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Mechanical stress produced in nano- and micro-scale structures can enhance materials properties, such as the high mobility of silicon in modern transistors or amplified magnetization dynamics in spintronic devices. Here, we report on the dynamics of coherent acoustic phonons excited by femtosecond light pulses and confined in a single freestanding nickel layer, acting as an acoustic cavity. By combining Fourier transform analysis of the experimental signal and numerical multi-physics simulations, we show that high-frequency (> 10 GHz) longitudinal acoustic pulses can resonate inside the cavity and display lower damping compared to a reference nickel film on SiO2 substrate given that the conditions of total reflection are nearly met in the cavity. Our results provide a thorough understanding of the opto-acoustic response in suspended membranes of magnetic materials, which we foresee can be used to amplify magnetization precession dynamics and to develop magneto-acousto-optical modulators.

Electro-optical modulation is widely employed for optical signal processing and in laser technology. To date, it is efficiently realized in integrated photonic systems as well as in bulk optics devices. Yet, the achievement of modulators exploiting Pockels effect in flat optics, essential to scale down the electric radiation-optical control in free space, currently lag behind bulk and on-chip integrated platforms in terms efficiency and speed. We bridge this gap realizing a metasurface based on lithium niobate (LiNbO3) on insulator that leverages on resonances with quality-factor as high as 8e3 to achieve fast electrical modulation of both linear and nonlinear optical properties. LiNbO3, well known for its high nonlinear susceptibility and wide transparency window across the infrared and visible spectrum, is employed to realize an asymmetric, one-dimensional array of nanowires, exhibiting resonances with linewidth < 0.2 nm. By applying a CMOS-compatible electrical bias, the metasurface imparts a relative reflectivity modulation around 0.1, with a modulation efficiency, defined as relative modulation per applied Volt, larger than 0.01 V^-1 on a bandwidth of about 1 GHz. We also demonstrated more than one order of magnitude intensity modulation of the second harmonic seeded by a continuous-wave laser, with a modulation efficiency of about 0.12 V^-1. This dual modulation capability, rooted in the interplay between optical resonances and electric field manipulation, holds significant potential for cutting-edge applications in high-speed photonics, nonlinear optics, and reconfigurable communication systems. Our findings highlight the transformative potential of LiNbO3-based metasurfaces for integration into next-generation optical technologies that demand rapid, efficient electrical control of light.

Space-time modulation of electromagnetic parameters offers novel exciting possibilities for advanced field manipulations. In this study, we explore wave scattering from a time-varying interface characterized by a Lorentz-type dispersion with a step-like temporal variation in its parameters. Our findings reveal a new process: an unconventional frequency generation at the natural resonances of the system. Remarkably, this phenomenon enables the coupling of propagating waves to evanescent ones, allowing the direct far-field excitation of surface-wave modes without the mediation of spatial gratings or prisms. These results suggest a novel strategy for designing compact and ultra-fast photonic devices, eliminating the necessity for subwavelength spatial structuring or prolonged temporal modulations., Comment: 7 pages; 4 figures; link to SM fixed; DOI added

Epsilon-near-zero materials are exceptional candidates for studying electrodynamics and nonlinear optical processes at the nanoscale. We demonstrate that by alternating a metal and a highly doped conducting-oxide, the epsilon-near-zero regime may be accessed resulting in an anisotropic, composite nanostructure that significantly enhances nonlinear interactions. Using two independent and different computation techniques we show that the structure can enhance the local field intensity by nearly two orders of magnitudes, in large part due to the onset of the effective anisotropy. The investigation of the multilayer nanostructure using a microscopic, hydrodynamic approach also sheds light on the roles of two competing contributions that are for the most part overlooked, but that can significantly modify linear and nonlinear responses of the structure: nonlocal effects, which blueshift the resulting resonance, and the hot electron nonlinearity, which redshifts the plasma frequency as the effective mass of free electrons increases as a function of incident power density. Finally, we show that, even in absence of second order bulk nonlinearity, second order nonlinear processes are also significantly enhanced by the layered structure.

