The Photoreaction of a Rhodamine 6g Monolayer Adsorbed on Quartz Studied by Surface Second Harmonic Generation

A monolayer of rhodamine 6G on quartz in air exhibited photochemistry upon laser irradiation in the first absorption band. The course of the reaction was followed in real time by the surface second harmonic generation method. It was observed that the photoproduct had an enhanced non‐linear coefficient, relative to rhodamine 6G. Absorption spectra showed that this was not a result of a stronger resonance enhancement of the signal by the photoproduct. Consideration of the factors to which the surface second harmonic signal is sensitive suggested that the enhancement arose from an increased charge transfer character of the photoproduct's electronic transitions, and a reorientation of its transition dipole.