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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.

Heavy pnictogen chalcohalide semiconductors are coming under the spotlight for energy conversion applications. Here we present the colloidal synthesis of phase pure AgBiSCl2nanocrystals. This quaternary chalcohalide compound features a quasi-two-dimensional crystal structure and a direct band gap, in contrast with the monodimensional structure and the indirect band gap peculiar to the orthorhombic, ternary Bi chalcohalides. Consistently, colloidal AgBiSCl2nanocrystals exhibit photoinduced luminescence compatible with both band edge excitons and midgap states. This is the first observation of band edge emission in chalcohalide nanomaterials at large, although exciton recombination in our AgBiSCl2nanocrystals mostly occurs via nonradiative pathways. This work further advances our knowledge on this class of mixed anion semiconductor nanomaterials and provides a contribution to establishing chalcohalides as a reliable alternative to metal chalcogenides and halides.

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 MoS2semiconductor whose propagation resembles that of a classical liquid as suggested by the nearly uniform photoluminescence through the MoS2monolayer regardless of crystallographic defects and geometric constraints. The exciton fluid flows over ultralong distances (at least 60 μm) at a speed of ~1.8 × 107m 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.

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 WS2monolayer 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.

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.

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 MoSe2homobilayers 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.

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 kstates in an adjacent branch. Our results strongly advocate the ability to reach the nonlinear regime essential for perovskite polaritonics working at room temperature.

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 CsPbBr3nanocrystal 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 CsPbBr3nanocrystals develop bulk-like CsPbBr3particles 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 CsPbBr3nanocrystal assemblies dramatically alters their emission properties and that should not be overlooked when studying collective optoelectronic phenomena nor confused with superfluorescence effects.

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.

Photonic crystal enhanced fluorescence biosensors have been proposed as a novel immunodiagnostic tool, due to the increased fluorescence excitation rates and angular redistribution of the emission. Among these, purely dielectric one-dimensional photonic crystals (1DPC) sustaining Bloch surface waves (BSW) at their truncation edge have recently attracted much interest. We report for the first time on the time-resolved experimental study of the effects of excess reabsorption of the BSW coupled fluorescence in the near-infrared range around 800 nm. Temporally and angularly resolved measurements of the BSW coupled fluorescence emission permit putting into evidence a strong reabsorption of the fluorescence emission when using highly resonant 1DPC. The results suggest that, when designing 1DPC sustaining BSW for quantitative diagnostic assays, it is necessary to choose a compromise quality factor, to exploit the features arising from the electromagnetic field enhancement while avoiding reabsorption.

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 devices5–11and 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. Hybrid light–matter states at the surface of a 2D material can interact strongly and propagate over macroscopic distances.

Superfluidity—the suppression of scattering in a quantum fluid at velocities below a critical value—is one of the most striking manifestations of the collective behaviour typical of Bose–Einstein condensates. This phenomenon, akin to superconductivity in metals, has until now been observed only at prohibitively low cryogenic temperatures. For atoms, this limit is imposed by the small thermal de Broglie wavelength, which is inversely related to the particle mass. Even in the case of ultralight quasiparticles such as exciton-polaritons, superfluidity has been demonstrated only at liquid helium temperatures. In this case, the limit is not imposed by the mass, but instead by the small binding energy of Wannier–Mott excitons, which sets the upper temperature limit. Here we demonstrate a transition from supersonic to superfluid flow in a polariton condensate under ambient conditions. This is achieved by using an organic microcavity supporting stable Frenkel exciton-polaritons at room temperature. This result paves the way not only for tabletop studies of quantum hydrodynamics, but also for room-temperature polariton devices that can be robustly protected from scattering.

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.

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.