Surface Plasmon Excitation of Second Harmonic light: Emission and Absorption

We aim to clarify the role that absorption plays in nonlinear optical processes in a variety of metallic nanostructures and show how it relates to emission and conversion efficiency. We define a figure of merit that establishes the structure's ability to either favor or impede second harmonic generation. Our findings suggest that, despite the best efforts embarked upon to enhance local fields and light coupling via plasmon excitation, nearly always the absorbed harmonic energy far surpasses the harmonic energy emitted in the far field. Qualitative and quantitative understanding of absorption processes is crucial in the evaluation of practical designs of plasmonic nanostructures for the purpose of frequency mixing

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