Room Temperature Polariton Condensation from Whispering Gallery Modes in CsPbBr3 Microplatelets.

Room temperature (RT) polariton condensate holds exceptional promise for revolutionizing various fields of science and technology, encompassing optoelectronics devices to quantum information processing. Using perovskite materials, like all-inorganic cesium lead bromide (CsPbBr3) single crystal, provides additional advantages, such as ease of synthesis, cost-effectiveness, and compatibility with existing semiconductor technologies. In this work, the formation of whispering gallery modes (WGM) in CsPbBr3 single crystals with controlled geometry is shown, synthesized using a low-cost and efficient capillary bridge method. Through the implementation of microplatelets geometry, enhanced optical properties and performance are achieved due to the presence of sharp edges and a uniform surface, effectively avoiding non-radiative scattering losses caused by defects. This allows not only to observe strong light matter coupling and formation of whispering gallery polaritons, but also to demonstrate the onset of polariton condensation at RT. This investigation not only contributes to the advancement of the knowledge concerning the exceptional optical properties of perovskite-based polariton systems, but also unveils prospects for the exploration of WGM polariton condensation within the framework of a 3D perovskite-based platform, working at RT. The unique characteristics of polariton condensate, including low excitation thresholds and ultrafast dynamics, open up unique opportunities for advancements in photonics and optoelectronics devices.

Collective excitations of a bound-in-the-continuum condensate.

Spectra of low-lying elementary excitations are critical to characterize properties of bosonic quantum fluids. Usually these spectra are difficult to observe, due to low occupation of non-condensate states compared to the ground state. Recently, low-threshold Bose-Einstein condensation was realised in a symmetry-protected bound state in the continuum, at a saddle point, thanks to coupling of this electromagnetic resonance to semiconductor excitons. While it has opened the door to long-living polariton condensates, their intrinsic collective properties are still unexplored. Here we unveil the peculiar features of the Bogoliubov spectrum of excitations in this system. Thanks to the dark nature of the bound-in-the-continuum state, collective excitations lying directly above the condensate become observable in enhanced detail. We reveal interesting aspects, such as energy-flat parts of the dispersion characterized by two parallel stripes in photoluminescence pattern, pronounced linearization at non-zero momenta in one of the directions, and a strongly anisotropic velocity of sound.

Strongly enhanced light-matter coupling of monolayer WS2 from a bound state in the continuum.

Exciton-polaritons derived from the strong light-matter interaction of an optical bound state in the continuum with an excitonic resonance can inherit an ultralong radiative lifetime and significant nonlinearities, but their realization in two-dimensional semiconductors remains challenging at room temperature. Here we show strong light-matter interaction enhancement and large exciton-polariton nonlinearities at room temperature by coupling monolayer tungsten disulfide excitons to a topologically protected bound state in the continuum moulded by a one-dimensional photonic crystal, and optimizing for the electric-field strength at the monolayer position through Bloch surface wave confinement. By a structured optimization approach, the coupling with the active material is maximized here in a fully open architecture, allowing to achieve a 100 meV photonic bandgap with the bound state in the continuum in a local energy minimum and a Rabi splitting of 70 meV, which results in very high cooperativity. Our architecture paves the way to a class of polariton devices based on topologically protected and highly interacting bound states in the continuum.

Rydberg polaritons in ReS2 crystals.

Rhenium disulfide belongs to group VII transition metal dichalcogenides (TMDs) with attractive properties such as exceptionally high refractive index and remarkable oscillator strength, large in-plane birefringence, and good chemical stability. Unlike most other TMDs, the peculiar optical properties of rhenium disulfide persist from bulk to the monolayer, making this material potentially suitable for applications in optical devices. In this work, we demonstrate with unprecedented clarity the strong coupling between cavity modes and excited states, which results in a strong polariton interaction, showing the interest of these materials as a solid-state counterpart of Rydberg atomic systems. Moreover, we definitively clarify the nature of important spectral features, shedding light on some controversial aspects or incomplete interpretations and demonstrating that their origin is due to the interesting combination of the very high refractive index and the large oscillator strength expressed by these TMDs.

Electrically tunable Berry curvature and strong light-matter coupling in liquid crystal microcavities with 2D perovskite.

