Origin of Exciton-Polariton Interactions and Decoupled Dark States Dynamics in 2D Hybrid Perovskite Quantum Wells.

The realization of efficient optical devices depends on the ability to harness strong nonlinearities, which are challenging to achieve with standard photonic systems. Exciton-polaritons formed in hybrid organic-inorganic perovskites offer a promising alternative, exhibiting strong interactions at room temperature (RT). Despite recent demonstrations showcasing a robust nonlinear response, further progress is hindered by an incomplete understanding of the microscopic mechanisms governing polariton interactions in perovskite-based strongly coupled systems. Here, we investigate the nonlinear properties of quasi-2D dodecylammonium lead iodide perovskite (n3-C12) crystals embedded in a planar microcavity. Polarization-resolved pump-probe measurements reveal the contribution of indirect exchange interactions assisted by dark states formation. Additionally, we identify a strong dependence of the unique spin-dependent interaction of polaritons on sample detuning. The results are pivotal for the advancement of polaritonics, and the tunability of the robust spin-dependent anisotropic interaction in n3-C12 perovskites makes this material a powerful choice for the realization of polaritonic circuits.

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.

Perovskite semiconductors for room-temperature exciton-polaritonics.

Lead-halide perovskites are generally excellent light emitters and can have larger exciton binding energies than thermal energy at room temperature, exhibiting great promise for room-temperature exciton-polaritonics. Rapid progress has been made recently, although challenges and mysteries remain in lead-halide perovskite semiconductors to push polaritons to room-temperature operation. In this Perspective, we discuss fundamental aspects of perovskite semiconductors for exciton-polaritons and review the recent rapid experimental advances using lead-halide perovskites for room-temperature polaritonics, including the experimental realization of strong light-matter interaction using various types of microcavities as well as reaching the polariton condensation regime in planar microcavities and lattices.

Ultralow Threshold Polariton Condensate in a Monolayer Semiconductor Microcavity at Room Temperature.

Exciton-polaritons, hybrid light-matter bosonic quasiparticles, can condense into a single quantum state, i.e., forming a polariton Bose-Einstein condensate (BEC), which represents a crucial step for the development of nanophotonic technology. Recently, atomically thin transition-metal dichalcogenides (TMDs) emerged as promising candidates for novel polaritonic devices. Although the formation of robust valley-polaritons has been realized up to room temperature, the demonstration of polariton lasing remains elusive. Herein, we report for the first time the realization of this important milestone in a TMD microcavity at room temperature. Continuous wave pumped polariton lasing is evidenced by the macroscopic occupation of the ground state, which undergoes a nonlinear increase of the emission along with the emergence of temporal coherence, the presence of an exciton fraction-controlled threshold and the buildup of linear polarization. Our work presents a critically important step toward exploiting nonlinear polariton-polariton interactions, as well as offering a new platform for thresholdless lasing.

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.

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.

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.

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.

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.

Topological order and thermal equilibrium in polariton condensates.

The Berezinskii-Kosterlitz-Thouless phase transition from a disordered to a quasi-ordered state, mediated by the proliferation of topological defects in two dimensions, governs seemingly remote physical systems ranging from liquid helium, ultracold atoms and superconducting thin films to ensembles of spins. Here we observe such a transition in a short-lived gas of exciton-polaritons, bosonic light-matter particles in semiconductor microcavities. The observed quasi-ordered phase, characteristic for an equilibrium two-dimensional bosonic gas, with a decay of coherence in both spatial and temporal domains with the same algebraic exponent, is reproduced with numerical solutions of stochastic dynamics, proving that the mechanism of pairing of the topological defects (vortices) is responsible for the transition to the algebraic order. This is made possible thanks to long polariton lifetimes in high-quality samples and in a reservoir-free region. Our results show that the joint measurement of coherence both in space and time is required to characterize driven-dissipative phase transitions and enable the investigation of topological ordering in open systems.

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.

Twist of generalized skyrmions and spin vortices in a polariton superfluid.

We study the spin vortices and skyrmions coherently imprinted into an exciton-polariton condensate on a planar semiconductor microcavity. We demonstrate that the presence of a polarization anisotropy can induce a complex dynamics of these structured topologies, leading to the twist of their circuitation on the Poincaré sphere of polarizations. The theoretical description of the results carries the concept of generalized quantum vortices in two-component superfluids, which are conformal with polarization loops around an arbitrary axis in the pseudospin space.

The road towards polaritonic devices.

