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Room-Temperature, Highly Pure Single-Photon Sources from All- Inorganic Lead Halide Perovskite Quantum Dots
Attaining pure single-photon emission is key for many quantum technologies, from optical quantum computing to quantum key distribution and quantum imaging. The past 20 years have seen the development of several solid-state quantum emitters, but most of them require highly sophisticated techniques (e.g., ultrahigh vacuum growth methods and cryostats for low-temperature operation). The system complexity may be significantly reduced by employing quantum emitters capable of working at room temperature. Here, we present a systematic study across ∼170 photostable single CsPbX3 (X: Br and I) colloidal quantum dots (QDs) of different sizes and compositions, unveiling that increasing quantum confinement is an effective strategy for maximizing single-photon purity due to the suppressed biexciton quantum yield. Leveraging the latter, we achieve 98% single-photon purity (g(2)(0) as low as 2%) from a cavity-free, nonresonantly excited single 6.6 nm CsPbI3 QDs, showcasing the great potential of CsPbX3 QDs as room-temperature highly pure single-photon sources for quantum technologies.
Ultra-narrow room-temperature emission from single CsPbBr3 perovskite quantum dots
Semiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr3 quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35−65 meV (vs. initial values of 70–120 meV), which are on par with the best values known for structurally rigid, colloidal II-VI quantum dots (20−60 meV). Ultra-narrow emission at room-temperature is desired for conventional light-emitting devices and paramount for emerging quantum light sources.
Solving the Max-3-Cut Problem with Coherent Networks
Many computational problems are intractable through classical computing and, as Moore’s law is drawing to a halt, demand for finding alternative methods in tackling these problems is growing. Here, we realize a liquid light machine for the NP-hard max-3-cut problem based on a network of synchronized exciton-polariton condensates. We overcome the binary limitation of the decision variables in Ising machines using the continuous-phase degrees of freedom of a coherent network of polariton condensates. The condensate network dynamical transients provide optically fast annealing of the XY Hamiltonian. We apply the Goemans and Williamson random hyperplane technique, discretizing the XY ground-state spin configuration to serve as ternary decision variables for an approximate optimal solution to the max-3-cut problem. Applications of the presented coherent network are investigated in image-segmentation tasks and in circuit design.
Exact Analytical Solution for the Density Matrix of a Nonequilibrium Polariton Bose-Einstein Condensate
In this Letter, we give an analytical quantum description of a nonequilibrium polariton Bose-Einstein condensate (BEC) based on the solution of the master equation for the full polariton density matrix in the limit of fast thermalization. We find the density matrix of a nonequilibrium BEC, that takes into account quantum correlations between all polariton states. We show that the formation of BEC is accompanied by the build-up of cross-correlations between the ground state and the excited states reaching their highest values at the condensation threshold. Despite the nonequilibrium nature of polariton systems, we show the average population of polariton states exhibits the Bose-Einstein distribution with an almost zero effective chemical potential above the condensation threshold similar to an equilibrium BEC. We demonstrate that above threshold the effective temperature of polaritons drops below the reservoir temperature.
Single CsPbX3 Perovskite QDs at Room Temperature
Lead-halide perovskite APbX3 (A=Cs or organic cation; X=Cl, Br, I) quantum dots (QDs) are subject of intense research due to their exceptional properties as both classical 1 and quantum light sources. Here, we report a comprehensive investigation of the room temperature single QD optical properties. The results reveal the origin of the QD homogeneous PL linewidths, and the peculiar size-dependent exciton photoluminescence line broadening and the exciton and multi-excitons recombination dynamics. Experimental results are corroborated by ab-initio molecular dynamics. Such findings guide the further design of robust single photon sources operating at room temperature.
