Several new high μβ chromophores have been synthesized. These chromophores were intentionally designedto study structure−property relationships. The synthetic strategy that was followed has been described in ourprevious publications. Chromophore photostability was investigated from a structural point of view. Contactand corona poling of the chromophores have also been accomplished with a 70 pm/V r33 being achieved atλ = 1550 nm. The same chromophores were also studied in two different polymer host systems to comparetheir dependence of the electrooptic coefficient and stability on the matrix material.