Harmonic generation from gold nanolayers: bound and hot electron contributions to nonlinear dispersion.

Understanding how light interacts with matter at the nanoscale is pivotal if one is to properly engineer nano-antennas, filters and other devices whose geometrical features approach atomic size. We report experimental results on second and third harmonic generation from 20 nm- and 70 nm-thick gold layers, for TE- and TM-polarized incident light pulses. We discuss the relative roles that bound electrons and an intensity dependent free electron density (hot electrons) play in third harmonic generation. While planar structures are generally the simplest to fabricate, metal layers that are only a few nanometers thick and partially transparent are almost never studied. Yet, transmission offers an additional reference point to compare experimental measurements with theoretical models. Our experimental results are explained well within the context of the microscopic hydrodynamic model that we employ to simulate second and third harmonic conversion efficiencies. Using our experimental observations we estimate ∣χ1064nm(3)∣≈10-18 (m/V)2, triggered mostly by hot electrons.

ENZ materials and anisotropy: enhancing nonlinear optical interactions at the nanoscale.

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 improves nonlinear interactions. The investigation of the multilayer nanostructure reveals the actual role of the anisotropy, showing that high degrees of anisotropy might be necessary to effectively boost nonlinear processes. Moreover, using a microscopic, hydrodynamic approach we shed 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 electrons nonlinearity, which redshifts the plasma frequency as the effective mass of free electrons increases as a function of incident power density and enhances the nonlinear signal by several orders of magnitude. Finally, we show that, even in the absence of second order bulk nonlinearity, second order nonlinear processes are also significantly enhanced by the layered structure.

Self-tuning of second-harmonic generation in GaAs nanowires enabled by nonlinear absorption.

We investigate the effects of nonlinear absorption of the pump beam on second-harmonic generation in GaAs nanowires. Our model includes nonlinear absorption of the pump and allows obtaining a self-consistent solution of the nonlinear Maxwell equations. First, we observe that SHG conversion efficiency can be limited from two-photon absorption and generated free-carriers depending on the pump intensity. Second, we show a method to modulate the SHG response by varying the pump beam intensity. We find that varying the pump intensity from 1 GW/cm2 up to 15 GW/cm2 can red-shift the SH peak wavelength up to 5 nm and modulate the conversion efficiency at a fixed pump wavelength up to 60%. Our results enable new applications of dielectric nanoresonators for nonlinear applications such as harmonic generation, optical switching, and all-optical ultrafast modulation.

Reevaluation of radiation reaction and consequences for light-matter interactions at the nanoscale.

In the context of electromagnetism and nonlinear optical interactions, damping is generally introduced as a phenomenological, viscous term that dissipates energy, proportional to the temporal derivative of the polarization. Here, we follow the radiation reaction method presented in [Phys. Lett. A157, 217 (1991)], which applies to non-relativistic electrons of finite size, to introduce an explicit reaction force in the Newtonian equation of motion, and derive a hydrodynamic equation that offers new insight on the influence of damping in generic plasmas, metal-based and/or dielectric structures. In these settings, we find new damping-dependent linear and nonlinear source terms that suggest the damping coefficient is proportional to the local charge density and nonlocal contributions that stem from the spatial derivative of the magnetic field. We discuss the conditions that could modify both linear and nonlinear electromagnetic responses.

Optically transparent microwave screens based on engineered graphene layers.

We propose an innovative approach for the realization of a microwave absorber fully transparent in the optical regime. This device is based on the Salisbury screen configuration, which consists of a lossless spacer, sandwiched between two graphene sheets whose sheet resistances are different and properly engineered. Experimental results show that it is possible to achieve near-perfect electromagnetic absorption in the microwave X-band. These findings are fully supported by an analytical approach based on an equivalent circuital model. Engineering and integration of graphene sheets could facilitate the realization of innovative microwave absorbers with additional electromagnetic and optical functionalities that could circumvent some of the major limitations of opaque microwave absorbers.

Anomalous nonlinear absorption in epsilon-near-zero materials: optical limiting and all-optical control.

We investigate nonlinear absorption in films of epsilon-near-zero materials. The combination of large local electric fields at the fundamental frequency and material losses at the harmonic frequencies induce unusual intensity-dependent phenomena. We predict that the second-order nonlinearity of a low-damping, epsilon-near-zero slab produces an optical limiting effect that mimics a two-photon absorption process. Anomalous absorption profiles that depend on low permittivity values at the pump frequency are also predicted for third-order nonlinearities. These findings suggest new opportunities for all-optical light control and novel ways to design reconfigurable and tunable nonlinear devices.

Graphene-based perfect optical absorbers harnessing guided mode resonances.

We investigate graphene-based optical absorbers that exploit guided mode resonances (GMRs) attaining theoretically perfect absorption over a bandwidth of few nanometers (over the visible and near-infrared ranges) with a 40-fold increase of the monolayer graphene absorption. We analyze the influence of the geometrical parameters on the absorption rate and the angular response for oblique incidence. Finally, we experimentally verify the theoretical predictions in a one-dimensional, dielectric grating by placing it near either a metallic or a dielectric mirror, thus achieving very good agreement between numerical predictions and experimental results.

Graphene-based absorber exploiting guided mode resonances in one-dimensional gratings.

