Inter-element miscibility driven stabilization of ordered pseudo-binary alloy.

An infinite number of crystal structures in a multicomponent alloy with a specific atomic ratio can be devised, although only thermodynamically-stable phases can be formed. Here, we experimentally show the first example of a layer-structured pseudo-binary alloy, theoretically called Z3-FePd3. This Z3 structure is achieved by adding a small amount of In, which is immiscible with Fe but miscible with Pd and consists of an alternate L10 (CuAu-type)-PdFePd trilayer and Pd-In ordered alloy monolayer along the c axis. First-principles calculations strongly support that the specific inter-element miscibility of In atoms stabilizes the thermodynamically-unstable Z3-FePd3 phase without significantly changing the original density of states of the Z3-FePd3 phase. Our results demonstrate that the specific inter-element miscibility can switch stable structures and manipulate the material nature with a slight composition change.

Observation of Cu Spin Fluctuations in High-Tc Cuprate Superconductor Nanoparticles Investigated by Muon Spin Relaxation.

The nano-size effects of high-Tc cuprate superconductor La2-xSrxCuO4 with x = 0.20 are investigated using X-ray diffractometry, Transmission electron microscopy, and muon-spin relaxation (µSR). It is investigated whether an increase in the bond distance of Cu and O atoms in the conducting layer compared to those of the bulk state might affect its physical and magnetic properties. The µSR measurements revealed the slowing down of Cu spin fluctuations in La2-xSrxCuO4 nanoparticles, indicating the development of a magnetic correlation at low temperatures. The magnetic correlation strengthens as the particle size reduces. This significantly differs from those observed in the bulk form, which show a superconducting state below Tc. It is indicated that reducing the particle size of La2-xSrxCuO4 down to nanometer size causes the appearance of magnetism. The magnetism enhances with decreasing particle size.

Ferroelectric Sr3 Sn2 O7 :Nd3+ : A New Multipiezo Material with Ultrasensitive and Sustainable Near-Infrared Piezoluminescence.

Ultrasensitive and sustainable near-infrared (NIR)-emitting piezoluminescence is observed from noncentrosymmetric and ferroelectric-phase Sr3 Sn2 O7 doped with rare earth Nd3+ ions. Sr3 Sn2 O7 :Nd3+ (SSN) with polar A21 am structure is demonstrated to emit piezoluminescence of wavelength of 800-1500 nm at microstrain levels, which is enhanced by the ferroelectrically polarized charges in the multipiezo material. These discoveries provide new research opportunities to study luminescence properties of multipiezo and piezo-photonic materials, and to explore their potential as novel ultrasensitive probes for deep-imaging of stress distributions in diverse materials and structures including artificial bone and other implanted structures (in vivo, in situ, etc).

Observation of vortex domain structures in multiferroic hexagonal manganites RMnO3 by transmission electron microscopy.

Multiferroic hexagonal manganite RMnO3 (R = rare-earth elements) shows improper ferroelectricity accompanied by tilting of MnO5 hexahedra as the primary order parameter. The ferroelectricity is originated from displacements of rare-earth ions along c-axis triggered by the MnO5 hexahedra tilting. Although coupling between ferroelectric and antiferromagnetic domains below the magnetic transition temperature of ∼90 K has been reported from previous work[1], the relationship between the ferroelectric domains and structural domains due to the MnO5 hexahedra tilting has not been well-studied. In this talk, we will report our studies on unique patterns of ferroelectric antiphase domains with a vorticity in hexagonal RMnO3, obtained from the results of transmission electron microscopy [2].The electron diffraction patterns obtained at room temperature exhibit superlattice reflection spots due to the MnO5 hexahedra tilting and displacements of rare-earth ions along c-axis, in addition to the fundamental reflections associated with the high symmetry structure with the space group of P63/mmc. Unique antiphase/ferroelectric "cloverleaf-like" domain patterns are clearly observed in dark-field images taken using superlattice spots. The fundamental and superlattice dark-field imaging combined with high-resolution imaging clearly demonstrates that in the cloverleaf-like domain patterns the antiphase and ferroelectric domains arrange periodically with certain rotation direction. In addition, there exist two types of cloverleaf-like domain patterns with the opposite rotations next to each other in the superlattice dark-field images. These results indicate that the cloverleaf-like domain patterns can be considered as the aggregation of vortices and antivortices consisting of ferroelectric and antiphase domains.

Color theorems, chiral domain topology, and magnetic properties of Fe(x)TaS2.

