No Arabic abstract
The switching of electric polarization induced by electric fields -a fundamental functionality of ferroelectrics- is closely associated with the motions of the domain walls that separate regions with distinct polarization directions. Therefore, understanding domain-walls dynamics is of essential importance for advancing ferroelectric applications. In this Letter, we show that the topology of the multidomain structure can have an intrinsic impact on the degree of switchable polarization. Using a combination of polarization hysteresis measurements and piezoresponse force microscopy on a uniaxial organic ferroelectric, alpha-6,6-dimethyl-2,2-bipyridinium chloranilate, we found that the head-to-head (or tail-to-tail) charged domain walls are strongly pinned and thus impede the switching process; in contrast, if the charged domain walls are replaced with electrically neutral antiparallel domain walls, bulk polarization switching is achieved. Our findings suggest that manipulation of the multidomain topology can potentially control the switchable polarization.
The behaviour of the cross-sectional polarization field is explored for thin nanowires of barium titanate from first-principles calculations. Topological defects of different winding numbers have been obtained, beyond the known textures in ferroelectric nanostructures. They result from the inward accommodation of the polarization patterns imposed at the surface of the wire by surface and edge effects. Close to a topological defect the polarization field orients out of the basal plane in some cases, maintaining a close to constant magnitude, whereas it virtually vanishes in other cases.
The classical spin-flop is the field-driven first-order reorientation transition in easy-axis antiferromagnets. A comprehensive phenomenological theory of easy-axis antiferromagnets displaying spin-flops is developed. It is shown how the hierarchy of magnetic coupling strengths in these antiferromagnets causes a strongly pronounced two-scale character in their magnetic phase structure. In contrast to the major part of the magnetic phase diagram, these antiferromagnets near the spin-flop region are described by an effective model akin to uniaxial ferromagnets. For a consistent theoretical description both higher-order anisotropy contributions and dipolar stray-fields have to be taken into account near the spin-flop. In particular, thermodynamically stable multidomain states exist in the spin-flop region, owing to the phase coexistence at this first-order transition. For this region, equilibrium spin-configurations and parameters of the multidomain states are derived as functions of the external magnetic field. The components of the magnetic susceptibility tensor are calculated for homogeneous and multidomain states in the vicinity of the spin-flop. The remarkable anomalies in these measurable quantities provide an efficient method to investigate magnetic states and to determine materials parameters in bulk and confined antiferromagnets, as well as in nanoscale synthetic antiferromagnets. The method is demonstrated for experimental data on the magnetic properties near the spin-flop region in the orthorhombic layered antiferromagnet (C_2H_5NH_3)_2CuCl_4.
Recent works suggest that the surface chemistry, in particular, the presence of oxygen vacancies can affect the polarization in a ferroelectric material. This should, in turn, influence the domain ordering driven by the need to screen the depolarizing field. Here we show using density functional theory that the presence of oxygen vacancies at the surface of BaTiO3 (001) preferentially stabilizes an inward pointing, P-, polarization. Mirror electron microscopy measurements of the domain ordering confirm the theoretical results.
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.
We report ferrielectricity in a single-phase crystal, TSCC -- tris-sarcosine calcium chloride [(CH3NHCH2COOH)3CaCl2]. Ferrielectricity is well known in smectic liquid crystals but almost unknown in true crystalline solids. Pulvari reported it in 1960 in mixtures of ferroelectrics and antiferroelectrics, but only at high fields. TSCC exhibits a second-order displacive phase transition near Tc = 130 K that can be lowered to a Quantum Critical Point at zero Kelvin via Br- or I-substitution, and phases predicted to be antiferroelectric at high pressure and low temperatures. Unusually, the size of the primitive unit cell does not increase. We measure hysteresis loops and polarization below T = 64 K and clear Raman evidence for this transition, as well of another transition near 47-50 K. X-ray and neutron studies below Tc = 130K show there is an antiferroelectric displacement out of plane of two sarcosine groups; but these are antiparallel displacements are of different magnitude, leading to a bias voltage that grows with decreasing T. A monoclinic subgroup C2 may be possible at the lowest temperatures (T<64K or T<48K), but no direct evidence exists for a crystal class lower than orthorhombic.