A one-dimensional dielectric grating, based on a simple geometry, is proposed and investigated to enhance light absorption in a monolayer graphene exploiting guided mode resonances. Numerical findings reveal that the optimized configuration is able to absorb up to 60% of the impinging light at normal incidence for both TE and TM polarizations resulting in a theoretical enhancement factor of about 26 with respect to the monolayer graphene absorption (≈2.3%). Experimental results confirm this behavior showing CVD graphene absorbance peaks up to about 40% over narrow bands of a few nanometers. The simple and flexible design points to a way to realize innovative, scalable and easy-to-fabricate graphene-based optical absorbers.

Nonlinear dynamics in low permittivity media: the impact of losses.

Slabs of materials with near-zero permittivity display enhanced nonlinear processes. We show that field enhancement due to the continuity of the longitudinal component of the displacement field drastically enhances harmonic generation. We investigate the impact of losses with and without bulk nonlinearities and demonstrate that in the latter scenario surface, magnetic and quadrupolar nonlinear sources cannot always be ignored.

Nonlinear control of absorption in one-dimensional photonic crystal with graphene-based defect.

Perfect, narrow-band absorption is achieved in an asymmetric 1D photonic crystal with a monolayer graphene defect. Thanks to the large third-order nonlinearity of graphene and field localization in the defect layer we demonstrate the possibility to achieve controllable, saturable absorption for the pump frequency.

Harmonic generation in metallic, GaAs-filled nanocavities in the enhanced transmission regime at visible and UV wavelengths.

We have conducted a theoretical study of harmonic generation from a silver grating having slits filled with GaAs. By working in the enhanced transmission regime, and by exploiting phase-locking between the pump and its harmonics, we guarantee strong field localization and enhanced harmonic generation under conditions of high absorption at visible and UV wavelengths. Silver is treated using the hydrodynamic model, which includes Coulomb and Lorentz forces, convection, electron gas pressure, plus bulk χ(3) contributions. For GaAs we use nonlinear Lorentz oscillators, with characteristic χ(2) and χ(3) and nonlinear sources that arise from symmetry breaking and Lorentz forces. We find that: (i) electron pressure in the metal contributes to linear and nonlinear processes by shifting/reshaping the band structure; (ii) TE- and TM-polarized harmonics can be generated efficiently; (iii) the χ(2) tensor of GaAs couples TE- and TM-polarized harmonics that create phase-locked pump photons having polarization orthogonal compared to incident pump photons; (iv) Fabry-Perot resonances yield more efficient harmonic generation compared to plasmonic transmission peaks, where most of the light propagates along external metal surfaces with little penetration inside its volume. We predict conversion efficiencies that range from 10(-6) for second harmonic generation to 10(-3) for the third harmonic signal, when pump power is 2 GW/cm2.

All-optical switching at the Fano resonances in subwavelength gratings with very narrow slits.

We theoretically discuss all-optical switching at the Fano resonances of subwavelength gratings made of a chalcogenide glass (As(2)S(3)). Particular attention is devoted to the case in which the grating possesses extremely narrow slits (channels ranging from a∼10 nm to a∼40 nm). The remarkable local field enhancement available in these situations conspires to yield low-threshold switching intensities (~50 MW/cm(2)) at telecommunication wavelengths for extremely thin (d∼200 nm) gratings when a realistic value of the As(2)S(3) cubic nonlinearity is used.

Enhanced second-harmonic generation from resonant GaAs gratings.

We theoretically study second harmonic generation in nonlinear, GaAs gratings. We find large enhancement of conversion efficiency when the pump field excites the guided mode resonances of the grating. Under these circumstances the spectrum near the pump wavelength displays sharp resonances characterized by dramatic enhancements of local fields and favorable conditions for second-harmonic generation, even in regimes of strong linear absorption at the harmonic wavelength. In particular, in a GaAs grating pumped at 1064 nm, we predict second-harmonic conversion efficiencies approximately 5 orders of magnitude larger than conversion rates achievable in either bulk or etalon structures of the same material.

Local treatment with deep percutaneous electrochemotherapy of different tumor lesions: pain relief and objective response results from an observational study.

OBJECTIVE: The aim of this investigation focuses on the evaluation of the efficacy of deep-seated Electrochemotherapy (ECT) in terms of pain relief and local objective response, in pre-treated patients with neither further available pharmacological treatments nor eligible for surgery. PATIENTS AND METHODS: Deep percutaneous ECT has been performed in 20 patients subjected to systemic anaesthesia. Bleomycin was administrated intravenously before the application of the electrical pulses on the target area, employing multiple single needles depending on the size and location of the target tumor. RESULTS: Pain assessment based on Visual Analogue Scale showed significant pain relief one month after treatment in all patients, reducing from 7.5 to 3 as a median value (p-value at Wilcoxon test <0.001). Local symptom-free survival median value was 5.5 months. At the first follow-up (1-2 months), a local disease control rate (LDCR) was observed in 19/20 (95%) patients: complete responses in 2 (10%), partial responses in 8 (40%) and stable disease in 9 (45%). Local progression-free survival median value was 5.7 months. Overall, no major adverse effects were observed. CONCLUSIONS: Our study indicates that deep percutaneous ECT can produce a significant pain reduction and a high LDCR in different tumor lesions, for anatomical site or histotype. In particular, ECT has demonstrated to be effective in various histotypes and deep-seated tumor lesions never treated before by this approach giving a new chance to physicians for reducing oncological pain in patients not eligible to other therapeutic routes. The innovative peculiarity of our study was the successful application of deep percutaneous ECT on adrenal metastasis, malignant pleural mesothelioma, uterine leiomyosarcoma and the uncommon case of a male müllerian tumor.