Capturing Coherent Magnons by Tip-Assisted Terahertz Spectroscopy.

Our study highlights the versatility of tip-assisted terahertz spectroscopy in probing coherent magnons, the elementary quanta of spin waves in magnetic materials. We identify two distinct coherent magnon types in canted antiferromagnet YFeO3. The remarkable consistency with far-field terahertz spectroscopy in crucial magnon parameters, such as coherence time and resonance frequency, firmly establishes the credibility of tip-assisted terahertz spectroscopy. Notably, we capture more coherent ferromagnetic magnons near the sample surface, underscoring the strength of the technique. This approach paves the way for local, free-standing, and real-space investigations of spin waves in solid magnets.

Electrical Transport Properties Driven by Unique Bonding Configuration in γ-GeSe.

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 γ-GeSe, a recently identified polymorph of GeSe. γ-GeSe exhibits high electrical conductivity (∼106 S/m) and a relatively low Seebeck coefficient (9.4 µV/K at room temperature) owing to its high p-doping level (5 × 1021 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 γ-GeSe is a unique polymorph in which the modified local bonding configuration leads to substantially different physical properties.

Type-II Red Phosphorus: Wavy Packing of Twisted Pentagonal Tubes.

Elemental phosphorus exhibits fascinating structural varieties and versatile properties. The unique nature of phosphorus bonds can lead to the formation of extremely complex structures, and detailed structural information on some phosphorus polymorphs is yet to be investigated. In this study, we investigated an unidentified crystalline phase of phosphorus, type-II red phosphorus (RP), by combining state-of-the-art structural characterization techniques. Electron diffraction tomography, atomic-resolution scanning transmission electron microscopy (STEM), powder X-ray diffraction, and Raman spectroscopy were concurrently used to elucidate the hidden structural motifs and their packing in type-II RP. Electron diffraction tomography, performed using individual crystalline nanowires, was used to identify a triclinic unit cell with volume of 5330 Å3 , which is the largest unit cell for elemental phosphorus crystals up to now and contains approximately 250 phosphorus atoms. Atomic-resolution STEM imaging, which was performed along different crystal-zone axes, confirmed that the twisted wavy tubular motif is the basic building block of type-II RP. Our study discovered and presented a new variation of building blocks in phosphorus, and it provides insights to clarify the complexities observed in phosphorus as well as other relevant systems.

Re-order parameter of interacting thermodynamic magnets.

Phase diagrams of materials are typically based on a static order parameter, but it faces challenges when distinguishing subtle phase changes, such as re-ordering. Here, we report a dynamic nonequilibrium order parameter termed re-order parameter to determine subtle phases and their transitions in interacting magnets. The dynamical precession of magnetization, so-called magnon, premises as a reliable re-order parameter of strong spin-orbit coupled magnets. We employ orthoferrites YFeO3 and its Mn-doped variations, where diverse magnetic phases, including canted antiferromagnetic (Γ4) and collinear antiferromagnetic (Γ1) states, have been well-established. Low-energy magnon uncovers the spin-orbit coupling-induced subtle magnetic structures, resulting in distinct terahertz emissions. The temporal and spectral parameters of magnon emission exhibit characteristics akin to BCS-type order parameters, constructing the magnetic phase diagram of Mn-doped YFeO3. This approach further reveals a concealed ferrimagnetic phase within the Γ1 state, underscoring its potential to search for hidden phases of materials, completing their phase diagrams.

Coherent charge hopping suppresses photoexcited small polarons in ErFeO3 by antiadiabatic formation mechanism.

Polarons are prevalent in condensed matter systems with strong electron-phonon coupling. The adiabaticity of the polaron relates to its transport properties and spatial extent. To date, only adiabatic small polaron formation has been measured following photoexcitation. The lattice reorganization energy is large enough that the first electron-optical phonon scattering event creates a small polaron without requiring substantial carrier thermalization. We measure that frustrating the iron-centered octahedra in the rare-earth orthoferrite ErFeO3 leads to antiadiabatic polaron formation. Coherent charge hopping between neighboring Fe3+─Fe2+ sites is measured with transient extreme ultraviolet spectroscopy and lasts several picoseconds before the polaron forms. The resulting small polaron formation time is an order of magnitude longer than previous measurements and indicates a shallow potential well, even in the excited state. The results emphasize the importance of considering dynamic electron-electron correlations, not just electron-phonon-induced lattice changes, for small polarons for transport, catalysis, and photoexcited applications.

