A ferroelectric crystal exhibits a stable and switchable electrical polarization that is manifested in the form of cooperative atomic displacements. A ferromagnetic crystal exhibits a stable and switchable magnetization that arises through the quantum mechanical phenomenon of exchange. There are very few 'multiferroic' materials that exhibit both of these properties, but the 'magnetoelectric' coupling of magnetic and electrical properties is a more general and widespread phenomenon. Although work in this area can be traced back to pioneering research in the 1950s and 1960s, there has been a recent resurgence of interest driven by long-term technological aspirations.

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Multiferroic and magnetoelectric materials

BiFeO3 is perhaps the only material that is both magnetic and a strong ferroelectric at room temperature. As a result, it has had an impact on the field of multiferroics that is comparable to that of yttrium barium copper oxide (YBCO) on superconductors, with hundreds of publications devoted to it in the past few years. In this Review, we try to summarize both the basic physics and unresolved aspects of BiFeO3 (which are still being discovered with several new phase transitions reported in the past few months) and device applications, which center on spintronics and memory devices that can be addressed both electrically and magnetically.

Physics and Applications of Bismuth Ferrite

State-of-the-art photovoltaics use high-purity, large-area, wafer-scale single-crystalline semiconductors grown by sophisticated, high-temperature crystal growth processes. We demonstrate a solution-based hot-casting technique to grow continuous, pinhole-free thin films of organometallic perovskites with millimeter-scale crystalline grains. We fabricated planar solar cells with efficiencies approaching 18%, with little cell-to-cell variability. The devices show hysteresis-free photovoltaic response, which had been a fundamental bottleneck for the stable operation of perovskite devices. Characterization and modeling attribute the improved performance to reduced bulk defects and improved charge carrier mobility in large-grain devices. We anticipate that this technique will lead the field toward synthesis of wafer-scale crystalline perovskites, necessary for the fabrication of high-efficiency solar cells, and will be applicable to several other material systems plagued by polydispersity, defects, and grain boundary recombination in solution-processed thin films.

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High-efficiency solution-processed perovskite solar cells with millimeter-scale grains

인공고관절의 세라믹 볼 헤드의 기계적 안정성 평가를 위한 3 차원 유한요소 해석

The room-temperature manipulation of magnetization by an electric field using the multiferroic BiFeO3 represents an essential step towards the magnetoelectric control of spintronics devices.

Multiferroics: Towards a magnetoelectric memory

From an experimental point of view, room-temperature ferroelectricity in $\mathrm{Bi}\mathrm{Fe}{\mathrm{O}}_{3}$ is raising many questions. Electric measurements made a long time ago on solid solutions of $\mathrm{Bi}\mathrm{Fe}{\mathrm{O}}_{3}$ with $\mathrm{Pb}(\mathrm{Ti},\mathrm{Zr}){\mathrm{O}}_{3}$ indicate that a spontaneous electric polarization exists in $\mathrm{Bi}\mathrm{Fe}{\mathrm{O}}_{3}$ below the Curie temperature ${T}_{C}=1143\phantom{\rule{0.3em}{0ex}}\mathrm{K}$. Yet in most reported works, the synthesized samples are too conductive at room temperature to get a clear polarization loop in the bulk without any effects of extrinsic physical or chemical parameters. Surprisingly, up to now there has been no report of a $P(E)$ (polarization versus electric field) loop at room temperature on single crystals of $\mathrm{Bi}\mathrm{Fe}{\mathrm{O}}_{3}$. We describe here our procedure to synthesize ceramics and to grow good quality sizeable single crystals by a flux method. We demonstrate that $\mathrm{Bi}\mathrm{Fe}{\mathrm{O}}_{3}$ is indeed ferroelectric at room temperature through evidence by piezoresponse force microscopy and $P(E)$ loops. The polarization is found to be large, around $60\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{C}∕{\mathrm{cm}}^{2}$, a value that has only been reached in thin films. Magnetic measurements using a superconducting quantum interference device magnetometer and M\"ossbauer spectroscopy are also presented. The latter confirms the results of nuclear magnetic resonance measurements concerning the anisotropy of the hyperfine field attributed to the magnetic cycloidal structure.

Room-temperature coexistence of large electric polarization and magnetic order in Bi Fe O 3 single crystals

Bismuth ferrite, BiFeO3, is the only known room-temperature magnetic ferroelectric material. We demonstrate here, using neutron scattering measurements in high quality single crystals, that the antiferromagnetic and ferroelectric order parameters are intimately coupled. Initially in a single ferroelectric state, our crystals have a canted antiferromagnetic structure describing a unique cycloid. Under electrical poling, polarization reorientation induces a spin flop. We argue here that the coupling between the two orders may be stronger in the bulk than in thin films where the cycloid is absent.

Electric-field-induced spin flop in BiFeO3 single crystals at room temperature.

We have explored the influence of deposition pressure and temperature on the growth of BiFeO3 thin films by pulsed laser deposition onto (001)-oriented SrTiO3 substrates. Single-phase BiFeO3 films are obtained in a region close to 10−2mbar and 580°C. In nonoptimal conditions, x-ray diffraction reveals the presence of Fe oxides or of Bi2O3. We address the influence of these parasitic phases on the magnetic and electrical properties of the films and show that films with Fe2O3 systematically exhibit a ferromagnetic behavior, while single-phase films have a low bulklike magnetic moment. Conductive-tip atomic force microscopy mappings also indicate that Bi2O3 conductive outgrowths create shortcuts through the BiFeO3 films, thus preventing their practical use as ferroelectric elements in functional heterostructures.

Influence of parasitic phases on the properties of BiFeO3 epitaxial thin films

We unravel the magnon spectra of ${\mathrm{BiFeO}}_{3}$ by means of low-energy inelastic light scattering. We show the existence of two species of magnons corresponding to spin wave excitations in and out of the cycloidal plane. These excitations might be interpreted as electromagnon modes. The present observations present an unique opportunity to study the competition between ferroelectric and magnetic orders.

Possible observation of cycloidal electromagnons in BiFeO3.

Micro-Raman spectroscopy has been used to study lattice dynamics associated with the ferroelectric domains of a BiFeO3 single crystal at low temperature. The phonon assignment shows a large frequency splitting between the transverse and longitudinal components of the A1 phonon mode related to the Bi–O bonds in contrast with thin films where the splitting is negligible. Applying an external electric field induces frequency shifts of the low energy modes related to the Bi–O bonds. These softenings are due to a tensile stress via the piezoelectric effect. The authors give estimates of the phonon deformation potentials.

D. Lebeugle

Papers

Room-temperature coexistence of large electric polarization and magnetic order in Bi Fe O 3 single crystals

Electric-field-induced spin flop in BiFeO3 single crystals at room temperature.

Influence of parasitic phases on the properties of BiFeO3 epitaxial thin films

Possible observation of cycloidal electromagnons in BiFeO3.

Electric field effect on BiFeO3 single crystal investigated by Raman spectroscopy