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Giuseppe Della Valle

Publications and source records attributed to Giuseppe Della Valle.

At least 19 recordsLinked to original sources

Spatiotemporal Metasurface for Ultrafast All-Optical Wavefront Shaping

Optical metasurfaces have established themselves as exceptional nanophotonic platforms to control the properties of light at subwavelength scales. By properly designing the geometry and spatial arrangement of their constituent meta-atoms, engineered phase gradients can be imparted to an incoming field, thereby tailoring its wavefront with a virtually unlimited number of control knobs. However, once fabricated, a metasurface has a permanently fixed optical response. Here, we introduce a strategy for dynamic control, by theoretically predicting and experimentally demonstrating all-optical, reversible, and ultrafast wavefront shaping in a periodic semiconductor nanowire metasurface. A strongly astigmatic femtosecond optical pump pulse is used to photoexcite the resonant metasurface non-uniformly, inducing a transient, spatially inhomogeneous permittivity modulation that reshapes the wavefront of a delayed probe pulse. Ultrafast imaging measurements reveal transient defocusing of the transmitted field at selected probe wavelengths, with a switching time below one picosecond. Quantitative numerical modelling elucidates the defocusing mechanism as arising from the interplay between the unperturbed optical response of the resonant metasurface and the pump-induced spatial permittivity gradient. Our work establishes a fully all-optical and ultrafast route to the dynamic analogue of passive wavefront shaping in gradient metasurfaces, paving the way to all-optically reconfigurable metalenses.

physics.optics↗

Broadband ultrafast self-heterodyned chiro-optical spectroscopy

Ultrafast chiro-optical spectroscopy provides unique access to the structural dynamics of molecules, spin-valley relaxation in semiconductors, and the non-equilibrium optical response of chiral nanophotonic systems. Yet, because chiral signals are intrinsically weak and time-resolved spectroscopy probes small photoinduced changes, transient chiro-optical responses are often difficult to isolate from parasitic achiral contributions. Here, we introduce a broadband ultrafast chiro-optical spectroscopy technique that integrates a birefringent common-path interferometer with an optical polarization bridge to sensitively detect photoinduced changes in the polarization state of light. Phase-sensitive self-heterodyned detection enables simultaneous measurement of transient circular dichroism and optical rotatory dispersion across a broad spectral range with ultrafast temporal resolution. Balanced detection suppresses excess laser noise, enabling exceptional sensitivity (<50 $μ$deg) close to shot-noise limit. We demonstrate this approach on an array of gold nano-helicoids, supported by a full-wave time-resolved model of the spatiotemporal dynamics of plasmonic non-equilibrium carriers and their associated optical nonlinearities. The model traces the system's transient chiro-optical response back to photoinduced modulations of the electric-magnetic dipole interaction in the nano-helicoid, elucidating the connection of near- and far-field dynamics in the non-equilibrium regime. We further investigate spin excitation, thermalization, and relaxation in a lead halide perovskite, establishing a novel approach to broadband time-resolved Faraday rotation. The simplicity, sensitivity, and wide applicability of this detection scheme provide a powerful platform for broadband ultrafast chiro-optical spectroscopy, opening new opportunities in biochemistry, solid-state physics, and nanophotonics.

physics.optics↗

Excitation of surface plasmon-polaritons through optically-induced ultrafast transient gratings

Ultrafast excitation of non-equilibrium carriers under intense pulses offer unique opportunities for controlling optical properties of semiconductor materials. In this work, we propose a scheme for ultrafast generation of surface plasmon polaritons (SPPs) via a transient metagrating formed under two interfering optical pump pulses in the semiconductor GaAs thin film. The grating can be formed due to modulation of the refractive index associated with the non-equilibrium carriers generation. The formed temporal grating structure enables generation of SPP waves at GaAs/Ag interface via weak probe pulse excitation. We propose a theoretical model describing non-equilibrium carriers formation and diffusion and their contribution to permittivity modulation via Drude and band-filling mechanisms. We predict that by tuning the parameters of the pump and probe one can reach critical coupling regime and achieve efficient generation of SPP at the times scales of 0.1-1 ps.

