale light emitter by use of a photonic cavity can significantly enhance its spontaneous emission rate, through cavity quantum electrodynamics in the Purcell regime. This effect can greatly reduce the lasing threshold of the emitter, providing a low-threshold laser system with small footprint, low power consumption and ultrafast modulation. An ultralow-threshold nanoscale laser has been successfully developed by embedding quantum dots into a photonic crystal cavity (PCC). However, several challenges impede the practical application of this architecture, including the random positions and compositional fluctuations of the dots, extreme difficulty in current injection, and lack of compatibility with electronic circuits. Here we report a new lasing strategy: an atomically thin crystalline semiconductor--that is, a tungsten diselenide monolayer--is non-destructively and deterministically introduced as a gain medium at the surface of a pre-fabricated PCC. A continuous-wave nanolaser operating in the visible regime is thereby achieved with an optical pumping threshold as low as 27 nanowatts at 130 kelvin, similar to the value achieved in quantum-dot PCC lasers. The key to the lasing action lies in the monolayer nature of the gain medium, which confines direct-gap excitons to within one nanometre of the PCC surface. The surface-gain geometry gives unprecedented accessibility and hence the ability to tailor gain properties via external controls such as electrostatic gating and current injection, enabling electrically pumped operation. Our scheme is scalable and compatible with integrated photonics for on-chip optical communication technologies.

Monolayer Semiconductor Auger Detector.

Auger recombination in semiconductors is a many-body phenomenon in which the recombination of electrons and holes is accompanied by excitation of other charge carriers. The excess energy of the excited carriers is normally rapidly converted to heat, making Auger processes difficult to probe directly. Here, we employ a technique in which the Auger-excited carriers are detected by their ability to tunnel out of the semiconductor through a thin barrier, generating a current. We use vertical van der Waals heterostructures with monolayer WSe2 as the semiconductor, with hexagonal boron nitride as the tunnel barrier, and a graphite collector electrode. The Auger processes combined with resonant absorption produce characteristic negative photoconductance. We detect holes Auger-excited by both neutral and charged excitons and find that the Auger scattering is surprisingly strong under weak excitation. Our work expands the range of techniques available for probing relaxation processes in 2D materials.

Interlayer Exciton Optoelectronics in a 2D Heterostructure p-n Junction.

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.

Single Defect Light-Emitting Diode in a van der Waals Heterostructure.

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.

Exciton Dynamics in Monolayer Transition Metal Dichalcogenides.

Since the discovery of semiconducting monolayer transition metal dichalcogenides, a variety of experimental and theoretical studies have been carried out seeking to understand the intrinsic exciton population recombination and valley relaxation dynamics. Reports of the exciton decay time range from hundreds of femtoseconds to ten nanoseconds, while the valley depolarization time can exceed one nanosecond. At present, however, a consensus on the microscopic mechanisms governing exciton radiative and non-radiative recombination is lacking. The strong exciton oscillator strength resulting in up to ~ 20% absorption for a single monolayer points to ultrafast radiative recombination. However, the low quantum yield and large variance in the reported lifetimes suggest that non-radiative Auger-type processes obscure the intrinsic exciton radiative lifetime. In either case, the electron-hole exchange interaction plays an important role in the exciton spin and valley dynamics. In this article, we review the experiments and theory that have led to these conclusions and comment on future experiments that could complement our current understanding.

Population pulsation resonances of excitons in monolayer MoSe2 with sub-1 µeV linewidths.

Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. Here, we investigate exciton relaxation in monolayer MoSe_{2} using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 and <0.2 µeV at low temperature. These linewidths are more than 3 orders of magnitude narrower than the photoluminescence and absorption linewidth, and indicate that a component of the exciton relaxation dynamics occurs on time scales longer than 1 ns. The ultranarrow resonance (<0.2 µeV) emerges with increasing excitation intensity, and implies the existence of a long-lived state whose lifetime exceeds 6 ns.

Slow light in a 2D semiconductor plasmonic structure.

Spectrally narrow optical resonances can be used to generate slow light, i.e., a large reduction in the group velocity. In a previous work, we developed hybrid 2D semiconductor plasmonic structures, which consist of propagating optical frequency surface-plasmon polaritons interacting with excitons in a semiconductor monolayer. Here, we use coupled exciton-surface plasmon polaritons (E-SPPs) in monolayer WSe2 to demonstrate slow light with a 1300 fold decrease of the SPP group velocity. Specifically, we use a high resolution two-color laser technique where the nonlinear E-SPP response gives rise to ultra-narrow coherent population oscillation (CPO) resonances, resulting in a group velocity on order of 105 m/s. Our work paves the way toward on-chip actively switched delay lines and optical buffers that utilize 2D semiconductors as active elements.

