Calix[4]arenes are a novel type of molecules for nonlinear optics. In
a single molecule four pi-conjugated systems are combined. Corona pole
d guest-host polymer systems [calix[4]arenes-poly(methyl-methacrylate)
] with transparency into the UV and loading up to 100% show a high deg
ree of orientation. The maximum resonant d33 nonlinear coefficient mea
sured at a fundamental wavelength of 590 nm is 51 pm/V. The d33 values
of the thin films relax after poling to 65% of their maximum value. R
esults indicate self-organization of the molecules upon poling.