Interplay between spin proximity effect and charge-dependent exciton dynamics in MoSe2/CrBr3 van der Waals heterostructures.

Semiconducting ferromagnet-nonmagnet interfaces in van der Waals heterostructures present a unique opportunity to investigate magnetic proximity interactions dependent upon a multitude of phenomena including valley and layer pseudospins, moiré periodicity, or exceptionally strong Coulomb binding. Here, we report a charge-state dependency of the magnetic proximity effects between MoSe2 and CrBr3 in photoluminescence, whereby the valley polarization of the MoSe2 trion state conforms closely to the local CrBr3 magnetization, while the neutral exciton state remains insensitive to the ferromagnet. We attribute this to spin-dependent interlayer charge transfer occurring on timescales between the exciton and trion radiative lifetimes. Going further, we uncover by both the magneto-optical Kerr effect and photoluminescence a domain-like spatial topography of contrasting valley polarization, which we infer to be labyrinthine or otherwise highly intricate, with features smaller than 400 nm corresponding to our optical resolution. Our findings offer a unique insight into the interplay between short-lived valley excitons and spin-dependent interlayer tunneling, while also highlighting MoSe2 as a promising candidate to optically interface with exotic spin textures in van der Waals structures.

Highly nonlinear trion-polaritons in a monolayer semiconductor.

Highly nonlinear optical materials with strong effective photon-photon interactions are required for ultrafast and quantum optical signal processing circuitry. Here we report strong Kerr-like nonlinearities by employing efficient optical transitions of charged excitons (trions) observed in semiconducting transition metal dichalcogenides (TMDCs). By hybridising trions in monolayer MoSe2 at low electron densities with a microcavity mode, we realise trion-polaritons exhibiting significant energy shifts at small photon fluxes due to phase space filling. We find the ratio of trion- to neutral exciton-polariton interaction strength is in the range from 10 to 100 in TMDC materials and that trion-polariton nonlinearity is comparable to that in other polariton systems. The results are in good agreement with a theory accounting for the composite nature of excitons and trions and deviation of their statistics from that of ideal bosons and fermions. Our findings open a way to scalable quantum optics applications with TMDCs.

Enhanced light-matter interaction in an atomically thin semiconductor coupled with dielectric nano-antennas.

Unique structural and optical properties of atomically thin two-dimensional semiconducting transition metal dichalcogenides enable in principle their efficient coupling to photonic cavities having the optical mode volume close to or below the diffraction limit. Recently, it has become possible to make all-dielectric nano-cavities with reduced mode volumes and negligible non-radiative losses. Here, we realise low-loss high-refractive-index dielectric gallium phosphide (GaP) nano-antennas with small mode volumes coupled to atomic mono- and bilayers of WSe[Formula: see text]. We observe a photoluminescence enhancement exceeding 10[Formula: see text] compared with WSe[Formula: see text] placed on planar GaP, and trace its origin to a combination of enhancement of the spontaneous emission rate, favourable modification of the photoluminescence directionality and enhanced optical excitation efficiency. A further effect of the coupling is observed in the photoluminescence polarisation dependence and in the Raman scattering signal enhancement exceeding 10[Formula: see text]. Our findings reveal dielectric nano-antennas as a promising platform for engineering light-matter coupling in two-dimensional semiconductors.

The valley Zeeman effect in inter- and intra-valley trions in monolayer WSe2.

Monolayer transition metal dichalcogenides (TMDs) hold great promise for future information processing applications utilizing a combination of electron spin and valley pseudospin. This unique spin system has led to observation of the valley Zeeman effect in neutral and charged excitonic resonances under applied magnetic fields. However, reported values of the trion valley Zeeman splitting remain highly inconsistent across studies. Here, we utilize high quality hBN encapsulated monolayer WSe2 to enable simultaneous measurement of both intervalley and intravalley trion photoluminescence. We find the valley Zeeman splitting of each trion state to be describable only by a combination of three distinct g-factors, one arising from the exciton-like valley Zeeman effect, the other two, trion specific, g-factors associated with recoil of the excess electron. This complex picture goes significantly beyond the valley Zeeman effect reported for neutral excitons, and eliminates the ambiguity surrounding the magneto-optical response of trions in tungsten based TMD monolayers.

Valley coherent exciton-polaritons in a monolayer semiconductor.

