Quantum Liquid States of Spin Solitons in a Ferroelectric Spin-Peierls State.

In this study, we performed high-magnetic-field magnetization, dielectric, and ultrasound measurements on an organic salt showing a ferroelectric spin-Peierls (FSP) state, which is in close proximity to a quantum critical point. In contrast to the sparsely distributed gaslike spin solitons typically observed in conventional spin-Peierls (SP) states, the FSP state exhibits dense liquidlike spin solitons resulting from strong quantum fluctuations, even at low fields. Nevertheless, akin to conventional SP systems, a magnetic-field-induced transition is observed in the FSP state. In conventional high-field SP states, an emergent wave vector results in the formation of a spin-soliton lattice. However, in the present high-field FSP state, the strong quantum fluctuations preclude the formation of such a soliton lattice, causing the dense solitons to remain in a quantum-mechanically melted state. This observation implies the realization of a quantum liquid-liquid transition of topological particles carrying spin and charge in a ferroelectric insulator.

Magnetoelectricity Enhanced by Electron Redistribution in a Spin Crossover [FeCo] Complex.

Molecular-based magnetoelectric materials are among the most promising materials for next-generation magnetoelectric memory devices. However, practical application of existing molecular systems has proven difficult largely because the polarization change is far lower than the practical threshold of the ME memory devices. Herein, we successfully obtained an [FeCo] dinuclear complex that exhibits a magnetic field-induced spin crossover process, resulting in a significant polarization change of 0.45 µC cm-2. Mössbauer spectroscopy and theoretical calculations suggest that the asymmetric structural change, coupled with electron redistribution, leads to the observed polarization change. Our approach provides a new strategy toward rationally enhancing the polarization change.

Pd2 MnGa Metamagnetic Shape Memory Alloy with Small Energy Loss.

Metamagnetic shape memory alloys (MMSMAs) are attractive functional materials owing to their unique properties such as magnetostrain, magnetoresistance, and the magnetocaloric effect caused by magnetic-field-induced transitions. However, the energy loss during the martensitic transformation, that is, the dissipation energy, Edis , is sometimes large for these alloys, which limits their applications. In this paper, a new Pd2 MnGa Heusler-type MMSMA with an extremely small Edis and hysteresis is reported. The microstructures, crystal structures, magnetic properties, martensitic transformations, and magnetic-field-induced strain of aged Pd2 MnGa alloys are investigated. A martensitic transformation from L21 to 10M structures is seen at 127.4 K with a small thermal hysteresis of 1.3 K. The reverse martensitic transformation is induced by applying a magnetic field with a small Edis (= 0.3 J mol-1 only) and a small magnetic-field hysteresis (= 7 kOe) at 120 K. The low values of Edis and the hysteresis may be attributed to good lattice compatibility in the martensitic transformation. A large magnetic-field-induced strain of 0.26% is recorded, indicating the proposed MMSMA's potential as an actuator. The Pd2 MnGa alloy with low values of Edis and hysteresis may enable new possibilities for high-efficiency MMSMAs.

Double dome structure of the Bose-Einstein condensation in diluted S = 3/2 quantum magnets.

Bose-Einstein condensation (BEC) in quantum magnets, where bosonic spin excitations condense into ordered ground states, is a realization of BEC in a thermodynamic limit. Although previous magnetic BEC studies have focused on magnets with small spins of S ≤ 1, larger spin systems potentially possess richer physics because of the multiple excitations on a single site level. Here, we show the evolution of the magnetic phase diagram of S = 3/2 quantum magnet Ba2CoGe2O7 when the averaged interaction J is controlled by a dilution of magnetic sites. By partial substitution of Co with nonmagnetic Zn, the magnetic order dome transforms into a double dome structure, which can be explained by three kinds of magnetic BECs with distinct excitations. Furthermore, we show the importance of the randomness effects induced by the quenched disorder: we discuss the relevance of geometrical percolation and Bose/Mott glass physics near the BEC quantum critical point.

