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    Influence of the Interaction Strength between Supramolecular Complexes on the Topography of Neutral Polymer Multilayer Films

    Year: 2014

    Journal: Langmuir, 2014, 30 (22), pp 6479–6488, 20141008

    Authors: Lydie Séon †‡§, Audrey Parat ‡§, Fabien Gaudière †,Jean-Claude Voegel ‡§, Rachel Auzély-Velty ∥,Philippe Lorchat †, Liliane Coche-Guérente ⊥#,Bernard Senger ‡§, Pierre Schaaf †‡§∇○◆, Loïc Jierry †∇○¶, and Fouzia Boulmedais †∇¶

    Last authors: Fouzia Boulmedais

    Organizations: † Institut Charles Sadron, Centre National de la Recherche Scientifique, Université de Strasbourg, UPR 22, 23 rue du Loess, BP 84047, 67034, Strasbourg Cedex 2, France ‡ INSERM, UMR-S 1121, “Biomatériaux et Bioingénierie”, 11 rue Humann, 67085 Strasbourg Cedex, France § Faculté de Chirurgie Dentaire, Université de Strasbourg, 8 rue Sainte Elisabeth, 67000, Strasbourg, France ∥ Centre de Recherches sur les Macromolécules Végétales, affiliated with Université Joseph Fourier, 601 rue de la Chimie, 38041 Grenoble, France ⊥ Université Grenoble Alpes, DCM UMR 5250, F-38000 Grenoble, France # CNRS, DCM UMR 5250, F-38000 Grenoble, France ∇ International Center for Frontier Research in Chemistry, 8 allée Gaspard Monge, 67083 Strasbourg,France ○ Ecole de Chimie, Polymères et Matériaux, Université de Strasbourg, 25 rue Becquerel, 67087 Strasbourg,France ◆ Institut Universitaire de France, 103 boulevard Saint-Michel, 75005 Paris, France ¶ Institut d’Etudes Avancées de l’Université de Strasbourg, 5 allée du Général Rouvillois, 67083 Strasbourg,France

    Country: France

    Step-by-step polymer film buildup processes lead to polymer coatings, e.g., polyelectrolyte multilayers, of various structures ranging from continuous smooth films to droplet like discontinuous coatings. Yet, the origin of these different behaviors depending upon the system is not yet known. This study is a first attempt to rationalize the evolution of the coating structure as a function of the strength of the interactions between the polymers constituting the film. We investigated the influence of the strength of noncovalent host–guest interactions between cyclodextrin (CD) and pyrene (Py), ferrocene (Fc) or adamantane (Ad) on the structure of neutral poly(N-hydroxypropylmethacrylamide) (PHPMA) multilayers films formed in a step-by-step manner. In solution, the strength of the inclusion complex (measured by log K where K is the complex association constant) is increasing in the order Py/β-CD < Fc/β-CD < Ad/β-CD and can be further varied in the presence of different sodium salts at different ionic strengths. Depending upon this strength, the buildup process is limited to the formation of isolated aggregates for PHPMA-CD/PHPMA-Py, leading to smooth continuous films for PHPMA-CD/PHPMA-Fc and to droplet-like films, not entirely covering the substrate, for PHPMA-CD/PHPMA-Ad. To study the influence of the strength of the host–guest interactions on the film topography, PHPMA-CD/PHPMA-Fc films were built in the presence of different sodium salts at different ionic strengths. For low host–guest interactions, only isolated aggregates are formed on the substrate. As the strength of the host–guest interactions increases (increase of log K), the formed films go through a droplet-like structure, before becoming continuous but rough for stronger interactions. When the interaction strength is further increased, the roughness of the films decreases, leading to a smooth continuous film before becoming rough again at still higher interaction strength. Smooth continuous multilayers seem thus to be obtained for an optimal range of the interaction strength.