Nonlinear-optical processes in lower-dimensional conjugated structures

J. W. Wu, J. R. Heflin, Robert A Norwood, K. Y. Wong, O. Zamani-Khamiri, A. F. Garito, P. Kalyanaraman, J. Sounik

Research output: Contribution to journalArticlepeer-review

95 Scopus citations

Abstract

Reduced dimensionality and quantum confinement in conjugated organic and polymer structures enhance the effects of electron correlation on virtual electronic excitation processes and nonlinear-optical responses. A microscopic many-electron description of the third-order susceptibilities Yijkl(−W4; w1, w2, w3) of conjugated structures is reviewed for one-dimensional chains and extended to two-dimensional conjugated cyclic structures. Electron correlation effects in effectively reduced dimensions result in highly correlated μ-electron virtual excitations that lead to large, ultrafast nonresonant nonlinear-optical responses. The increase of dimensionality from linear to cyclic chains is found to reduce the nonresonant isotropic third-order susceptibility yg. Resonant experimental studies of saturable absorption and optical bistability in ultrathin films of quasi-two-dimensional naphthalocyanine oligomers are also presented. In the saturable-absorption studies, the resonant nonlinear refractive index n was measured to be 1 × 10−4 cm2/kW in the wavelength range of operating laser diodes. Based on this result, electronic absorptive optical bistability is observed on a nanosecond time scale in a nonlinear Fabry-Perot interferometer employing the saturably absorbing naphthalocyanine film as the nonlinear-optical medium.

Original languageEnglish (US)
Pages (from-to)707-720
Number of pages14
JournalJournal of the Optical Society of America B: Optical Physics
Volume6
Issue number4
DOIs
StatePublished - 1989
Externally publishedYes

ASJC Scopus subject areas

  • Statistical and Nonlinear Physics
  • Atomic and Molecular Physics, and Optics

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