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Antonio Fieramosca

Publications and source records attributed to Antonio Fieramosca.

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Fully Integrated Perovskite Polaritonic Circuits with Tunable Lasing and Nonlinear Amplification

Photonic integrated circuits are emerging as a key technology for compact and energy-efficient optical information processing. Yet, their practical implementation remains limited by the intrinsically weak optical nonlinearities of conventional materials, which demand high power and large footprints to achieve significant nonlinear responses. Exciton-polaritons, hybrid light-matter excitations of semiconducting materials, offer a promising solution by combining strong optical nonlinearities with the high speed and large scalability typical of photonic devices. However, despite their potential, working on-chip polaritonic elements demonstrating room temperature coherent lasing, controllable nonlinear propagation, or amplification have remained elusive. Here we demonstrate a fully integrated perovskite polaritonic circuit that overcomes these limitations. Using a single-step microfluidic lithographic technique, we realize waveguide circuits with integrated gratings that simultaneously act as couplers and mirrors, forming in-plane Fabry-Pérot cavities. These structures support robust in-plane polariton lasing between gratings, yielding coherent emission along the waveguide. Furthermore, we observe clear signatures of strong nonlinear self-phase modulation and, for the first time, optical amplification of guided polaritons at room temperature. Our simple, scalable platform opens the way to low-power, highly nonlinear optical circuits for integrated photonics and neuromorphic architectures operating at room temperature.

physics.optics

Microfluidic-Assisted Growth of Perovskite Microwires for Room-Temperature All-Optical Switching Based on Total Internal Reflection

The development of efficient integrated photonic circuits is fundamental for ongoing research in information processing and computer science. The greatest challenge in strong light-matter regime facing photonic systems is achieving strong nonlinearities, which are exploitable in strongly coupled systems, leading to the formation of exciton-polaritons. In this context, the use of hybrid organic-inorganic perovskites offers a promising alternative, exhibiting robust interactions at Room Temperature (RT). However, the development of perovskite-based integrated devices requires both the ability to achieve long in-plane propagation, and the development of alternative fabrication approaches tailored to perovskite materials, designed to preserve their optical properties and prevent degradation. Herein, we present the realization of a proof-of-concept all-optical switch using propagating polaritons confined in Total Internal Reflection (TIR), which ensures long in-plane propagation and limited optical losses. We realized an efficient injection/extraction of the TIR-confined waveguide polariton modes by employing gold grating couplers prepatterned on the substrate.

physics.optics

Room temperature spin-layer locking of exciton-polariton nonlinearities

Recent advancements in transition metal dichalcogenides (TMDs) have unveiled exceptional optical and electronic characteristics, opened up new opportunities, and provided a unique platform for exploring light-matter interactions under the strong coupling regime. The exploitation of exciton-polaritons, with their peculiar hybrid light-matter properties, for the development of spintronic customizable devices that enhance both the information capacity and functionality at ambient temperatures is often suggested as a promising route. However, although TMD polaritons have shown promising potential, the microscopic mechanisms leading to nonlinearities in TMD polaritons are complex and their spin-anisotropy, a crucial requirement for many proposed polaritonic devices, has been missing. Here, we demonstrate the absence of spin-anisotropic interaction in a monolayer WS2 microcavity (at room temperature) and show how spin-dependent interactions can be controlled and spin anisotropy recovered by engineering double WS2 layer structures with varied interlayer spacing. We attribute this phenomenon to a distinctive feature in exciton-polariton physics: layer-dependent polariton-phonon coupling. We use theoretical calculations of the phonon electrostatic potentials finding a drastically different coupling strength for single and double monolayer samples and discuss qualitatively how this explains the observed spin-anisotropic response. This is further consistent with experiments on multi WS2 layer samples and the identification of a critical separation distance, above which an effective single monolayer spin-anisotropic response is recovered, both in experiment and theory. Our work lays the groundwork for the development of spin-optronic polaritonic devices at room temperature.