Common mathematical theories can have profound applications in understanding real materials. The intrinsic connection between aperiodic orders observed in the Fibonacci sequence, Penrose tiling, and quasicrystals is a well-known example. Another example is the self-similarity in fractals and dendrites. From transmission electron microscopy experiments, we found that FexTaS2 crystals with x = 1/4 and 1/3 exhibit complicated antiphase and chiral domain structures related to ordering of intercalated Fe ions with 2a × 2a and √3a × âˆš3a superstructures, respectively. These complex domain patterns are found to be deeply related with the four color theorem, stating that four colors are sufficient to identify the countries on a planar map with proper coloring and its variations for two-step proper coloring. Furthermore, the domain topology is closely relevant to their magnetic properties. Our discovery unveils the importance of understanding the global topology of domain configurations in functional materials.

Transferring MBE-grown topological insulator films to arbitrary substrates and metal-insulator transition via Dirac gap.

Mechanical exfoliation of bulk crystals has been widely used to obtain thin topological insulator (TI) flakes for device fabrication. However, such a process produces only microsized flakes that are highly irregular in shape and thickness. In this work, we developed a process to transfer the entire area of TI Bi2Se3 thin films grown epitaxially on Al2O3 and SiO2 to arbitrary substrates, maintaining their pristine morphology and crystallinity. Transport measurements show that these transferred films have lower carrier concentrations and comparable or higher mobilities than before the transfer. Furthermore, using this process we demonstrated a clear metal-insulator transition in an ultrathin Bi2Se3 film by gate-tuning its Fermi level into the hybridization gap formed at the Dirac point. The ability to transfer large area TI films to any substrate will facilitate fabrication of TI heterostructure devices, which will help explore exotic phenomena such as Majorana fermions and topological magnetoelectricity.

Duality of topological defects in hexagonal manganites.

We show that the spontaneous symmetry breaking in multiferroic hexagonal manganites can be chemically manipulated to yield two complementary ground states: the well-known ferroelectric P6(3)cm and an antipolar P3c phase. Both symmetry breakings yield topologically protected vortex defects, with the antipolar vortices dual to those of the ferroelectric. This duality stems from the existence of 12 possible angles of MnO5 tilting, and broad strain-free walls with low energy spontaneously emerge through an intermediate P3c1 state, providing a complete unified symmetry description.

Magnetic and dielectric properties of InFe2O4, InFeCuO4, and InGaCuO4.

The magnetic and dielectric properties of InFe2O4, InFeCuO4, and InGaCuO4 have been investigated. All these materials are isostructural with RFe2O4 (R = Y, Ho-Lu), which shows ferroelectricity due to iron-valence ordering. InFe2O4 exhibits ferrimagnetic ordering at T(C) approximately 242 K and a dielectric constant (epsilon) of approximately 10,000 at around room temperature. These properties resemble those of RFe2O4; the origins of the magnetic and dielectric phenomena are likely common in InFe2O4 and RFe2O4. From measurements of the other two materials, we found that both T(C) and epsilon are decreased in the order of InFe2O4, InFeCuO4, and InGaCuO4. This result strongly supports the previously reported explanation based on an electron transfer between the Fe-site ions for the corresponding rare-earth systems. Therefore, we propose that the dielectric properties of the oxides isostructural with RFe2O4 are plausibly governed by electron transfer; this situation is different from that of ordinary ferroelectrics and dielectrics, in which the displacement of cations and anions is important. In addition, InFeCuO4 and InGaCuO4 exhibit large epsilon values (epsilon > approximately 1500). In consideration of this property, we discuss the possible applications of these oxides.

Ferroelectricity from iron valence ordering in the charge-frustrated system LuFe2O4.

Ferroelectric materials are widely used in modern electric devices such as memory elements, filtering devices and high-performance insulators. Ferroelectric crystals have a spontaneous electric polarization arising from the coherent arrangement of electric dipoles (specifically, a polar displacement of anions and cations). First-principles calculations and electron density analysis of ferroelectric materials have revealed that the covalent bond between the anions and cations, or the orbital hybridization of electrons on both ions, plays a key role in establishing the dipolar arrangement. However, an alternative model-electronic ferroelectricity-has been proposed in which the electric dipole depends on electron correlations, rather than the covalency. This would offer the attractive possibility of ferroelectric materials that could be controlled by the charge, spin and orbital degrees of freedom of the electron. Here we report experimental evidence for ferroelectricity arising from electron correlations in the triangular mixed valence oxide, LuFe(2)O(4). Using resonant X-ray scattering measurements, we determine the ordering of the Fe(2+) and Fe(3+) ions. They form a superstructure that supports an electric polarization consisting of distributed electrons of polar symmetry. The polar ordering arises from the repulsive property of electrons-electron correlations-acting on a frustrated geometry.