Giant and highly anisotropic magnetocaloric effects in single crystals of disordered-perovskite RCr0.5Fe0.5O3 (R = Gd, Er).

Magnetic anisotropy is crucial in examining suitable materials for magnetic functionalities because it affects their magnetic characteristics. In this study, disordered-perovskite RCr0.5Fe0.5O3 (R = Gd, Er) single crystals were synthesized and the influence of magnetic anisotropy and additional ordering of rare-earth moments on cryogenic magnetocaloric properties was investigated. Both GdCr0.5Fe0.5O3 (GCFO) and ErCr0.5Fe0.5O3 (ECFO) crystallize in an orthorhombic Pbnm structure with randomly distributed Cr3+ and Fe3+ ions. In GCFO, the long-range order of Gd3+ moments emerges at a temperature of TGd (the ordering temperature of Gd3+ moments) = 12 K. The relatively isotropic nature of large Gd3+ moment originating from zero orbital angular momentum exhibits giant and virtually isotropic magnetocaloric effect (MCE), with a maximum magnetic entropy change of [Formula: see text] ≈ 50.0 J/kg·K. In ECFO, the highly anisotropic magnetizations result in a large rotating MCE characterized by a rotating magnetic entropy change [Formula: see text] = 20.8 J/kg·K. These results indicate that a detailed understanding of magnetically anisotropic characteristics is the key for exploring improved functional properties in disordered perovskite oxides.

Gapless superconductivity in Nb thin films probed by terahertz spectroscopy.

Time reversal symmetry (TRS) breaking often generates exotic quantum phases in condensed matter. In superconductors, TRS breaking by an external magnetic field not only suppresses superconductivity but also leads to a novel quantum state called the gapless superconducting state. Here we show that magneto-terahertz spectroscopy provides us with a rare opportunity to access and explore the gapless superconducting state of Nb thin films. We present the complete functional form of the superconducting order parameter for an arbitrary magnetic field, for which a fully self-consistent theory is, surprisingly, yet unavailable. We observe a Lifshitz topological phase transition with a vanishing quasiparticle gap everywhere on the Fermi surface, whereas the superconducting order parameter smoothly crosses over from the gapped to the gapless regime. Our observation of the magnetic pair-breaking effects in Nb challenges traditional perturbative theories and opens a pathway to further exploring and manipulating the exotic state of gapless superconductivity.

Spin-flip-driven anomalous Hall effect and anisotropic magnetoresistance in a layered Ising antiferromagnet.

The influence of magnetocrystalline anisotropy in antiferromagnets is evident in a spin flip or flop transition. Contrary to spin flops, a spin-flip transition has been scarcely presented due to its specific condition of relatively strong magnetocrystalline anisotropy and the role of spin-flips on anisotropic phenomena has not been investigated in detail. In this study, we present antiferromagnet-based functional properties on an itinerant Ising antiferromagnet Ca0.9Sr0.1Co2As2. In the presence of a rotating magnetic field, anomalous Hall conductivity and anisotropic magnetoresistance are demonstrated, the effects of which are maximized above the spin-flip transition. Moreover, a joint experimental and theoretical study is conducted to provide an efficient tool to identify various spin states, which can be useful in spin-processing functionalities.

Kondo interaction in FeTe and its potential role in the magnetic order.

Finding d-electron heavy fermion states has been an important topic as the diversity in d-electron materials can lead to many exotic Kondo effect-related phenomena or new states of matter such as correlation-driven topological Kondo insulator. Yet, obtaining direct spectroscopic evidence for a d-electron heavy fermion system has been elusive to date. Here, we report the observation of Kondo lattice behavior in an antiferromagnetic metal, FeTe, via angle-resolved photoemission spectroscopy, scanning tunneling spectroscopy and transport property measurements. The Kondo lattice behavior is represented by the emergence of a sharp quasiparticle and Fano-type tunneling spectra at low temperatures. The transport property measurements confirm the low-temperature Fermi liquid behavior and reveal successive coherent-incoherent crossover upon increasing temperature. We interpret the Kondo lattice behavior as a result of hybridization between localized Fe 3dxy and itinerant Te 5pz orbitals. Our observations strongly suggest unusual cooperation between Kondo lattice behavior and long-range magnetic order.

Low-field magnetic anisotropy of Sr2IrO4.

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 Sr2IrO4for 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 thebaxis 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 Sr2IrO4for future studies.

Spin-flip-driven reversal of the angle-dependent magnetic torque in layered antiferromagnetic Ca0.9Sr0.1Co2As2.

