Nonlinear optical chromophores can be organized as orientationally correlat
ed side groups of polypeptides with a rigid backbone. In such an organizati
on, each chromophore contributes coherently to the second-order nonlinear r
esponse of the polymer structure. The synthesis of poly-l-tyrosine, functio
nalized with the NLO-phores 4-nitroaniline, 2,4-dinitroaniline, 2-cyano-4-n
itroaniline and 4-nitro-4'-nitroazobenzene, which is organized in alpha-hel
ix conformation are presented. Solvatochromic measurements show that the hy
perpolarizability of the supramolecular structure is a module factor of 18.
7 higher than that of the model chromophore and that conformational organiz
ation leads to a strong enhancement of the molecular hyperpolarizability be
ta.