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.

Lateral heterojunctions within monolayer MoSe2-WSe2 semiconductors.

Heterojunctions between three-dimensional (3D) semiconductors with different bandgaps are the basis of modern light-emitting diodes, diode lasers and high-speed transistors. Creating analogous heterojunctions between different 2D semiconductors would enable band engineering within the 2D plane and open up new realms in materials science, device physics and engineering. Here we demonstrate that seamless high-quality in-plane heterojunctions can be grown between the 2D monolayer semiconductors MoSe2 and WSe2. The junctions, grown by lateral heteroepitaxy using physical vapour transport, are visible in an optical microscope and show enhanced photoluminescence. Atomically resolved transmission electron microscopy reveals that their structure is an undistorted honeycomb lattice in which substitution of one transition metal by another occurs across the interface. The growth of such lateral junctions will allow new device functionalities, such as in-plane transistors and diodes, to be integrated within a single atomically thin layer.

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.

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.

Electrically tunable excitonic light-emitting diodes based on monolayer WSe2 p-n junctions.

The development of light-emitting diodes with improved efficiency, spectral properties, compactness and integrability is important for lighting, display, optical interconnect, logic and sensor applications. Monolayer transition-metal dichalcogenides have recently emerged as interesting candidates for optoelectronic applications due to their unique optical properties. Electroluminescence has already been observed from monolayer MoS2 devices. However, the electroluminescence efficiency was low and the linewidth broad due both to the poor optical quality of the MoS2 and to ineffective contacts. Here, we report electroluminescence from lateral p-n junctions in monolayer WSe2 induced electrostatically using a thin boron nitride support as a dielectric layer with multiple metal gates beneath. This structure allows effective injection of electrons and holes, and, combined with the high optical quality of WSe2, yields bright electroluminescence with 1,000 times smaller injection current and 10 times smaller linewidth than in MoS2 (refs 17,18). Furthermore, by increasing the injection bias we can tune the electroluminescence between regimes of impurity-bound, charged and neutral excitons. This system has the required ingredients for new types of optoelectronic device, such as spin- and valley-polarized light-emitting diodes, on-chip lasers and two-dimensional electro-optic modulators.

Vapor-solid growth of high optical quality MoS2 monolayers with near-unity valley polarization.

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.

Electrical control of neutral and charged excitons in a monolayer semiconductor.

Monolayer group-VI transition metal dichalcogenides have recently emerged as semiconducting alternatives to graphene in which the true two-dimensionality is expected to illuminate new semiconducting physics. Here we investigate excitons and trions (their singly charged counterparts), which have thus far been challenging to generate and control in the ultimate two-dimensional limit. Utilizing high-quality monolayer molybdenum diselenide, we report the unambiguous observation and electrostatic tunability of charging effects in positively charged (X(+)), neutral (X(o)) and negatively charged (X(-)) excitons in field-effect transistors via photoluminescence. The trion charging energy is large (30 meV), enhanced by strong confinement and heavy effective masses, whereas the linewidth is narrow (5 meV) at temperatures <55 K. This is greater spectral contrast than in any known quasi-two-dimensional system. We also find the charging energies for X(+) and X(-) to be nearly identical implying the same effective mass for electrons and holes.

Optical generation of excitonic valley coherence in monolayer WSe2.

As a consequence of degeneracies arising from crystal symmetries, it is possible for electron states at band-edges ('valleys') to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseudospins, analogous to that implemented using true spin, in the quest for quantum technologies. Here, we show that valley coherence can be generated and detected. Because excitons in a single valley emit circularly polarized photons, linear polarization can only be generated through recombination of an exciton in a coherent superposition of the two valley states. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley excitons and trions. We then demonstrate coherence between valley excitons through the observation of linearly polarized luminescence, whose orientation coincides with that of the linearly polarized excitation, for any given polarization angle. In contrast, the corresponding photoluminescence from trions is not observed to be linearly polarized, consistent with the expectation that the emitted photon polarization is entangled with valley pseudospin. The ability to address coherence, in addition to valley polarization, is a step forward towards achieving quantum manipulation of the valley index necessary for coherent valleytronics.

Ultrafast hot-carrier-dominated photocurrent in graphene.

The combination of its high electron mobility, broadband absorption and ultrafast luminescence make graphene attractive for optoelectronic and photonic applications, including transparent electrodes, mode-locked lasers and high-speed optical modulators. Photo-excited carriers that have not cooled to the temperature of the graphene lattice are known as hot carriers, and may limit device speed and energy efficiency. However, their roles in charge and energy transport are not fully understood. Here, we use time-resolved scanning photocurrent microscopy to demonstrate that hot carriers, rather than phonons, dominate energy transport across a tunable graphene p-n junction excited by ultrafast laser pulses. The photocurrent response time varies from 1.5 ps at room temperature to 4 ps at 20 K, implying a fundamental bandwidth of ∼500 GHz (refs 12, 13, 21). Gate-dependent pump-probe measurements demonstrate that both thermoelectric and built-in electric field effects contribute to the photocurrent, with the contribution from each depending on the junction configuration. The photocurrent produced by a single pulsed laser also displays multiple polarity reversals as a function of carrier density, which is a possible signature of impact ionization.