The field of spinoptronics is underpinned by good control over photonic spin-orbit coupling in devices that have strong optical nonlinearities. Such devices might hold the key to a new era of optoelectronics where momentum and polarization degrees of freedom of light are interwoven and interfaced with electronics. However, manipulating photons through electrical means is a daunting task given their charge neutrality. In this work, we present electrically tunable microcavity exciton-polariton resonances in a Rashba-Dresselhaus spin-orbit coupling field. We show that different spin-orbit coupling fields and the reduced cavity symmetry lead to tunable formation of the Berry curvature, the hallmark of quantum geometrical effects. For this, we have implemented an architecture of a photonic structure with a two-dimensional perovskite layer incorporated into a microcavity filled with nematic liquid crystal. Our work interfaces spinoptronic devices with electronics by combining electrical control over both the strong light-matter coupling conditions and artificial gauge fields.

Shaping the topology of light with a moving Rabi-oscillating vortex.

Quantum vortices are the analogue of classical vortices in optics, Bose-Einstein condensates, superfluids and superconductors, where they provide the elementary mode of rotation and orbital angular momentum. While they mediate important pair interactions and phase transitions in nonlinear fluids, their linear dynamics is useful for the shaping of complex light, as well as for topological entities in multi-component systems, such as full Bloch beams. Here, setting a quantum vortex into directional motion in an open-dissipative fluid of microcavity polaritons, we observe the self-splitting of the packet, leading to the trembling movement of its center of mass, whereas the vortex core undergoes ultrafast spiraling along diverging and converging circles, in a sub-picosecond precessing fashion. This singular dynamics is accompanied by vortex-antivortex pair creation and annihilation and a periodically changing topological charge. The spiraling and branching mechanics represent a direct manifestation of the underlying Bloch pseudospin space, whose mapping is shown to be rotating and splitting itself. Its reshaping is due to three simultaneous drives along the distinct directions of momentum and complex frequency, by means of the differential group velocities, Rabi frequency and dissipation rates, which are natural assets in coupled fields such as polaritons. This state, displaying linear momentum dressed with oscillating angular momentum, confirms the richness of multi-component and open quantum fluids and their innate potentiality to implement sophisticated and dynamical topological textures of light.

Tuning of the Berry curvature in 2D perovskite polaritons.

The engineering of the energy dispersion of polaritons in microcavities through nanofabrication or through the exploitation of intrinsic material and cavity anisotropies has demonstrated many intriguing effects related to topology and emergent gauge fields such as the anomalous quantum Hall and Rashba effects. Here we show how we can obtain different Berry curvature distributions of polariton bands in a strongly coupled organic-inorganic two-dimensional perovskite single-crystal microcavity. The spatial anisotropy of the perovskite crystal combined with photonic spin-orbit coupling produce two Hamilton diabolical points in the dispersion. An external magnetic field breaks time-reversal symmetry owing to the exciton Zeeman splitting and lifts the degeneracy of the diabolical points. As a result, the bands possess non-zero integral Berry curvatures, which we directly measure by state tomography. In addition to the determination of the different Berry curvatures of the multimode microcavity dispersions, we can also modify the Berry curvature distribution, the so-called band geometry, within each band by tuning external parameters, such as temperature, magnetic field and sample thickness.

Dynamics of a Vortex Lattice in an Expanding Polariton Quantum Fluid.

If a quantum fluid is driven with enough angular momentum, at equilibrium the ground state of the system is given by a lattice of quantized vortices whose density is prescribed by the quantization of circulation. We report on the first experimental study of the Feynman-Onsager relation in a nonequilibrium polariton fluid, free to expand and rotate. Upon initially imprinting a lattice of vortices in the quantum fluid, we track the vortex core positions on picosecond timescales. We observe an accelerated stretching of the lattice and an outward bending of the linear trajectories of the vortices, due to the repulsive polariton interactions. Access to the full density and phase fields allows us to detect a small deviation from the Feynman-Onsager rule in terms of a transverse velocity component, due to the density gradient of the fluid envelope acting on the vortex lattice.

Demonstration of Self-Starting Nonlinear Mode Locking in Random Lasers.

