Abstract

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=1.91µm. In a guest–host polymer very high electro-optic (EO) coefficients, of up to 55 pm/V, have been determined at λ=1.31µm 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.

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