The spectrophotometric characterization of high efficiency, optically-active samples such as light-emitting organic bulks and thin films can be problematic because their broad-band luminescence is detected together with the monochromatic transmitted
and reflected signals, hence perturbing measurements of optical transmittance and reflectance at wavelengths within the photoexcitation band. As a matter of fact, most commercial spectrophotometers apply spectral filtering before the light beam reaches the sample, not after it. In this Report, we introduce and discuss the method we have developed to correct photometric spectra that are perturbed by photoluminescence.
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 Lorent
z 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.
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 X(3) contributions. For GaAs we use nonlinear Lorentz oscillators, with characteristic X(2) and X(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) TEand TM-polarized harmonics can be generated efficiently; (iii) the X(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 2GW/cm2.
We demonstrate second and third harmonic generation from a GaP substrate 500{mu}m thick. The second harmonic field is tuned at the absorption resonance at 335nm, and the third harmonic signal is tuned at 223nm, in a range where the dielectric functio
n 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.
We numerically demonstrate inhibition of absorption, optical transparency, and anomalous momentum states of phase locked harmonic pulses in semiconductors, at UV and extreme UV frequencies, in spectral regions where the dielectric constant of typical
semiconductors is negative. We show that a generated harmonic signal can propagate through a bulk metallic medium without being absorbed as a result of a phase locking mechanism between the pump and its harmonics. These findings may open new regimes in nonlinear optics and are particularly relevant to the emerging fields of nonlinear negative index meta-materials and nano-plasmonics, especially in the ultrafast pulse regime.
We theoretically investigate second harmonic generation that originates from the nonlinear, magnetic Lorentz force term from single and multiple apertures carved on thick, opaque metal substrates. The linear transmission properties of apertures on me
tal substrates have been previously studied in the context of the extraordinary transmission of light. The transmission process is driven by a number of physical mechanisms, whose characteristics and relative importance depend on the thickness of the metallic substrate, slit size, and slit separation. In this work we show that a combination of cavity effects and surface plasmon generation gives rise to enhanced second harmonic generation in the regime of extraordinary transmittance of the pump field. We have studied both forward and backward second harmonic generation conversion efficiencies as functions of the geometrical parameters, and how they relate to pump transmission efficiency. The resonance phenomenon is evident in the generated second harmonic signal, as conversion efficiency depends on the duration of incident pump pulse, and hence its bandwidth. Our results show that the excitation of tightly confined modes as well as the combination of enhanced transmission and nonlinear processes can lead to several potential new applications such as photo-lithography, scanning microscopy, and high-density optical data storage devices.
We discuss propagation effects in realistic, transparent, metallo-dielectric photonic band gap structures in the context of negative refraction and super-resolution in the visible and near infrared ranges. In the resonance tunneling regime, we find t
hat for transverse-magnetic incident polarization, field localization effects contribute to a waveguiding phenomenon that makes it possible for the light to remain confined within a small fraction of a wavelength, without any transverse boundaries, due to the suppression of diffraction. This effect is related to negative refraction of the Poynting vector inside each metal layer, balanced by normal refraction inside the adjacent dielectric layer: The degree of field localization and material dispersion together determine the total momentum that resides within any given layer, and thus the direction of energy flow. We find that the transport of evanescent wave vectors is mediated by the excitation of quasi-stationary, low group velocity surface waves responsible for relatively large losses. As representative examples we consider transparent metallo-dielectric stacks such as Ag/TiO2 and Ag/GaP and show in detail how to obtain the optimum conditions for high transmittance of both propagating and evanescent modes for super-guiding and super resolution applications across the visible and near IR ranges. Finally, we study the influence of gain on super-resolution. We find that the introduction of gain can compensate the losses caused by the excitation of surface plasmons, improves the resolving characteristics of the lens, and leads to gain-tunable super-resolution.