Two-dimensional transition metal dichalcogenides (TMDs) provide a unique possibility to generate and read-out excitonic valley coherence using linearly polarized light, opening the way to valley information transfer between distant systems. However, these excitons have short lifetimes (ps) and efficiently lose their valley coherence via the electron-hole exchange interaction. Here, we show that control of these processes can be gained by embedding a monolayer of WSe2 in an optical microcavity, forming part-light-part-matter exciton-polaritons. We demonstrate optical initialization of valley coherent polariton populations, exhibiting luminescence with a linear polarization degree up to 3 times higher than displayed by bare excitons. We utilize an external magnetic field alongside selective exciton-cavity-mode detuning to control the polariton valley pseudospin vector rotation, which reaches 45° at B = 8 T. This work provides unique insight into the decoherence mechanisms in TMDs and demonstrates the potential for engineering the valley pseudospin dynamics in monolayer semiconductors embedded in photonic structures.

WSe2 Light-Emitting Tunneling Transistors with Enhanced Brightness at Room Temperature.

Monolayers of molybdenum and tungsten dichalcogenides are direct bandgap semiconductors, which makes them promising for optoelectronic applications. In particular, van der Waals heterostructures consisting of monolayers of MoS2 sandwiched between atomically thin hexagonal boron nitride (hBN) and graphene electrodes allows one to obtain light emitting quantum wells (LEQWs) with low-temperature external quantum efficiency (EQE) of 1%. However, the EQE of MoS2- and MoSe2-based LEQWs shows behavior common for many other materials: it decreases fast from cryogenic conditions to room temperature, undermining their practical applications. Here we compare MoSe2 and WSe2 LEQWs. We show that the EQE of WSe2 devices grows with temperature, with room temperature EQE reaching 5%, which is 250× more than the previous best performance of MoS2 and MoSe2 quantum wells in ambient conditions. We attribute such different temperature dependences to the inverted sign of spin-orbit splitting of conduction band states in tungsten and molybdenum dichalcogenides, which makes the lowest-energy exciton in WSe2 dark.

Exciton-polaritons in van der Waals heterostructures embedded in tunable microcavities.

Layered materials can be assembled vertically to fabricate a new class of van der Waals heterostructures a few atomic layers thick, compatible with a wide range of substrates and optoelectronic device geometries, enabling new strategies for control of light-matter coupling. Here, we incorporate molybdenum diselenide/hexagonal boron nitride (MoSe2/hBN) quantum wells in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe2 excitons and cavity photons, evidenced from a clear anticrossing between the neutral exciton and the cavity modes with a splitting of 20 meV for a single MoSe2 monolayer, enhanced to 29 meV in MoSe2/hBN/MoSe2 double-quantum wells. The splitting at resonance provides an estimate of the exciton radiative lifetime of 0.4 ps. Our results pave the way for room-temperature polaritonic devices based on multiple-quantum-well van der Waals heterostructures, where polariton condensation and electrical polariton injection through the incorporation of graphene contacts may be realized.

Light-emitting diodes by band-structure engineering in van der Waals heterostructures.

The advent of graphene and related 2D materials has recently led to a new technology: heterostructures based on these atomically thin crystals. The paradigm proved itself extremely versatile and led to rapid demonstration of tunnelling diodes with negative differential resistance, tunnelling transistors, photovoltaic devices and so on. Here, we take the complexity and functionality of such van der Waals heterostructures to the next level by introducing quantum wells (QWs) engineered with one atomic plane precision. We describe light-emitting diodes (LEDs) made by stacking metallic graphene, insulating hexagonal boron nitride and various semiconducting monolayers into complex but carefully designed sequences. Our first devices already exhibit an extrinsic quantum efficiency of nearly 10% and the emission can be tuned over a wide range of frequencies by appropriately choosing and combining 2D semiconductors (monolayers of transition metal dichalcogenides). By preparing the heterostructures on elastic and transparent substrates, we show that they can also provide the basis for flexible and semi-transparent electronics. The range of functionalities for the demonstrated heterostructures is expected to grow further on increasing the number of available 2D crystals and improving their electronic quality.

Suppression of nuclear spin bath fluctuations in self-assembled quantum dots induced by inhomogeneous strain.

Interaction with nuclear spins leads to decoherence and information loss in solid-state electron-spin qubits. One particular, ineradicable source of electron decoherence arises from decoherence of the nuclear spin bath, driven by nuclear-nuclear dipolar interactions. Owing to its many-body nature nuclear decoherence is difficult to predict, especially for an important class of strained nanostructures where nuclear quadrupolar effects have a significant but largely unknown impact. Here, we report direct measurement of nuclear spin bath coherence in individual self-assembled InGaAs/GaAs quantum dots: spin-echo coherence times in the range 1.2-4.5 ms are found. Based on these values, we demonstrate that strain-induced quadrupolar interactions make nuclear spin fluctuations much slower compared with lattice-matched GaAs/AlGaAs structures. Our findings demonstrate that quadrupolar effects can potentially be used to engineer optically active III-V semiconductor spin-qubits with a nearly noise-free nuclear spin bath, previously achievable only in nuclear spin-0 semiconductors, where qubit network interconnection and scaling are challenging.

