SOLVENT EFFECTS ON FIRST-ORDER MOLECULAR HYPERPOLARIZABILITY - A STUDY BASED ON VIBRATIONAL OBSERVABLES

Using a recently developed method, we show here that solvent effects o n the first molecular hyperpolarizabilities of push-pull polyenes can be predicted by evaluation of the relaxation contribution beta(r) to t he hyperpolarizability from vibrational infrared and Raman intensities and vibrational frequencies. The molecules studied in this work are a few organic polymethine dyes with different donor and acceptor groups . The analysis of their vibrational spectra confirms the key role play ed by the structural parameters of the polyene chain in determining th e nonlinear optical response. (C) 1995 American Institute of Physics.