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Group-IV monochalcogenides have recently shown great potential for their thermoelectric, ferroelectric, and other intriguing properties. The electrical properties of group-IV monochalcogenides exhibit a strong dependence on the chalcogen type. For example, GeTe exhibits high doping concentration, whereas S/Se-based chalcogenides are semiconductors with sizable bandgaps. Here, we investigate the electrical and thermoelectric properties of gamma-GeSe, a recently identified polymorph of GeSe. gamma-GeSe exhibits high electrical conductivity (~106 S/m) and a relatively low Seebeck coefficient (9.4 uV/K at room temperature) owing to its high p-doping level (5x1021 cm-3), which is in stark contrast to other known GeSe polymorphs. Elemental analysis and first-principles calculations confirm that the abundant formation of Ge vacancies leads to the high p-doping concentration. The magnetoresistance measurements also reveal weak-antilocalization because of spin-orbit coupling in the crystal. Our results demonstrate that gamma-GeSe is a unique polymorph in which the modified local bonding configuration leads to substantially different physical properties.

Magnetic properties can be manipulated to enhance certain functionalities by tuning different material processing parameters. Here, we present the controllable magnetization steps of hysteresis loops in double-perovskite single crystals of Eu2CoMnO6. Ferromagnetic order emerges below TC ≈ 122 K along the crystallographic c axis. The difficulty in altering Co2+ and Mn4+ ions naturally induces additional antiferromagnetic clusters in this system. Annealing the crystals in different gas environments modifies the mixed magnetic state, and results in the retardation (after O2-annealing) and bifurcation (after Ar-annealing) of the magnetization steps of isothermal magnetization. This remarkable variation offers an efficient approach for improving the magnetic properties of double-perovskite oxides.

Emerging from competing exchange interactions, the helimagnetic order describes a noncollinear spin texture of antiferromagnets. Although collinear antiferromagnets act as the elemental building blocks of antiferromagnetic (AFM) spintronics, until now, the potential of implementing spintronic functionality in noncollinear antiferromagnets has not been clarified. Here, we propose an AFM helimagnet of EuCo2As2 as a novel single-phase spintronic material that exhibits a remarkable sign reversal of anisotropic magnetoresistance (AMR). The contrast in the AMR arises from two electrically distinctive magnetic phases with spin reorientation that is driven by the magnetic field prevailing in the easy plane, which converts the AMR from positive to negative. Furthermore, based on an easy-plane anisotropic spin model, we theoretically identified various AFM memory states associated with the evolution of the spin structure under magnetic fields. The results revealed the potential of noncollinear antiferromagnets for application in the development of spintronic devices.

Magnetic anisotropy in strontium iridate (Sr

We investigated Ru-doped single-crystal $5d$ iridates, ${\mathrm{Sr}}_{2}{\mathrm{Ir}}_{1\ensuremath{-}x}{\mathrm{Ru}}_{x}{\mathrm{O}}_{4}$, at three different doping concentrations ($x=0.01$, 0.07, and 0.10) using optical spectroscopy. The undoped pristine compound (${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$) is known as a novel ${J}_{\text{eff}}=1/2$ Mott insulator. Remarkably, the optical conductivity spectra of all three samples exhibited insulating behavior, although we observed weak Drude components in the optical conductivity spectra down to the lowest temperature of 30 K. The charge-carrier densities of the Ru-doped iridates estimated from the Drude components are significantly smaller than the expected values estimated from the nominal Ru-doping concentrations. Herein, we provide the temperature- and doping-dependent electronic structure evolution of Ru-doped iridates. We expect that our results will be useful for understanding the intriguing Ru-doping-dependent properties of $5d$ iridate ${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$.