Two Distinct Cu(II)-V(IV) Superexchange Interactions with Similar Bond Angles in a Triangular "CuV2" Fragment.

The strength and sign of superexchange interactions are often predicted on the basis of the bond angles between magnetic ions, but complications may arise in situations with a nontrivial arrangement of the magnetic orbitals. We report on a novel molecular tetramer compound [Cu(H2O)dmbpy]2[V2O2F8] (dmbpy = 4,4'-dimethyl-2,2'-bipyridyl) that is composed of triangular "CuV2" fragments and displays a spin gap behavior. By combining first-principles calculations and electronic models, we reveal that superexchange Cu-V interactions carry drastically different coupling strengths along two Cu-F-V pathways with comparable bond angles in the triangular "CuV2" fragment. Counterintuitively, their strong disparity is found to originate from the restricted symmetry of the half-filled Cu dx2-y2 orbital stabilized by the crystal field, leading to one dominating antiferromagnetic Cu-V coupling in each fragment. We revisit the magnetic properties of the reported spin-gapped chain compound [enH2]Cu(H2O)2[V2O2F8] (enH2 = ethylene diammonium) containing similar triangular "CuV2" fragments, and the magnetic behavior of the molecular tetramer and the chain compounds is rationalized as that of weakly coupled spin dimers and spin trimers, respectively. This work demonstrates that fundamentally different magnetic couplings can be observed between magnetic ions with similar bond angles in a single spin motif, thus providing a strategy to introduce various exchange interactions combined with low dimensionality in heterometallic Cu(II)-V(IV) compounds.

Extremely high upper critical field in BiCh2-based (Ch: S and Se) layered superconductor LaO0.5F0.5BiS2-xSex (x = 0.22 and 0.69).

Centrosymmetric compounds with local inversion symmetry breaking have tremendously interesting and intriguing physical properties. In this study, we focus on a BiCh2-based (Ch: S, Se) layered superconductor, as a system with local inversion asymmetry, because spin polarisation based on the Rashba-Dresselhaus-type spin-orbit coupling has been observed in centrosymmetric BiCh2-based LaOBiS2 systems, while the BiCh2 layer lacks local inversion symmetry. Herein, we report the existence of extremely high in-plane upper critical fields in the BiCh2-based system LaO0.5F0.5BiS2-xSex (x = 0.22 and 0.69). The superconducting states are not completely suppressed by the applied magnetic fields with strengths up to 55 T. Thus, we consider that the in-plane upper critical field is enhanced by the local inversion symmetry breaking and its layered structure. Our study will open a new pathway for the discovery of superconductors that exhibit a high upper critical field by focusing on the local inversion symmetry breaking.

Above-ordering-temperature large anomalous Hall effect in a triangular-lattice magnetic semiconductor.

While anomalous Hall effect (AHE) has been extensively studied in the past, efforts for realizing large Hall response have been mainly limited within intrinsic mechanism. Lately, however, a theory of extrinsic mechanism has predicted that magnetic scattering by spin cluster can induce large AHE even above magnetic ordering temperature, particularly in magnetic semiconductors with low carrier density, strong exchange coupling, and finite spin chirality. Here, we find out a new magnetic semiconductor EuAs, where Eu2+ ions with large magnetic moments form distorted triangular lattice. In addition to colossal magnetoresistance, EuAs exhibits large AHE with an anomalous Hall angle of 0.13 at temperatures far above antiferromagnetic ordering. As also demonstrated by model calculations, observed AHE can be explained by the spin cluster scattering in a hopping regime. Our findings shed light on magnetic semiconductors hosting topological spin textures, developing a field targeting diluted carriers strongly coupled to noncoplanar spin structures.

Coexistence of Magnetoelectric and Antiferroelectric-like Orders in Mn3Ta2O8.

