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.

Ultrafast exciton fluid flow in an atomically thin MoS2 semiconductor.

Excitons (coupled electron-hole pairs) in semiconductors can form collective states that sometimes exhibit spectacular nonlinear properties. Here, we show experimental evidence of a collective state of short-lived excitons in a direct-bandgap, atomically thin MoS2 semiconductor whose propagation resembles that of a classical liquid as suggested by the nearly uniform photoluminescence through the MoS2 monolayer regardless of crystallographic defects and geometric constraints. The exciton fluid flows over ultralong distances (at least 60 µm) at a speed of ~1.8 × 107 m s-1 (~6% the speed of light). The collective phase emerges above a critical laser power, in the absence of free charges and below a critical temperature (usually Tc ≈ 150 K) approaching room temperature in hexagonal-boron-nitride-encapsulated devices. Our theoretical simulations suggest that momentum is conserved and local equilibrium is achieved among excitons; both these features are compatible with a fluid dynamics description of the exciton transport.

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.

Nonlinear polariton parametric emission in an atomically thin semiconductor based microcavity.

Parametric nonlinear optical processes are at the heart of nonlinear optics underpinning the central role in the generation of entangled photons as well as the realization of coherent optical sources. Exciton-polaritons are capable to sustain parametric scattering at extremely low threshold, offering a readily accessible platform to study bosonic fluids. Recently, two-dimensional transition-metal dichalcogenides (TMDs) have attracted great attention in strong light-matter interactions due to robust excitonic transitions and unique spin-valley degrees of freedom. However, further progress is hindered by the lack of realizations of strong nonlinear effects in TMD polaritons. Here, we demonstrate a realization of nonlinear optical parametric polaritons in a WS2 monolayer microcavity pumped at the inflection point and triggered in the ground state. We observed the formation of a phase-matched idler state and nonlinear amplification that preserves the valley population and survives up to room temperature. Our results open a new door towards the realization of the future for all-optical valley polariton nonlinear devices.

All-optical switching based on interacting exciton polaritons in self-assembled perovskite microwires.

Ultrafast all-optical switches and integrated circuits call for giant optical nonlinearity to minimize energy consumption and footprint. Exciton polaritons underpin intrinsic strong nonlinear interactions and high-speed propagation in solids, thus affording an intriguing platform for all-optical devices. However, semiconductors sustaining stable exciton polaritons at room temperature usually exhibit restricted nonlinearity and/or propagation properties. Delocalized and strongly interacting Wannier-Mott excitons in metal halide perovskites highlight their advantages in integrated nonlinear optical devices. Here, we report all-optical switching by using propagating and strongly interacting exciton-polariton fluids in self-assembled CsPbBr3 microwires. Strong polariton-polariton interactions and extended polariton fluids with a propagation length of around 25 µm have been reached. All-optical switching on/off of polariton propagation can be realized in picosecond time scale by locally blue-shifting the dispersion with interacting polaritons. The all-optical switching, together with the scalable self-assembly method, highlights promising applications of solution-processed perovskites toward integrated photonics operating in strong coupling regime.

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.

Managing Growth and Dimensionality of Quasi 2D Perovskite Single-Crystalline Flakes for Tunable Excitons Orientation.

Hybrid perovskites are among the most promising materials for optoelectronic applications. Their 2D crystalline form is even more interesting since the alternating inorganic and organic layers naturally forge a multiple quantum-well structure, leading to the formation of stable excitonic resonances. Nevertheless, a controlled modulation of the quantum well width, which is defined by the number of inorganic layers (n) between two organic ones, is not trivial and represents the main synthetic challenge in the field. Here, a conceptually innovative approach to easily tune n in lead iodide perovskite single-crystalline flakes is presented. The judicious use of potassium iodide is found to modulate the supersaturation levels of the precursors solution without being part of the final products. This allows to obtain a fine tuning of the n value. The excellent optical quality of the as synthesized flakes guarantees an in-depth analysis by Fourier-space microscopy, revealing that the excitons orientation can be manipulated by modifying the number of inorganic layers. Excitonic out-of-plane component, indeed, is enhanced when "n" is increased. The combined advances in the synthesis and optical characterization fill in the picture of the exciton behavior in low-dimensional perovskite, paving the way to the design of materials with improved optoelectronic characteristics.

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.

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.

Evidence for Moiré Trions in Twisted MoSe2 Homobilayers.