Magnetic anisotropy in strontium iridate (Sr2IrO4) is essential because of its strong spin-orbit coupling and crystal field effect. In this study, we investigated the detailed mapping of the out-of-plane (OOP) magnetic anisotropy in Sr2IrO4 for different sample orientations using torque magnetometry measurements in the low-magnetic-field region before the isospins are fully ordered. Dominant in-plane anisotropy was identified at low fields, confirming the b axis as an easy magnetization axis. Based on the fitting analysis of the strong uniaxial magnetic anisotropy, we observed that the main anisotropic effect arises from a spin–orbit-coupled magnetic exchange interaction that affects the OOP interaction. The interlayer exchange interaction results in additional anisotropic terms owing to the tilting of the isospins. Our results are relevant for understanding OOP magnetic anisotropy and provide a new way to analyze the effects of spin–orbit-coupling and interlayer magnetic exchange interactions. This study provides a new insight into the understanding of bulk magnetic, magneto-transport, and spintronic behavior of Sr2IrO4 for future studies.

We investigated the magnetic and dielectric properties of perovskite HoCr0.5Fe0.5O3. The coexistence of various magnetic interactions resulting from disordered transition-metal ions leads to an intricate temperature dependence of the magnetic properties. From the examination of the temperature dependence of magnetic susceptibility and heat capacity, an antiferromagnetic order of Cr3+/Fe3+ moments arises below TN = 304 K and a spin reorientation transition occurs at TSR = 170 K. In addition, an antiferromagnetic order of Ho3+ spins emerges at THo = 18 K. Based on the sufficiently low dielectric loss below 150 K, excluding the influence of extrinsic effects, a highly nonlinear variation in the isothermal dielectric constant, with a similar hysteretic behavior of the magnetic-field derivative of magnetization, is observed. In comparison to the lack of a noticeable magnetodielectric effect in YCr0.5Fe0.5O3, the strong correlation between magnetic and dielectric order parameters in HoCr0.5Fe0.5O3 suggests the important role of magnetic rare-earth Ho3+ ions. Our results accompanied by intricate magnetic correlations in the disordered HoCr0.5Fe0.5O3 are expected to trigger fundamental and applied research on magnetic materials through the scope of specific magnetic characteristics in disordered perovskites.

Exploring new magnetic materials is essential for finding advantageous functional properties such as magnetoresistance, magnetocaloric effect, spintronic functionality, and multiferroicity. Versatile classes of double perovskite compounds have been recently investigated because of intriguing physical properties arising from the proper combination of several magnetic ions. In this study, it is observed that the dominant ferrimagnetic phase is coexisted with a minor multiferroic phase in single-crystalline double-perovskite Er2CoMnO6. The majority portion of the ferrimagnetic order is activated by the long-range order of Er3+ moments below TEr = 10 K in addition to the ferromagnetic order of Co2+ and Mn4+ moments arising at TC = 67 K, characterized by compensated magnetization at TComp = 3.15 K. The inverted magnetic hysteresis loop observed below TComp can be described by an extended Stoner–Wohlfarth model. The additional multiferroic phase is identified by the ferroelectric polarization of ~0.9 μC/m2 at 2 K. The coexisting ferrimagnetic and multiferroic phases appear to be strongly correlated in that metamagnetic and ferroelectric transitions occur simultaneously. The results based on intricate magnetic correlations and phases in Er2CoMnO6 enrich fundamental and applied research on magnetic materials through the scope of distinct magnetic characteristics in double perovskites.

Magnetic frustration can produce exotic spin configurations and dynamics. Here, the authors explore the seemingly simple competition between ferromagnetic nearest- and antiferromagnetic next-nearest neighbor interactions along Ising spin chains, as realized in the magnetoelectric compound Lu${}_{2}$CoMnO${}_{6}$. Commonly, this situation is described by the axial next-nearest-neighbor Ising model. For the first time, the authors measure and calculate its correlated magnetic dynamics, resulting from a characteristic fractal set of first-order phase boundaries. Experiments and Monte Carlo simulations reveal a dynamics slowdown while approaching the phase transition regime.

