Harmonic generation and energy transport in dielectric and semiconductors at visible and UV wavelengths: the case of GaP

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 vide

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

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

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

Enhanced second harmonic generation from resonant GaAs gratings

We 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 1064nm, we predict second harmonic conversion efficiencies approximately five orders of magnitude larger than conversion rates achievable in either bulk or etalon structures of the same material.Comment: 8 page

Dynamical Model of Harmonic Generation in Centrosymmetric Semiconductors at Visible and UV Wavelengths

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 spatial symmetry breaking, the magnetic portion of the Lorentz force, and quadrupolar contributions from inner core electrons. The material is assumed to have a nonzero, third-order nonlinearity that gives rise to most of the third harmonic signal. Using the parameters of bulk silicon we predict that cavity environments modify the dependence of second harmonic generation on incident angle, while improving third harmonic conversion efficiency by several orders of magnitude relative to bulk silicon. This occurs despite the fact that the harmonic signals may be tuned to a wavelength range where the dielectric function of the material is negative: A phase-locking mechanism binds the generated signals to the pump and inhibits their absorption. These results point the way to alternative uses and flexibility of materials such as silicon as nonlinear media in the visible and UV ranges