We study electromagnetic pulse propagation in an indium tin oxide nanolayer in the linear and nonlinear regimes. We use the constitutive relations to reconstruct the effective dielectric constant of the medium, and show that nonlocal effects induce additional absorption resonances and anisotropic dielectric response: longitudinal and transverse effective dielectric functions are modulated differently along the propagation direction, and display different epsilon-near-zero crossing points with a discrepancy that increases with increasing intensity. We predict that hot carriers induce a dynamic redshift of the plasma frequency and a corresponding translation of the effective nonlinear dispersion curves that can be used to predict and quantify nonlinear refractive index changes as a function of incident laser peak power density. Our results suggest that large, nonlinear refractive index changes can occur without the need for epsilon-near-zero modes to couple with plasmonic resonators. At sufficiently large laser pulse intensities, we predict the onset of optical bistability, while the presence of additional pump absorption resonances that arise from longitudinal oscillations of the free electron gas give way to corresponding resonances in the second and third harmonic spectra. A realistic propagation model is key to unraveling the basic physical mechanisms that play a fundamental role in the dynamics.

We report that the second and third harmonic signal reductions with insulator film surface coverage over a gold substrate gives a measure of the electron density in the spill out volume of the insulator, which is dubbed metal insulator gap states. For metal-insulator-metal (MIM) structures we observe enhancement saturation and quenching of the third harmonic efficiencies well above the efficiencies for metal-insulator (MI) samples. The measured optical harmonics of scattered light from MI and MIM systems are compared with detailed simulations of the nonlinear interactions including free electron spill out into the insulator, nonlocal and electron quantum tunneling effects. Gold coated substrates are covered with variable thin insulator film thicknesses using atomic layer deposition. Optical harmonics of light scattered from two insulator materials (ZnO and Al2O3) are measured in our experiments. Based on our simulations we conclude that the observed MIM signal enhancement effects are primarily due to nonlocal phenomena in an electron gas., Comment: 12 pages, 6 figures, Supplementary material 12 pages, 10 figures. Submitted for publication in a refereed journal

Optical nonlocalities are elusive and hardly observable in traditional plasmonic materials like noble and alkali metals. Here we report experimental observation of viscoelastic nonlocalities in the infrared optical response of doped cadmium-oxide, epsilon-near-zero nanofilms. The nonlocality is detectable thanks to the low damping rate of conduction electrons and the virtual absence of interband transitions at infrared wavelengths. We describe the motion of conduction electrons using a hydrodynamic model for a viscoelastic fluid, and find excellent agreement with experimental results. The electrons elasticity blue-shifts the infrared plasmonic resonance associated with the main epsilon-near-zero mode, and triggers the onset of higher-order resonances due to the excitation of electron-pressure modes above the bulk plasma frequency. We also provide evidence of the existence of nonlocal damping, i.e., viscosity, in the motion of optically-excited conduction electrons using a combination of spectroscopic ellipsometry data and predictions based on the viscoelastic hydrodynamic model., Comment: 19 pages, 5 figures

We aim to clarify the role that absorption plays in nonlinear optical processes in a variety of metallic nanostructures and show how it relates to emission and conversion efficiency. We define a figure of merit that establishes the structure's ability to either favor or impede second harmonic generation. Our findings suggest that, despite the best efforts embarked upon to enhance local fields and light coupling via plasmon excitation, nearly always the absorbed harmonic energy far surpasses the harmonic energy emitted in the far field. Qualitative and quantitative understanding of absorption processes is crucial in the evaluation of practical designs of plasmonic nanostructures for the purpose of frequency mixing.

