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Andrea Toma

Publications and source records attributed to Andrea Toma.

17 recordsLinked to original sources

Efficient photon-pair emission from a nanostructured resonator and its theoretical description

Spontaneous parametric down-conversion (SPDC) in subwavelength nanostructures is a promising source of quantum light, owing to its multifunctionality and ability to generate complex quantum states. Nevertheless, the mechanisms governing photon-pair generation in such systems remain only partially understood. In particular, experimental investigations of key emission properties in individual resonators, such as directionality and spectral distribution, are still lacking, and predictive theoretical frameworks have not yet been experimentally validated. Here, we report the first measurement of the directional and spectral distributions of photon pairs generated via SPDC in a nanostructured resonator. Both distributions exhibit resonant behaviour, which we describe using an extended quasi-normal-mode theory. This comparison is enabled by photon-pair count rates of up to 0.45 Hz/mW -- to our knowledge, the highest reported for a nanostructured resonator. Our results provide new physical insight into nanoscale SPDC and represent an important step toward designing of efficient miniaturized quantum light sources.

quant-ph

Halide Perovskite-Chalcohalide Nanocrystal Heterostructures as a Platform for the Synthesis and Investigation of the CsPbCl3-CsPbI3 Epitaxial Interface

Halide exchange in lead-based halide perovskites has been studied extensively. While mixed Cl-Br or Br-I alloy compositions can be formed with no miscibility gaps, this is precluded for mixed Cl-I compositions, due to the large difference in Cl and I ionic radii. Here, we exploit perovskite-chalcohalide CsPbCl3-Pb4S3Cl2 heterostructures to study the Cl-I exchange and isolate new types of intermediate structures. The epitaxial interface between the Pb4S3Cl2 chalcohalide and the CsPbCl3 perovskite domain significantly influences the intermediate stages of halide exchange in the perovskite domain, leading to coexisting CsPbCl3 and CsPbI3 domains, thereby delivering segmented CsPbI3-CsPbCl3-Pb4S3Cl2 energetically favorable heterostructures, with partial iodide alloying of the CsPbCl3 domain and at the perovskite-chalcohalide interface. The I:CsPbCl3 domain between CsPbI3 and Pb4S3Cl2 enables a gradual lattice expansion across the heterostructure. This design accommodates interfacial strain, with a 5.6% mismatch at the CsPbCl3-CsPbI3 interface and a 3.4% mismatch at the perovskite-chalcohalide interface. Full halide exchange leads to CsPbI3-Pb4S3Cl2 heterostructures. Both in intermediate and fully exchanged heterostructures, the CsPbI3 domain is emissive. In the intermediate structures, the band alignment between the two perovskite domains is type-I, with carriers photogenerated in the CsPbCl3 domain quickly transferring to the CsPbI3 domain, where they can recombine radiatively.

cond-mat.mtrl-sci

Polarization control via artificial optical nonlinearity in dielectric metasurfaces

Nonlinear optical phenomena are generally governed by geometry in matter systems, as they depend on the spatial arrangement of atoms within materials or molecules. Metasurfaces, through precisely designed geometries on a subwavelength scale, allow tailoring the optical response of a material far beyond its natural properties. Therefore, metasurfaces are highly appealing to enable the engineering of nonlinear optical interactions at an unprecedented level. Current studies on nonlinear metasurfaces predominantly focus on the phase control of the generated light. Nonetheless, investigating the tensorial nature of the nonlinearity of metasurfaces and its effect on the polarization of the generated light is critical to fully unlock a range of applications, such as nonlinear vector beam generation and nonlinear polarization imaging. Here, we study the artificial optical nonlinearity of a dielectric metasurface originating from its meta-atom symmetry and describe the third-order nonlinear behavior by considering the polarization degree of freedom. We establish an effective nonlinear medium model that serves as a design toolbox for developing amorphous silicon-based geometric metasurfaces with customizable features in third harmonic generation. We further extract quantitative values of the artificial nonlinear susceptibility tensor elements related to the investigated nonlinear process and geometry. The implemented functional devices demonstrate the versatility of dielectric metasurfaces in shaping the emitted light in terms of amplitude, phase, and polarization, for the precise engineering of novel nonlinear architectures targeting applications in nonlinear imaging and complex light generation.