Two-dimensional metal-chalcogenide films in tunable optical microcavities.

Integration of quasi-two-dimensional (2D) films of metal-chalcogenides in optical microcavities permits new photonic applications of these materials. Here we present tunable microcavities with monolayer MoS2 or few monolayer GaSe films. We observe significant modification of spectral and temporal properties of photoluminescence (PL): PL is emitted in spectrally narrow and wavelength-tunable cavity modes with quality factors up to 7400; a 10-fold PL lifetime shortening is achieved, a consequence of Purcell enhancement of the spontaneous emission rate.

Optical investigation of the natural electron doping in thin MoS2 films deposited on dielectric substrates.

Two-dimensional (2D) compounds provide unique building blocks for novel layered devices and hybrid photonic structures. However, large surface-to-volume ratio in thin films enhances the significance of surface interactions and charging effects requiring new understanding. Here we use micro-photoluminescence (PL) and ultrasonic force microscopy to explore the influence of the dielectric environment on optical properties of a few monolayer MoS2 films. PL spectra for MoS2 films deposited on SiO2 substrates are found to vary widely. This film-to-film variation is suppressed by additional capping of MoS2 with SiO2 and Si(x)N(y), improving mechanical coupling of MoS2 with surrounding dielectrics. We show that the observed PL non-uniformities are related to strong variation in the local electron charging of MoS2 films. In completely encapsulated films, negative charging is enhanced leading to uniform optical properties. Observed great sensitivity of optical characteristics of 2D films to surface interactions has important implications for optoelectronics applications of layered materials.

Nuclear spin effects in semiconductor quantum dots.

The interaction of an electronic spin with its nuclear environment, an issue known as the central spin problem, has been the subject of considerable attention due to its relevance for spin-based quantum computation using semiconductor quantum dots. Independent control of the nuclear spin bath using nuclear magnetic resonance techniques and dynamic nuclear polarization using the central spin itself offer unique possibilities for manipulating the nuclear bath with significant consequences for the coherence and controlled manipulation of the central spin. Here we review some of the recent optical and transport experiments that have explored this central spin problem using semiconductor quantum dots. We focus on the interaction between 10(4)-10(6) nuclear spins and a spin of a single electron or valence-band hole. We also review the experimental techniques as well as the key theoretical ideas and the implications for quantum information science.

III-V quantum light source and cavity-QED on silicon.

Non-classical light sources offer a myriad of possibilities in both fundamental science and commercial applications. Single photons are the most robust carriers of quantum information and can be exploited for linear optics quantum information processing. Scale-up requires miniaturisation of the waveguide circuit and multiple single photon sources. Silicon photonics, driven by the incentive of optical interconnects is a highly promising platform for the passive optical components, but integrated light sources are limited by silicon's indirect band-gap. III-V semiconductor quantum-dots, on the other hand, are proven quantum emitters. Here we demonstrate single-photon emission from quantum-dots coupled to photonic crystal nanocavities fabricated from III-V material grown directly on silicon substrates. The high quality of the III-V material and photonic structures is emphasized by observation of the strong-coupling regime. This work opens-up the advantages of silicon photonics to the integration and scale-up of solid-state quantum optical systems.

Effect of a GaAsP shell on the optical properties of self-catalyzed GaAs nanowires grown on silicon.

We realize the growth of self-catalyzed core-shell GaAs/GaAsP nanowires (NWs) on Si substrates using molecular-beam epitaxy. Transmission electron microscopy of single GaAs/GaAsP NWs demonstrates their high crystal quality and shows domination of the GaAs zinc-blende phase. Using continuous-wave and time-resolved photoluminescence (PL), we make a detailed comparison with uncapped GaAs NWs to emphasize the effect of the GaAsP capping in suppressing the nonradiative surface states. Significant PL enhancement in the core-shell structures exceeding 3 orders of magnitude at 10 K is observed; in uncapped NWs PL is quenched at 60 K, whereas single core-shell GaAs/GaAsP structures exhibit bright emission even at room temperature. From analysis of the PL temperature dependence in both types of NW we are able to determine the main carrier escape mechanisms leading to the PL quench.

