Lateral piezoelectric response across ferroelectric domain walls in thin films

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.Comment: 31 pages, 10 figures. to appear in J. Appl. Phys. Special topic: invited papers from the international symposium on piezoresponse force microscopy and nanoscale phenomena in polar materials. Aveiro - portugal 200

Theoretical Approach to Electroresistance in Ferroelectric Tunnel Junctions

In this paper, a theoretical approach, comprising the non-equilibrium Green's function method for electronic transport and Landau-Khalatnikov equation for electric polarization dynamics, is presented to describe polarization-dependent tunneling electroresistance (TER) in ferroelectric tunnel junctions. Using appropriate contact, interface, and ferroelectric parameters, measured current-voltage characteristic curves in both inorganic (Co/BaTiO$_{3}$/La$_{0.67}$Sr$_{0.33}$MnO$_{3}$) and organic (Au/PVDF/W) ferroelectric tunnel junctions can be well described by the proposed approach. Furthermore, under this theoretical framework, the controversy of opposite TER signs observed experimentally by different groups in Co/BaTiO$_{3}$/La$_{0.67}$Sr$_{0.33}$MnO$_{3}$ systems is addressed by considering the interface termination effects using the effective contact ratio, defined through the effective screening length and dielectric response at the metal/ferroelectric interfaces. Finally, our approach is extended to investigate the role of a CoO$_{x}$ buffer layer at the Co/BaTiO$_{3}$ interface in a ferroelectric tunnel memristor. It is shown that, to have a significant memristor behavior, not only the interface oxygen vacancies but also the CoO$_{x}$ layer thickness may vary with the applied bias.Comment: 12 page

High-Symmetry Polarization Domains in Low-Symmetry Ferroelectrics

We present experimental evidence for hexagonal domain faceting in the ferroelectric polymer PVDF-TrFE films having the lower orthorhombic crystallographic symmetry. This effect can arise from purely electrostatic depolarizing forces. We show that in contrast to magnetic bubble shape domains where such type of deformation instability has a predominantly elliptical character, the emergence of more symmetrical circular harmonics is favored in ferroelectrics with high dielectric constant

Electromechanical Imaging of Biological Systems with Sub-10 nm Resolution

Electromechanical imaging of tooth dentin and enamel has been performed with sub-10 nm resolution using piezoresponse force microscopy. Characteristic piezoelectric domain size and local protein fiber ordering in dentin have been determined. The shape of a single collagen fibril in enamel is visualized in real space and local hysteresis loops are measured. Because of the ubiquitous presence of piezoelectricity in biological systems, this approach is expected to find broad application in high-resolution studies of a wide range of biomaterials.Comment: 12 pages, 4 figures, submitted for publication in Appl. Phys. Let

On the persistence of polar domains in ultrathin ferroelectric capacitors

The instability of ferroelectric ordering in ultra-thin films is one of the most important fundamental issues pertaining realization of a number of electronic devices with enhanced functionality, such as ferroelectric and multiferroic tunnel junctions or ferroelectric field effect transistors. In this paper, we investigate the polarization state of archetypal ultrathin (several nanometres) ferroelectric heterostructures: epitaxial single-crystalline BaTiO$_3$ films sandwiched between the most habitual perovskite electrodes, SrRuO$_3$, on top of the most used perovskite substrate, SrTiO$_3$. We use a combination of piezoresponse force microscopy, dielectric measurements and structural characterization to provide conclusive evidence for the ferroelectric nature of the relaxed polarization state in ultrathin BaTiO$_3$ capacitors. We show that even the high screening efficiency of SrRuO$_3$ electrodes is still insufficient to stabilize polarization in SrRuO$_3$/BaTiO$_3$/SrRuO$_3$ heterostructures at room temperature. We identify the key role of domain wall motion in determining the macroscopic electrical properties of ultrathin capacitors and discuss their dielectric response in the light of the recent interest in negative capacitance behaviour.Comment: 13 pages, 4 figure

Polarization imaging in ferroelectric polymer thin film capacitors by pyroelectric scanning microscopy

A Pyroelectric Scanning Microscopy system, which uses laser-induced thermal modulation for mapping the pyroelectric response, has been used to image a bipolar domain pattern in a ferroelectric polymer thin film capacitor. This system has achieved a resolution of 660±28 nm by using a violet laser and high f-number microscope objective to reduce the optical spot size, and by operating at high modulation frequencies to reduce the thermal diffusion length. The results agree well with a thermal model implemented numerically using finite element analysis

Shear effects in lateral piezoresponse force microscopy at 180∘^\circ ferroelectric domain walls

In studies using piezoresponse force microscopy, we observe a non-zero lateral piezoresponse at 180$^\circ$ domain walls in out-of-plane polarized, c-axis-oriented tetragonal ferroelectric Pb(Zr$_{0.2}$Ti$_{0.8}$)O$_3$ epitaxial thin films. We attribute these observations to a shear strain effect linked to the sign change of the $d_{33}$ piezoelectric coefficient through the domain wall, in agreement with theoretical predictions. We show that in monoclinically distorted tetragonal BiFeO$_3$ films, this effect is superimposed on the lateral piezoresponse due to actual in-plane polarization, and has to be taken into account in order to correctly interpret the ferroelectric domain configuration.Comment: 4 pages, 3 figure

Choice of tip, signal stability, and practical aspects of piezoresponse-force-microscopy

Piezoresponse force-microscopy (PFM) has become the standard tool to investigate ferroelectrics on the micro- and nanoscale. However, reliability of PFM signals is often problematic and their quantification is challenging and thus not widely applied. Here, we present a study of the reproducibility of PFM signals and of the so-called PFM background signal which has been reported in the literature. We find that PFM signals are generally reproducible to certain extents. The PFM signal difference between 180°domains on periodically poled lithium niobate (PPLN) is taken as the reference signal in a large number of measurements, carried out in a low frequency regime (30-70 kHz). We show that in comparison to Pt coated tips, diamond coated tips exhibit improved signal stability, lower background signal, and less imaging artifacts related to PFM which is reflected in the spread of measurements. This is attributed to the improved mechanical stability of the conductive layer. The average deviation of the mean PFM signal is 38.3%, for a diamond coated tip. Although this deviation is relatively high, it is far better than values from the literature which showed a deviation of approx. 73.1%. Additionally, we find that the average deviation of the background signal from 0 is 11.6% of the PPLN domain contrast. Thus, the background signal needs to be taken into account when quantifying PFM signals and should be subtracted from PFM signals. Those results are important for quantification of PFM signals, since PPLN might be used for this purpose when PFM signals measured on PPLN are related to its macroscopic d33 coefficient. Finally, the crucial influence of sample polishing on PFM signals is shown and we recommend to use a multistep polishing route with a final step involving 200 nm sized colloidal silica particles