Abstract

Degenerate four-wave mixing experiments (along with saturated absorption experiments) were carried out in and below the excitonic-state resonance in polydiacetylenes. A self-consistent analysis of the data was obtained with a two (electronic) level molecularlike model. The excitonic-state lifetime was determined to be 1.8 psec, and an initial excited-state process with a 100-fsec time constant was resolved. The time constant of the nonresonant third-order nonlinear-optical susceptibility was determined to be less than the resolution of the four-wave mixing experiment, -300 fsec, which was limited by the optical pulse duration.

© 1987 Optical Society of America

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