In materials showing a linear magnetoelectric (ME) effect, unconventional functionalities can be anticipated such as electric control of magnetism and nonreciprocal optical responses. Thus, the search for new linear ME materials is of interest in materials science. Here, using a recently proposed design principle of linear ME materials, which is based on the combination of local structural asymmetry and collinear antiferromagnetism, we demonstrate that an anion-deficient fluorite derivative, Mn3Ta2O8, is a new linear ME material. This is evidenced by the onset of magnetic-field-induced electric polarization in its collinear antiferromagnetic phase below TN = 24 K. Furthermore, we also find an antiferroelectric-like phase transition at TS = 55 K, which is attributable to an off-center displacement of magnetic Mn2+ ions. The present study shows that Mn3Ta2O8 is a rare material that exhibits both ME and antiferroelectric-like transitions. Thus, Mn3Ta2O8 may provide an opportunity to investigate the physics associated with complicated interactions between magnetic (spin) and electric dipole degrees of freedom.

Giant anomalous Hall effect from spin-chirality scattering in a chiral magnet.

The electrical Hall effect can be significantly enhanced through the interplay of the conduction electrons with magnetism, which is known as the anomalous Hall effect (AHE). Whereas the mechanism related to band topology has been intensively studied towards energy efficient electronics, those related to electron scattering have received limited attention. Here we report the observation of giant AHE of electron-scattering origin in a chiral magnet MnGe thin film. The Hall conductivity and Hall angle, respectively, reach [Formula: see text] Ω-1 cm-1 and [Formula: see text]% in the ferromagnetic region, exceeding the conventional limits of AHE of intrinsic and extrinsic origins, respectively. A possible origin of the large AHE is attributed to a new type of skew-scattering via thermally excited spin-clusters with scalar spin chirality, which is corroborated by the temperature-magnetic-field profile of the AHE being sensitive to the film-thickness or magneto-crystalline anisotropy. Our results may open up a new platform to explore giant AHE responses in various systems, including frustrated magnets and thin-film heterostructures.

Improved accuracy in high-frequency AC transport measurements in pulsed high magnetic fields.

We show theoretically and experimentally that accurate transport measurements are possible even within the short time provided by pulsed magnetic fields. For this purpose, a new method has been devised, which removes the noise component of a specific frequency from the signal by taking a linear combination of the results of numerical phase detection using multiple integer periods. We also established a method to unambiguously determine the phase rotation angle in AC transport measurements using a frequency range of tens of kilohertz. We revealed that the dominant noise in low-frequency transport measurements in pulsed magnetic fields is the electromagnetic induction caused by mechanical vibrations of wire loops in inhomogeneous magnetic fields. These results strongly suggest that accurate transport measurements in short-pulsed magnets are possible when mechanical vibrations are well suppressed.

Capacitive detection of magnetostriction, dielectric constant, and magneto-caloric effects in pulsed magnetic fields.

We report on the development of a capacitance measuring system that allows measurements of capacitance in pulsed magnetic fields up to 61 T. By using this system, magnetic-field responses of various physical quantities, such as magnetostriction, magnetic-field-induced change in complex dielectric constant, and magneto-caloric effect, can be investigated in pulsed-magnetic-field conditions. Here, we examine the validity of our system for investigations of these magnetic-field-induced phenomena in pulse magnets. For the magnetostriction measurement, magnetostriction of a specimen can be measured through a change in the capacitance between two aligned electrodes glued on the specimen and a dilatometer. We demonstrate a precise detection of valley polarization in semimetallic bismuth through a magnetostriction signal with a resolution better than 10-6 of the relative length change. For the magnetic-field-induced change in complex dielectric constant, we successfully observed clear dielectric anomalies accompanied by magnetic/magnetoelectric phase transitions in multiferroic Pb(TiO)Cu4(PO4)4. For the measurement of magneto-caloric effect, a magnetic-field-induced change in sample temperature was verified for Gd3Ga5O12 with a capacitance thermometer made of a non-magnetic ferroelectric compound KTa1-xNbxO3 (x = 0.02) whose capacitance is nearly field-independent. These results show that our capacitance measuring system is a promising tool to study various magnetic-field-induced phenomena, which have been difficult to detect in pulsed magnetic fields.

Synthesis, Structure, and Anomalous Magnetic Ordering of the Spin-1/2 Coupled Square Tetramer System K(NbO)Cu4(PO4)4.

