To demonstrate the feasibility of preparing ordered multilayers compos
ed of charged macromolecule/dye bilayers, we used an electrostatic sel
f-assembly technique to prepare polypeptide/dye multilayers. We immers
ed previously protonated silanized glass slides in aqueous solutions (
1 mM) of two representative anionic dyes: rod-shaped congo red or plat
e-shaped copper phthalocyanine tetrasulfonic acid sodium salt and cati
onic polypeptide poly(L-lysine) solutions (15 mM monomer). Films resul
ting from up to 100 dipping cycles were characterized by UV-vis absorp
tion spectra, ellipsometry, CD, and FT IR. FT IR spectra of film mater
ial embedded in KBr pelf ets showed an amide I band at 1654 cm(-1), su
ggesting thin film alpha-helical conformation. In both systems, the dy
e absorbance increased with the number of layers. In the copper phthal
ocyanine system, the absorption spectrum was a combination of phthaloc
yanine monomer and dimer contributions, with no evidence of higher agg
regates. The congo red film dye absorption maximum was a function of t
he number of bilayers, suggesting congo red resided in a polar, hydrop
hilic environment that became less polar with increasing bilayer numbe
r. From ellipsometry measurements, the bilayer thickness in both films
was determined to be 20 Angstrom. The phthalocyanine Q band showed ne
gative-induced CD, while the congo red pi pi band exhibited positive-
induced CD The CD measurements gave evidence for ordered dye-polypepti
de complexes in films greater than 100-Angstrom thickness. The current
work suggested a bilayer structure where monomeric congo red or dimer
ic copper phthalocyanine tetrasulfonate were randomly distributed amon
g excess poly(K) monomer bindings sites, giving clear films with no sc
attering centers.