Spontaneous polarization is a characteristic feature of a ferroelectric material that can be switched by the application of an external electric field. However, in a practical scenario, the switched polarization should be stable for the realization of functional devices. In this study, an ultrathin (≈40 nm) poly(vinylidene fluoride‐trifluoroethylene (PVDF‐TrFE) film self‐assembled on a monolayer (≈1 nm) graphene oxide (GO) film is exploited. Oxygen‐functional groups and defective structure of GO can act as domain pinning sites to provide strong ferroelectric domain stability along with a specific crystal orientation to PVDF‐TrFE through hydrogen bonds and columbic interactions. Scanning probe microscopy based switching experiments reveal excellent piezoelectric response (d33 = −145 pm V−1) along with high polarization retention (over 1500 h with no volatilization) in these ultrathin films, paving new pathways toward high performance miniaturized organic ferroelectric devices.
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