Thermally Induced Charge Reversal of Layer-by-Layer Assembled Single-Component Polymer Films

Joseph J. Richardson, Blaise L. Tardy, Hirotaka Ejima, Junling Guo, Jiwei Cui, Kang Liang, Gwan H. Choi, Pil J. Yoo, Bruno G. De Geest, Frank Caruso

Research output: Contribution to journalArticlepeer-review

28 Scopus citations


Temperature can be harnessed to engineer unique properties for materials useful in various contexts and has been shown to affect the layer-by-layer (LbL) assembly of polymer thin films and cause physical changes in preassembled polymer thin films. Herein we demonstrate that exposure to relatively low temperatures (≤100 °C) can induce physicochemical changes in cationic polymer thin films. The surface charge of polymer films containing primary and secondary amines reverses after heating (from positive to negative), and different characterization techniques are used to show that the change in surface charge is related to oxidation of the polymer that specifically occurs in the thin film state. This charge reversal allows for single-polymer LbL assembly to be performed with poly(allylamine) hydrochloride (PAH) through alternating heat/deposition steps. Furthermore, the negative charge induced by heating reduces the fouling and cell-association of PAH-coated planar and particulate substrates, respectively. This study highlights a unique property of thin films which is relevant to LbL assembly and biofouling and is of interest for the future development of thin polymer films for biomedical systems.

Original languageBritish English
Pages (from-to)7449-7455
Number of pages7
JournalACS Applied Materials and Interfaces
Issue number11
StatePublished - 30 Mar 2016


  • cell adhesion
  • charge conversion
  • layer-by-layer assembly
  • low-fouling
  • single-polymer


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