Controlling electric polarization with a magnetic field is of technological and fundamental significance. This can be achieved in magnetoelectric materials. ${A}_{4}$${B}_{2}$${O}_{9}$ ($A$=Fe, Co; $B$=Nb, Ta) are promising magnetoelectrics because they combine magnetic ions possessing large orbital moments with heavy elements exhibiting strong spin-orbit coupling. Magnetic symmetry is key for the magnetoelectric properties. Neutron diffraction and anisotropic magnetic susceptibility measurements reported in this paper revise the magnetic structure of Co${}_{4}$Ta${}_{2}$O${}_{9}$ and explain its previously puzzling magnetoelectric tensor.

Strongly correlated materials with multiple order parameters provide unique insights into the fundamental interactions in condensed matter systems and present opportunities for innovative technological applications. A class of antiferromagnetic honeycomb lattices compounds, A4B2O9 (A = Co, Fe, Mn; B = Nb, Ta), have been explored owing to the occurrence of linear magnetoelectricity. From our investigation of magnetoelectricity on single crystalline Co4Ta2O9, we discovered strongly nonlinear and antisymmetric magnetoelectric behavior above the spin-flop transition for magnetic fields applied along two orthogonal in-plane directions. This observation suggests that two types of inequivalent Co2+ sublattices generate magnetic-field-dependent ferroelectric polarization with opposite signs. The results motivate fundamental and applied research on the intriguing magnetoelectric characteristics of these buckled-honeycomb lattice materials.

Magnetic anisotropy in strontium iridate (Sr2IrO4) is essential because of its strong spin–orbit coupling and crystal field effect. In this paper, we present a detailed mapping of the out-of-plane (OOP) magnetic anisotropy in Sr2IrO4 for different sample orientations using torque magnetometry measurements in the low-magnetic-field region before the isospins are completely ordered. Dominant in-plane anisotropy was identified at low fields, confirming the b axis as an easy magnetization axis. Based on the fitting analysis of the strong uniaxial magnetic anisotropy, we observed that the main anisotropic effect arises from a spin–orbit-coupled magnetic exchange interaction affecting the OOP interaction. The effect of interlayer exchange interaction results in additional anisotropic terms owing to the tilting of the isospins. The results are relevant for understanding OOP magnetic anisotropy and provide a new way to analyze the effects of spin–orbit-coupling and interlayer magnetic exchange interactions. This study provides insight into the understanding of bulk magnetic, magnetotransport, and spintronic behavior on Sr2IrO4 for future studies.

Two-dimensional (2D) transition metal dichalcogenides (TMDs)-based van der Waals (vdW) PN junctions have been used for heterojunction diodes, which basically utilize out-of-plane current across the junction interface. In fact, the same vdW PN junction structure can be utilized for another important device application, junction field effect transistors (JFETs), where in-plane current is possible along with 2D–2D heterojunction interface. Moreover, the 2D TMD-based JFET can use both p- and n-channel for low voltage operation, which might be its unique feature. Here we report vdW JFETs as an in-plane current device with heterojunction between semiconducting p- and n-TMDs. Since this vdW JFET would have low-density traps at the vdW interface unlike 2D TMD-based metal insulator semiconductor field effect transistors (MISFETs), little hysteresis of 0.0–0.1 V and best subthreshold swing of ~100 mV/dec were achieved. Easy saturation was observed either from n-channel or p-channel JFET as another advantage over 2D MISFETs, exhibiting early pinch-off at ~1 V. Operational gate voltage for threshold was near 0 V and our highest mobility reaches to ~>500 cm2/V·s for n-channel JFET with MoS2 channel. For 1 V JFET operation, our best ON/OFF current ratio was observed to be ~104. Van der Waals heterostructures of atomically thin semiconductors enable junction field effect transistors (JFETs). A team led by Seongil Im at Yonsei University fabricated JFETs using a heterojunction of semiconducting p-MoTe2 (or p-WSe2) and n-MoS2. The p-type transition metal dichalcogenide (TMDC) works as a gate for the n-type TMDC channel, whereas the n-type TMDC operates as a gate for the p-type TMDC channel. Owing to the low density of traps at the van der Waals interface, the devices exhibit low hysteresis of 0.05–0.1 V and achieve a subthreshold swing of ~100 mV/decade. The highest mobility reaches 500 cm2/V·s for the n-channel JFET with MoS2, whereas the p-channel JFET with MoTe2 is characterized by a much lower mobility of ~13 cm2/V·s. The highest ON/OFF current ratio was observed to be >104.

