Thickness-dependent evolution of piezoresponses and a/c domains in [101]-oriented PbTiO3 ferroelectric films

It is known that high-index perovskite ferroelectric thin films exhibit giant permittivity, piezoelectric response, and a particular switching behavior. However, the fine domain configuration in high-index ferroelectric films is not yet clarified, which triggers difficulties to further modulate their electric properties. In this work, we focus on the tetragonal PbTiO3 thin films with thicknesses of 20, 40, 55, and 70nm deposited on a [101]-oriented KTaO3 substrate. By using piezoresponse force microscopy and state-of-the-art scanning transmission electron microscopy, the stripe a/c domains with alternately wide c and narrow a domains are observed in all these PbTiO3 films. The periodic stripe a/c domains with {101} domain walls extend along the in-plane [ 11 1 <overbar></mml:mover> ] or [ 1 1 <overbar></mml:mover> <mml:mover> 1 <mml:mo stretchy="false"><overbar></mml:mover> <mml:mo stretchy="false">] direction, which almost completely relaxes the misfit strain between the PbTiO3 films and the KTaO3 substrate. The domain width decreases as the film thickness is reduced following the square root dependence. This results in an increase of ferroelastic a/c domain walls and promotes the enhancement of the piezoresponse amplitude for the thinner PbTiO3 films. In addition, the piezoresponse amplitude of a 20nm PbTiO3 film is comparable to that of a 40nm PbTiO3 film, which indicates that the piezoelectric response of ferroelectric films may saturate at a certain film thickness and scarcely increase even after the film thickness reduces further. These results clarify the domain configurations of [101]-oriented PbTiO3 thin films and provide useful information for understanding the relationship between microstructures and piezoelectric properties in ferroelectric films.