In ultrafast multimode lasers, mode locking is implemented by means of saturable absorbers or modulators, allowing for very short pulses. This occurs because of nonlinear interactions of modes with well equispaced frequencies. Though theory predicts that, in the absence of any device, mode locking would occur in random lasers, this has never been demonstrated so far. Through the analysis of multimode correlations we provide clear evidence for nonlinear mode coupling in random lasers. The behavior of multiresonance intensity correlations is tested against the nonlinear frequency matching condition equivalent to the one underlying phase locking in ordered ultrafast lasers. Nontrivially large correlations are clearly observed for spatially overlapping resonances that sensitively depend on the frequency matching condition to be satisfied, eventually demonstrating the occurrence of nonlinear mode-locked mode coupling. This is the first example, to our knowledge, of an experimental realization of self-starting mode locking in random lasers, allowing for many new developments in the design and use of nanostructured devices.

Improved Photostability in Fluorinated 2D Perovskite Single Crystals.

Hybrid organic-inorganic perovskites are very promising semiconductors for many optoelectronic applications, although their extensive use is limited by their poor stability under environmental conditions. In this work, we synthesize two-dimensional perovskite single crystals and investigate their optical and structural evolution under continuous light irradiation. We found that the hydrophobic nature of the fluorinated component, together with the absence of grain boundary defects, lead to improved material stability thanks to the creation of a robust barrier that preserve the crystalline structure, hindering photo-degradation processes usually promoted by oxygen and moisture.

Neuromorphic Binarized Polariton Networks.

The rapid development of artificial neural networks and applied artificial intelligence has led to many applications. However, current software implementation of neural networks is severely limited in terms of performance and energy efficiency. It is believed that further progress requires the development of neuromorphic systems, in which hardware directly mimics the neuronal network structure of a human brain. Here, we propose theoretically and realize experimentally an optical network of nodes performing binary operations. The nonlinearity required for efficient computation is provided by semiconductor microcavities in the strong quantum light-matter coupling regime, which exhibit exciton-polariton interactions. We demonstrate the system performance against a pattern recognition task, obtaining accuracy on a par with state-of-the-art hardware implementations. Our work opens the way to ultrafast and energy-efficient neuromorphic systems taking advantage of ultrastrong optical nonlinearity of polaritons.

Quantum hydrodynamics of a single particle.

Semiconductor devices are strong competitors in the race for the development of quantum computational systems. In this work, we interface two semiconductor building blocks of different dimensionalities with complementary properties: (1) a quantum dot hosting a single exciton and acting as a nearly ideal single-photon emitter and (2) a quantum well in a 2D microcavity sustaining polaritons, which are known for their strong interactions and unique hydrodynamic properties, including ultrafast real-time monitoring of their propagation and phase mapping. In the present experiment, we can thus observe how the injected single particles propagate and evolve inside the microcavity, giving rise to hydrodynamic features typical of macroscopic systems despite their genuine intrinsic quantum nature. In the presence of a structural defect, we observe the celebrated quantum interference of a single particle that produces fringes reminiscent of wave propagation. While this behavior could be theoretically expected, our imaging of such an interference pattern, together with a measurement of antibunching, constitutes the first demonstration of spatial mapping of the self-interference of a single quantum particle impinging on an obstacle.

Polaritonic Neuromorphic Computing Outperforms Linear Classifiers.

Machine learning software applications are ubiquitous in many fields of science and society for their outstanding capability to solve computationally vast problems like the recognition of patterns and regularities in big data sets. In spite of these impressive achievements, such processors are still based on the so-called von Neumann architecture, which is a bottleneck for faster and power-efficient neuromorphic computation. Therefore, one of the main goals of research is to conceive physical realizations of artificial neural networks capable of performing fully parallel and ultrafast operations. Here we show that lattices of exciton-polariton condensates accomplish neuromorphic computing with outstanding accuracy thanks to their high optical nonlinearity. We demonstrate that our neural network significantly increases the recognition efficiency compared with the linear classification algorithms on one of the most widely used benchmarks, the MNIST problem, showing a concrete advantage from the integration of optical systems in neural network architectures.

Directional Goldstone waves in polariton condensates close to equilibrium.

Quantum fluids of light are realized in semiconductor microcavities using exciton-polaritons, solid-state quasi-particles with a light mass and sizeable interactions. Here, we use the microscopic analogue of oceanographic techniques to measure the excitation spectrum of a thermalised polariton condensate. Increasing the fluid density, we demonstrate the transition from a free-particle parabolic dispersion to a linear, sound-like Goldstone mode characteristic of superfluids at equilibrium. Notably, we reveal the effect of an asymmetric pumping by showing that collective excitations are created with a definite direction with respect to the condensate. Furthermore, we measure the critical sound speed for polariton superfluids close to equilibrium.

