CARS-background suppression by phase-controlled nonlinear interferometry.

We have developed a new technique for efficient suppression of the nonresonant background in coherent anti-Stokes Raman scattering (CARS). The advantage of this technique, which is based upon phase-controlled superposition of an appropriately selected reference signal, is presented in theory and demonstrated experimentally by the example of the S(3) (pure rotational) transition of molecular hydrogen

Second harmonic generation in planar optical waveguides.

We study optical second harmonic generation (SHG) in planar waveguide structures composed of several layers with different dielectric constants. We develop a general formalism for the calculation of mode generation by a planar antenna embedded in the waveguide. As an application we consider a monolayer of high second-order susceptibility adsorbed at the interface between two layers of the waveguide structure. Periodic modulation of the nonlinear susceptibility allows phase matching leading to dramatically enhanced second harmonic intensities. We investigate the SHG-efficiency of various experimentally realizable geometries

Anisotropic second-order nonlinearities of organic monolayers.

Monolayers prepared from hemicyanine chromophores of high second-order nonlinearity (β=1.3×10−26 esu at resonance) have been used to study anisotropies of the concomitant χ(2)-susceptibility tensor. All components of this third-rank tensor have been determined by Fourier analysis of the anisotropic coverage density Ns(φ) with respect to the angle of rotation about surface normal. Depending on the preparation both Cs and C2v symmetry could be identified

Symmetry superposition studied by surface second-harmonic generation.

The components of a third-rank χ(2) tensor have been split into contributions due to 1-fold, 2-fold, 3-fold, and ∞-fold or isotropic rotation axes for a surface of Cs symmetry. Theoretical analysis of the rotation patterns obtained by the surface second-harmonic (SH) generation indicates that a complete symmetry analysis cannot be performed without knowledge of the relevant distribution functions. Rotation axes of lower symmetry create via ‘‘overtones’’ or ‘‘harmonics’’ contributions apparent in the analysis of the rotation axes of higher symmetry. An experimental example is the observation of structural changes of Au(111) surfaces in an aqueous electrolytic environment. Potential-dependent buildup and removal of a Au(111)-(1×23) surface could be monitored in situ and in real time. Symmetry analysis of the SH rotation patterns reveals both contributions due to a 3-fold axis due to the regular (1×1) structure and simultaneously a 1-fold and a 2-fold axis due to the (1×23) reconstruction

Surface-enhanced optical third-harmonic generation in Ag island films

Surface-enhanced optical third-harmonic generation (THG) is observed in silver island films. The THG intensity from Ag nanoparticles is enhanced by more than two orders of magnitude with respect to the THG intensity from a smooth and homogeneous silver surface. This enhancement is attributed to local plasmon excitation and resonance of the local field at the third-harmonic wavelength. The diffuse and depolarized component of the enhanced THG is associated with the third-order hyper-Rayleigh scattering in a 2-D random array of silver nanoparticles.Comment: 4 pages, 2 figure

Laser performance of perylenebis (dicarboximide) dyes with long secondary alkyl chains

The laser performance and related photophysical properties of two very soluble perylene dyes with long chain secondary alkyl groups were investigated in cyclohexane solution. With a dye laser as pump source a tuning range of 555–580 nm was obtained at an optimum concentration of 3×10–4 M. The quantum efficiencies (=0.29 and 0.21) were better than 1/2 that of rhodamine 6G. No photodegradation was observed over an excitation period of several hours