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Effects of Charge Density on Spread Hyperbranched Polyelectrolyte/Surfactant Films at the Air/Water Interface.

  • Carrascosa-Tejedor, Javier1, 2
  • Tummino, Andrea2, 3
  • Fehér, Bence4
  • Kardos, Attila4, 5
  • Efstratiou, Marina1
  • Skoda, Maximilian W A6
  • Gutfreund, Philipp2
  • Maestro, Armando7, 8
  • Lawrence, M Jayne1
  • Campbell, Richard A1
  • Varga, Imre4, 5
  • 1 Division of Pharmacy and Optometry, Faculty of Biology, Medicine and Health, University of Manchester, Oxford Road, Manchester M13 9PT, U.K.
  • 2 Institut Laue-Langevin, 71 Avenue des Martyrs, CS20156, Grenoble 38042, France. , (France)
  • 3 CEA Commissariat à l'Energie Atomique et aux Energies Alternatives, 17 Rue des Martyrs, Grenoble Cedex 9 38054, France. , (France)
  • 4 Institute of Chemistry, Eötvös Loránd University, 112, Budapest H-1518, Hungary. , (Hungary)
  • 5 Department of Chemistry, Faculty of Education, J. Selye University, Komárno 945 01, Slovakia. , (Slovakia)
  • 6 ISIS Neutron and Muon Source, Rutherford Appleton Laboratory, Harwell Campus, Didcot OX11 0QX, U.K.
  • 7 Basque Foundation for Science, Plaza Euskadi 5, Bilbao 48009, Spain. , (Spain)
  • 8 Centro de Fısica de Materiales (CSIC, UPV/EHU)─Materials Physics Center MPC, Paseo Manuel de Lardizabal 5, San Sebastián E-20018, Spain. , (Spain)
Published Article
American Chemical Society
Publication Date
Oct 24, 2023
DOI: 10.1021/acs.langmuir.3c01514
PMID: 37839073


The interfacial structure and morphology of films spread from hyperbranched polyethylene imine/sodium dodecyl sulfate (PEI/SDS) aggregates at the air/water interface have been resolved for the first time with respect to polyelectrolyte charged density. A recently developed method to form efficient films from the dissociation of aggregates using a minimal quantity of materials is exploited as a step forward in enhancing understanding of the film properties with a view to their future use in technological applications. Interfacial techniques that resolve different time and length scales, namely, ellipsometry, Brewster angle microscopy, and neutron reflectometry, are used. Extended structures of both components are formed under a monolayer of the surfactant with bound polyelectrolytes upon film compression on subphases adjusted to pH 4 or 10, corresponding to high and low charge density of the polyelectrolyte, respectively. A rigid film is related to compact conformation of the PEI in the interfacial structure at pH 4, while it is observed that aggregates remain embedded in mobile films at pH 10. The ability to compact surfactants in the monolayer to the same extent as its maximum coverage in the absence of polyelectrolyte is distinct from the behavior observed for spread films involving linear polyelectrolytes, and intriguingly evidence points to the formation of extended structures over the full range of surface pressures. We conclude that the molecular architecture and charge density can be important parameters in controlling the structures and properties of spread polyelectrolyte/surfactant films, which holds relevance to a range of applications, such as those where PEI is used, including CO2 capture, electronic devices, and gene transfection.

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