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Semi-metallic graphene and semiconducting monolayer transition-metal dichalcogenides are the most intensively studied two-dimensional materials of recent years. Lately, black phosphorus has emerged as a promising new two-dimensional material due to its widely tunable and direct bandgap, high carrier mobility and remarkable in-plane anisotropic electrical, optical and phonon properties. However, current progress is primarily limited to its thin-film form. Here, we reveal highly anisotropic and strongly bound excitons in monolayer black phosphorus using polarization-resolved photoluminescence measurements at room temperature. We show that, regardless of the excitation laser polarization, the emitted light from the monolayer is linearly polarized along the light effective mass direction and centres around 1.3 eV, a clear signature of emission from highly anisotropic bright excitons. Moreover, photoluminescence excitation spectroscopy suggests a quasiparticle bandgap of 2.2 eV, from which we estimate an exciton binding energy of ∼0.9 eV, consistent with theoretical results based on first principles. The experimental observation of highly anisotropic, bright excitons with large binding energy not only opens avenues for the future explorations of many-electron physics in this unusual two-dimensional material, but also suggests its promising future in optoelectronic devices. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The generation of a current by light is a key process in optoelectronic and photovoltaic devices. In band semiconductors, depletion fields associated with interfaces separate long-lived photo-induced carriers. However, in systems with strong electron-electron and electron-phonon correlations it is unclear what physics will dominate the photoresponse. Here, we investigate photocurrent in VO2, an exemplary strongly correlated material known for its dramatic metal-insulator transition at Tc ? 68 °C, which could be useful for optoelectronic detection and switching up to ultraviolet wavelengths. Using scanning photocurrent microscopy on individual suspended VO2 nanobeams we observe a photoresponse peaked at the metal-insulator boundary but extending throughout both insulating and metallic phases. We determine that the response is photothermal, implying efficient carrier relaxation to a local equilibrium in a manner consistent with strong correlations. Temperature-dependent measurements reveal subtle phase changes within the insulating state. We further demonstrate switching of the photocurrent by optical control of the metal-insulator boundary arrangement. Our work shows the value of applying scanning photocurrent microscopy to nanoscale crystals in the investigation of strongly correlated materials, and the results are relevant for designing and controlling optoelectronic devices employing such materials. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]