physics.optics↗

Visualizing hot carrier dynamics by nonlinear optical microscopy at the atomic length scale

Probing and manipulating the spatiotemporal dynamics of hot carriers in nanoscale metals is crucial to a plethora of applications ranging from nonlinear nanophotonics to single molecule photochemistry. The direct investigation of these highly non-equilibrium carriers requires the experimental capability of high energy resolution (~ meV) broadband femtosecond spectroscopy. When considering the ultimate limits of atomic scale structures, this capability has remained out of reach until date. Using a two color femtosecond pump-probe spectroscopy, we present here the real-time tracking of hot carrier dynamics in a well-defined plasmonic picocavity, formed in the tunnel junction of a scanning tunneling microscope (STM). The excitation of hot carriers in the picocavity enables ultrafast all optical control over the broadband (~ eV) anti Stokes electronic resonance Raman scattering (ERRS) and the four-wave mixing (FWM) signals generated at the atomic length scale. By mapping the ERRS and FWM signals from a single graphene nanoribbon (GNR), we demonstrate that both signals are more efficiently generated along the edges of the GNR: a manifestation of atomic-scale nonlinear optical microscopy. This demonstration paves the way to the development of novel ultrafast nonlinear picophotonic platforms, affording unique opportunities in a variety of contexts, from the direct investigation of non equilibrium light matter interactions in complex quantum materials, to the development of robust strategies for hot carriers harvesting in single molecules and the next generation of active metasurfaces with deep-sub-wavelength meta-atoms.

physics.optics↗

Directional coupling to a $λ/5000$ nano-waveguide

Silicon-based micro-devices are considered promising candidates for consolidating several terahertz technologies into a common and practical platform. The practicality stems from the relatively low loss, device compactness, ease of fabrication, and wide range of available passive and active functionalities. Nevertheless, typical device footprints are limited by diffraction to several hundreds of micrometers, which hinders emerging nanoscale applications of terahertz frequencies. While metallic gap modes provide nanoscale terahertz confinement, efficiently coupling to them is difficult. Here we present and experimentally demonstrate a strategy for efficiently interfacing sub-terahertz radiation (λ=1 mm) to a waveguide formed by a nanogap, etched in a gold film, that is 200 nm (λ/5000) wide and up to 4.5 mm long. The design principle relies on phase matching dielectric and nanogap waveguide modes, resulting in efficient directional coupling between them when placed side-by-side. Broadband far field terahertz transmission experiments through the dielectric waveguide reveal a transmission dip near the designed wavelength due to resonant coupling. Near field measurements on the surface of the gold layer confirm that such a dip is accompanied by a transfer of power to the nanogap, with an estimated coupling efficiency of ~10%. Our approach provides a pathway for efficiently interfacing millimeter-wave and near-infrared photonic circuits, providing controlled and tailored nanoscale terahertz confinement, with important implications for on-chip nanospectroscopy, telecommunications, and quantum technologies.

physics.optics↗

Resonant Fully dielectric metasurfaces for ultrafast Terahertz pulse generation

Metasurfaces represent a new frontier in materials science paving for unprecedented methods of controlling electromagnetic waves, with a range of applications spanning from sensing to imaging and communications. For pulsed terahertz generation, metasurfaces offer a gateway to tuneable thin emitters that can be utilised for large-area imaging, microscopy and spectroscopy. In literature THz-emitting metasurfaces generally exhibit high absorption, being based either on metals or on semiconductors excited in highly resonant regimes. Here we propose the use of a fully dielectric semiconductor exploiting morphology-mediated resonances and inherent quadratic nonlinear response. Our system exhibits a remarkable 40-fold efficiency enhancement compared to the unpatterned at the peak of the optimised wavelength range, demonstrating its potential as scalable emitter design.

