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Epitaxial oxide ferroelectric films exhibit emerging phenomena arising from complex domain configurations even at pseudoequilibrium, including the creation of domain states unfavored in nature and abrupt piezoelectric coefficients around morphotropic phase boundaries. The nanometer-sized domain configurations and their domain switching dynamics under external stimuli are directly linked to the ultrafast manipulation of ferroelectric thin films; however, complex domain switching dynamics under homogeneous electric fields has not been fully explored, especially at the nanosecond timescale. This Letter reports the nanosecond dynamics of ferroelastic-domain switching from the 90° to 180° direction using time-resolved x-ray microdiffraction under homogeneous electric fields onto an epitaxial Pb(Zr_{0.35},Ti_{0.65})O_{3} film capacitor. It is found that the application of electric fields induces spatially heterogeneous domain switching processes via intermediate domain structures with rotated polarization vectors. In addition, the domain switching time is shown to be inversely proportional to the magnitude of the applied electric field, and electric fields higher than 480  kV/cm are found to complete the ferroelastic switching within nanoseconds.

The nanosecond response of a PbTiO(3)/SrTiO(3) ferroelectric/dielectric superlattice to applied electric fields is closely linked to the dynamics of striped domains of the remnant polarization. The intensity of domain satellite reflections observed with time-resolved x-ray microdiffraction decays in 5-100 ns depending on the magnitude of the electric field. The piezoelectric response of the superlattice within stripe domains is strongly suppressed due to electromechanical clamping between adjacent regions of opposite polarization. Regions of the superlattice that have been switched into a uniform polarization state by the applied electric field, however, exhibit piezoelectricity during the course of the switching process. We propose a switching model different from previous models of the switching of superlattices, based instead on a spatially heterogeneous transformation between striped and uniform polarization states., (© 2011 American Physical Society)

The origin of the functional properties of complex oxide superlattices can be resolved using time-resolved synchrotron x-ray diffraction into contributions from the component layers making up the repeating unit. The CaTiO3 layers of a CaTiO3/BaTiO3 superlattice have a piezoelectric response to an applied electric field, consistent with a large continuous polarization throughout the superlattice. The overall piezoelectric coefficient at large strains, 54  pm/V, agrees with first-principles predictions in which a tetragonal symmetry is imposed on the superlattice by the SrTiO3 substrate.

We investigated the ferroelectric domain-wall propagation in epitaxial Pb(Zr,Ti)O3 thin film over a wide temperature range (3-300 K). We measured the domain-wall velocity under various electric fields and found that the velocity data is strongly nonlinear with electric fields, especially at low temperature. We found that, as one of surface growth issues, our domain-wall velocity data from ferroelectric epitaxial film could be classified into the creep, depinning, and flow regimes due to competition between disorder and elasticity. The measured values of velocity and dynamical exponents indicate that the ferroelectric domain walls in the epitaxial films are fractal and pinned by a disorder-induced local field.

We investigated domain kinetics by measuring the polarization switching behaviors of (111)-preferred polycrystalline Pb(Zr,Ti)O3 films, which are widely used in ferroelectric memories. Their switching behaviors at various electric fields and temperatures could be explained by assuming the Lorentzian distribution of logarithmic domain-switching times. We suggested that the local field variation due to dipole defects at domain pinning sites could explain the Lorentzian distribution.

In most ferroelectrics, the domain nucleation barrier (U*) is thermally insurmountable; this is called "Landauer's paradox." However, we showed that, in ultrathin films, the large depolarization fields could lower U* to a level comparable to thermal energy (k(B)T), resulting in power-law decay of polarization. We empirically found a universal relation between the power-law decay exponent and U*/k(B)T. This relation will provide a practical but fundamental limit for capacitor-type ferroelectric devices, analogous to the superparamagnetic limit for magnetic memory devices.

Time-dependent polarization relaxation behavior induced by a depolarization field E(d) was investigated on high-quality ultrathin SrRuO3/BaTiO3/SrRuO3 capacitors. The E(d) values were determined experimentally from an applied external field to stop the net polarization relaxation. These values agree with those from the electrostatic calculations, demonstrating that a large E(d) inside the ultrathin ferroelectric layer could cause severe polarization relaxation. For numerous ferroelectric devices of capacitor configuration, this effect will set a stricter size limit than the critical thickness issue.