Single-photon emission from localized excitons in an atomically thin semiconductor

Monolayer transition metal dichalcogenides have recently attracted great interests because the quantum dots embedded in monolayer can serve as optically active single-photon emitters. Here, we provide an interpretation of the recombination mechanisms of these quantum emitters through polarization-resolved and magneto-optical spectroscopy at low temperature. Three types of defect-related quantum emitters in monolayer tungsten diselenide (WSe2) are observed, with different exciton g-factors of 2.02, 9.36, and unobservable Zeeman shift, respectively. The various magnetic response of the spatially localized excitons strongly indicate that the radiative recombination stems from the different transitions between defect-induced energy levels, valance, and conduction bands. Furthermore, the different g-factors and zero-field splittings of the three types of emitters strongly show that quantum dots embedded in monolayer have various types of confining potentials for localized excitons, resulting in electron–hole exchange interaction with a range of values in the presence of anisotropy. Our work further sheds light on the recombination mechanisms of defect-related quantum emitters and paves a way toward understanding the role of defects in single-photon emitters in atomically thin semiconductors.

Semiconductor quantum dots have emerged as promising candidates for the implementation of quantum information processing, because they allow for a quantum interface between stationary spin qubits and propagating single photons. In the meantime, transition-metal dichalcogenide monolayers have moved to the forefront of solid-state research due to their unique band structure featuring a large bandgap with degenerate valleys and non-zero Berry curvature. Here, we report the observation of zero-dimensional anharmonic quantum emitters, which we refer to as quantum dots, in monolayer tungsten diselenide, with an energy that is 20-100 meV lower than that of two-dimensional excitons. Photon antibunching in second-order photon correlations unequivocally demonstrates the zero-dimensional anharmonic nature of these quantum emitters. The strong anisotropic magnetic response of the spatially localized emission peaks strongly indicates that radiative recombination stems from localized excitons that inherit their electronic properties from the host transition-metal dichalcogenide. The large ∼1 meV zero-field splitting shows that the quantum dots have singlet ground states and an anisotropic confinement that is most probably induced by impurities or defects. The possibility of achieving electrical control in van der Waals heterostructures and to exploit the spin-valley degree of freedom renders transition-metal-dichalcogenide quantum dots interesting for quantum information processing.

In this paper, temperature dependence of the excitonic bands in a mechanically exfoliated tungsten diselenide (WSe2) monolayer is studied using photoluminescence and circular dichroic photoluminescence (PL) in the temperature range between 8 and 300 K. The peak energies associated with the neutral exciton (A), charged exciton (trion) and localized excitons are extracted from the PL spectra revealing a trion binding energy of around 30 meV. The circular dichroic PL measured at 8 K shows about 45% valley polarisation that sharply reduces with increasing temperature to 5% at 300 K with photoexcitation energy of 1.96 eV. A detailed analysis of the emission line-width suggests that the rapid decrease of valley polarisation with the increase of temperature is caused by the strong exciton–phonon interactions which efficiently scatter the excitons into different excitonic states that are easily accessible due to the supply of excess photoexcitation energy. The emission line-width broadening with the increase of temperature indicate residual exciton dephasing lifetime < 100 fs, that correlates with the observed rapid valley depolarisation. Circular dichroic photoluminescence spectra in monolayer WSe2 and the influence of temperature on valley depolarization is shown.

We observe stable and narrowband single photon emission from localized quantum emitters in a WSe2 monolayer. Photoluminescence excitation spectroscopy reveals that the emission originates from single excitons trapped in a local potential well.

