Enhancement of polarization and related properties in heteroepitaxially constrained thin films of the ferroelectromagnet, BiFeO3, is reported. Structure analysis indicates that the crystal structure of film is monoclinic in contrast to bulk, which is rhombohedral. The films display a room-temperature spontaneous polarization (50 to 60 microcoulombs per square centimeter) almost an order of magnitude higher than that of the bulk (6.1 microcoulombs per square centimeter). The observed enhancement is corroborated by first-principles calculations and found to originate from a high sensitivity of the polarization to small changes in lattice parameters. The films also exhibit enhanced thickness-dependent magnetism compared with the bulk. These enhanced and combined functional responses in thin film form present an opportunity to create and implement thin film devices that actively couple the magnetic and ferroelectric order parameters.
We report on the coupling between ferroelectric and magnetic order parameters in a nanostructured BaTiO3-CoFe2O4 ferroelectromagnet. This facilitates the interconversion of energies stored in electric and magnetic fields and plays an important role in many devices, including transducers, field sensors, etc. Such nanostructures were deposited on single-crystal SrTiO3 (001) substrates by pulsed laser deposition from a single Ba-Ti-Co-Fe-oxide target. The films are epitaxial in-plane as well as out-of-plane with self-assembled hexagonal arrays of CoFe2O4 nanopillars embedded in a BaTiO3 matrix. The CoFe2O4 nanopillars have uniform size and average spacing of 20 to 30 nanometers. Temperature-dependent magnetic measurements illustrate the coupling between the two order parameters, which is manifested as a change in magnetization at the ferroelectric Curie temperature. Thermodynamic analyses show that the magnetoelectric coupling in such a nanostructure can be understood on the basis of the strong elastic interactions between the two phases.
The dielectric relaxation of a solid solution of 10-mol % lead titanate in lead magnesium niobate is found to be similar to the magnetic relaxation in spin-glass systems.1–3 Based on this analogy, it is proposed that the relaxor ferroelectric is a polar-glassy system which has thermally activated polarization fluctuations above a static freezing temperature. An activation energy and freezing temperature of 0.0407 eV and 291.5 K, respectively, were found by analyzing the frequency dependence of the temperature of the dielectric maximum using the Vogel–Fulcher relationship.4,5 It has also been shown that a macroscopic polarization is sustained on heating up to this freezing temperature. A coupling between nanometer scale clusters is believed to control the kinetics of the fluctuations and the development of a frustration as the system freezes into states of local equilibrium. The possibility of an orientational freezing associated with the ferroelastic nature of the nanosized polar regions in the rhombohedral relaxor families as well as a polar freezing is discussed. A diffuse phase transformation is believed to arise due to a dispersion in the fluctuation frequency of the polarization. A qualitative model for the relaxation time spectrum is also proposed in which the width of the spectrum broadens strongly near the freezing temperature.
Reversibility of structural phase transformations has profound technological implications in a wide range of applications from fatigue life in shape-memory alloys (SMAs) to magnetism in multiferroic oxides. The geometric nonlinear theory of martensite universally applicable to all structural transitions has been developed. It predicts the reversibility of the transitions as manifested in the hysteresis behaviour based solely on crystal symmetry and geometric compatibilities between phases. In this article, we report on the verification of the theory using the high-throughput approach. The thin-film composition-spread technique was devised to rapidly map the lattice parameters and the thermal hysteresis of ternary alloy systems. A clear relationship between the hysteresis and the middle eigenvalue of the transformation stretch tensor as predicted by the theory was observed for the first time. We have also identified a new composition region of titanium-rich SMAs with potential for improved control of SMA properties.
Dramatically enhanced polarization has been found for (001), (101), and (111) films, relative to that of BiFeO3 crystals. The easy axis of spontaneous polarization lies close to (111), for the various oriented films. BiFeO3 films grown on (111) have a rhombohedral structure, identical to that of single crystals; whereas films grown on (101) or (001) are monoclinically distorted from the rhombohedral structure, due to the epitaxial constraint.
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