Spontaneous and Stimulated Raman Scattering near Metal Nanostructures in the Ultrafast, High-Intensity regime

The inclusion of atomic inversion in Raman scattering can significantly alter field dynamics in plasmonic settings. Our calculations show that large local fields and femtosecond pulses combine to yield: (i) population inversion within hot spots; (ii) gain saturation; and (iii) conversion efficiencies characterized by a switch-like transition to the stimulated regime that spans twelve orders of magnitude. While in Raman scattering atomic inversion is usually neglected, we demonstrate that in some circumstances full accounting of the dynamics of the Bloch vector is required

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

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