We show that the organic polyene crystal 2-{3-(4-hydroxystyryl)-5,5-dimethylcyclohex-2-enylidene}malononitrile (OH1) is a new material with excellent nonlinear optical and electro-optical properties. The principal refractive indices and the absorption constants have been determined over a broad wavelength range from $0.6\text{to}2.2\mu \mathrm{m}$ . OH1 shows a large birefringence of $\Delta n>0.55$ and a low absorption of $\alpha <1{\mathrm{cm}}^{-1}$ in a large wavelength range between 800 and $1400\mathrm{nm}$ . Furthermore, the nonlinear optical tensor elements $d_{333}=120\pm 10\mathrm{pm}∕\mathrm{V}$ , $d_{223}=13\pm 2\mathrm{pm}∕\mathrm{V}$ , and $d_{322}=8.5\pm 2\mathrm{pm}∕\mathrm{V}$ have been determined by the Maker-fringe technique at the fundamental wavelength of $1.9\mu \mathrm{m}$ . The electro-optic coefficients $r_{333}$ , $r_{223}$ , and $r_{113}$ have been measured at the wavelengths of 633, 785, 1064, and $1319\mathrm{nm}$ , and it is shown that the dispersion can be described by a one-oscillator model. OH1 is a promising material for nonlinear optical and electro-optical applications due to the large nonlinear coefficient $d_{333}$ , the large electro-optic coefficient $r_{333}=109\pm 4\mathrm{pm}∕\mathrm{V}$ at $632.8\mathrm{nm}$ , the favorable crystal growth properties, as well as the orthorhombic crystal symmetry (point group $mm2$ ), which renders crystal preparation and orientation much simpler than in most organic nonlinear optical crystals.

© 2008 Optical Society of America

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