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↗

Quantitative Ultrafast Electron-Temperature Dynamics in Photo-Excited Au Nanoparticles

The femtosecond evolution of the electronic temperature of laser-excited gold nanoparticles is measured, by means of ultrafast time-resolved photoemission spectroscopy induced by extreme-ultraviolet radiation pulses. The temperature of the electron gas is deduced by recording and fitting high-resolution photo emission spectra around the Fermi edge of gold nanoparticles providing a direct, unambiguous picture of the ultrafast electron-gas dynamics. These results will be instrumental to the refinement of existing models of femtosecond processes in laterally-confined and bulk condensed-matter systems, and for understanding more deeply the role of hot electrons in technological applications.

cond-mat.mtrl-sci↗

Enhanced generation of non-degenerate photon-pairs in nonlinear metasurfaces

We reveal a novel regime of photon-pair generation driven by the interplay of multiple bound states in the continuum resonances in nonlinear metasurfaces. This non-degenerate photon-pair generation is derived from the hyperbolic topology of the transverse phase-matching and can enable orders-of-magnitude enhancement of the photon rate and spectral brightness, as compared to the degenerate regime. We show that the entanglement of the photon-pairs can be tuned by varying the pump polarization, which can underpin future advances and applications of ultra-compact quantum light sources.

physics.optics↗

Thermometric Calibration of the Ultrafast Relaxation Dynamics in Plasmonic Au Nanoparticles

The excitation of plasmonic nanoparticles by ultrashort laser pulses sets in motion a complex ultrafast relaxation process involving the gradual re-equilibration of the system's electron gas, lattice and environment. One of the major hurdles in studying these processes is the lack of direct measurements of the dynamic temperature evolution of the system subcomponents. We measured the dynamic optical response of ensembles of plasmonic Au nanoparticles following ultrashort-pulse excitation and we compared it with the corresponding static optical response as a function of the increasing temperature of the thermodynamic bath. Evaluating the two sets of data, the optical fingerprints of equilibrium or off-equilibrium responses could be clearly identified, allowing us to extract a dynamic thermometric calibration scale of the relaxation process, yielding the experimental ultrafast temperature evolution of the plasmonic particles as a function of time.

physics.optics↗

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↗

Color Routing via Cross-Polarized Detuned Plasmonic Nanoantennas in Large Area Metasurfaces

Bidirectional nanoantennas are of key relevance for advanced functionalities to be implemented at the nanoscale, and in particular for color routing in an ultracompact flat-optics configuration. Here we demonstrate a novel approach avoiding complex collective geometries and/or restrictive morphological parameters, based on cross-polarized detuned plasmonic nanoantennas in a uniaxial (quasi-1D) bimetallic configuration. The nanofabrication of such a flat-optics system is controlled over a large-area (cm^2) by a novel self-organized technique exploiting ion-induced nanoscale wrinkling instability on glass templates to engineer tilted bimetallic nanostrip dimers. These nanoantennas feature broadband color routing with superior light scattering directivity figures, which are well described by numerical simulations and turn out to be competitive with the response of lithographic nanoantennas. These results demonstrate that our large-area self-organized metasurfaces can be implemented in real world applications of flat optics color routing from telecom photonics to optical nanosensing.

physics.optics↗

One-dimensional disordered photonic structures with two or more materials

Here we would like to discuss the light transmission modulation by periodic and disordered one dimensional (1D) photonic structures. In particular, we will present some theoretical and experimental findings highlighting the peculiar optical properties of: i) 1D periodic and disordered photonic structures made with two or more materials; ii) 1D photonic structures in which the homogeneity or the aggregation of the high refractive index layers is controlled. We will focus also on the fabrication aspects of these structures.

physics.optics↗

Nonlinear anisotropic dielectric metasurfaces for ultrafast nanophotonics

We report on the broadband transient optical response from anisotropic nanobrick amorphous silicon particles, exhibiting Mie-type resonances. A quantitative model is developed to identify and disentangle the three physical processes that govern the ultrafast changes of the nanobrick optical properties, namely two-photon absorption, free-carrier relaxation, and lattice heating. We reveal a set of operating windows where ultrafast all-optical modulation of transmission is achieved with full return to zero in 20 ps. This is made possible due to the interplay between the competing nonlinear processes and despite the slow (nanosecond) internal lattice dynamics. The observed ultrafast switching behavior can be independently engineered for both or- thogonal polarizations using the large anisotropy of nanobricks thus allowing ultrafast anisotropy control. Our results categorically ascertain the potential of all-dielectric resonant nanophotonics as a platform for ultrafast optical devices, and reveal the pos- sibility for ultrafast polarization-multiplexed displays and polarization rotators.

