Inversion of exciton level splitting in quantum dots

The demonstration of degeneracy of exciton spin states is an important step toward the production of entangled photon pairs from the biexciton cascade. We measure the fine structure of exciton and biexciton states for a large number of single InAs quantum dots in a GaAs matrix; the energetic splitting of the horizontally and vertically polarized components of the exciton doublet is shown to decrease as the exciton confinement decreases, crucially passing through zero and changing sign. Thermal annealing is shown to reduce the exciton confinement, thereby increasing the number of dots with splitting close to zero

Dielectric nano-antennas for strain engineering in atomically thin two-dimensional semiconductors

Atomically thin two-dimensional semiconducting transition metal dichalcogenides (TMDs) can withstand large levels of strain before their irreversible damage occurs. This unique property offers a promising route for control of the optical and electronic properties of TMDs, for instance by depositing them on nano-structured surfaces, where position-dependent strain can be produced on the nano-scale. Here, we demonstrate strain-induced modifications of the optical properties of mono- and bilayer TMD WSe$_2$ placed on photonic nano-antennas made from gallium phosphide (GaP). Photoluminescence (PL) from the strained areas of the TMD layer is enhanced owing to the efficient coupling with the confined optical mode of the nano-antenna. Thus, by following the shift of the PL peak, we deduce the changes in the strain in WSe$_2$ deposited on the nano-antennas of different radii. In agreement with the presented theory, strain up to $\approx 1.4 \%$ is observed for WSe$_2$ monolayers. We also estimate that $>3\%$ strain is achieved in bilayers, accompanied with the emergence of a direct bandgap in this normally indirect-bandgap semiconductor. At cryogenic temperatures, we find evidence of the exciton confinement in the most strained nano-scale parts of the WSe$_2$ layers, as also predicted by our theoretical model. Our results, of direct relevance for both dielectric and plasmonic nano-antennas, show that strain in atomically thin semiconductors can be used as an additional parameter for engineering light-matter interaction in nano-photonic devices

All-optical formation of coherent dark states of silicon-vacancy spins in diamond

Spin impurities in diamond can be versatile tools for a wide range of solid-state-based quantum technologies, but finding spin impurities which offer sufficient quality in both photonic and spin properties remains a challenge for this pursuit. The silicon-vacancy center has recently attracted a lot of interest due to its spin-accessible optical transitions and the quality of its optical spectrum. Complementing these properties, spin coherence is essential for the suitability of this center as a spin-photon quantum interface. Here, we report all-optical generation of coherent superpositions of spin states in the ground state of a negatively charged silicon-vacancy center using coherent population trapping. Our measurements reveal a characteristic spin coherence time, T2*, exceeding 250 nanoseconds at 4 K. We further investigate the role of phonon-mediated coupling between orbital states as a source of irreversible decoherence. Our results indicate the feasibility of all-optical coherent control of silicon-vacancy spins using ultrafast laser pulses.Comment: Additional data and analysis is available for download in PDF format at the publications section of http://www.amop.phy.cam.ac.uk/amop-m

Full coherent control of nuclear spins in an optically pumped single quantum dot

Highly polarized nuclear spins within a semiconductor quantum dot (QD) 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 QD-based spin quantum bits. However, only static long-lived Overhauser fields could be used. Here we demonstrate fast redirection on the microsecond time-scale of Overhauser fields of the order of 0.5 T experienced by a single electron spin in an optically pumped GaAs quantum dot. This has been achieved using full coherent control of an ensemble of 10^3-10^4 optically polarized nuclear spins by sequences of short radio-frequency (rf) pulses. These results open the way to a new class of experiments using rf techniques to achieve highly-correlated nuclear spins in quantum dots, such as adiabatic demagnetization in the rotating frame leading to sub-micro K nuclear spin temperatures, rapid adiabatic passage, and spin squeezing

Exciton and trion dynamics in atomically thin MoSe2 and WSe2: effect of localization

We present a detailed investigation of the exciton and trion dynamics in naturally doped MoSe2 and WSe2 single atomic layers as a function of temperature in the range 10-300K under above band-gap laser excitation. By combining time-integrated and time-resolved photoluminescence (PL) spectroscopy we show the importance of exciton and trion localization in both materials at low temperatures. We also reveal the transition to delocalized exciton complexes at higher temperatures where the exciton and trion thermal energy exceeds the typical localization energy. This is accompanied with strong changes in PL including suppression of the trion PL and decrease of the trion PL life-time, as well as significant changes for neutral excitons in the temperature dependence of the PL intensity and appearance of a pronounced slow PL decay component. In MoSe2 and WSe2 studied here, the temperatures where such strong changes occur are observed at around 100 and 200 K, respectively, in agreement with their inhomogeneous PL linewidth of 8 and 20 meV at T~10K. The observed behavior is a result of a complex interplay between influences of the specific energy ordering of bright and dark excitons in MoSe2 and WSe2, sample doping, trion and exciton localization and various temperature-dependent non-radiative processes

