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Article Abstract
Applications of ferroelectric films critically depend on their polar ordering, which is highly sensitive to the film size and substrate constraint. Previous studies have revealed a much enhanced piezoresponse in ferroelectric nanoislands relaxed from substrate clamping, yet the proposed mechanisms were completely opposite. We revisit this problem utilizing clamped epitaxial and freestanding PbTiO (PTO) films as our model system for systematic investigation via scanning transmission electron microscopy, piezoresponse force microscopy, and second harmonic generation. It is found that freestanding PTO exhibits 97% higher atomic-scale polar displacement compared to the one clamped on the SrAlO/SrTiO (SAO/STO) substrate, with ferroelectric -domains coarsened significantly accompanied by notable polarization rotation and vanishing -domains. These structural changes yield 141% enhancement in the effective piezoelectric coefficient and 404% increase in second harmonic generation intensity for freestanding PTO compared to its epitaxial counterpart clamped by SAO/STO substrate, highlighting the important influence of substrate constraint on ferroelectric films.
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