Reaching ultimate perovskite quantum dot optical properties with a new synthetic approach
A new synthetic method for colloidal perovskite nanocrystals has been designed, which offers slow thermodynamic control instead of conventional kinetic growth. The reaction time is increased up to 30 minutes while a wide size range of nanoparticles, some even reaching the strong confinement regime, is obtained with high level control of size and shape. The synthesized quantum dots (QDs) turn out to have a spheroidal shape on average with remarkably well-separated higher absorption peaks. For the first time, this allows for a direct comparison between theory and experimental data related to the transitions beyond the lowest absorption line. Using empirical modelling with second-order many body perturbation theory, we are able to predict the energy positions as well as the oscillator strength of not only the lowest 1s-1s exciton but also of the higher excitonic transitions. The calculated values are in fair agreement with the experimental data. Besides, by taking into consideration the spherical and cuboidal confining potentials, our theory offers an explanation for the well-defined higher transitions in the spheroidal QDs compared to cuboidal ones obtaining from more standard synthetic approaches. The accuracy of the theoretical methods will be also critically discussed.
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Superfluorescence from Binary Perovskite
Lead-halide perovskite APbX3 (A=Cs or organic cation; X=Cl, Br, I) quantum dots (QDs) are subject of intense research due to their exceptional properties as both classical 1 and quantum light sources. Here we present perovskite-type (ABO3) binary nanocrystal superlattices, created via the shape-directed co-assembly of steric-stabilized, highly luminescent cubic CsPbBr 3 nanocrystals (which occupy the B and/or O lattice sites), assembled in combination with spherical Fe 3O4 or NaGdF4 nanocrystals (A sites). These ABO3 superlattices, as well as the binary NaCl and AlB 2 superlattice structures that we demonstrated, exhibit a high degree of orientational ordering of the CsPbBr 3 nanocubes which preserve their high oscillator strength and long exciton coherence time in the assembly. Such superlattices exhibit superfluorescence—a collective emission that results in a burst of photons with ultrafast radiative decay (22 picoseconds) that could be tailored, by structural engineering of the nanoparticle assembly, for use in ultrabright (quantum) light sources. Our work paves the way for further exploration of complex, ordered and functionally useful perovskite mesostructures.
Realizing Persistent-Spin-Helix Lasing in the Regime of Rashba-Dresselhaus Spin-Orbit Coupling in a Dye-Filled Liquid-Crystal Optical Microcavity
In the presence of Rashba-Dresselhaus coupling, strong spin-orbit interactions in liquid-crystal optical cavities result in a distinctive spin-split entangled dispersion. Spin coherence between such modes gives rise to an optically persistent spin helix. In this paper, we introduce optical gain in such a system, by dispersing a molecular dye in a liquid-crystal microcavity, and demonstrate an optically persistent spin-helix lasing in the Rashba-Dresselhaus regime.
GDR NBODY GENERAL MEETING 2022
Perovskite nanocrystals (NCs) are among the most fashionable names nowadays in the field of colloidal synthesis owing to their superior photoluminescence quantum yield and blinking-free properties, which make them promising materials for both classical and quantum light sources. Their brightness and sub-nanosecond radiative decay originates from the inherent correlation effects. The many-body Coulomb interaction has generally been studied for semiconductor quantum dots. Perovskites, as a consequence of the unique properties of their dielectric functions, possess enhanced Coulomb interaction between the charge carriers. This leads to large binding energies of multi-exciton systems such as trion and biexciton in these NCs or the sizable splitting in the fine structure of single exciton states. Considering each NC as an artificial atom under the envelope function approximation, this problem of correlation effects can be approached at first by using second-order many-body techniques. This offers an elegant and efficient method that provides qualitative results for the trion and biexciton binding energies. In going beyond the second-order description, configuration interaction can be employed to include the correlation energies between the various charge carriers in a more holistic manner.
En savoir plusReservoir optics with exciton-polariton condensates
We investigate an all-optical microscale planar lensing technique based on coherent fluids of semiconductor cavity exciton-polariton condensates. Our theoretical analysis underpins the potential in using state-of-the-art spatial light modulation of nonresonant excitation beams to guide and focus polariton condensates away from their pumping region. The nonresonant excitation profile generates an excitonic reservoir that blueshifts the polariton mode and provides gain, which can be spatially tailored into lens shapes at the microscale to refract condensate waves. We propose several different avenues in controlling the condensate fluid, and demonstrate formation of highly enhanced and localized condensates away from the pumped reservoirs. This opens new perspectives in guiding quantum fluids of light and generating polariton condensates that are removed from detrimental reservoir dephasing effects.