Robust massless Dirac states with helical spin textures were realized at the boundaries of topological insulators such as van der Waals (vdW) layered Bi2Se3 family compounds. Topological properties of massless Dirac states can be controlled by varying the film thickness, external stimuli, or environmental factors. Here, we report single-crystal-quality growth of ultrathin Bi2Se3 films on flexible polyimide sheets and manipulation of the Dirac states by varying the vdW gap. X-ray diffraction unambiguously demonstrates that under uniaxial bending stress the vdW gap substantially changes with interatomic-layer distances unaltered. Terahertz and photoelectron spectroscopy indicate tuning of the number of quantum conducting channels and of work function, by the stress, respectively. Surprisingly, under compressive strain, transport measurements reveal dimensional crossover and suppressed weak antilocalization. First-principles calculations support the observation. Our findings suggest that variation of vdW gap...

We have conducted a terahertz spectroscopic study of antiferromagnetic resonances in bulk orthoferrite YFe1−xMnxO3 0≤x≤0.4. Both the quasi-ferromagnetic resonance mode and the quasi-antiferromagnetic resonance mode in the weak ferromagnetic Γ4 phase disappear near the spin reorientation temperature, TSR, for the onset of the collinear antiferromagnetic Γ1 phase (x ≥ 0.1). Below TSR, an antiferromagnetic resonance mode emerges and exhibits a large blueshift with decreasing temperature. However, below 50 K, this mode softens considerably, and this tendency becomes stronger with Mn doping. We provide a deeper understanding of such behaviors of the antiferromagnetic resonance modes in terms of the influence of the Mn3+ ions on the magnetocrystalline anisotropy. Our results show that terahertz time-domain spectroscopy is a useful, complementary tool in tracking magnetic transitions and probing the interaction between disparate magnetic subsystems in antiferromagnetic materials with multiple ionic species.

The magnetocaloric effect (MCE) is described by the change in temperature of a material by magnetic field variation and is a crucial subject in magnetism; it is motivated by the desire to enhance energy-efficient magnetic refrigeration for clean technology. Despite the recent discovery of the giant cryogenic MCE in double perovskites, the role of magnetic anisotropy has not yet been clearly discussed, because of the averaging effect of polycrystalline samples. Here, we investigated the anisotropic MCE in the single-crystal double perovskite Gd2CoMnO6. In addition to the ferromagnetic order of the Co2+ and Mn4+ moments, the large Gd3+ moments align below TGd = 21 K, exhibiting an isotropic nature. Because of the intricate temperature development of magnetically hysteretic behaviour and metamagnetism, the change in magnetic entropy along the c-axis appears to be relatively small. On the contrary, the smaller but almost reversible magnetization perpendicular to the c-axis leads to a large MCE with a maximum entropy change of 25.4 J/kg·K. The anisotropic MCE generates a giant rotational MCE, estimated as 16.6 J/kg·K. Our results demonstrate the importance of magnetic anisotropy for understanding the MCE and reveal essential clues for exploring suitable magnetic refrigerant compounds aiming at magnetic functional applications.

