Controlled Molecular Orientation through Intercalation in PVDF Thin Films: Exhibiting Ultralong Retention and...

Ferroelectric switching and retention performance of poly(vinylidene fluoride) (PVDF) thin films improve by the incorporation of unmodified smectite montmorillonite (MMT) clay nanodielectric. In the present study, an intercalated PVDF (clay/PVDF) thin film with edge-on β-crystallite is fabricated via a heat-controlled spin coating (HCSC) technique. This provides an efficient and simple way to fabricate the edge-on oriented crystallite lamellae with an electroactive β-phase, facilitating nanoscale ferroelectric switching at a lower voltage compared to the face-on orientation. Here, we demonstrate the polarization retention for periods longer than 20 days (∼480 h, i.e., 1.8 × 10⁶ s), with no degradation in switched nanoscale domains. In addition, by maintaining the relatively high dielectric constant, the incorporation of nanoclay effectively lowers the leakage current by 10² factors. The obtained memory window in the edge-on orientation is 7 V, approximately twice the memory window obtained in the face-on orientation. In short, our findings provide a simple and promising route to fabricate edge-on oriented PVDF thin films, with ultralong retention, high dielectric constant, and improved leakage current.