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
Original Manuscript: January 21, 1987
Manuscript Accepted: February 13, 1987
Published: June 1, 1987
Gary M. Carter, "Excited-state dynamics and temporally resolved nonresonant nonlinear-optical processes in polydiacetylenes," J. Opt. Soc. Am. B 4, 1018-1024 (1987)