Ferromagnetism and exotic topological structures in SrRuO$_3$ (SRO) induce sign-changing anomalous Hall effect (AHE). Recently, hump structures have been reported in the Hall resistivity of SRO thin films, especially in the ultra-thin regime. We investigate the AHE and hump structure in the Hall resistivity of SRO ultra-thin films with an SrTiO$_3$ (STO) capping layer and ionic liquid gating. STO capping results in sign changes in the AHE and modulation of the hump structure. In particular, the hump structure in the Hall resistivity is strongly modulated and even vanishes in STO-capped 4 unit cell (uc) films. In addition, the conductivity of STO-capped SRO ultra-thin films is greatly enhanced with restored ferromagnetism. We also performed ionic liquid gating to modulate the electric field at SRO/STO interface. Drastic changes in the AHE and hump structure are observed with different gate voltages. Our study shows that the hump structure as well as the AHE can be controlled by tuning inversion symmetry and the electric field at the interface., Comment: 5 pages, 5 figures

We developed Schottky junction photovoltaic cells based on multilayer Mo1–xWxSe2 with x = 0, 0.5, and 1. To generate built-in potentials, Pd and Al were used as the source and drain electrodes in a lateral structure, and Pd and graphene were used as the bottom and top electrodes in a vertical structure. These devices exhibited gate-tunable diode-like current rectification and photovoltaic responses. Mo0.5W0.5Se2 Schottky diodes with Pd and Al electrodes exhibited higher photovoltaic efficiency than MoSe2 and WSe2 devices with Pd and Al electrodes, likely because of the greater adjusted band alignment in Mo0.5W0.5Se2 devices. Furthermore, we showed that Mo0.5W0.5Se2-based vertical Schottky diodes yield a power conversion efficiency of ∼16% under 532 nm light and ∼13% under a standard air mass 1.5 spectrum, demonstrating their remarkable potential for photovoltaic applications.

We investigated the anisotropy of the magnetic and magnetocaloric properties of single-crystalline double-perovskite $\mathrm{T}{\mathrm{b}}_{2}\mathrm{CoMn}{\mathrm{O}}_{6}$, which crystallizes in a monoclinic $P{2}_{1}/n$ structure. Due to dissimilar magnetic anisotropy, the ferromagnetic order of the $\mathrm{C}{\mathrm{o}}^{2+}$ and $\mathrm{M}{\mathrm{n}}^{4+}$ moments emerges along the $c$ axis at ${T}_{\mathrm{C}}=100\phantom{\rule{0.16em}{0ex}}\mathrm{K}$, and the larger $\mathrm{T}{\mathrm{b}}^{3+}$ moments align perpendicular to the $c$ axis, below ${T}_{\mathrm{Tb}}=15\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. The intricate temperature development of the metamagnetism along the $c$ axis results in a large negative change in the magnetic entropy at low temperature. On the other hand, the larger but almost reversible magnetization, perpendicular to the $c$ axis, results in a small and positive entropy change. This highly anisotropic magnetocaloric effect (MCE) leads to a giant rotational MCE, estimated to be $20.8\phantom{\rule{0.16em}{0ex}}\mathrm{J}/\mathrm{kg}\phantom{\rule{0.16em}{0ex}}\mathrm{K}$. Our findings, based on the magnetic anisotropy in $\mathrm{T}{\mathrm{b}}_{2}\mathrm{CoMn}{\mathrm{O}}_{6}$, enrich fundamental and applied research on magnetic materials, considering the distinct magnetic characteristics of double perovskites.

The novel electronic state of the canted antiferromagnetic (AFM) insulator, strontium iridate (Sr2IrO4) has been well described by the spin-orbit-entangled isospin Jeff = 1/2, but the role of isospin in transport phenomena remains poorly understood. In this study, antiferromagnet-based spintronic functionality is demonstrated by combining unique characteristics of the isospin state in Sr2IrO4. Based on magnetic and transport measurements, large and highly anisotropic magnetoresistance (AMR) is obtained by manipulating the antiferromagnetic isospin domains. First-principles calculations suggest that electrons whose isospin directions are strongly coupled to in-plane net magnetic moment encounter the isospin mismatch when moving across antiferromagnetic domain boundaries, which generates a high resistance state. By rotating a magnetic field that aligns in-plane net moments and removes domain boundaries, the macroscopically-ordered isospins govern dynamic transport through the system, which leads to the extremely angle-sensitive AMR. As with this work that establishes a link between isospins and magnetotransport in strongly spin-orbit-coupled AFM Sr2IrO4, the peculiar AMR effect provides a beneficial foundation for fundamental and applied research on AFM spintronics., Advanced Materials, online published (2018)