physics.app-ph

Enhanced vibrational optical activity by near-zero index chiral effective media

The enhancement of the inherently weak optical activity of solvated molecules by superchiral fields, crucial for detecting their chirality, is a research frontier of photonics and the basis of novel chiroptical detection schemes. Here, we show that an effective medium consisting of randomly dispersed metal-based nanoparticles embedded within an optically active solvated drug (aqueous reparixin) can enhance vibrational optical rotation and circular dichroism thanks to superchirality produced by slow light in near-zero index conditions. We evaluate from first principles the effective bianisotropic response of the bulk chiral effective medium, showing that, by adjusting the nanoparticles filling fraction, vibrational optical activity is greatly enhanced by a factor $\simeq 10^2-10^3$ at the near-zero index resonance. Our results are relevant for the development of innovative devices capable of detecting the chirality of low-volume samples, with applications in quantum chemistry and nanomedicine.

physics.optics

Enhanced Terahertz Spectroscopy of a Monolayer Transition Metal Dichalcogenide

Two-dimensional materials, including transition metal dichalcogenides, are attractive for a variety of applications in electronics as well as photonics and have recently been envisioned as an appealing platform for phonon polaritonics. However, their direct characterization in the terahertz spectral region, of interest for retrieving, e.g., their phonon response, represents a major challenge, due to the limited sensitivity of typical terahertz spectroscopic tools and the weak interaction of such long-wavelength radiation with sub-nanometer systems. In this work, by exploiting an ad-hoc engineered metallic surface enabling a ten-thousand-fold local absorption boost, we perform enhanced terahertz spectroscopy of a monolayer transition metal dichalcogenide (tungsten diselenide) and extract its dipole-active phonon resonance features. In addition, we use these data to obtain the monolayer effective permittivity around its phonon resonance. Via the direct terahertz characterization of the phonon response of such two-dimensional systems, this method opens the path to the rational design of phonon polariton devices exploiting monolayer transition metal dichalcogenides.

physics.optics

Plasmon-enhanced circular dichroism spectroscopy of chiral drug solutions

We investigate the potential of surface plasmon polaritons at noble metal interfaces for surface-enhanced chiroptical sensing of dilute chiral drug solutions. The high quality factor of surface plasmon resonances in both Otto and Kretschmann configurations enables the enhancement of circular dichroism differenatial absorption thanks to the large near-field intensity of such plasmonic excitations. Furthermore, the subwavelength confinement of surface plasmon polaritons is key to attain chiroptical sensitivity to small amounts of drug volumes placed around $\simeq 100$ nm by the metal surface. Our calculations focus on reparixin, a pharmaceutical molecule currently used in clinical studies for patients with community-acquired pneumonia, including COVID-19 and acute respiratory distress syndrome. Considering realistic dilute solutions of reparixin dissolved in water with concentration $\leq 5$ mg$/$ml, we find a circular-dichroism differential absorption enhancement factor of the order $\simeq 20$ and chirality-induced polarization distortion upon surface plasmon polariton excitation.

physics.optics

Bound states in the continuum and long-range coupling of polaritons in hexagonal boron nitride nanoresonators

Bound states in the continuum (BICs) garnered significant for their potential to create new types of nanophotonic devices. Most prior demonstrations were based on arrays of dielectric resonators, which cannot be miniaturized beyond the diffraction limit, reducing the applicability of BICs for advanced functions. Here, we demonstrate BICs and quasi-BICs based on high-quality factor phonon-polariton resonances in isotopically pure h11BN and how these states can be supported by periodic arrays of nanoresonators with sizes much smaller than the wavelength. We theoretically illustrate how BICs emerge from the band structure of the arrays and verify both numerically and experimentally the presence of these states and enhanced quality factor. Furthermore, we identify and characterize simultaneously quasi-BICs and bright states. Our method can be generalized to create a large number of optical states and to tune their coupling with the environment, paving the way to miniaturized nanophotonic devices with more advanced functions.

physics.optics

Meta-Optics with Lithium Niobate

The rapid development of metasurfaces - 2D ensembles of engineered nanostructures - is presently fostering a steady drive towards the miniaturization of many optical functionalities and devices to a subwavelength size. The material platforms for optical metasurfaces are rapidly expanding and for the past few years, we are seeing a surge in establishing meta-optical elements from high-index, highly transparent materials with strong nonlinear and electro-optic properties. Crystalline lithium niobate (LN), a prime material of choice in integrated photonics, has shown great promise for future meta-optical components, thanks to its large electro-optical coefficient, second-order nonlinear response and broad transparency window ranging from the visible to the mid-infrared. Recent advances in nanofabrication technology have indeed marked a new milestone in the miniaturization of LN platforms, hence enabling the first demonstrations of LN-based metasurfaces. These seminal works set the first steppingstone towards the realization of ultra-flat monolithic nonlinear light sources with emission ranging from the visible to the infrared, efficient sources of correlated photon pairs, as well as electro-optical devices. Here, we review these recent advances, discussing potential perspectives for applications in light conversion and modulation shaping as well as quantum optics, with a critical eye on the potential setbacks and limitations of this emerging field.

