Holographic capture of femtosecond pulse propagation

We have implemented a holographic system to study the propagation of femtosecond laser pulses with high temporal (150 fs) and spatial resolutions (4 µm). The phase information in the holograms allows us to reconstruct both positive and negative index changes due to the Kerr nonlinearity (positive) and plasma formation (negative), and to reconstruct three-dimensional structure. Dramatic differences were observed in the interaction of focused femtosecond pulses with air, water, and carbon disulfide. The air becomes ionized in the focal region, while in water long plasma filaments appear before the light reaches a tight focus. In contrast, in carbon disulfide the optical beam breaks up into multiple filaments but no plasma is measured. We explain these different propagation regimes in terms of the different nonlinear material properties

A Dynamical Model of Harmonic Generation in Centrosymmetric Semiconductors

We study second and third harmonic generation in centrosymmetric semiconductors at visible and UV wavelengths in bulk and cavity environments. Second harmonic generation is due to a combination of symmetry breaking, the magnetic portion of the Lorentz force, and quadrupolar contributions that impart peculiar features to the angular dependence of the generated signals, in analogy to what occurs in metals. The material is assumed to have a non-zero, third order nonlinearity that gives rise to most of the third harmonic signal. Using the parameters of bulk Silicon we predict that cavity environments can significantly modify second harmonic generation (390nm) with dramatic improvements for third harmonic generation (266nm). This occurs despite the fact that the harmonics may be tuned to a wavelength range where the dielectric function of the material is negative: a phase locking mechanism binds the pump to the generated signals and inhibits their absorption. These results point the way to novel uses and flexibility of materials like Silicon as nonlinear media in the visible and UV ranges

Resonant, broadband and highly efficient optical frequency conversion in semiconductor nanowire gratings at visible and UV wavelengths

Using a hydrodynamic approach we examine bulk- and surface-induced second and third harmonic generation from semiconductor nanowire gratings having a resonant nonlinearity in the absorption region. We demonstrate resonant, broadband and highly efficient optical frequency conversion: contrary to conventional wisdom, we show that harmonic generation can take full advantage of resonant nonlinearities in a spectral range where nonlinear optical coefficients are boosted well beyond what is achievable in the transparent, long-wavelength, non-resonant regime. Using femtosecond pulses with approximately 500 MW/cm2 peak power density, we predict third harmonic conversion efficiencies of approximately 1% in a silicon nanowire array, at nearly any desired UV or visible wavelength, including the range of negative dielectric constant. We also predict surface second harmonic conversion efficiencies of order 0.01%, depending on the electronic effective mass, bistable behavior of the signals as a result of a reshaped resonance, and the onset fifth order nonlinear effects. These remarkable findings, arising from the combined effects of nonlinear resonance dispersion, field localization, and phase-locking, could significantly extend the operational spectral bandwidth of silicon photonics, and strongly suggest that neither linear absorption nor skin depth should be motivating factors to exclude either semiconductors or metals from the list of useful or practical nonlinear materials in any spectral range.Comment: 12 pages, 4 figure

Third harmonic generation at 223 nm in the metallic regime of GaP

We demonstrate second and third harmonic generation from a GaP substrate 500 μm thick. The second harmonic field is tuned at the absorption resonance at 335 nm, and the third harmonic signal is tuned at 223 nm, in a range where the dielectric function is negative. These results show that a phase locking mechanism that triggers transparency at the harmonic wavelengths persists regardless of the dispersive properties of the medium, and that the fields propagate hundreds of microns without being absorbed even when the harmonics are tuned to portions of the spectrum that display metallic behavior.Peer ReviewedPostprint (published version

Gap solitons in a nonlinear quadratic negative index cavity

By integrating the full Maxwell's equations we predict the existence of gap solitons in a quadratic, Fabry-Perot negative index cavity. An intense, fundamental pump pulse shifts the band structure that forms when magnetic and electric plasma frequencies are different so that a weak, second harmonic pulse initially tuned inside the gap is almost entirely transmitted. The process is due cascading, which occurs far from phase matching conditions, and causes pulse compression. A nonlinear polarization spawns a dark soliton, while a nonlinear magnetization produces a bright soliton

Second and Third Harmonic Generation in Metal-Based Nanostructures

We present a new theoretical approach to the study of second and third harmonic generation from metallic nanostructures and nanocavities filled with a nonlinear material, in the ultrashort pulse regime. We model the metal as a two-component medium, using the hydrodynamic model to describe free electrons, and Lorentz oscillators to account for core electron contributions to both the linear dielectric constant and to harmonic generation. The active nonlinear medium that may fill a metallic nanocavity, or be positioned between metallic layers in a stack, is also modeled using Lorentz oscillators and surface phenomena due to symmetry breaking are taken into account. We study the effects of incident TE- and TM-polarized fields and show that a simple re-examination of the basic equations reveals additional exploitable dynamical features of nonlinear frequency conversion in plasmonic nanostructures.Comment: 33 pages, including 11 figures and 74 references; corrected affiliations and some typo

Graphene-based perfect optical absorbers harnessing guided mode resonances

We numerically and experimentally investigate graphene-based optical absorbers that exploit guided mode resonances (GMRs) achieving 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 and placing it near either a metallic or a dielectric mirror

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 (about 2.3%). Experimental results confirm this behaviour showing CVD graphene absorbance peaks up to about 40% over narrow bands of few nanometers. The simple and flexible design paves the way for the realization of innovative, scalable and easy-to-fabricate graphene-based optical absorbers