Structural analysis of strained quantum dots using nuclear magnetic resonance.

Strained semiconductor nanostructures can be used to make single-photon sources, detectors and photovoltaic devices, and could potentially be used to create quantum logic devices. The development of such applications requires techniques capable of nanoscale structural analysis, but the microscopy methods typically used to analyse these materials are destructive. NMR techniques can provide non-invasive structural analysis, but have been restricted to strain-free semiconductor nanostructures because of the significant strain-induced quadrupole broadening of the NMR spectra. Here, we show that optically detected NMR spectroscopy can be used to analyse individual strained quantum dots. Our approach uses continuous-wave broadband radiofrequency excitation with a specially designed spectral pattern and can probe individual strained nanostructures containing only 1 × 10(5) quadrupole nuclear spins. With this technique, we are able to measure the strain distribution and chemical composition of quantum dots in the volume occupied by the single confined electron. The approach could also be used to address problems in quantum information processing such as the precise control of nuclear spins in the presence of strong quadrupole effects.

Laser location and manipulation of a single quantum tunneling channel in an InAs quantum dot.

We use a femtowatt focused laser beam to locate and manipulate a single quantum tunneling channel associated with an individual InAs quantum dot within an ensemble of dots. The intensity of the directed laser beam tunes the tunneling current through the targeted dot with an effective optical gain of 10(7) and modifies the curvature of the dot's confining potential and the spatial extent of its ground state electron eigenfunction. These observations are explained by the effect of photocreated hole charges which become bound close to the targeted dot, thus acting as an optically induced gate electrode.

Fast control of nuclear spin polarization in an optically pumped single quantum dot.

Highly polarized nuclear spins within a semiconductor quantum dot induce effective magnetic (Overhauser) fields of up to several Tesla acting on the electron spin, or up to a few hundred mT for the hole spin. Recently this has been recognized as a resource for intrinsic control of quantum-dot-based spin quantum bits. However, only static long-lived Overhauser fields could be used. Here we demonstrate fast redirection on the microsecond timescale of Overhauser fields on the order of 0.5 T experienced by a single electron spin in an optically pumped GaAs quantum dot. This has been achieved using coherent control of an ensemble of 10(5) optically polarized nuclear spins by sequences of short radiofrequency pulses. These results open the way to a new class of experiments using radiofrequency techniques to achieve highly correlated nuclear spins in quantum dots, such as adiabatic demagnetization in the rotating frame leading to sub-µK nuclear spin temperatures, rapid adiabatic passage, and spin squeezing.

Direct measurement of the hole-nuclear spin interaction in single InP/GaInP quantum dots using photoluminescence spectroscopy.

We measure the hyperfine interaction of the valence band hole with nuclear spins in single InP/GaInP semiconductor quantum dots. Detection of photoluminescence (PL) of both "bright" and "dark" excitons enables direct measurement of the Overhauser shift of states with the same electron but opposite hole spin projections. We find that the hole hyperfine constant is ≈11% of that of the electron and has the opposite sign. By measuring the degree of circular polarization of the PL, an upper limit to the contribution of the heavy-light hole mixing to the measured value of the hole hyperfine constant is deduced. Our results imply that environment-independent hole spins are not realizable in III-V semiconductor, a result important for solid-state quantum information processing using hole spin qubits.

Pumping of nuclear spins by optical excitation of spin-forbidden transitions in a quantum dot.

We demonstrate that efficient optical pumping of nuclear spins in semiconductor quantum dots (QDs) can be achieved by resonant pumping of optically forbidden transitions. This process corresponds to one-to-one conversion of a photon absorbed by the dot into a polarized nuclear spin, and also has potential for initialization of hole spin in QDs. We find that by employing this spin-forbidden process, nuclear polarization of 65% can be achieved, markedly higher than from pumping the allowed transition, which saturates due to the low probability of electron-nuclear spin flip-flop.

Nuclear spin switch in semiconductor quantum dots.

We show that by illuminating an InGaAs/GaAs self-assembled quantum dot with circularly polarized light, the nuclei of atoms constituting the dot can be driven into a bistable regime, in which either a thresholdlike enhancement or reduction of the local nuclear field by up to 3 T can be generated by varying the pumping intensity. The excitation power threshold for such a nuclear spin "switch" is found to depend on both the external magnetic and electric fields. The switch is shown to arise from the strong feedback of the nuclear spin polarization on the dynamics of the spin transfer from electrons to the nuclei of the dot.