Second-order nonlinear optical properties and relaxation characteristics of poled linear epoxy polymers with tolane chromophores

  • D. Jungbauer
    IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, California 95120-6099
  • I. Teraoka
    IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, California 95120-6099
  • D. Y. Yoon
    IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, California 95120-6099
  • B. Reck
    IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, California 95120-6099
  • J. D. Swalen
    IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, California 95120-6099
  • R. Twieg
    IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, California 95120-6099
  • C. G. Willson
    IBM Research Division, Almaden Research Center, 650 Harry Road, San Jose, California 95120-6099

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<jats:p>A new linear epoxy polymer containing 4-amino-4′-nitrotolane chromophores attached to the chain backbone was synthesized in an attempt to enhance both the poling-induced nonlinear optical susceptibility and its long-term stability. The polymer films poled by corona discharge showed very large nonlinear optical doubling coefficients of d33 ≂ 89 pm/V and d31≂25 pm/V for incident light of 1.06 μm wavelength, and a linear electro-optic coefficient r13≂8 pm/V at 633 nm wavelength. Poling-induced alignment of the nonlinear optical moieties showed no detectable decay in two weeks at ambient temperature, as studied by the birefringence. Even at 100 °C the relaxation time estimated from the birefringence decay was ca. 450 h, consistent with roughly 16% decrease in dij coefficients in 20 h at this temperature and also the extrapolation from the dielectric α relaxation characteristics. The dielectric α relaxation temperatures of the poled polymer samples exhibited higher values than that of the unpoled counterpart. This unusual behavior may be due to a significant contribution of Maier–Saupe thermotropic interactions among the tolane moieties that favor parallel alignment.</jats:p>

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