We report our continuing investigations of the cumulenes, a novel class of compounds proposed for use as the active second- and third-order nonlinear optical component materials for electro-optic and all-optical devices. Unlike conjugated organic nonlinear optical molecules based on alternating multiple and single bonds, these molecules contain a contiguous, or `cumulated' system of double bonds, leading to a highly rigid one-dimensional backbone of polarizable (pi) -electrons. A series of symmetrically- and asymmetrically-substituted tetraphenyl cumulenes has been synthesized and characterized. Direct-current electric field- induced second harmonic generation experiments show significant second-order nonlinear susceptibilities in a series of polar cumulenes. These experiments have been performed at 1.9 micrometers to avoid dispersion effects. Thermogravimetric analysis indicates survival of a butatriene to 300 degree(s)C.
A novel passive optical device type is described yielding enhanced reflectance with increasing optical intensity at visible wavelengths. The device is a multilayered thin film Bragg structure, consisting of alternating layers of a transparent polymer and a transparent polymer doped with organic nonlinear optical (NLO) materials. The device operates through the intensity dependent charge of the optical index of refraction of the NLO material. Multilayer optical thin film computer codes were developed and used in the design, modeling, and fabrication of this device. The Bragg structure transmits under low intensity conditions and changes to a reflector with increasing intensity. Present devices were fabricated with poly- (methylmethacrylate) PMMA and PMMA doped with silicon naphthalocyanine (SiNc), an off- resonant electronic third-order organic NLO material. Intensity dependent increases in reflectivity were measured on picosecond time scales with fractional reflectance changes greater than 40% being observed. Along with the device performance results, characterization efforts on the NLO materials are discussed.
We report our investigations of the cumulenes, a novel class of compounds proposed for use as the active second- and thirdorder
nonlinear optical component materials for electro-optic and all-optical devices. Unlike conjugated organic nonlinear
optical molecules based on alternating multiple and single bonds, these molecules contain a contiguous, or "cumulated" system
of double bonds, leading to a highly rigid one-dimensional backbone of polarizable ic-electrons. A series of symmetrically- and
asymmetrically-substituted teiraphenyl cumulenes has been synthesized and characterized. D.C. electric field-induced second
harmonic generation experiments show significant second-order nonlinear susceptibilities in a series of polar cumulenes.
Preliminary results showing evidence of resonant and nonresonant third-order nonlinear optical activity are also reported.
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