A series of symmetric derivatives of
4-(dicyanomethylene)-2-methyl-6-(p-(dimethylamino)styryl)-4H-pyran
(DCM laser dye) has been synthesized, and the nonlinear optical
properties and thermal decomposition temperatures
of each of the chromophores has been measured. The symmetric
chromophores all have larger hyperpolarizabilities
than one would expect based on their absorption maxima.
Estimations of their oscillator strengths based upon
UV/vis spectra are all well above 1.0. It is proposed that these
compounds possess two excited electronic states close
to each other in energy, both contributing to the hyperpolarizability
in an additive fashion. Electro-optical absorption
spectroscopy data and semiempirical calculations on a model compound
support this hypothesis. The implications
of these results with regard to the tradeoff between nonlinearity and
transparency are discussed. The large dipole
moments and high decomposition temperatures of these chromophores make
them attractive candidates for use in
electro-optic polymers.
The performance of amorphous organic photorefractive (PR) materials in applications such as optical data storage is generally limited by the concentration of active molecules (chromophores) that can be incorporated into the host without forming a crystalline material with poor optical quality. In polymeric PR systems described previously, performance has been limited by the necessity of devoting a large fraction of the material to inert polymer and plasticizing components in order to ensure compositional stability. A new class of organic PR materials composed of multifunctional glass-forming organic chromophores is described that have long-term stability and greatly improved PR properties.
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