It is safe to say that, when the concept of the photon was first introduced, the generation of single photons was not being considered. Until the emergence of the ideas and methods of quantum optics, the `single-photon regime' was attained by strongly attenuating a laser beam to ensure that the probability of having more than one photon became negligible. However, such attenuated beams differ from `true' single photons in at least two respects: first, the vacuum probability is much higher than the probability of detecting a photon, so one gets predominantly a `no-photon' regime with occasional detection of a photon; second, the probability of getting two photons is never zero, but essentially follows a Poisson law.Although the weak beam has been useful in quantum optics, the advent of quantum information science has placed stringent demands on optical sources, namely that sources produce single photons either on demand or heralded. In particular secure quantum cryptography and linear optical quantum computing depend on the availability of such single-photon sources. The combination of strict requirements for single photons, plus new technologies, is driving an exciting research effort into single-photon generation.This Focus Issue recognizes that single-photon sources are rapidly developing and presents research articles covering the spectrum of activity in the field. Significant advances are reported for single-photon and photon-pair sources constructed from quantum dots in pillar microcavities, parametric down converters, falling neutral atoms and trapped ions in cavities, defects in diamond nanocrystals and a single molecule in a solid. In addition to producing single-photon pulses, one article reports on the latest developments regarding the production of photon number states in a microwave cavity. Another article discusses the application of a nitrogen-vacancy-based single-photon source to an experimental demonstration of quantum key distribution in open air. Photodetection performs a critical role in assessing single-photon sources as well as heralding the arrival of a single photon based on detecting a correlated partner, and this issue presents the latest results on single-photon counting with a superconducting niobium nitride hot-electron bolometer. Another article provides a detailed study of how to characterize single-photon sources via intensity noise analyses. Photodetection is also important for post-selection-based processing for non-deterministic quantum information tasks, and this issue presents an analysis of photodetection and post-selection used in another way: enhancing the efficiency of single-photon sources by interferometry,photodetection and post-selection.New Journal of Physics appreciates the rapid pace of development in the area of single photons on demand. This Focus Issue presents the latest developments and also points to a bright future with better photon sources.Focus on Single Photons on Demand ContentsPhoton statistics characterization of a single-photon source R Alléaume, F Treussart, J-M Courty and J-F RochPhoton statistics of a non-stationary periodically driven single-photon source M Hennrich, T Legero, A Kuhn and G RempeOn the measurement of two-photon single-mode coupling efficiency in parametric down-conversion photon sources S Castelletto, I P Degiovanni, A Migdall and M WareSingle-photon sources based on single molecules in solids W E MoernerSingle-photon generation with InAs quantum dots Charles Santori, David Fattal, Jelena Vuckovic, Glenn S Solomon and Yoshihisa YamamotoVisible single-photon generation from semiconductor quantum dots Thomas Aichele, Valéry Zwiller and Oliver BensonEnhanced correlated photon pair emission from a pillar microcavity M Benyoucef, S M Ulrich, P Michler, J Wiersig, F Jahnke and A ForchelExperimental open-air quantum key distribution with a single-photon source R Alléaume, F Treussart, G Messin, Y Dumeige, J-F Roch, A Beveratos, R Brouri-Tualle, J-P Poizat and P GrangierPost-processing with linear optics for improving the quality of single-photon sources Dominic W Berry, Stefan Scheel, Casey R Myers, Barry C Sanders, Peter L Knight and Raymond LaflammeA single-photon source based on a single Ca+ ion Christian Maurer, Christoph Becher, Carlos Russo, Jürgen Eschner and Rainer BlattA calcium ion in a cavity as a controlled single-photon source M Keller, B Lange, K Hayasaka, W Lange and H WaltherQuantum optics with single quantum dot devices Valéry Zwiller, Thomas Aichele and Oliver BensonThe creation and detection of arbitrary photon number states using cavity QED Benjamin T H Varcoe, Simon Brattke and Herbert WaltherStable single-photon source in the near infrared T Gaebel, I Popa, A Gruber, M Domhan, F Jelezko and J WrachtrupColloidal CdSe/ZnS quantum dots as single-photon sources X Brokmann, G Messin, P Desbiolles, E Giacobino, M Dahan and J P HermierTowards a periodic deterministic source of arbitrary single-photon states Evan Jeffrey, Nicholas A Peters and Paul G KwiatFabrication of a superconducting niobium nitride hot electron bolometer for single-photon counting R Romestain, B Delaet, P Renaud-Goud, I Wang, C Jorel, J-C Villegier and J-Ph PoizatHigh-quality asynchronous heralded single-photon source at telecom wavelength Sylvain Fasel, Olivier Alibart, Sébastien Tanzilli, Pascal Baldi, Alexios Beveratos, Nicolas Gisin and Hugo ZbindenPhilippe Grangier, Institut d'Optique Théorique et Appliquée, Orsay, France Barry Sanders, University of Calgary, Canada Jelena Vuckovic, Stanford University, CA, USA

Monolayer transition metal dichalcogenides (TMDs) have a crystalline structure with broken spatial inversion symmetry, making them promising candidates for valleytronic applications. However, the degree of valley polarization is usually not high due to the presence of intervalley scattering. Here, we use the nanoindentation technique to fabricate strained structures of WSe2 on Au arrays, thus demonstrating the generation and detection of strained localized excitons in monolayer WSe2. Enhanced emission of strain-localized excitons was observed as two sharp photoluminescence (PL) peaks measured using low-temperature PL spectroscopy. We attribute these emerging sharp peaks to excitons trapped in potential wells formed by local strains. Furthermore, the valley polarization of monolayer WSe2 is modulated by a magnetic field, and the valley polarization of strained localized excitons is increased, with a high value of up to approximately 79.6%. Our results show that tunable valley polarization and localized excitons can be realized in WSe2 monolayers, which may be useful for valleytronic applications.

