Improved nonlinear organic chromophores of varying conjugation length with either thiobarbituric acid or 3-dicyanomethylene-2,3-dihydrobenzothiophene-1,1-dioxide (FORON^® Blue) acceptors have been synthesized and investigated for their nonlinear optical properties. Very large quadratic hyperpolarizabilities β(−2ω; ω, ω) have been found, up to 25,700×10⁻⁴⁸ esu at λ=1.91 μm. In a guest–host polymer very high electro-optic (EO) coefficients, of up to 55 pm/V, have been determined at λ=1.31 μm with 20-wt % chromophore loading. We find good agreement between molecular parameters evaluated by electric-field-induced second-harmonic generation (EFISH) and the measurements of guest–host solid–solid solutions. The latter method is well suited to the determination of the product of dipole moment μ and hyperpolarizability β quickly and reliably at the wavelength of interest for EO applications without the complications associated with EFISH measurements.

© 1996 Optical Society of America

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