Quasi-zero-dimensional antiferromagnets with weakly coupled clusters of multiple spins can provide an excellent platform for exploring exotic quantum states of matter. Here, we report the synthesis and the characterization of a copper-based insulating antiferromagnet, K(NbO)Cu4(PO4)4. Single-crystal X-ray diffraction measurements reveal that the crystal structure belongs to the tetragonal space group P4/nmm, in which Cu2+ ions align to form a quasi-two-dimensional layer of spin-1/2 coupled square tetramers. The structure is quasi-isostructural to recently reported magnetoelectric antiferromagnets, A(TiO)Cu4(PO4)4 (A = Ba, Sr, and Pb) with the P4212 space group. Despite their structural similarities, whereas the antiferromagnetic transition in A(TiO)Cu4(PO4)4 produces conventional anomalies in magnetization and heat capacity, that in K(NbO)Cu4(PO4)4 has several unusual features such as an upturn in magnetic susceptibility and a very weak specific heat anomaly that corresponds to a spin entropy release as small as 3%. These results indicate that the magnetism of K(NbO)Cu4(PO4)4 is far different from that of A(TiO)Cu4(PO4)4 and suggest that the ground state is very close to a quantum nonmagnetic singlet state. The origin of the distinct magnetism in K(NbO)Cu4(PO4)4 is discussed in terms of structural modifications of a Cu4O12 unit forming a square tetramer. Our study demonstrates that the present material family, represented by an extended chemical formula A(BO)Cu4(PO4)4 (AB = KNb, BaTi, SrTi, and PbTi), has broad chemical controllability of their magnetism. This makes this system an attractive material platform to study the physics of quantum spin-1/2 coupled square tetramers.

Anisotropic Quantum Transport through a Single Spin Channel in the Magnetic Semiconductor EuTiO3.

Magnetic semiconductors are a vital component in the understanding of quantum transport phenomena. To explore such delicate, yet fundamentally important, effects, it is crucial to maintain a high carrier mobility in the presence of magnetic moments. In practice, however, magnetization often diminishes the carrier mobility. Here, it is shown that EuTiO3 is a rare example of a magnetic semiconductor that can be desirably grown using the molecular beam epitaxy to possess a high carrier mobility exceeding 3000 cm2 V-1 s-1 at 2 K, while intrinsically hosting a large magnetization value, 7 µB per formula unit. This is demonstrated by measuring the Shubnikov-de Haas (SdH) oscillations in the ferromagnetic state of EuTiO3 films with various carrier densities. Using first-principles calculations, it is shown that the observed SdH oscillations originate genuinely from Ti 3d-t2g states which are fully spin-polarized due to their energetical proximity to the in-gap Eu 4f bands. Such an exchange coupling is further shown to have a profound effect on the effective mass and fermiology of the Ti 3d-t2g electrons, manifested by a directional anisotropy in the SdH oscillations. These findings suggest that EuTiO3 film is an ideal magnetic semiconductor, offering a fertile field to explore quantum phenomena suitable for spintronic applications.

High-Mobility 2D Hole Gas at a SrTiO3 Interface.

Strontium titanate (SrTiO3 or STO) is important for oxide-based electronics as it serves as a standard substrate for a wide range of high-temperature superconducting cuprates, colossal magnetoresistive manganites, and multiferroics. Moreover, in its heterostructures with different materials, STO exhibits a broad spectrum of important physics such as superconductivity, magnetism, the quantum Hall effect, giant thermoelectric effect, and colossal ionic conductivity, most of which emerge in a two-dimensional (2D) electron gas (2DEG) formed at an STO interface. However, little is known about its counterpart system, a 2D hole gas (2DHG) at the STO interface. Here, a simple way of realizing a 2DHG with an ultrahigh mobility of 24 000 cm2 V-1 s-1 is demonstrated using an interface between STO and a thin amorphous FeOy layer, made by depositing a sub-nanometer-thick Fe layer on an STO substrate at room temperature. This mobility is the highest among those reported for holes in oxides. The carrier type can be switched from p-type (2DHG) to n-type (2DEG) by controlling the Fe thickness. This unprecedented method of forming a 2DHG at an STO interface provides a pathway to unexplored hole-related physics in this system and enables extremely low-cost and high-speed oxide electronics.

