Searcharxiv⌕ Search

arXiv subjects

Daniele Sanvitto

Publications and source records attributed to Daniele Sanvitto.

At least 55 records · Page 3Linked to original sources

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↗

Tuning the Berry curvature in 2D Perovskite

Topological physics and in particular its connection with artificial gauge fields is a forefront topic in different physical systems, ranging from cold atoms to photonics and more recently semiconductor dressed exciton-photon states, called polaritons. Engineering the energy dispersion of polaritons in microcavities through nanofabrication or exploiting the intrinsic material and cavity anisotropies has demonstrated many intriguing effects related to topology and emergent gauge fields. Here, we show that we can control the Berry curvature distribution of polariton bands in a strongly coupled organic-inorganic 2D perovskite single crystal. The spatial anisotropy of the perovskite crystal combined with photonic spin-orbit coupling make emerge two Hamilton's diabolical points in the dispersion. The application of an external magnetic field breaks time reversal symmetry thanks to the exciton Zeeman splitting. It splits the diabolical points degeneracy. The resulting bands show non-zero integral Berry curvature which we directly measure by state tomography. Crucially, we show that we can control the Berry curvature distribution in the band, the so-called band geometry, within the same microcavity.

physics.optics↗

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↗

Directional Goldstone waves in polariton condensates close to equilibrium

Quantum fluids of light are realized in semiconductor microcavities by 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 show that excitations are created with a definite direction with respect to the condensate, analogous to how a sea breeze develops surface waves aligned with the wind. These results reveal the effect of asymmetric pumping on the collective excitations of a condensate. Furthermore, we measure the critical sound speed for polariton superfluids close to equilibrium.

cond-mat.quant-gas↗

Self-starting nonlinear mode-locking in random lasers

In ultra-fast multi-mode lasers, mode-locking is implemented by means of ad hoc devices, like saturable absorbers or modulators, allowing for very short pulses. This comes about because of nonlinear interactions induced among modes at different, well equispaced, frequencies. Theory predicts that the same locking of modes would occur in random lasers but, in absence of any device, its detection is unfeasible so far. Because of the general interest in the phenomenology and understanding of random lasers and, moreover, because it is a first example of self-starting mode-locking we devise and test a way to measure such peculiar non-linear coupling. Through a detailed analysis of multi-mode correlations we provide clear evidence for the occurrence of nonlinear mode-coupling in the cavity-less random laser made of a powder of GaAs crystals and its self-starting mode-locking nature. The behavior of multi-point correlations among intensity peaks is tested against the nonlinear frequency matching condition equivalent to the one underlying phase-locking in ordered ultrafast lasers. Non-trivially large multi-point correlations are clearly observed for spatially overlapping resonances and turn out to sensitively depend on the frequency matching being satisfied, eventually demonstrating the occurrence of non-linear mode-locked mode-coupling.

physics.optics↗

Josephson vortices in a long Josephson junction formed by phase twist in a polariton superfluid

Quantum fluids of light are an emerging platform for energy efficient signal processing, ultra-sensitive interferometry and quantum simulators at elevated temperatures. Here we demonstrate the optical control of the topological excitations induced in a large polariton condensate, realising the bosonic analog of a long Josephson junction and reporting the first observation of bosonic Josephson vortices. When a phase difference is imposed at the boundaries of the condensate, two extended regions become separated by a sharp $π$-slippage of the phase and a solitonic depletion of the density, forming an insulating barrier with a suppressed order parameter. The superfluid behavior, that is a smooth phase gradient across the system instead of the sharp phase jump, is recovered at higher polariton densities and it is mediated by the nucleation of Josephson vortices within the barrier. Our results contribute to the understanding of dissipation and stability of elementary excitations in macroscopic quantum systems.

cond-mat.quant-gas↗

Magnetic control of polariton spin transport

We show the full control of the polarization dynamics of a propagating exciton-polariton condensate in a planar microcavity by using a magnetic field applied in the Voigt geometry. The change of the spin-beat frequency, the suppression of the optical spin Hall effect and the rotation of the polarization pattern by the magnetic field are theoretically reproduced by accounting for the magneto-induced mixing of exciton-polariton and dark, spin forbidden, exciton states.

cond-mat.quant-gas↗

Self-trapping of exciton-polariton condensates

The self-trapping of exciton-polariton condensates is demonstrated and explained by the formation of a new polaron-like state. Above the polariton lasing threshold, local variation of the lattice temperature provides the mechanism for an attractive interaction between polaritons. Due to 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 strike contrast to the conventional single-particle polaron state.

cond-mat.quant-gas↗

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.

cond-mat.quant-gas↗

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↗

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.

cond-mat.quant-gas↗

Topological order and equilibrium in a condensate of exciton-polaritons

We report the observation of the Berezinskii-Kosterlitz-Thouless transition for a 2D gas of exciton-polaritons, and through the joint measurement of the first-order coherence both in space and time we bring compelling evidence of a thermodynamic equilibrium phase transition in an otherwise open driven/dissipative system. This is made possible thanks to long polariton lifetimes in high-quality samples with small disorder and in a reservoir-free region far away from the excitation spot, that allow topological ordering to prevail. The observed quasi-ordered phase, characteristic for an equilibrium 2D 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. Finally, measurements in the weak-coupling regime confirm that polariton condensates are fundamentally different from photon lasers and constitute genuine quantum degenerate macroscopic states.

cond-mat.quant-gas↗

Visible quantum plasmonics from metallic nanodimers

We report theoretical evidence that bulk nonlinear materials weakly interacting with highly localized plasmonic modes in ultra-sub-wavelength metallic nanostructures can lead to nonlinear effects at the single plasmon level in the visible range. In particular, the two-plasmon interaction energy in such systems is numerically estimated to be comparable with the typical plasmon linewidths. Localized surface plasmons are thus predicted to exhibit a purely nonclassical behavior, which can be clearly identified by a sub-Poissonian second-order correlation in the signal scattered from the quantized plasmonic field under coherent electromagnetic excitation. We explicitly show that systems sensitive to single-plasmon scattering can be experimentally realized by combining electromagnetic confinement in the interstitial region of gold nanodimers with local infiltration or deposition of ordinary nonlinear materials. We also propose configurations that could allow to realistically detect such an effect with state-of-the-art technology, overcoming the limitations imposed by the short plasmonic lifetime.

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↗

Merging of vortices and antivortices in polariton superfluids

Quantised vortices are remarkable manifestations on a macroscopic scale of the coherent nature of quantum fluids, and the study of their properties is of fundamental importance for the understanding of this peculiar state of matter. Cavity-polaritons, due to their double light-matter nature, offer a unique controllable environment to investigate these properties. In this work we theoretically investigate the possibility to deterministically achieve the annihilation of a vortex with an antivortex through the increase of the polariton density in the region surrounding the vortices. Moreover we demonstrate that by means of this mechanism an array of vortex-antivortex pairs can be completely washed out.

cond-mat.other↗