The effect of carbon-ion irradiation on surface microstructure and photoluminescence properties in monolayer tungsten diselenide

In monolayer transition-metal dichalcogenides, localized strain can be used to design nanoarrays of single photon sources. Despite strong empirical correlation, the nanoscale interplay between excitons and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopic analysis of excitons in nanobubbles of monolayer WSe2 with atomistic models to study how strain induces nanoscale confinement potentials and localized exciton states. The imaging of nanobubbles in monolayers with low defect concentrations reveals localized excitons on length scales of around 10 nm at multiple sites around the periphery of individual nanobubbles, in stark contrast to predictions of continuum models of strain. These results agree with theoretical confinement potentials atomistically derived from the measured topographies of nanobubbles. Our results provide experimental and theoretical insights into strain-induced exciton localization on length scales commensurate with exciton size, realizing key nanoscale structure-property information on quantum emitters in monolayer WSe2.

Transition metal dichalcogenides, such as MoS2 and WSe2, have recently gained tremendous interest for electronic and optoelectronic applications. MoS2 and WSe2 monolayers are direct bandgap and show bright photoluminescence (PL), whereas multilayers exhibit much weaker PL due to their indirect optical bandgap. This presents an obstacle for a number of device applications involving light harvesting or detection where thicker films with direct optical bandgap are desired. Here, we experimentally demonstrate a drastic enhancement in PL intensity for multilayer WSe2 (2-4 layers) under uniaxial tensile strain of up to 2%. Specifically, the PL intensity of bilayer WSe2 is amplified by ∼ 35× , making it comparable to that of an unstrained WSe2 monolayer. This drastic PL enhancement is attributed to an indirect to direct bandgap transition for strained bilayer WSe2, as confirmed by density functional theory (DFT) calculations. Notably, in contrast to MoS2 multilayers, the energy difference between the direct and indirect bandgaps of WSe2 multilayers is small, thus allowing for bandgap crossover at experimentally feasible strain values. Our results present an important advance toward controlling the band structure and optoelectronic properties of few-layer WSe2 via strain engineering, with important implications for practical device applications.

Two experiments observe the so-called Mollow triplet in the emission spectrum of a quantum dot—originating from resonantly driving a dot transition—and demonstrate the potential of these systems to act as single-photon sources, and as a readout modality for electron-spin states. Single-quantum emitters emit only one photon at a time1,2, but the properties of the photon depend on how the emitter is excited3. Incoherent excitation is simple and broadly used with solid-state emitters such as quantum dots, but does not allow direct manipulation of the quantum state. Coherent, resonant excitation on the other hand is used in pump–probe techniques to examine the quantum state of the emitter4, but does not permit collection of the single-photon emission. Coherent control with simultaneous generation of photons has been an elusive goal in solid-state approaches, where, because of strong laser scattering at the detection wavelength, measurement of resonant emission has been limited to cross-polarized detection5 or Stokes-shift techniques6,7. Here we demonstrate that a semiconductor quantum dot in a microcavity can be resonantly driven and its single-photon emission extracted background free. Under strong continuous-wave excitation, the dot undergoes several Rabi oscillations before emitting, which are visible as oscillations in the second-order correlation function. The quantum-dot states are therefore ‘dressed’, resulting in a Mollow-triplet emission spectrum. Such coherent control will be necessary for future high-efficiency sources of indistinguishable single photons3,8, which can be used for quantum key distribution9 or through post-selection10 to generate entangled photon pairs11,12.

Due to their unique band structure, single layers of transition metal dichalcogenides are promising for new atomic-scale physics and devices. It has been shown that the band structure and the excitonic transitions can be tuned by straining the material. Recently, the discovery of single-photon emission from localized excitons has put monolayer WSe2 in the spotlight. The localized light emitters might be related to local strain potentials in the monolayer. Here, we measure strain-dependent energy shifts for the A, B, C, and D excitons for uniaxial tensile strain up to 1.4% in monolayer WSe2 by performing absorption measurements. A gauge factor of and is derived for the A, B, C, and D exciton, respectively. These values are in good agreement with ab initio GW-BSE calculations. Furthermore, we examine the spatial strain distribution in the WSe2 monolayer at different applied strain levels. We find that the size of the monolayer is crucial for an efficient transfer of strain from the substrate to the monolayer.