physics.optics↗

Shortcut to adiabaticity in full-wave optics for ultra-compact waveguide junctions

We extend the concept of shortcut to adiabaticity to full-wave optics and provide application to the design of an ultra-compact waveguide junction. In particular, we introduce a procedure allowing one to synthesize a purely dielectric optical potential that precisely compensates for the non-adiabatic losses of the transverse-electric fundamental mode in any (sufficiently regular) two-dimensional waveguide junction. Our results are corroborated by finite-element method numerical simulations in a Poschl-Teller waveguide mode expander.

physics.optics↗

Non-Hermitian transparency and one-way transport in low-dimensional lattices by an imaginary gauge field

Unidirectional and robust transport is generally observed at the edge of two- or three-dimensional quantum Hall and topological insulator systems. A hallmark of these systems is topological protection, i.e. the existence of propagative edge states that cannot be scattered by imperfections or disorder in the system. A different and less explored form of robust transport arises in non-Hermitian systems in the presence of an {\it imaginary} gauge field. As compared to topologically-protected transport in quantum Hall and topological insulator systems, robust non-Hermitian transport can be observed in {\it lower} dimensional (i.e. one dimensional) systems. In this work the transport properties of one-dimensional tight-binding lattices with an imaginary gauge field are theoretically investigated, and the physical mechanism underlying robust one-way transport is highlighted. Back scattering is here forbidden because reflected waves are evanescent rather than propagative. Remarkably, the spectral transmission of the non-Hermitian lattice is shown to be mapped into the one of the corresponding Hermitian lattice, i.e. without the gauge field, {\it but} computed in the complex plane. In particular, at large values of the gauge field the spectral transmittance becomes equal to one, even in the presence of disorder or lattice imperfections. This phenomenon can be referred to as {\it one-way non-Hermitian transparency}. Robust one-way transport can be also realized in a more realistic setting, namely in heterostructure systems, in which a non-Hermitian disordered lattice is embedded between two homogeneous Hermitian lattices. Such a double heterostructure realizes asymmetric (non-reciprocal) wave transmission. A physical implementation of non-Hermtian transparency, based on light transport in a chain of optical microring resonators, is suggested.

cond-mat.mes-hall↗

Robust light transport in non-Hermitian photonic lattices

Combating the effects of disorder on light transport in micro- and nano-integrated photonic devices is of major importance from both fundamental and applied viewpoints. In ordinary waveguides, imperfections and disorder cause unwanted back-reflections, which hinder large-scale optical integration. Topological photonic structures, a new class of optical systems inspired by quantum Hall effect and topological insulators, can realize robust transport via topologically-protected unidirectional edge modes. Such waveguides are realized by the introduction of synthetic gauge fields for photons in a two-dimensional structure, which break time reversal symmetry and enable one-way guiding at the edge of the medium. Here we suggest a different route toward robust transport of light in lower-dimensional (1D) photonic lattices, in which time reversal symmetry is broken because of the {\it non-Hermitian} nature of transport. While a forward propagating mode in the lattice is amplified, the corresponding backward propagating mode is damped, thus resulting in an asymmetric transport that is rather insensitive to disorder or imperfections in the structure. Non-Hermitian transport in two lattice models is considered: a tight-binding lattice with an imaginary gauge field (Hatano-Nelson model), and a non-Hermitian driven binary lattice. In the former case transport in spite of disorder is ensured by a mobility edge that arises because of a non-Hermitian delocalization transition. The possibility to observe non-Hermitian delocalization induced by a synthetic 'imaginary' gauge field is suggested using an engineered coupled-resonator optical waveguide (CROW) structure.

physics.optics↗