We experimentally demonstrate efficient third harmonic generation from an indium tin oxide (ITO) nanofilm (lambda/42 thick) on a glass substrate for a pump wavelength of 1.4 um. A conversion efficiency of 3.3x10^-6 is achieved by exploiting the field enhancement properties of the epsilon-near-zero (ENZ) mode with an enhancement factor of 200. This nanoscale frequency conversion method is applicable to other plasmonic materials and reststrahlen materials in proximity of the longitudinal optical phonon frequencies., Comment: 13 pages, 5 figures

Fano resonances are features in transmissivity/reflectivity/absorption that owe their origin to the interaction between a bright resonance and a dark (i.e., sub-radiant) narrower resonance, and may emerge in the optical properties of planar two-dimensional (2D) periodic arrays (metasurfaces) of plasmonic nanoparticles. In this Letter, we provide a thorough assessment of their nature for the general case of normal and oblique plane wave incidence, highlighting when a Fano resonance is affected by the mutual coupling in an array and its capability to support free modal solutions. We analyze the representative case of a metasurface of plasmonic nanoshells at ultraviolet frequencies and compute its absorption under TE- and TM-polarized, oblique plane-wave incidence. In particular, we find that plasmonic metasurfaces display two distinct types of resonances observable as absorption peaks: one is related to the Mie, dipolar resonance of each nanoparticle; the other is due to the forced excitation of free modes with small attenuation constant, usually found at oblique incidence. The latter is thus an array-induced collective Fano resonance. This realization opens up to manifold flexible designs at optical frequencies mixing individual and collective resonances. We explain the physical origin of such Fano resonances using the modal analysis, which allows to calculate the free modes with complex wavenumber supported by the metasurface. We define equivalent array dipolar polarizabilities that are directly related to the absorption physics at oblique incidence and show a direct dependence between array modal phase and attenuation constant and Fano resonances. We thus provide a more complete picture of Fano resonances that may lead to the design of filters, energy-harvesting devices, photodetectors, and sensors at ultraviolet frequencies., Comment: 6 pages, 5 figures

Our theoretical examination of second and third harmonic generation from metal-based nanostructures predicts that nonlocal and quantum tunneling phenomena can significantly exceed expectations based solely on local, classical electromagnetism. Mindful that the diameter of typical transition metal atoms is approximately 3{\AA}, we adopt a theoretical model that treats nanometer-size features and/or sub-nanometer size gaps or spacers by taking into account: (i) the limits imposed by atomic size to fulfill the requirements of continuum electrodynamics; (ii) spillage of the nearly-free electron cloud into the surrounding vacuum; and (iii) the increased probability of quantum tunneling as objects are placed in close proximity. Our approach also includes the treatment of bound charges, which add crucial, dynamical components to the dielectric constant that are neglected in the conventional hydrodynamic model, especially in the visible and UV ranges, where interband transitions are important. The model attempts to inject into the classical electrodynamic picture a simple, perhaps more realistic description of the metal surface by incorporating a thin patina of free-electrons that screens an internal, polarizable medium., Comment: Submitted to PRA

We present a methodology based on quantum mechanics for assigning quantum conductivity when an ac field is applied across a variable gap between two plasmonic nanoparticles with an insulator sandwiched between them. The quantum tunneling effect is portrayed by a set of quantum conductivity coefficients describing the linear ac conductivity responding at the frequency of the applied field and nonlinear coefficients that modulate the field amplitude at the fundamental frequency and its harmonics. The quantum conductivity, determined with no fit parameters, has both frequency and gap dependence that can be applied to determine the nonlinear quantum effects of strong applied electromagnetic fields even when the system is composed of dissimilar metal nanostructures. Our methodology compares well to results on quantum tunneling effects reported in the literature and it is simple to extend it to a number of systems with different metals and different insulators between them.

We study the formation of second harmonic double-resonance cones in hyperbolic metamaterials. An electric dipole on the surface of the structure induces second harmonic light to propagate into two distinct volume plasmon-polariton channels: A signal that propagates within its own peculiar resonance cone; and a phase-locked signal that is trapped under the pump's resonance cone. Metamaterial dispersion and birefringence induce a large angular divergence between the two volume plasmon-polaritons, making these structures ideal for subwavelength second and higher harmonic imaging microscopy.

