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Engineering Surface Chemistry to Enhance Ferroelectric Phase Formation in Ultrathin PVDF-TrFE Films
Andres Mosquera-Vallin1, Arnaud Hemmerle2, Jon Maiz1,3
1Centro de Fisica de Materiales (CFM-MPC), CSIC-EHU, 20018 Donostia - San Sebastian, Spain.
Macromolecules
|March 2, 2026
Summary
Modifying substrate surface chemistry with polymer brushes significantly impacts ultrathin ferroelectric polymer films. Hydrophobic surfaces enhance film coverage, crystallinity, and the electroactive beta-phase for flexible electronics.
Area of Science:
- Materials Science
- Polymer Science
- Nanotechnology
Background:
- Growing interest in ferroelectric polymers like poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) for flexible electronics.
- Challenges in controlling crystallization and morphology of ultrathin (below 50 nm) PVDF-TrFE films due to interfacial sensitivity.
Purpose of the Study:
- To investigate the influence of controlled substrate surface chemistry modifications on the crystallization behavior of ultrathin PVDF-TrFE films.
- To establish a framework for optimizing ferroelectric polymer films by controlling interfacial interactions.
Main Methods:
- Grafting polymer brushes of varying polarity onto silicon oxide substrates to create a surface energy gradient.
- Spin-coating ultrathin PVDF-TrFE films (VDF:TrFE ratios 80:20, 75:25, 70:30) below 50 nm.
- Characterizing film properties using ellipsometry, contact-angle measurements, ATR-FTIR, GIWAXS, and AFM.
Main Results:
- Hydrophobic surfaces promoted superior film coverage, larger crystalline domains, and higher electroactive beta-phase content compared to hydrophilic surfaces.
- Both brush chemistry and copolymer composition were found to significantly affect beta-phase content and crystalline texture.
- Demonstrated a correlation between surface energy and the resulting film's crystalline structure and morphology.
Conclusions:
- Controlled modification of substrate surface chemistry offers a simple and effective strategy for improving ultrathin ferroelectric polymer films.
- Tailoring interfacial properties, rather than the material itself, provides design guidelines for enhancing performance in flexible electronic applications.
- Opens new research directions in nanoscale polymer engineering for advanced electronic devices.
