The present invention relates generally to mercaptofunctional high .mu..beta. EO chromophores and EO polymers, and particularly to mercaptofunctional high .mu..beta. EO chromophores and EO polymers useful for making electro-optical devices and systems. Mercaptofunctional high .mu..beta. EO chromophores are covalently bonded to poly(imido sulfide) polymers producing high Tg, low optical loss, covalently bonded, high .mu..beta. EO chromophore containing polymers. Methods of synthesizing these EO materials using mild polymerization conditions are also described.

 
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