We observed a hump-like feature in Hall effects of SrRuO$_3$ ultrathin films, and systematically investigated it with controlling thicknesses, temperatures and magnetic fields. The hump-like feature is extremely stable, even surviving as a magnetic field is tilted by as much as 85$^\circ$. Based on the atomic-level structural analysis of a SrRuO$_3$ ultrathin film with a theoretical calculation, we reveal that atomic rumplings at the thin-film surface enhance Dzyaloshinskii-Moriya interaction, which can generate stable chiral spin textures and a hump-like Hall effect. Moreover, temperature dependent resonant X-ray measurements at Ru L-edge under a magnetic field showed that the intensity modulation of unexpected peaks was correlated with the hump region in the Hall effect. We verify that the two-dimensional property of ultrathin films generates stable non-coplanar spin textures having a magnetic order in a ferromagnetic oxide material.

In type-I multiferroics, where ferroelectricity and magnetism arise from different origins, the explicit measurement of magnetoelectric effect is commonly prohibited due to the weak magnetoelectric coupling. From our investigation of magnetic and dielectric properties in a perovskite PbFe0.5Ti0.25W0.25O3, we have directly demonstrated magnetic-field-driven change of dielectric constant in a highly non-linear fashion. Our result offers a potential utilization of magnetoelectric functionality in type-I multiferroics.

We have investigated the influence of different annealing conditions on the magnetic properties on the single crystals of double-perovskite Y2CoMnO6. The ferromagnetic moment along the c-axis with the large magnetic coercivity and high squareness ratio was observed. Particularly, in the quenched specimen, the magnetic functionality has been greatly improved compared to that of the as-grown crystal. The magnetic coercivity and maximum energy product have been increased by ∼120% and ∼50%, respectively, by comprising substantial disorders and defects. Our result renders an efficient route to improve the magnetic functionality in mixed-valent magnets. (© 2015 WILEY-VCH Verlag GmbH &Co. KGaA, Weinheim)

We have successfully synthesized the high-quality single crystals of double perovskite La 2 CoMnO 6 by flux method and investigated the effects of different annealing conditions on the magnetic properties. In an as-grown crystal, ferromagnetic order along the c axis arises below 204 K, and the spin-glass-type behavior inherent from ionic disorders is also observed. Upon annealing in different gas environments, the reconstructed magnetic states induce a metamagnetic transition (after Ar annealing), and increase Curie temperature (after O 2 annealing). After quenching, the magnetic transition temperature decreases significantly, comprising lots of defects and disorders. Our results provide adequate procedures to control magnetic properties of double-perovskite compounds.

We report on the growth of multiferroic Yb2CoMnO6 and Lu2CoMnO6 single crystals which were synthesized by the flux method with Bi2O3. Yb2CoMnO6 and Lu2CoMnO6 crystallize in a double-perovskite structure with a monoclinic P2(1)/n space group. Bulk magnetization measurements of both specimens revealed strong magnetic anisotropy and metamagnetic transitions. We observed a dielectric anomaly perpendicular to the c axis. The strongly coupled magnetic and dielectric states resulted in the variation of both the dielectric constant and the magnetization by applying magnetic fields, offering an efficient approach to accomplish intrinsically coupled functionality in multiferroics.