Polaritons are quasiparticles that form in semiconductors when an elementary excitation such as an exciton or a phonon interacts sufficiently strongly with light. In particular, exciton-polaritons have attracted tremendous attention for their unique properties, spanning from an ability to undergo ultra-efficient four-wave mixing to superfluidity in the condensed state. These quasiparticles possess strong intrinsic nonlinearities, while keeping most characteristics of the underlying photons. Here we review the most important features of exciton-polaritons in microcavities, with a particular emphasis on the emerging technological applications, the use of new materials for room-temperature operation, and the possibility of exploiting polaritons for quantum computation and simulation.

Macroscopic Two-Dimensional Polariton Condensates.

We report a record-size, two-dimensional polariton condensate of a fraction of a millimeter radius free from the presence of an exciton reservoir. This macroscopically occupied state is formed by the ballistically expanding polariton flow that relaxes and condenses over a large area outside of the excitation spot. The density of this trap-free condensate is <1 polariton/µm^{2}, reducing the phase noise induced by the interaction energy. Moreover, the backflow effect, recently predicted for the nonparabolic polariton dispersion, is observed here for the first time in the fast-expanding wave packet.

Room temperature Bloch surface wave polaritons.

Polaritons are hybrid light-matter quasi-particles that have gathered a significant attention for their capability of showing room temperature and out-of-equilibrium Bose-Einstein condensation. More recently, a novel class of ultrafast optical devices have been realized by using flows of polariton fluids, such as switches, interferometers, and logical gates. However, polariton lifetimes and propagation distances are strongly limited by photon losses and accessible in-plane momenta in normal microcavity samples. In this work, we show experimental evidence of the formation of room temperature propagating polariton states arising from the strong coupling between organic excitons and a Bloch surface wave. This result, which was only recently predicted, paves the way for the realization of polariton devices that could allow lossless propagation up to macroscopic distances.

Relaxation oscillations in the formation of a polariton condensate.

We report observation of oscillations in the dynamics of a microcavity polariton condensate formed under pulsed nonresonant excitation. While oscillations in a condensate have always been attributed to Josephson mechanisms due to a chemical potential unbalance, here we show that under some localization conditions of the condensate, they may arise from relaxation oscillations, a pervasive classical dynamics that repeatedly provokes the sudden decay of a reservoir, shutting off relaxation as the reservoir is replenished. Using nonresonant excitation, it is thus possible to obtain condensate injection pulses with a record frequency of 0.1 THz.

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.

Energy transfer driven brightening of MoS2 by ultrafast polariton relaxation in microcavity MoS2/hBN/WS2 heterostructures.

Energy transfer is a ubiquitous phenomenon that delivers energy from a blue-shifted emitter to a red-shifted absorber, facilitating wide photonic applications. Two-dimensional (2D) semiconductors provide unique opportunities for exploring novel energy transfer mechanisms in the atomic-scale limit. Herein, we have designed a planar optical microcavity-confined MoS2/hBN/WS2 heterojunction, which realizes the strong coupling among donor exciton, acceptor exciton, and cavity photon mode. This configuration demonstrates an unconventional energy transfer via polariton relaxation, brightening MoS2 with a record-high enhancement factor of ~440, i.e., two-order-of-magnitude higher than the data reported to date. The polariton relaxation features a short characteristic time of ~1.3 ps, resulting from the significantly enhanced intra- and inter-branch exciton-exciton scattering. The polariton relaxation dynamics is associated with Rabi energies in a phase diagram by combining experimental and theoretical results. This study opens a new direction of microcavity 2D semiconductor heterojunctions for high-brightness polaritonic light sources and ultrafast polariton carrier dynamics.

Exciton polariton interactions in Van der Waals superlattices at room temperature.

Monolayer transition-metal dichalcogenide (TMD) materials have attracted a great attention because of their unique properties and promising applications in integrated optoelectronic devices. Being layered materials, they can be stacked vertically to fabricate artificial van der Waals lattices, which offer unique opportunities to tailor the electronic and optical properties. The integration of TMD heterostructures in planar microcavities working in strong coupling regime is particularly important to control the light-matter interactions and form robust polaritons, highly sought for room temperature applications. Here, we demonstrate the systematic control of the coupling-strength by embedding multiple WS2 monolayers in a planar microcavity. The vacuum Rabi splitting is enhanced from 36 meV for one monolayer up to 72 meV for the four-monolayer microcavity. In addition, carrying out time-resolved pump-probe experiments at room temperature we demonstrate the nature of polariton interactions which are dominated by phase space filling effects. Furthermore, we also observe the presence of long-living dark excitations in the multiple monolayer superlattices. Our results pave the way for the realization of polaritonic devices based on planar microcavities embedding multiple monolayers and could potentially lead the way for future devices towards the exploitation of interaction-driven phenomena at room temperature.