physics.optics

Radially and azimuthally pure vortex beams from phase-amplitude metasurfaces

To exploit the full potential of the transverse spatial structure of light using the Laguerre-Gaussian basis, it is necessary to control the azimuthal and radial components of the photons. Vortex phase elements are commonly used to generate these modes of light, offering precise control over the azimuthal index but neglect the radially dependent amplitude term which defines their associated corresponding transverse profile. Here we experimentally demonstrate the generation of high purity Laguerre-Gaussian beams with a single step on-axis transformation implemented with a dielectric phase-amplitude metasurface. By vectorially structuring the input beam and projecting it onto an orthogonal polarisation basis, we can sculpt any vortex beam in phase and amplitude. We characterize the azimuthal and radial purity of the generated vortex beams, reaching a purity of 98% for a vortex beam with $\ell=50$ and $p=0$. Furthermore, we comparatively show that the purity of the generated vortex beams outperform those generated with other well-established phase-only metasurface approaches. In addition, we highlight the formation of 'ghost' orbital angular momentum orders from azimuthal gratings (analogous to ghost orders in ruled gratings), which have not been widely studied to date. Our work brings higher-order vortex beams and their unlimited potential within reach of wide adoption.

physics.optics

All-optical Reconfiguration of Ultrafast Dichroism in Gold Metasurfaces

Optical metasurfaces have come into the spotlight as a promising platform for light manipulation at the nanoscale, including ultrafast all-optical control via excitation with femtosecond laser pulses. Recently, dichroic metasurfaces have been exploited to modulate the polarization state of light with unprecedented speed. Here, we theoretically predict and experimentally demonstrate by pump-probe spectroscopy the capability to reconfigure the ultrafast dichroic signal of a gold metasurface by simply acting on the polarization of the pump pulse, which is shown to reshape the spatio-temporal distribution of the optical perturbation. The photoinduced anisotropic response, driven by out-of-equilibrium carriers and extinguished in a sub-picosecond temporal window, is readily controlled in intensity by tuning the polarization direction of the excitation up to a full sign reversal. This work proves that nonlinear metasurfaces offer the flexibility to tailor their ultrafast optical response in a fully all-optically reconfigurable platform.

physics.optics

Optical vortex crystals with dynamic topologies

Vortex crystals are geometric arrays of vortices found in various physics fields, owing their regular internal structure to mutual interactions within a spatially confined system. In optics, vortex crystals may form spontaneously within a nonlinear resonator but their usefulness is limited by the lack of control over their topology. On the other hand, programmable devices used in free space, like spatial light modulators, allow the design of nearly arbitrary vortex distributions but without any intrinsic dynamics. By combining non-Hermitian optics with on-demand topological transformations enabled by metasurfaces, we report a solid-state laser that generates vortex crystals with mutual interactions and actively-tunable topologies. We demonstrate 10x10 coherent vortex arrays with nonlocal coupling networks that are not limited to nearest-neighbor coupling but rather dictated by the crystal's topology. The vortex crystals exhibit sharp Bragg diffraction peaks, witnessing their coherence and high topological charge purity, which we resolve spatially over the whole lattice by introducing a parallelized analysis technique. By structuring light at the source, we enable complex transformations that allow to arbitrarily partition the orbital angular momentum inside the cavity and to heal topological charge defects, making these resonators a robust and versatile tool for advanced applications in topological optics.

physics.optics

Nonlinear Hall effect as a local probe of plasmonic magnetic hot spots

Recently developed plasmonic nanostructures are able to generate intense and localized magnetic hot spots in a large spectral range from the terahertz to the visible. However, a direct measurement of the magnetic field at the hot spot has not been performed yet, due to the absence of magnetic field detectors that work at those high frequencies and that fit the hot-spot area. We propose to place a graphene ribbon in the hot spot of a plasmonic nanostructure driven by a laser beam, such that a current is generated due to both the magnetic field at the hot spot and the electric field of the laser. We demonstrate that a nonlinear Hall voltage, which can be measured by standard electrical means, builds up across the ribbon, making it possible to directly probe the magnetic field at the hot spot.

cond-mat.mes-hall

Transient optical symmetry breaking for ultrafast broadband dichroism in plasmonic metasurfaces

