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Positively charged poly(allylamine hydrochloride) (PAH) and poly(acrylic acid) (PAA) complexes (noted as PAH-PAA) with a molar excess of PAH were layer-by-layer (LbL) assembled with polyanion poly(sodium 4-styrenesulfonate) (PSS) to produce multilayer films. The film structure and deposition behavior of the PAH-PAA/PSS films were influenced by the structure of PAH-PAA complexes in solution. For the PAH-PAA complexes with a low ratio of PAA to PAH the PAH-PAA complexes have low-level cross-linking and are flexible. The resultant PAH-PAA/PSS films have a thin film thickness and smooth surface and exhibit a nonlinear deposition behavior where the amount of PAH-PAA complexes and PSS deposited in each deposition cycle are larger than in its previous cycle. The PAH-PAA complexes with a high ratio of PAA to PAH have high-level cross-linking and are rigid. The PAH-PAA/PSS films constructed from the rigid PAH-PAA complexes have a large film thickness and rough surface and exhibit a linear deposition behavior. Deposition of the PAH-PAA/PSS films was well characterized by quartz crystal microbalance, atomic force microscopy, and scanning electron microscopy. The thermally cross-linked PAH-PAA/PSS films can be released from substrate to form stable free-standing films by an ion-triggered exfoliation method. Meanwhile, positively charged PAH-PAA complexes can be LbL assembled with negatively charged PAH-PAA complexes with a molar excess of PAA to produce multilayer films. Use of polyelectrolyte-polyelectrolyte complexes as building blocks for LbL fabrication provides a facile way to tailor the structures of the resultant films by simply changing the structure of the complexes in solution.

Noncharged pyrene molecules were incorporated into multilayer films by first loading pyrene into poly(acrylic acid) (PAA)-stabilized cetyltrimethylammonium bromide (CTAB) micelles (noted as PAA&(Py@CTAB)) and then layer-by-layer (LbL) assembled with poly(diallyldimethylammonium chloride) (PDDA). The stable incorporation of pyrene into multilayer films was confirmed by quartz crystal microbalance (QCM) measurements and UV-vis absorption spectroscopy. The resultant PAA&(Py@CTAB)/PDDA multilayer films show an exponential growth behavior because of the increased surface roughness with increasing number of film deposition cycles. The present study will open a general and cost-effective avenue for the incorporation of noncharged species, such as organic molecules, nanoparticles, and so forth, into LbL-assembled multilayer films by using polyelectrolyte-stabilized surfactant micelles as carriers.

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