Dale M. Willard

White light continuum as a tunable radiation source for second-harmonic generation experiments

We have used a white light continuum generated with ultrashort laser pulses from a Ti:sapphire laser system as the radiation source for second-harmonic generation measurements. The white light continuum provides easily tuned radiation for experiments requiring a range of wavelengths. Despite the small coherence length of the radiation, parametric processes, such as second-harmonic generation, are possible with this source. In particular, surface second-harmonic generation using the white light continuum is reasonable because the extent of the interface is much smaller than the coherence length of the radiation. We demonstrate second-harmonic generation from a gold surface and show that surface second-harmonic generation using the white light continuum can be used to measure absorption spectroscopy of molecules adsorbed to surfaces via resonance enhancement of the surface second-harmonic signals.

Absorption spectroscopy at liquid interfaces by resonant surface second harmonic generation

We have measured the absorption spectrum of the laser dye IR125 (also known as indocyanine green) at the water/air interface using resonant enhanced surface second harmonic generation. The spectra of the dye molecules at the interface are extremely sensitive to the bulk concentration. All the surface spectra reflect aggregation of the dye at the interface, even at the smallest concentrations detectable, below 1 (mu) M. Resonant enhanced second harmonic generation appears to be a good technique for measuring spectra at liquid interfaces.

Solvation Dynamics in Restricted Environments: Solvent Immobilization in Reverse Micelles

Polar solvation dynamics in various reverse micellar environments are investigated. The solvent is immobilized in the smallest micelles and becomes more mobile with increasing water content and micellar size.