Three-wave-mixing spectroscopy is used to determine the dispersive and absorptive parts of a strongly allowed two-photon transition in a series of polydiacetylene solutions. The data analysis yields the energy, width, symmetry assignment, and oscillator strength for the two-photon transition. The data conclusively demonstrate that strong two-photon absorption is a fundamental property of the polydiacetylene backbone. The remarkably large two-photon absorption coefficients are explained by large oscillator strengths for both transitions involved in the two-photon absorption combined with strong one-photon resonance effects. The experimental results are shown to be consistent with a simple theoretical model for the energies and oscillator strengths of the one- and two-photon-allowed transitions.

• Received 22 May 1980

DOI:https://doi.org/10.1103/PhysRevB.22.3540