We developed Schottky junction photovoltaic cells based on multilayer Mo

Lu${}_{2}$MnCoO${}_{6}$ is a rare example of a double-perovskite material exhibiting multiferroic behavior -- coupling of magnetic and electric order -- and a rare example of hysteretic coupling in a bulk material. Here, the authors lay to rest questions about whether it occurs in single crystals and verify that it is an intrinsic effect. The Mn and Co spins are arranged in a frustrated up-up-down-down ordering along the $c$ axis. Data from single crystals show that exchange striction produces electric polarization, albeit with a twist. Unlike other `up up down down' multiferroics, the ferroelectricity emerges orthogonal to the magnetic ordering easy axis. This may be explained by a model taking into account the oxygen bond distortion in Lu${}_{2}$MnCoO${}_{6}$. Consequently, the system has a rich phase diagram: a dielectric response emerges below the magnetic ordering temperature, whereas a hysteretic polarization emerges in the region of magnetic hysteresis, as shown in this paper.

The magnetocrystalline contribution to magnetic anisotropy was studied in the canted antiferromagnetic state of layered ${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$ single crystals. We performed torque measurements in magnetic fields up to 9 T under various magnetic field orientations. The strong dependence of torque on the magnetic field revealed that the magnetic easy axis is along the in-plane direction and that the observed field-induced weak ferromagnetic order is attributed only to the in-plane component of the external magnetic field. The dependence of torque on the angle produces a twofold symmetric sawtoothlike shape. A simple model consisting of canted antiferromagnetic and magnetic induction terms showed good agreement with the measured torque. These results show that magnetic anisotropy is closely related to the anisotropy of the exchange between antiferromagnetic moments whose canting is mediated by the Dzyaloshinsky-Moriya interaction. Our study demonstrates that torque magnetometry can be extended to the investigation of the magnetic anisotropy of complex magnetic phases.

Hexagonal YMnO(3) shows a unique improper ferroelectricity induced by structural trimerization. Extensive research on this system is primarily due to its candidacy for ferroelectric memory as well as the intriguing coexistence of ferroelectricity and magnetism. Despite this research, the true ferroelectric domain structure and its relationship with structural domains have never been revealed. Using transmission electron microscopy and conductive atomic force microscopy, we observed an intriguing conductive 'cloverleaf' pattern of six domains emerging from one point--all distinctly characterized by polarization orientation and structural antiphase relationships. In addition, we discovered that the ferroelectric domain walls and structural antiphase boundaries are mutually locked and this strong locking results in incomplete poling even when large electric fields are applied. Furthermore, the locked walls are found to be insulating, which seems consistent with the surprising result that the ferroelectric state is more conducting than the paraelectric state. These fascinating results reveal the rich physics of the hexagonal system with a truly semiconducting bandgap where structural trimerization, ferroelectricity, magnetism and charge conduction are intricately coupled.

We have successfully synthesized the series of the double-perovskite R2CoMnO6 (R = rare earth: La to Lu) single crystals and have investigated their magnetic properties. The ferromagnetic order of Co(2+)/Mn(4+) spins emerges mainly along the c axis. Upon decreasing the size of rare earth ion, the magnetic transition temperature decreases linearly from 204 K for La2CoMnO6 to 48 K for Lu2CoMnO6, along with the enhancement of monoclinic distortion. The temperature and magnetic-field dependences of magnetization reveal the various magnetic characteristics such as the metamagnetic transition in R = Eu, the isotropic nature of rare earth moment in R = Gd, and the reversal of magnetic anisotropy in R = Tb and Dy. Our results offer comprehensive information for understanding the roles of mixed-valent magnetic ions and rare earth magnetic moments on the magnetic properties.

We have grown single crystals of multiferroic double-perovskite Lu2CoMnO6 and studied the directional dependence of their magnetic and dielectric properties. The ferromagnetic order emerges below TC ≈ 48 K along the crystallographic c axis. Dielectric anomaly arises along the b axis at TC, contrary to the polycrystalline work suggesting ferroelectricity along the c axis. Through the strongly coupled ferromagnetic and dielectric states, the highly non-linear variation of both dielectric constant and magnetization was achieved in application of magnetic fields. This concurrent tunability provides an efficient route to manipulation of multiple order parameters in multiferroics.