Quantized surface transport in topological Dirac semimetal films.

Unconventional surface states protected by non-trivial bulk orders are sources of various exotic quantum transport in topological materials. One prominent example is the unique magnetic orbit, so-called Weyl orbit, in topological semimetals where two spatially separated surface Fermi-arcs are interconnected across the bulk. The recent observation of quantum Hall states in Dirac semimetal Cd3As2 bulks have drawn attention to the novel quantization phenomena possibly evolving from the Weyl orbit. Here we report surface quantum oscillation and its evolution into quantum Hall states in Cd3As2 thin film samples, where bulk dimensionality, Fermi energy, and band topology are systematically controlled. We reveal essential involvement of bulk states in the quantized surface transport and the resultant quantum Hall degeneracy depending on the bulk occupation. Our demonstration of surface transport controlled in film samples also paves a way for engineering Fermi-arc-mediated transport in topological semimetals.

Thermodynamic evidence of magnetic-field-induced complete valley polarization in bismuth.

We investigated the fundamental physical properties in the ultra-quantum limit state of bismuth through measurements of magnetoresistance, magnetization, magnetostriction, and ultrasound attenuation in magnetic fields up to 60T. For magnetic fields applied along the bisectrix direction of a single crystal, a drastic sign reversal in magnetostriction was observed at approximately 39T, which could be ascribed to the complete valley polarization in the electron Fermi pockets. The application of magnetic fields along the binary direction presented an anomalous feature at approximately 50T only in the magnetoresistance. The emergence of a field-induced splitting of a valley was proposed as a possible origin of this anomaly.

Observation of Poiseuille flow of phonons in black phosphorus.

The travel of heat in insulators is commonly pictured as a flow of phonons scattered along their individual trajectory. In rare circumstances, momentum-conserving collision events dominate, and thermal transport becomes hydrodynamic. One of these cases, dubbed the Poiseuille flow of phonons, can occur in a temperature window just below the peak temperature of thermal conductivity. We report on a study of heat flow in bulk black phosphorus between 0.1 and 80 K. We find a thermal conductivity showing a faster than cubic temperature dependence between 5 and 12 K. Consequently, the effective phonon mean free path shows a nonmonotonic temperature dependence at the onset of the ballistic regime, with a size-dependent Knudsen minimum. These are hallmarks of Poiseuille flow previously observed in a handful of solids. Comparing the phonon dispersion in black phosphorus and silicon, we show that the phase space for normal scattering events in black phosphorus is much larger. Our results imply that the most important requirement for the emergence of Poiseuille flow is the facility of momentum exchange between acoustic phonon branches. Proximity to a structural transition can be beneficial for the emergence of this behavior in clean systems, even when they do not exceed silicon in purity.

Quantum Hall states observed in thin films of Dirac semimetal Cd3As2.

A well known semiconductor Cd3As2 has reentered the spotlight due to its unique electronic structure and quantum transport phenomena as a topological Dirac semimetal. For elucidating and controlling its topological quantum state, high-quality Cd3As2 thin films have been highly desired. Here we report the development of an elaborate growth technique of high-crystallinity and high-mobility Cd3As2 films with controlled thicknesses and the observation of quantum Hall effect dependent on the film thickness. With decreasing the film thickness to 10 nm, the quantum Hall states exhibit variations such as a change in the spin degeneracy reflecting the Dirac dispersion with a large Fermi velocity. Details of the electronic structure including subband splitting and gap opening are identified from the quantum transport depending on the confinement thickness, suggesting the presence of a two-dimensional topological insulating phase. The demonstration of quantum Hall states in our high-quality Cd3As2 films paves a road to study quantum transport and device application in topological Dirac semimetal and its derivative phases.