Moiré superlattices of van der Waals structures offer a powerful platform for engineering band structure and quantum states. For instance, Moiré superlattices in magic-angle twisted bilayer graphene, ABC trilayer graphene have been shown to harbor correlated insulating and superconducting states, while in transition metal dichalcogenide (TMD) twisted bilayers, Moiré excitons have been identified. Here we show that the effects of a Moiré superlattice on the band structure are general: In TMD twisted bilayers, excitons and exciton complexes can be trapped in the superlattice in a manner analogous to ultracold bosonic or Fermionic atoms in optical lattices. Using twisted MoSe2 homobilayers as a model system, we present evidence for Moiré trions. Our results thus open possibilities for designer van der Waals structures hosting arrays of Fermionic or bosonic quasiparticles, which can be used to realize tunable many-body states crucial for quantum simulation and quantum information processing.

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.

Nonlinear Parametric Scattering of Exciton Polaritons in Perovskite Microcavities.

Comparing with pure photons, higher nonlinearity in polariton systems has been exploited in various proof-of-principle demonstrations of efficient optical devices based on the parametric scattering effect. However, most of them demand cryogenic temperatures limited by the small exciton binding energy of traditional semiconductors or exhibit weak nonlinearity resulting from Frenkel excitons. Lead halide perovskites, possessing both a large binding energy and a strong polariton interaction, emerge as ideal platforms to explore nonlinear polariton physics toward room temperature operation. Here, we report the first observation of nonlinear parametric scattering in a lead halide perovskite microcavity with multiple polariton branches at room temperature. Driven by the scattering source from condensation in one polariton branch, correlated polariton pairs are obtained at high k states in an adjacent branch. Our results strongly advocate the ability to reach the nonlinear regime essential for perovskite polaritonics working at room temperature.

Aging of Self-Assembled Lead Halide Perovskite Nanocrystal Superlattices: Effects on Photoluminescence and Energy Transfer.

Excitonic coupling, electronic coupling, and cooperative interactions in self-assembled lead halide perovskite nanocrystals were reported to give rise to a red-shifted collective emission peak with accelerated dynamics. Here we report that similar spectroscopic features could appear as a result of the nanocrystal reactivity within the self-assembled superlattices. This is demonstrated by studying CsPbBr3 nanocrystal superlattices over time with room-temperature and cryogenic micro-photoluminescence spectroscopy, X-ray diffraction, and electron microscopy. It is shown that a gradual contraction of the superlattices and subsequent coalescence of the nanocrystals occurs over several days of keeping such structures under vacuum. As a result, a narrow, low-energy emission peak is observed at 4 K with a concomitant shortening of the photoluminescence lifetime due to the energy transfer between nanocrystals. When exposed to air, self-assembled CsPbBr3 nanocrystals develop bulk-like CsPbBr3 particles on top of the superlattices. At 4 K, these particles produce a distribution of narrow, low-energy emission peaks with short lifetimes and excitation fluence-dependent, oscillatory decays. Overall, the aging of CsPbBr3 nanocrystal assemblies dramatically alters their emission properties and that should not be overlooked when studying collective optoelectronic phenomena nor confused with superfluorescence effects.

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.

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.

High-speed flow of interacting organic polaritons.

The strong coupling of an excitonic transition with an electromagnetic mode results in composite quasi-particles called exciton polaritons, which have been shown to combine the best properties of their individual components in semiconductor microcavities. However, the physics and applications of polariton flows in organic materials and at room temperature are still unexplored because of the poor photon confinement in such structures. Here, we demonstrate that polaritons formed by the hybridization of organic excitons with a Bloch surface wave are able to propagate for hundreds of microns showing remarkable third-order nonlinear interactions upon high injection density. These findings pave the way for the study of organic nonlinear light-matter fluxes and for a technologically promising route of the realization of dissipation-less on-chip polariton devices operating at room temperature.

Combining label-free and fluorescence operation of Bloch surface wave optical sensors.

We report on the design, fabrication, and characterization of optical sensors based on Bloch surface waves propagating at the truncation edge of one-dimensional photonic crystals. The sensors can be simultaneously operated in both a label-free mode, where small refractive index changes at the surface are detected, and a fluorescence mode, where the fluorescence from a novel heptamethyne dye label in the proximity of the surface is collected. The two modes operate in the near-infrared spectral range with the same configuration of the optical reading apparatus. The limit of detection is shown to be smaller than that of equivalent surface plasmon sensors and the fluorescence collection efficiency is such that it can be efficiently analyzed by the same camera sensor used for label-free operation.