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Register a new userDomain wall conductivity in semiconducting hexagonal ferroelectric TbMnO$_3$ thin films
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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.
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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.
Domain walls in ferroelectrics exhibit a plethora of phases and functionalities not found in the bulk. The interplay of electrostatic, chemical, topological, and distortive inhomogeneities at the walls can be so complex, however, that this obstructs their technological performance. In tetragonal ferroelectrics like PbZrxTi1-xO3, for example, the desired functional 180{deg} domain walls within out-of-plane-polarized c-domains are interspersed by in-plane-polarized a-domains and the associated network of domain walls remains challenging to analyze. Here we use a combination of STEM and optical second harmonic generation (SHG) to determine the relation between strain, film thickness, local electric fields and the resulting domain and domain-wall structures across the entire thickness of a set of PZT films. We quantify the distribution of a-domains in the c-domain matrix of the films. Using locally applied electric fields we control the a/c distribution and induce the technologically preferable 180{deg} domain walls. We find that these voltage induced walls are tilted and exhibit a mixed Ising-Neel type transverse rotation of polarization across the wall with a specific nonlinear optical response.
The static configuration of ferroelectric domain walls was investigated using atomic force microscopy on epitaxial PbZr0.2Ti0.8O3 thin films. Measurements of domain wall roughness reveal a power law growth of the correlation function of relative displacements B(L) ~ L^(2zeta) with zeta ~ 0.26 at short length scales L, followed by an apparent saturation at large L. In the same films, the dynamic exponent mu was found to be ~ 0.6 from independent measurements of domain wall creep. These results give an effective domain wall dimensionality of d=2.5, in good agreement with theoretical calculations for a two-dimensional elastic interface in the presence of random-bond disorder and long range dipolar interactions.
The ideal intrinsic barriers to domain switching in c-phase PbTiO_3 (PTO), PbZrO_3 (PZO), and PbZr_{1-x}Ti_xO_3 (PZT) are investigated via first-principles computational methods. The effects of epitaxial strain on the atomic structure, ferroelectric response, barrier to coherent domain reversal, domain-wall energy, and barrier to domain-wall translation are studied. It is found that PTO has a larger polarization, but smaller energy barrier to domain reversal, than PZO. Consequentially the idealized coercive field is over two times smaller in PTO than PZO. The Ti--O bond length is more sensitive to strain than the other bonds in the crystals. This results in the polarization and domain-wall energy in PTO having greater sensitivity to strain than in PZO. Two ordered phases of PZT are considered, the rock-salt structure and a (100) PTO/PZO superlattice. In these simple structures we find that the ferroelectric properties do not obey Vergards law, but instead can be approximated as an average over individual 5-atom unit cells.
Using Landau-Ginzburg-Devonshire theory we calculated numerically the static conductivity of both inclined and counter domain walls in the uniaxial ferroelectrics-semiconductors of n-type. We used the effective mass approximation for the electron and holes density of states, which is valid at arbitrary distance from the domain wall. Due to the electrons accumulation, the static conductivity drastically increases at the inclined head-to-head wall by 1 order of magnitude for small incline angles theta pi/40 by up 3 orders of magnitude for the counter domain wall (theta=pi/2). Two separate regions of the space charge accumulation exist across an inclined tail-to-tail wall: the thin region in the immediate vicinity of the wall with accumulated mobile holes and the much wider region with ionized donors. The conductivity across the tail-to-tail wall is at least an order of magnitude smaller than the one of the head-to-head wall due to the low mobility of holes, which are improper carries. The results are in qualitative agreement with recent experimental data for LiNbO3 doped with MgO.
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