physics.optics

Enhanced polariton interactions in suspended WS2 monolayer microcavity

Transition-metal dichalcogenides monolayers exhibit strong exciton resonances that enable intense light-matter interactions at room temperature (RT). However, the sensitivity of these materials to the surrounding environment and their intense interactions with the sustaining substrate result in the enhancement of excitonic losses through scattering, dissociation and defects formation, hindering their full potential for the excitation of optical nonlinearities in exciton-polariton platforms. From this point of view, the use of suspended monolayers holds the potential to completely eliminate substrate-induced losses, offering unique advantages for the investigation and exploitation of intrinsic electronic, mechanical, and optical properties of 2D materials based polaritonic systems, without any influence of proximity effects of all sort. In this work, we report a novel fabrication approach enabling the realization of a planar λ/2 microcavity filled with a suspended WS2 monolayer in its centre. In such a system, we experimentally demonstrate a 2-fold enhancement of the strong coupling at RT, due to reduced overall losses as compared to similar systems based on dielectric-filled microcavities. Moreover, as a result of minimized losses, spin-dependent polaritonic interactions in our platform are significantly amplified, leading to achievement of a record exciton interaction constant approaching the theoretically predicted value at RT, without making use of theoretical hypothesis on the effective polariton densities. This approach holds promises for pushing 2D materials-based polaritonic systems to their intrinsic limits, paving the way for the realization of novel polaritonic devices with superior performance.

physics.optics

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 CsPbBr3 single crystal provides additional advantages, such as ease of synthesis, cost-effectiveness, and compatibility with existing semiconductor technologies. In this work, we show the formation of whispering gallery modes (WGM) in CsPbBr3 single crystals with controlled geometry, synthesized using a lowcost and efficient capillary bridge method. Through the implementation of microplatelets geometry, we achieve enhanced optical properties and performance thanks to the presence of sharp edges and a uniform surface, effectively avoiding non-radiative scattering losses caused by defects. This allows us 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 our 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.

physics.optics

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 quantised vortices whose density is prescribed by the quantization of circulation. We report on the first experimental study of the Feynman-Onsager relation in a non-equilibrium 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 time scales. 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.

cond-mat.quant-gas

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

Atomically thin transition metal dichalcogenides possess valley dependent functionalities that are usually available only at crogenic temperatures, constrained by various valley depolarization scatterings. The formation of exciton polaritons by coherently superimposing excitons and microcavity photons potentially harnesses the valley polarized polariton polariton interactions for novel valleytronics devices. Robust EPs have been demonstrated at room temperature in TMDs microcavity, however, the coherent polariton lasing and condensation remain elusive. Herein, we demonstrate for the first time the realization of EP condensation in a TMD microcavity at room temperature. The continuous wave pumped EP condensation and lasing with ultralow thresholdsis evidenced by the macroscopic occupation of the ground state, that undergoes a nonlinear increase of the emission and a continuous blueshift, a build up of spatial coherence, and a detuning-controlled threshold. Our work presents a critically important step towards exploiting nonlinear polariton polariton interactions and polaritonic devices with valley functionality at room temperature.

physics.optics

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

Excitonic/electronic coupling and cooperative interactions in self-assembled lead halide perovskite nanocrystals were reported to give rise to a collective low energy 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 using CsPbBr3 nanocrystal superlattices under room temperature and cryogenic micro-photoluminescence spectroscopy. It is shown that keeping such structures under vacuum, a gradual contraction of the superlattices and subsequent coalescence of the nanocrystals occurs over several days. 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, resembling the features of superfluorescence. Overall, the reactivity of CsPbBr3 nanocrystals dramatically alters the emission of their assemblies, which should not be overlooked when studying collective optoelectronic properties nor confused with superfluorescence effects.

physics.app-ph

Observation of two thresholds leading to polariton condensation in 2D hybrid perovskites