Sculpting oscillators with light within a nonlinear quantum fluid

Seeing macroscopic quantum states directly remains an elusive goal. Particles with boson symmetry can condense into such quantum fluids producing rich physical phenomena as well as proven potential for interferometric devices [1-10]. However direct imaging of such quantum states is only fleetingly possible in high-vacuum ultracold atomic condensates, and not in superconductors. Recent condensation of solid state polariton quasiparticles, built from mixing semiconductor excitons with microcavity photons, offers monolithic devices capable of supporting room temperature quantum states [11-14] that exhibit superfluid behaviour [15,16]. Here we use microcavities on a semiconductor chip supporting two-dimensional polariton condensates to directly visualise the formation of a spontaneously oscillating quantum fluid. This system is created on the fly by injecting polaritons at two or more spatially-separated pump spots. Although oscillating at tuneable THz-scale frequencies, a simple optical microscope can be used to directly image their stable archetypal quantum oscillator wavefunctions in real space. The self-repulsion of polaritons provides a solid state quasiparticle that is so nonlinear as to modify its own potential. Interference in time and space reveals the condensate wavepackets arise from non-equilibrium solitons. Control of such polariton condensate wavepackets demonstrates great potential for integrated semiconductor-based condensate devices.Comment: accepted in Nature Physic

Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature

Strong-coupling of monolayer metal dichalcogenide semiconductors with light offers encouraging prospects for realistic exciton devices at room temperature. However, the nature of this coupling depends extremely sensitively on the optical confinement and the orientation of electronic dipoles and fields. Here, we show how plasmon strong coupling can be achieved in compact robust easily-assembled gold nano-gap resonators at room temperature. We prove that strong coupling is impossible with monolayers due to the large exciton coherence size, but resolve clear anti-crossings for greater than 7 layer devices with Rabi splittings exceeding 135 meV. We show that such structures improve on prospects for nonlinear exciton functionalities by at least 10$^{4}$, while retaining quantum efficiencies above 50%, and show evidence for superlinear light emission.We acknowledge support from EPSRC grants EP/G060649/1, EP/L027151/1, EP/G037221/1, EPSRC NanoDTC, and ERC grant LINASS 320503. J.M. acknowledges support from the Winton Programme of the Physics of Sustainability. R.C. acknowledges support from the Dr Manmohan Singh scholarship from St John’s College, University of Cambridge. AIT and EMA acknowledge support from EPSRC grant EP/M012727/1, Graphene Flagship grant 696656, and ITN Spin-NANO 676108. CC acknowledges support from the UK National Physical Laboratory. CG acknowledges support by the A. v. Humboldt Foundation

Measurement of local optomechanical properties of a direct bandgap 2D semiconductor

Strain engineering is a powerful tool for tuning physical properties of 2D materials, including monolayer transition metal dichalcogenides (TMDs)—direct bandgap semiconductors with strong excitonic response. Deformation of TMD monolayers allows inducing modulation of exciton potential and, ultimately, creating single-photon emitters at desired positions. The performance of such systems is critically dependent on the exciton energy profile and maximum possible exciton energy shift that can be achieved under local impact until the monolayer rupture. Here, we study the evolution of two-dimensional exciton energy profile induced in a MoSe2 monolayer under incremental local indentation until the rupture. We controllably stress the flake with an atomic force microscope tip and perform in situ spatiospectral mapping of the excitonic photoluminescence in the vicinity of the indentation point. In order to accurately fit the experimental data, we combine numerical simulations with a simple model of strain-induced modification of the local excitonic response and carefully account for the optical resolution of the setup. This allows us to extract deformation, strain, and exciton energy profiles obtained at each indentation depth. The maximum exciton energy shift induced by local deformation achieved at 300 nm indentation reaches the value of 36.5 meV and corresponds to 1.15% strain of the monolayer. Our approach is a powerful tool for in situ characterization of local optomechanical properties of 2D direct bandgap semiconductors with strong excitonic response

Vortices in polariton OPO superfluids

This chapter reviews the occurrence of quantised vortices in polariton fluids, primarily when polaritons are driven in the optical parametric oscillator (OPO) regime. We first review the OPO physics, together with both its analytical and numerical modelling, the latter being necessary for the description of finite size systems. Pattern formation is typical in systems driven away from equilibrium. Similarly, we find that uniform OPO solutions can be unstable to the spontaneous formation of quantised vortices. However, metastable vortices can only be injected externally into an otherwise stable symmetric state, and their persistence is due to the OPO superfluid properties. We discuss how the currents charactering an OPO play a crucial role in the occurrence and dynamics of both metastable and spontaneous vortices.Comment: 40 pages, 16 figure

Interspecies exciton interactions lead to enhanced nonlinearity of dipolar excitons and polaritons in MoS2 homobilayers

This is the final version. Available from Nature Research via the DOI in this record. Data availability: The data that support the findings of this study are available in the MARVEL public repository (MARVEL Materials Cloud Archive: https:// archive.materialscloud.org) with the same title as this paper.Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS2 to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons (dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS2 monolayers, both hIX and dipolaritons exhibit ≈ 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This provides access to an unusual nonlinear regime which we describe theoretically as a mixed effect of Pauli exclusion and exciton-exciton interactions enabled through charge tunnelling. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.Engineering and Physical Sciences Research Council (EPSRC)European Graphene Flagship ProjectEngineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research Council (EPSRC)European Union Marie Sklodowska-Curie ActionsEngineering and Physical Sciences Research Council (EPSRC)JSPS KAKENHIJSPS KAKENHIJSPS KAKENHIWorld Premier International Research Centre Initiative (WPI)Royal Society, ERC Consolidator grant QTWISTEngineering and Physical Sciences Research Council (EPSRC)Engineering and Physical Sciences Research CouncilEngineering and Physical Sciences Research CouncilEuropean Quantum Technology Flagship Project 2DSIPCNATO SPS projectEngineering and Physical Sciences Research Council (EPSRC)European Union’s Horizon 202