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We investigated domain kinetics by measuring the polarization switching behaviors of polycrystalline Pb(Zr,Ti)O$_{3}$ films, which are widely used in ferroelectric memory devices. Their switching behaviors at various electric fields and temperatures could be explained by assuming the Lorentzian distribution of domain switching times. We viewed the switching process under an electric field as a motion of the ferroelectric domain through a random medium, and we showed that the local field variation due to dipole defects at domain pinning sites could explain the intriguing distribution.
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A long standing problem of domain switching process - how domains nucleate - is examined in ultrathin ferroelectric films. We demonstrate that the large depolarization fields in ultrathin films could significantly lower the nucleation energy barrier (U*) to a level comparable to thermal energy (kBT), resulting in power-law like polarization decay behaviors. The Landauers paradox: U* is thermally insurmountable is not a critical issue in the polarization switching of ultrathin ferroelectric films. We empirically find a universal relation between the polarization decay behavior and U*/kBT.
In purely c-axis oriented PbZr$_{0.2}$Ti$_{0.8}$O$_3$ ferroelectric thin films, a lateral piezoresponse force microscopy signal is observed at the position of 180{deg}domain walls, where the out-of-plane oriented polarization is reversed. Using electric force microscopy measurements we exclude electrostatic effects as the origin of this signal. Moreover, our mechanical simulations of the tip/cantilever system show that the small tilt of the surface at the domain wall below the tip does not satisfactorily explain the observed signal either. We thus attribute this lateral piezoresponse at domain walls to their sideways motion (shear) under the applied electric field. From simple elastic considerations and the conservation of volume of the unit cell, we would expect a similar lateral signal more generally in other ferroelectric materials, and for all types of domain walls in which the out-of-plane component of the polarization is reversed through the domain wall. We show that in BiFeO$_3$ thin films, with 180, 109 and 71{deg}domain walls, this is indeed the case.
Although enhanced conductivity at ferroelectric domain boundaries has been found in BiFeO$_3$ films, Pb(Zr,Ti)O$_3$ films, and hexagonal rare-earth manganite single crystals, the mechanism of the domain wall conductivity is still under debate. Using conductive atomic force microscopy, we observe enhanced conductance at the electrically-neutral domain walls in semiconducting hexagonal ferroelectric TbMnO$_3$ thin films where the structure and polarization direction are strongly constrained along the c-axis. This result indicates that domain wall conductivity in ferroelectric rare-earth manganites is not limited to charged domain walls. We show that the observed conductivity in the TbMnO$_3$ films is governed by a single conduction mechanism, namely, the back-to-back Schottky diodes model tuned by the segregation of defects.
Deterministic polarization reversal in ferroelectric and multiferroic films is critical for their exploitation in nanoelectronic devices. While ferroelectricity has been studied for nearly a century, major discrepancies in the reported values of coercive fields and saturation polarization persist in literature for many materials. This raises questions about the atomic-scale mechanisms behind polarization reversal. Unconventional ferroelectric switching in $epsilon$-Fe2O3 films, a material that combines ferrimagnetism and ferroelectricity at room temperature, is reported here. High-resolution in-situ scanning transmission electron microscopy (STEM) experiments and first-principles calculations demonstrate that polarization reversal in $epsilon$-Fe2O3 occurs around pre-existing domain walls only, triggering local domain wall motion in moderate electric fields of 250 - 500 kV/cm. Calculations indicate that the activation barrier for switching at domain walls is nearly a quarter of that corresponding to the most likely transition paths inside $epsilon$-Fe2O3 domains. Moreover, domain walls provide symmetry lowering, which is shown to be necessary for ferroelectric switching. Local polarization reversal in $epsilon$-Fe2O3 limits the macroscopic ferroelectric response and offers important hints on how to tailor ferroelectric properties by domain structure design in other relevant ferroelectric materials.
Mechanical restoring forces acting on ferroelastic domain walls displaced from the equilibrium positions in epitaxial films are calculated for various modes of their cooperative translational oscillations. For vibrations of the domain-wall superlattice with the wave vectors corresponding to the center and boundaries of the first Brillouin zone, the soft modes are singled out that are distinguished by a minimum magnitude of the restoring force. It is shown that, in polydomain ferroelectric thin films, the soft modes of wall vibrations may create enormously large contribution to the film permittivity.
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