SPECTRAL CHARACTERISTICS OF 2ND-ORDER OPTICAL NONLINEARITIES IN POLEDPOLYMER-FILMS CONTAINING CHARGED CHROMOPHORE AGGREGATES

We report measurements of the frequency dependence of anomalous second -order electric susceptibilities of polymer films containing hyperpola rizable chromophore guest molecules and poled using coplanar electrode s. The frequency dependence, polarization dependence, and magnitude of the observed second-order susceptibilities are radically different fr om those of conventional corona-field poling experiments and cannot be explained by isolated chromophore models. These observations and the results of sum-over-states perturbative electronic structure calculati ons for the importance of positively charged chromophore aggregates.