Vito Roppo

Second- and third-harmonic generation in metal-based structures

We present a theoretical approach to the study of second- and third-harmonic generation from metallic structures 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 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 reexamination of the basic equations reveals additional, exploitable dynamical features of nonlinear frequency conversion in plasmonic nanostructures.

Čerenkov third-harmonic generation in χ(2) nonlinear photonic crystal

The authors acknowledge the financial supports from Australian Research Council and Israeli Science Foundation Grant No. 774/09.

Inhibition of Linear Absorption in Opaque Materials Using Phase-Locked Harmonic Generation

We theoretically predict and experimentally demonstrate inhibition of linear absorption for phase and group velocity mismatched second- and third-harmonic generation in strongly absorbing materials, GaAs, in particular, at frequencies above the absorption edge. A 100-fs pump pulse tuned to 1300 nm generates 650 and 435 nm second- and third-harmonic pulses that propagate across a 450-microm-thick GaAs substrate without being absorbed. We attribute this to a phase-locking mechanism that causes the pump to trap the harmonics and to impress on them its dispersive properties.

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.

Planar second-harmonic generation with noncollinear pumps in disordered media

We study experimentally the process of the second harmonic generation by two noncollinear beams in quadratic nonlinear crystals with a disordered structure of ferroelectric domains. We show that the second-harmonic radiation is emitted in the form of two cones as well as in a plane representing the cross-correlation of the two fundamental pulses. We demonstrate the implementation of this parametric process for characterisation of femtosecond pulses, enabling the estimation of pulse width, chirp, and front tilt. This is achieved through monitoring the evolution of the autocorrelation trace inside the nonlinear crystal.

Third-harmonic generation via broadband cascading in disordered quadratic nonlinear media

We study parametric frequency conversion in quadratic nonlinear media with disordered ferroelectric domains. We demonstrate that disorder allows realizing broadband third-harmonic generation via cascading of two second-order quasi-phase matched nonlinear processes. We analyze both spatial and polarization properties of the emitted radiation and find the results in agreement with our theoretical predictions.

Role of a localized modulation of χ(2) in Čerenkov second-harmonic generation in nonlinear bulk medium.

We study the second-harmonic generation in quadratic nonlinear media with localized spatial modulation of χ((2)) response. We demonstrate that the emission of Čerenkov second-harmonic takes place only when the fundamental beam illuminates the region of χ((2)) variation. This proves that the sharp modulation of the χ((2)) nonlinearity constitutes a sufficient condition for the emission of Čerenkov second harmonic in bulk materials. Our calculations are in excellent agreement with simple analytical approach utilizing the concept of reciprocal vectors representing the Fourier spectrum of the modulation of χ((2)).

Theoretical study of Čerenkov-type second-harmonic generation in periodically poled ferroelectric crystals

We study theoretically the Cerenkov-type second-harmonic generation by a Gaussian beam in quadratic nonlinear media with periodically reverted ferroelectric domains. In particular, we consider the role of fundamental beam width on the harmonic emission process. We show that varying the beam width of the fundamental wave not only affects the strength of the emitted Cerenkov harmonic signal but also changes the sensitivity of the emission process to wavelength tuning.

Field localization and enhancement of phase-locked second- and third-order harmonic generation in absorbing semiconductor cavities

We predict and experimentally observe the enhancement by three orders of magnitude of phase mismatched second and third harmonic generation in a GaAs cavity at 650 and 433 nm, respectively, well above the absorption edge. Phase locking between the pump and the harmonics changes the effective dispersion of the medium and inhibits absorption. Despite hostile conditions the harmonics resonate inside the cavity and become amplified leading to relatively large conversion efficiencies. Field localization thus plays a pivotal role despite the presence of absorption, and ushers in a new class of semiconductor-based devices in the visible and uv ranges.

The role of ferroelectric domain structure in second harmonic generation in random quadratic media.

We study theoretically and numerically the second harmonic generation in a nonlinear crystal with random distribution of ferroelectric domains. We show that the specific features of disordered domain structure greatly affect the emission pattern of the generated harmonics. This phenomena can be used to characterize the degree of disorder in nonlinear photonic structures.