Skewed electronic band structure induced by electric polarization in ferroelectric BaTiO3.

Skewed band structures have been empirically described in ferroelectric materials to explain the functioning of recently developed ferroelectric tunneling junction (FTJs). Nonvolatile ferroelectric random access memory (FeRAM) and the artificial neural network device based on the FTJ system are rapidly developing. However, because the actual ferroelectric band structure has not been elucidated, precise designing of devices has to be advanced through appropriate heuristics. Here, we perform angle-resolved hard X-ray photoemission spectroscopy of ferroelectric BaTiO3 thin films for the direct observation of ferroelectric band skewing structure as the depth profiles of atomic orbitals. The depth-resolved electronic band structure consists of three depth regions: a potential slope along the electric polarization in the core, the surface and interface exhibiting slight changes. We also demonstrate that the direction of the energy shift is controlled by the polarization reversal. In the ferroelectric skewed band structure, we found that the difference in energy shifts of the atomic orbitals is correlated with the atomic configuration of the soft phonon mode reflecting the Born effective charges. These findings lead to a better understanding of the origin of electric polarization.

A novel perovskite oxide chemically designed to show multiferroic phase boundary with room-temperature magnetoelectricity.

There is a growing activity in the search of novel single-phase multiferroics that could finally provide distinctive magnetoelectric responses at room temperature, for they would enable a range of potentially disruptive technologies, making use of the ability of controlling polarization with a magnetic field or magnetism with an electric one (for example, voltage-tunable spintronic devices, uncooled magnetic sensors and the long-searched magnetoelectric memory). A very promising novel material concept could be to make use of phase-change phenomena at structural instabilities of a multiferroic state. Indeed, large phase-change magnetoelectric response has been anticipated by a first-principles investigation of the perovskite BiFeO3-BiCoO3 solid solution, specifically at its morphotropic phase boundary between multiferroic polymorphs of rhombohedral and tetragonal symmetries. Here, we report a novel perovskite oxide that belongs to the BiFeO3-BiMnO3-PbTiO3 ternary system, chemically designed to present such multiferroic phase boundary with enhanced ferroelectricity and canted ferromagnetism, which shows distinctive room-temperature magnetoelectric responses.

Simulating the Radio-Frequency Dielectric Response of Relaxor Ferroelectrics: Combination of Coarse-Grained Hamiltonians and Kinetic Monte Carlo Simulations.

The radio-frequency dielectric response of the lead-free Ba(Zr_{0.5}Ti_{0.5})O_{3} relaxor ferroelectric is simulated using a coarse-grained Hamiltonian. This concept, taken from real-space renormalization group theories, allows us to depict the collective behavior of correlated local modes gathered in blocks. Free-energy barriers for their thermally activated collective hopping are deduced from this ab initio-based approach, and used as input data for kinetic Monte Carlo simulations. The resulting numerical scheme allows us to simulate the dielectric response for external field frequencies ranging from kHz up to a few tens of MHz for the first time and to demonstrate, e.g., that local (electric or elastic) random fields lead to the dielectric relaxation in the radio-frequency range that has been observed in relaxors.

Morphogenesis mechanisms in the solvothermal synthesis of BaTiO3 from titanate nanorods and nanotubes.

A rich variety of single crystalline BaTiO3 (BT) nanostructures have been synthesized by two different routes using titanate nanorods and nanotubes as precursors. Free standing, mixed or agglomerated nanotori, solid or hollow nanospheres and nanocubes were obtained. A careful analysis of the shape evolution of the resulting BT nano-objects obtained with both types of precursors and different parameters (precursor composition and shape, temperature, Ba/Ti molar ratio) allowed an improved understanding of the nanostructure formation. The morphogenesis models at play such as Ostwald ripening and the Kirkendall effect have been identified. Other mechanisms hereafter called the self and merging rebuilding processes and a tentative Turing-reaction-diffusion-model are proposed to explain the formation of these obtained nanoparticles.