Localized interlayer excitons in MoSe2-WSe2 heterostructures without a moiré potential.

Interlayer excitons (IXs) in MoSe2-WSe2 heterobilayers have generated interest as highly tunable light emitters in transition metal dichalcogenide (TMD) heterostructures. Previous reports of spectrally narrow (<1 meV) photoluminescence (PL) emission lines at low temperature have been attributed to IXs localized by the moiré potential between the TMD layers. We show that spectrally narrow IX PL lines are present even when the moiré potential is suppressed by inserting a bilayer hexagonal boron nitride (hBN) spacer between the TMD layers. We compare the doping, electric field, magnetic field, and temperature dependence of IXs in a directly contacted MoSe2-WSe2 region to those in a region separated by bilayer hBN. The doping, electric field, and temperature dependence of the narrow IX lines are similar for both regions, but their excitonic g-factors have opposite signs, indicating that the origin of narrow IX PL is not the moiré potential.

2D semiconductor nonlinear plasmonic modulators.

A plasmonic modulator is a device that controls the amplitude or phase of propagating plasmons. In a pure plasmonic modulator, the presence or absence of a plasmonic pump wave controls the amplitude of a plasmonic probe wave through a channel. This control has to be mediated by an interaction between disparate plasmonic waves, typically requiring the integration of a nonlinear material. In this work, we demonstrate a 2D semiconductor nonlinear plasmonic modulator based on a WSe2 monolayer integrated on top of a lithographically defined metallic waveguide. We utilize the strong interaction between the surface plasmon polaritons (SPPs) and excitons in the WSe2 to give a 73 % change in transmission through the device. We demonstrate control of the propagating SPPs using both optical and SPP pumps, realizing a 2D semiconductor nonlinear plasmonic modulator, with an ultrafast response time of 290 fs.

Defect-Mediated Alloying of Monolayer Transition-Metal Dichalcogenides.

Alloying plays a central role in tailoring the material properties of 2D transition-metal dichalcogenides (TMDs). However, despite widespread reports, the details of the alloying mechanism in 2D TMDs have remained largely unknown and are yet to be further explored. Here, we combine a set of systematic experiments with ab initio density functional theory (DFT) calculations to unravel a defect-mediated mechanism for the alloying of monolayer TMD crystals. In our alloying approach, a monolayer MoSe2 film serves as a host crystal in which exchanging selenium (Se) atoms with sulfur (S) atoms yields a MoS2 xSe2(1- x) alloy. Our study reveals that the driving force required for the alloying of CVD-grown films with abundant vacancy-type defects is significantly lower than that required for the alloying of exfoliated films with fewer vacancies. Indeed, we show that pre-existing Se vacancies in the host MoSe2 lattice mediate the replacement of chalcogen atoms and facilitate the synthesis of MoS2 xSe2(1- x) alloys. Our DFT calculations suggest that S atoms can bind to Se vacancies and then diffuse throughout the host MoSe2 lattice via exchanging the position with Se vacancies, further supporting our proposed defect-mediated alloying mechanism. Beside native vacancy defects, we show that the existence of large-scale defects in CVD-grown MoSe2 films causes the fracture of alloys under the alloying-induced strain, while no such effect is observed in exfoliated MoSe2 films. Our study provides a deep insight into the details of the alloying mechanism and enables the synthesis of 2D alloys with tunable properties.

Ultrafast optical pump-probe studies of the cytochrome b(6)f complex in solution and crystalline states.

The cytochrome b6f complex of oxygenic photosynthesis contains a single chlorophyll a (Chl a) molecule whose function is presently unknown. The singlet excited state of the Chl a molecule is quenched by the surrounding protein matrix, and thus the Chl a molecule in the b6f complex may serve as an exceptionally sensitive probe of the protein structure. For the first time, singlet excited-state dynamics were measured in well-diffracting crystals using femtosecond time-resolved optical pump-probe methodology. Lifetimes of the Chl a molecule in crystals of the cytochrome b6f complex having different space groups were 3-6 times longer than those determined in detergent solutions of the b6f. The observed differences in excited state dynamics may arise from small (1-1.5 A) changes in the local protein structure caused by crystal packing. The Chl a excited state lifetimes measured in the dissolved cytochrome b6f complexes from several different species are essentially the same, in spite of differences in the local amino acid sequences around the Chl a. This supports an earlier hypothesis that the short excited state lifetime of Chl a is critical for the function of the b6f complex.

Directional interlayer spin-valley transfer in two-dimensional heterostructures.