Two dimensional (2D) perovskites are promising materials for photonic applications, given their outstanding nonlinear optical properties, ease of fabrication and versatility. In particular, exploiting their high oscillator strength, the crystalline form of 2D perovskites can be used as excitonic medium in optical microcavities, allowing for the study of their optical properties in the strong light-matter coupling regime. While polariton condensation has been observed in different materials at room temperature, here we observe for the first time two distinct threshold processes in a 2D perovskite, a material that has never shown spontaneous phase transition up to now. In particular, we demonstrate lasing from the bi-exciton state which contributes to populate the lower polariton branch and, at higher excitation powers, eventually leads to the formation of a polariton condensate. The emission linewidth narrowing and a spatial coherence over 50 x 50 um2 area are the smoking gun, the formation of a quantum coherent state in 2D hybrid perovskite. Our results not only show the formation of a polariton condensate in 2D perovskites but they are also crucial for the understanding of the physical mechanisms that leads to coherent phase transition in perovskite-based polariton microcavities.

physics.optics

Interaction and coherence of a plasmon-exciton polariton condensate

Polaritons are quasiparticles arising from the strong coupling of electromagnetic waves in cavities and dipolar oscillations in a material medium. In this framework, localized surface plasmon in metallic nanoparticles defining optical nanocavities have attracted increasing interests in the last decade. This interest results from their sub-diffraction mode volume, which offers access to extremely high photonic densities by exploiting strong scattering cross-sections. However, high absorption losses in metals have hindered the observation of collective coherent phenomena, such as condensation. In this work we demonstrate the formation of a non-equilibrium room temperature plasmon-exciton-polariton condensate with a long range spatial coherence, extending a hundred of microns, well over the excitation area, by coupling Frenkel excitons in organic molecules to a multipolar mode in a lattice of plasmonic nanoparticles. Time-resolved experiments evidence the picosecond dynamics of the condensate and a sizeable blueshift, thus measuring for the first time the effect of polariton interactions in plasmonic cavities. Our results pave the way to the observation of room temperature superfluidity and novel nonlinear phenomena in plasmonic systems, challenging the common belief that absorption losses in metals prevent the realization of macroscopic quantum states.

cond-mat.mtrl-sci

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 devices. 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 mirror. Here we demonstrate that monolayer tungsten disulfide ($\text{WS}_2$) can sustain Bloch surface wave polaritons (BSWPs) with a Rabi splitting of 43 meV and propagation constants reaching 33 $μ$m. In addition, we evidence strong polariton-polariton nonlinearities within BSWPs, which manifest themselves as a reversible blueshift of the lower polariton resonance by up to 12.9$\pm$0.5 meV. Such nonlinearities are at the heart of polariton devices 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.

cond-mat.quant-gas

Entangling one polariton with a photon: effect of interactions on a single-polariton quantum state

Polaritons are quasi-particles originating from the coupling of light with matter that demonstrated quantum phenomena at the many-particle mesoscopic level, such as BEC 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 behaviour has remained fully accountable for by classical and mean-field theories. In this Article, we report the first experimental demonstration of a genuinely-quantum manifestation of microcavity polaritons, by swapping, in a two-photon entangled state generated by parametric down-conversion, a photon for a polariton. Furthermore, we show how single polaritons are affected by polariton-polariton interactions in a propaedeutic demonstration of their qualities for quantum information applications.

cond-mat.mes-hall

Room-temperature superfluidity in a polariton condensate

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 only been observed 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 only been demonstrated at liquid helium temperatures. In this case, the limit is not imposed by the mass, but instead by the small exciton binding energy of Wannier-Mott excitons, which places the upper temperature limit. Here we demonstrate a transition from normal to superfluid flow in an organic microcavity supporting stable Frenkel exciton-polaritons at room temperature. This result paves the way not only to table-top studies of quantum hydrodynamics, but also to room-temperature polariton devices that can be robustly protected from scattering.

cond-mat.quant-gas

Ultrafast 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 bare 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 studies of organic nonlinear light-matter fluxes and for a technological promising route of dissipation-less on-chip polariton devices working at room temperature.

physics.optics