Spin-flip transition can occur in antiferromagnets with strong magnetocrystalline anisotropy, inducing a significant modification of the anisotropic magnetic properties through phase conversion. In contrast to ferromagnets, antiferromagnets have not been thoroughly examined in terms of their anisotropic characteristics. We investigated the magnetic-field and angle-dependent magnetic properties of Ising-type antiferromagnetic Ca0.9Sr0.1Co2As2 using magnetic torque measurements. An A-type antiferromagnetic order emerges below TN = 97 K aligned along the magnetically easy c-axis. The reversal of the angle-dependent torque across the spin-flip transition was observed, revealing the strong influence of the magnetocrystalline anisotropy on the magnetic properties. Based on the easy-axis anisotropic spin model, we theoretically generated torque data and identified specific spin configurations associated with the magnetic torque variation in the presence of a rotating magnetic field. Our results enrich fundamental and applied research on diverse antiferromagnetic compounds by shedding new light on the distinct magnetic features of the Ising-type antiferromagnet.

Tunable magnetization steps in mixed valent ferromagnet Eu2CoMnO6.

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.

Behavior of magnetoelectric hysteresis and role of rare earth ions in multiferroicity in double perovskite Yb2CoMnO6.

Double-perovskite multiferroics have been investigated because alternating orders of magnetic ions act as distinct magnetic origins for ferroelectricity. In Yb2CoMnO6, the frustrated antiferromagnetic order emerging at TN = 52 K induces ferroelectric polarization perpendicular to the c axis through cooperative O2- shifts via the symmetric exchange striction. In our detailed measurements of the magnetoelectric properties of single-crystalline Yb2CoMnO6, we observe full ferromagnetic-like hysteresis loops that are strongly coupled to the dielectric constant and ferroelectric polarization at various temperatures below TN. Unlike Lu2CoMnO6 with non-magnetic Lu3+ ions, we suggest the emergence of additional ferroelectric polarization along the c axis below the ordering temperature of magnetic Yb3+ ions, TYb ≈ 20 K, based on the spin structure established from recent neutron diffraction experiments. While the proposed description for additional ferroelectricity, ascribed to the symmetric exchange striction between Yb3+ and Co2+/Mn4+ magnetic moments, is clearly given, anomalies of dielectric constants along the c axis are solely observed. Our interesting findings on magnetoelectric hysteresis and the possible development of additional ferroelectricity reveal notable characteristics of double perovskites and provide essential guidance for the further examination of magnetoelectric functional properties.

Anisotropic and nonlinear magnetodielectric effects in orthoferrite ErFeO3 single crystals.

In rare-earth orthoferrites, strongly correlated order parameters have been thoroughly investigated, which aims to find multiple functionalities such as multiferroic or magnetoelectric properties. We have discovered highly anisotropic and nonlinear magnetodielectric effects from detailed measurements of magnetoelectric properties in single-crystalline orthoferrite, ErFeO3. Isothermal dielectric constant varies in shapes and signs depending on the relative orientations between the external electric and magnetic fields, which may be ascribed to the spin-phonon couplings. In addition, a dielectric constant with both electric and magnetic fields along the c axis exhibits two symmetric sharp anomalies, which are closely relevant to the spin-flop transition, below the ordering temperature of Er3+ spins, TEr = 3.4 K. We speculate that the magnetostriction from the exchange couplings between Er3+ and Fe3+ magnetic moments would be responsible for this relationship between electric and magnetic properties. Our results present significant characteristics of the orthoferrite compounds and offer a crucial guide for exploring suitable materials for magnetoelectric functional applications.

Highly nonlinear magnetoelectric effect in buckled-honeycomb antiferromagnetic Co4Ta2O9.

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.

Antiferromagnet-Based Spintronic Functionality by Controlling Isospin Domains in a Layered Perovskite Iridate.

The novel electronic state of the canted antiferromagnetic (AFM) insulator strontium iridate (Sr2 IrO4 ) is 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 the unique characteristics of the isospin state in Sr2 IrO4 . Based on magnetic and transport measurements, a large and highly anisotropic magnetoresistance (AMR) is obtained by manipulating the AFM isospin domains. First-principles calculations suggest that electrons whose isospin directions are strongly coupled to the in-plane net magnetic moment encounter an isospin mismatch when moving across the AFM 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 this work establishes a link between isospins and magnetotransport in strongly spin-orbit-coupled AFM Sr2 IrO4 , the peculiar AMR effect provides a beneficial foundation for fundamental and applied research on AFM spintronics.

Mo1-xWxSe2-Based Schottky Junction Photovoltaic Cells.

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.