Novel Route for Enhancing Piezoelectricity of Ferroelectric Films: Controlling Nontrivial Polarization States in Pb(Zr, Ti)O3 Monodomain Superlattice Structure

Artificial superlattice films made of Pb(Zr0.4Ti0.6)O-3 and Pb(Zr0.6Ti0.4)O-3 were investigated for their polarization states and piezoelectric properties theoretically and experimentally in this study. The developed theory predicts nontrivial polarization along neither [001] nor [111] directions in (111)-epitaxial monodomain superlattice films with uniform compressive strain. Such films were achieved via pulsed laser deposition. When the layer thickness is reduced to 3 nm, d(33) becomes 128 +/- 3.8 pm/V at 100 kV/cm and 71.3 +/- 2.83 pm/V at 600 kV/cm, comparable to that of (111)-oriented Pb(Zr0.4Ti0.6)O-3 or Pb(Zr0.6Ti0.4)O-3 bulks and clearly exceeding that of the typical clamped films. The measurement agrees with the theoretical analysis, which reveals that the enhanced piezoelectricity is due to rotation of the nontrivial polarization. Furthermore, the theoretical study predicts an even larger d(33) exceeding 300 pm/V for specific parameters in superlattice films with uniform tensile strain, which is promising for applications of microelectromechanical systems.