Van der Waals heterostructures formed by two different monolayer semiconductors have emerged as a promising platform for new optoelectronic and spin/valleytronic applications. In addition to its atomically thin nature, a two-dimensional semiconductor heterostructure is distinct from its three-dimensional counterparts due to the unique coupled spin-valley physics of its constituent monolayers. Here, we report the direct observation that an optically generated spin-valley polarization in one monolayer can be transferred between layers of a two-dimensional MoSe2-WSe2 heterostructure. Using non-degenerate optical circular dichroism spectroscopy, we show that charge transfer between two monolayers conserves spin-valley polarization and is only weakly dependent on the twist angle between layers. Our work points to a new spin-valley pumping scheme in nanoscale devices, provides a fundamental understanding of spin-valley transfer across the two-dimensional interface, and shows the potential use of two-dimensional semiconductors as a spin-valley generator in two-dimensional spin/valleytronic devices for storing and processing information.

Valley-polarized exciton dynamics in a 2D semiconductor heterostructure.

Heterostructures comprising different monolayer semiconductors provide an attractive setting for fundamental science and device technologies, such as in the emerging field of valleytronics. We realized valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We created interlayer exciton spin-valley polarization by means of circularly polarized optical pumping and determined a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several micrometers. The spatial pattern of the polarization evolves into a ring with increasing exciton density, a manifestation of valley exciton exchange interactions. Our work introduces van der Waals heterostructures as a promising platform from which to study valley exciton physics.

Electrical control of second-harmonic generation in a WSe2 monolayer transistor.

Nonlinear optical frequency conversion, in which optical fields interact with a nonlinear medium to produce new field frequencies, is ubiquitous in modern photonic systems. However, the nonlinear electric susceptibilities that give rise to such phenomena are often challenging to tune in a given material and, so far, dynamical control of optical nonlinearities remains confined to research laboratories as a spectroscopic tool. Here, we report a mechanism to electrically control second-order optical nonlinearities in monolayer WSe2, an atomically thin semiconductor. We show that the intensity of second-harmonic generation at the A-exciton resonance is tunable by over an order of magnitude at low temperature and nearly a factor of four at room temperature through electrostatic doping in a field-effect transistor. Such tunability arises from the strong exciton charging effects in monolayer semiconductors, which allow for exceptional control over the oscillator strengths at the exciton and trion resonances. The exciton-enhanced second-harmonic generation is counter-circularly polarized to the excitation laser due to the combination of the two-photon and one-photon valley selection rules, which have opposite helicity in the monolayer. Our study paves the way towards a new platform for chip-scale, electrically tunable nonlinear optical devices based on two-dimensional semiconductors.

Observation of long-lived interlayer excitons in monolayer MoSe2-WSe2 heterostructures.

Van der Waals bound heterostructures constructed with two-dimensional materials, such as graphene, boron nitride and transition metal dichalcogenides, have sparked wide interest in device physics and technologies at the two-dimensional limit. One highly coveted heterostructure is that of differing monolayer transition metal dichalcogenides with type-II band alignment, with bound electrons and holes localized in individual monolayers, that is, interlayer excitons. Here, we report the observation of interlayer excitons in monolayer MoSe2-WSe2 heterostructures by photoluminescence and photoluminescence excitation spectroscopy. We find that their energy and luminescence intensity are highly tunable by an applied vertical gate voltage. Moreover, we measure an interlayer exciton lifetime of ~1.8 ns, an order of magnitude longer than intralayer excitons in monolayers. Our work demonstrates optical pumping of interlayer electric polarization, which may provoke further exploration of interlayer exciton condensation, as well as new applications in two-dimensional lasers, light-emitting diodes and photovoltaic devices.

Single quantum emitters in monolayer semiconductors.

Single quantum emitters (SQEs) are at the heart of quantum optics and photonic quantum-information technologies. To date, all the demonstrated solid-state single-photon sources are confined to one-dimensional (1D; ref. 3) or 3D materials. Here, we report a new class of SQEs based on excitons that are spatially localized by defects in 2D tungsten-diselenide (WSe2) monolayers. The optical emission from these SQEs shows narrow linewidths of ∼130 µeV, about two orders of magnitude smaller than those of delocalized valley excitons. Second-order correlation measurements revealed a strong photon antibunching, which unambiguously established the single-photon nature of the emission. The SQE emission shows two non-degenerate transitions, which are cross-linearly polarized. We assign this fine structure to two excitonic eigenmodes whose degeneracy is lifted by a large ∼0.71 meV coupling, probably because of the electron-hole exchange interaction in the presence of anisotropy. Magneto-optical measurements also reveal an exciton g factor of ∼8.7, several times larger than those of delocalized valley excitons. In addition to their fundamental importance, establishing new SQEs in 2D quantum materials could give rise to practical advantages in quantum-information processing, such as an efficient photon extraction and a high integratability and scalability.