We investigate second harmonic generation, low-threshold multistability, all-optical switching, and inherently nonlocal effects due to the free-electron gas pressure in an epsilon-near-zero (ENZ) metamaterial slab made of cylindrical, plasmonic nanoshells illuminated by TM-polarized light. Damping compensation in the ENZ frequency region, achieved by using gain medium inside the shells' dielectric cores, enhances the nonlinear properties. Reflection is inhibited and the electric field component normal to the slab interface is enhanced near the effective pseudo-Brewster angle, where the effective \epsilon-near-zero condition triggers a non-resonant, impedance-matching phenomenon. We show that the slab displays a strong effective, spatial nonlocality associated with leaky modes that are mediated by the compensation of damping. The presence of these leaky modes then induces further spectral and angular conditions where the local fields are enhanced, thus opening new windows of opportunity for the enhancement of nonlinear optical processes.

We investigate local field enhancement phenomena in subwavelength, {\epsilon}-near-zero (ENZ) slabs that do not exploit Fabry-P\'erot resonances. In particular, we study the linear response of engineered metamaterial slabs of finite thickness based on plasmonic nanoshells that show an ENZ band in the visible range, and naturally occurring materials (e.g., SiO2) that also display ENZ properties, under oblique, TM-polarized plane wave incidence. We then introduce active gain material in engineered metamaterial slabs that adds peculiar spectral and angular features to transmission, reflection, and absorption properties, and leads to a further local field enhancement. These findings are supported by two theoretical studies: First, a simple interface between two semi-infinite media, namely free space and a generic ENZ medium; then, an ENZ slab of finite thickness, with the aim of understanding the system's behavior when varying the ENZ properties as well as the incident angle. For either case we report three distinct physical conditions for which we explain spectral and angular features that might result in strong field enhancement. The gain-assisted metamaterial implementation has the potential of triggering and enhancing low-threshold nonlinear phenomena thanks to the large local fields found at specific frequency and angular bands.

We investigate enhanced harmonic generation processes in gain-assisted, near-zero permittivity metamaterials composed of spherical plasmonic nanoshells. We report the presence of narrow-band features in transmission, reflection and absorption induced by the presence of an active material inside the core of the nanoshells. The damping-compensation mechanism used to achieve the near-zero effective permittivity condition also induces a significant increase in field localization and strength and, consequently, enhancement of linear absorption. When only metal nonlinearities are considered, second and third harmonic generation efficiencies obtained by probing the structure in the vicinity of the near-zero permittivity condition approach values as high as for irradiance value as low as . These results clearly demonstrate that a relatively straightforward path now exists to the development of exotic and extreme nonlinear optical phenomena in the KW/cm2 range

We discuss the possibility of implementing a novel bio-sensing platform based on the observation of the shift of the leaky surface plasmon mode that occurs at the edge of the plasmonic band gap of metal gratings when an analyte is deposited on top of the metallic structure. We provide experimental proof of the sensing capabilities of a two-dimensional array of gold nano-patches by observing color variations in the diffracted field when the air overlayer is replaced with a small quantity of Isopropyl Alcohol (IPA). Effects of rounded corners and surface imperfections are also discussed. Finally, we also report proof of changes in color intensities as a function of the air/filling ratio of the structure and discuss their relation with the diffracted spectra.

We study inhibition of absorption, transparency, energy and momentum transport of the inhomogeneous component of harmonic pulses in dielectrics and semiconductors, at visible and UV wavelengths, focusing on materials like GaP. In these spectral regions GaP is characterized by large absorption, metallic behavior or a combination of both. We show that phase locking causes the generated inhomogeneous signals to propagate through a bulk metallic medium without being absorbed, that is occurs even in centrosymmetric materials via the magnetic Lorentz force, and that the transport of energy and momentum is quite peculiar and seemingly anomalous. These results make it clear that there are new opportunities in ultrafast nonlinear optics and nano-plasmonics in new wavelength ranges., Comment: 16 pages, 5 figures, 1 video