Ultrafast nanophotonics is an emerging research field aimed at the development of nanodevices capable of light modulation with unprecedented speed. A promising approach exploits the optical nonlinearity of nanostructured materials (either metallic or dielectric) to modulate their effective permittivity via interaction with intense ultrashort laser pulses. While the ultrafast temporal dynamics of such nanostructures following photoexcitation has been studied in depth, sub-ps transient spatial inhomogeneities taking place at the nanoscale have been so far almost ignored. Here we theoretically predict and experimentally demonstrate that the inhomogeneous space-time distribution of photogenerated hot carriers induces a transient symmetry breaking in a plasmonic metasurface made of highly symmetric metaatoms. The process is fully reversible, and results in a broadband transient dichroic optical response with a recovery of the initial isotropic state in less than 1 picosecond, overcoming the speed bottleneck caused by slower relaxation processes, such as electron-phonon and phonon-phonon scattering. Our results pave the way to the development of ultrafast dichroic devices, capable of Tera bit/s modulation of light polarization.

physics.optics

Photoinduced Temperature Gradients in Sub-wavelength Plasmonic Structures: The Thermoplasmonics of Nanocones

Plasmonic structures are renowned for their capability to efficiently convert light into heat at the nanoscale. However, despite the possibility to generate deep sub-wavelength electromagnetic hot spots, the formation of extremely localized thermal hot spots is an open challenge of research, simply because of the diffusive spread of heat along the whole metallic nanostructure. Here we tackle this challenge by exploiting single gold nanocones. We theoretically show how these structures can indeed realize extremely high temperature gradients within the metal, leading to deep sub-wavelength thermal hot spots, owing to their capability of concentrating light at the apex under resonant conditions even under continuous wave illumination. A three-dimensional Finite Element Method model is employed to study the electromagnetic field in the structure and subsequent thermoplasmonic behaviour, in terms of the three-dimensional temperature distribution. We show how the latter is affected by nanocone size, shape, and composition of the surrounding environment. Finally, we anticipate the use of photoinduced temperature gradients in nanocones for applications in optofluidics and thermoelectrics or for thermally induced nanofabrication.

physics.optics

Fractal-like plasmonic self-similar material with a tailorable plasma frequency in the near-infrared

In this work, we show that modulating the fractal dimension of nanoporous gold allows its effective dielectric response to be tailored over a wide spectral range of infrared wavelengths. In particular, the plasma edge and effective plasma frequency depend linearly on the fractal dimension, which can be controlled by varying the pore and ligament sizes. Importantly, the fractal porous metal exhibits superior plasmonic properties compared to its bulk counterpart. These properties, combined with a longer skin depth on the order of 100-200 nm, enables the penetration of optical energy deep into the nanopores where molecules can be loaded, thus achieving more effective light-matter coupling. These findings may open new pathways to engineering the optical response of fractal-like or self-similar metamaterials without the need for sophisticated lithographic patterning.

cond-mat.mes-hall

Magnetic Control of Transmission and Helicity of Nano-Structured Optical Beams in Magnetoplasmonic Vortex Lenses

We theoretically investigate the generation of far-field propagating optical beams with a desired orbital angular momentum by using an archetypical magnetoplasmonic tip surrounded by a gold spiral slit. The use of a magnetic material can lead to important implications once magneto-optical activity is activated through the application of an external magnetic field. The physical model and the numerical study presented here introduce the concept of magnetically tunable plasmonic vortex lens, namely a magnetoplasmonic vortex lens, which ensures a tunable selectivity in the polarization state of the generated nanostructured beam. The presented system provides a promising platform for a localized excitation of plasmonic vortices followed by their beaming in the far-field with an active modulation of both light's transmittance and helicity.

physics.optics

Emitter Localisation from Reception Timestamps in Asynchronous Networks

We address the problem of localising a mobile terminal ("blind" node) in unknown position from a set of "anchor" nodes in known positions. The proposed method does not require any form of node synchronisation nor measurement (or control) of the transmission times, which is difficult or anyway costly to achieve in practice. It relies exclusively on reception timestamps collected by the anchor nodes, according to their local clocks, that overhear packets transmitted by the blind node and by (at least one) other transmitting node(s) in known position, e.g., other anchors. The clock differences between the nodes are not eliminated ex ante through clock synchronisation, as in traditional ToA and TDoA methods. Instead, they are counteracted ex post, during the data processing stage, leveraging the data redundancy that is intrinsic to the multiple reception of the same packet by different (anchor) nodes. We validate the proposed method in different experimental settings, indoor and outdoor, using exclusively low-cost Commercial-Off-The-Shelf WiFi devices, achieving sub-meter accuracy in full Line-of-Sight conditions and meter-level accuracy in mild Non-line-of-sight environment. The proposed method does not require that the blind node participate actively to the localisation procedure and can use "opportunistically" any legacy signal or packet available over-the-air for communication purposes. Considering the very minimal requirement on the system - basically, only that anchors in known positions are able to collect and share reception timestamps - the proposed approach can enable practical adoption of opportunistic and/or cooperative localisation on top of existing radio communication systems.

cs.NI