Toward integrated optoelectronic circuits, electrically‐driven nanoscale light sources remain a key challenge in nanophotonics. 2D monolayer semiconductors, especially transition metal dichalcogenides (TMDs) represent as promising materials for developing room‐temperature tunable exciton light sources, where their exciton emission behaviors can be well controlled via strain engineering. Here, strain‐enhanced electroluminescence (EL) is demonstrated from monolayer tungsten diselenide (WSe2), which is further coupled to an optical waveguide for signal transmission. Under the alternating current (AC) gate voltage, EL emission is collected from the monolayer WSe2 and the light emission is selectively enhanced at the local strained position due to the exciton funneling effect. Furthermore, using a molybdenum trioxide (MoO3) nanoribbon as both the strain source and the optical waveguide, strain‐confined and waveguide‐integrated EL emission is visualized from the monolayer WSe2 with a coupling efficiency of 5.7%. The work provides new insights for realizing electrically‐driven on‐chip light sources based on monolayer semiconductors.

The outstanding optoelectronic and valleytronic properties of transition metal dichalcogenides (TMDs) have triggered intense research efforts by the scientific community. An alternative to induce long-range ferromagnetism (FM) in TMDs is by introducing magnetic dopants to form a dilute magnetic semiconductor. Enhancing ferromagnetism in these semiconductors not only represents a key step toward modern TMD-based spintronics, but also enables exploration of new and exciting dimensionality-driven magnetic phenomena. To this end, tunable ferromagnetism at room temperature and a thermally induced spin flip (TISF) in monolayers of V-doped WSe2 are shown. As vanadium concentration increases, the saturation magnetization increases, which is optimal at ≈4 at% vanadium; the highest doping level ever achieved for V-doped WSe2 monolayers. The TISF occurs at ≈175 K and becomes more pronounced upon increasing the temperature toward room temperature. The TISF can be manipulated by changing the vanadium concentration. The TISF is attributed to the magnetic-field- and temperature-dependent flipping of the nearest W-site magnetic moments that are antiferromagnetically coupled to the V magnetic moments in the ground state. This is fully supported by a recent spin-polarized density functional theory study. The findings pave the way for the development of novel spintronic and valleytronic nanodevices and stimulate further research.

We have investigated the optical and magneto-optical properties of monolayer (ML) WSe2 on flakes of β-Ga2O3 under high magnetic fields. Remarkably, sharp emission peaks were observed and associated with localized excitons related to point defects. A detailed study of low-temperature photoluminescence (PL) and magneto-PL under high perpendicular magnetic field up to 9 T was carried out. Several sharp emission peaks have shown valley g-factors values close to −4, which is an unusual result for localized excitons in WSe2. Furthermore, some PL peaks have shown higher g-factor values of ≈−7 and ≈−12, which were associated with the hybridization of strain localized dark excitons and defects. The reported results suggest that β-Ga2O3 is, indeed, a promising dielectric substrate for ML WSe2 and also to explore fundamental physics in view of possible applications in quantum information technology.

Solid-state quantum emitters coupled to integrated photonic nanostructures are quintessential for exploring fundamental phenomena in cavity quantum electrodynamics and widely employed in photonic quantum technologies such as non-classical light sources, quantum repeaters, and quantum transducers, etc. One of the most exciting promises from integrated quantum photonics is the potential of scalability that enables massive productions of miniaturized devices on a single chip. In reality, the yield of efficient and reproducible light-matter couplings is greatly hindered by the spectral and spatial mismatches between the single solid-state quantum emitters and confined or propagating optical modes supported by the photonic nanostructures, preventing the high-throughput realization of large-scale integrated quantum photonic circuits for more advanced quantum information processing tasks. In this work, we introduce the concept of hyperspectral imaging in quantum optics, for the first time, to address such a long-standing issue. By exploiting the extended mode with a unique dispersion in a 1D planar cavity, the spectral and spatial information of each individual quantum dot in an ensemble can be accurately and reliably extracted from a single wide-field photoluminescence image with super-resolutions. With the extracted quantum dot positions and emission wavelengths, surface-emitting quantum light sources and in-plane photonic circuits can be deterministically fabricated with a high-throughput by etching the 1D confined planar cavity into 3D confined micropillars and 2D confined waveguides. Further extension of this technique by employing an open planar cavity could be exploited for pursuing a variety of compact quantum photonic devices with expanded functionalities for large-scale integration. Our work is expected to change the landscape of integrated quantum photonic technology in which solid-state quantum emitters play essential roles as superior quantum light sources and efficient spin-photon interfaces.