Self-Trapping of Exciton-Polariton Condensates in GaAs Microcavities.

The self-trapping of exciton-polariton condensates is demonstrated and explained by the formation of a new polaronlike state. Above the polariton lasing threshold, local variation of the lattice temperature provides the mechanism for an attractive interaction between polaritons. Because of this attraction, the condensate collapses into a small bright spot. Its position and momentum variances approach the Heisenberg quantum limit. The self-trapping does not require either a resonant driving force or a presence of defects. The trapped state is stabilized by the phonon-assisted stimulated scattering of excitons into the polariton condensate. While the formation mechanism of the observed self-trapped state is similar to the Landau-Pekar polaron model, this state is populated by several thousands of quasiparticles, in a striking contrast to the conventional single-particle polaron state.

Quantum Nature of Light in Nonstoichiometric Bulk Perovskites.

Sources of single photons are a fundamental brick in the development of quantum information technologies. Great efforts have been made so far in the realization of reliable, highly efficient, and on demand quantum sources that could show an easy integration with quantum devices. This has recently culminated in the use of solid state quantum dots as promising candidates for future sources of quantum technologies. However, some challenges, like their complex fabrication, random distribution, and difficult integrability with silicon technology, could hinder their broad application, making necessary the study of alternative systems. In this work, we clearly demonstrate single photon emission from quantum dots formed in nonstoichiometric bulk perovskites. Their simple growing procedures, exceptional stability under constant illumination, easy control of their optical properties, as well as ease of integrability make these materials very interesting candidates for the development of quantum light sources in the near-infrared.

Interacting polariton fluids in a monolayer of tungsten disulfide.

Atomically thin transition metal dichalcogenides (TMDs) possess a number of properties that make them attractive for realizing room-temperature polariton devices1. An ideal platform for manipulating polariton fluids within monolayer TMDs is that of Bloch surface waves, which confine the electric field to a small volume near the surface of a dielectric mirror2-4. Here we demonstrate that monolayer tungsten disulfide can sustain Bloch surface wave polaritons (BSWPs) with a Rabi splitting of 43 meV and propagation lengths reaching 33 µm. In addition, we show strong polariton-polariton nonlinearities within BSWPs, which manifest themselves as a reversible blueshift of the lower polariton resonance. Such nonlinearities are at the heart of polariton devices5-11 and have not yet been demonstrated in TMD polaritons. As a proof of concept, we use the nonlinearity to implement a nonlinear polariton source. Our results demonstrate that BSWPs using TMDs can support long-range propagation combined with strong nonlinearities, enabling potential applications in integrated optical processing and polaritonic circuits.

First observation of the quantized exciton-polariton field and effect of interactions on a single polariton.

Polaritons are quasi-particles that originate from the coupling of light with matter and that demonstrate quantum phenomena at the many-particle mesoscopic level, such as Bose-Einstein condensation and superfluidity. A highly sought and long-time missing feature of polaritons is a genuine quantum manifestation of their dynamics at the single-particle level. Although they are conceptually perceived as entangled states and theoretical proposals abound for an explicit manifestation of their single-particle properties, so far their behavior has remained fully accounted for by classical and mean-field theories. We report the first experimental demonstration of a genuinely quantum state of the microcavity polariton field, by swapping a photon for a polariton in a two-photon entangled state generated by parametric downconversion. When bringing this single-polariton quantum state in contact with a polariton condensate, we observe a disentangling with the external photon. This manifestation of a polariton quantum state involving a single quantum unlocks new possibilities for quantum information processing with interacting bosons.

Interactions and scattering of quantum vortices in a polariton fluid.

Quantum vortices, the quantized version of classical vortices, play a prominent role in superfluid and superconductor phase transitions. However, their exploration at a particle level in open quantum systems has gained considerable attention only recently. Here we study vortex pair interactions in a resonant polariton fluid created in a solid-state microcavity. By tracking the vortices on picosecond time scales, we reveal the role of nonlinearity, as well as of density and phase gradients, in driving their rotational dynamics. Such effects are also responsible for the split of composite spin-vortex molecules into elementary half-vortices, when seeding opposite vorticity between the two spinorial components. Remarkably, we also observe that vortices placed in close proximity experience a pull-push scenario leading to unusual scattering-like events that can be described by a tunable effective potential. Understanding vortex interactions can be useful in quantum hydrodynamics and in the development of vortex-based lattices, gyroscopes, and logic devices.