Colossal angular magnetoresistance in ferrimagnetic nodal-line semiconductors.

Efficient magnetic control of electronic conduction is at the heart of spintronic functionality for memory and logic applications1,2. Magnets with topological band crossings serve as a good material platform for such control, because their topological band degeneracy can be readily tuned by spin configurations, dramatically modulating electronic conduction3-10. Here we propose that the topological nodal-line degeneracy of spin-polarized bands in magnetic semiconductors induces an extremely large angular response of magnetotransport. Taking a layered ferrimagnet, Mn3Si2Te6, and its derived compounds as a model system, we show that the topological band degeneracy, driven by chiral molecular orbital states, is lifted depending on spin orientation, which leads to a metal-insulator transition in the same ferrimagnetic phase. The resulting variation of angular magnetoresistance with rotating magnetization exceeds a trillion per cent per radian, which we call colossal angular magnetoresistance. Our findings demonstrate that magnetic nodal-line semiconductors are a promising platform for realizing extremely sensitive spin- and orbital-dependent functionalities.

Magnetochiral tunneling in paramagnetic Co1/3NbS2.

Electric currents have the intriguing ability to induce magnetization in nonmagnetic crystals with sufficiently low crystallographic symmetry. Some associated phenomena include the non-linear anomalous Hall effect in polar crystals and the nonreciprocal directional dichroism in chiral crystals when magnetic fields are applied. In this work, we demonstrate that the same underlying physics is also manifested in the electronic tunneling process between the surface of a nonmagnetic chiral material and a magnetized scanning probe. In the paramagnetic but chiral metallic compound Co1/3NbS2, the magnetization induced by the tunneling current is shown to become detectable by its coupling to the magnetization of the tip itself. This results in a contrast across different chiral domains, achieving atomic-scale spatial resolution of structural chirality. To support the proposed mechanism, we used first-principles theory to compute the chirality-dependent current-induced magnetization and Berry curvature in the bulk of the material. Our demonstration of this magnetochiral tunneling effect opens up an avenue for investigating atomic-scale variations in the local crystallographic symmetry and electronic structure across the structural domain boundaries of low-symmetry nonmagnetic crystals.

Light-induced electronic polarization in antiferromagnetic Cr2O3.

In a solid, the electronic subsystem can exhibit incipient order with lower point group symmetry than the crystal lattice. Ultrafast external fields that couple exclusively to electronic order parameters have rarely been investigated, however, despite their potential importance in inducing exotic effects. Here we show that when inversion symmetry is broken by the antiferromagnetic order in Cr2O3, transmitting a linearly polarized light pulse through the crystal gives rise to an in-plane rotational symmetry-breaking (from C3 to C1) via optical rectification. Using interferometric time-resolved second harmonic generation, we show that the ultrafast timescale of the symmetry reduction is indicative of a purely electronic response; the underlying spin and crystal structures remain unaffected. The symmetry-broken state exhibits a dipole moment, and its polar axis can be controlled with the incident light. Our results establish a coherent nonlinear optical protocol by which to break electronic symmetries and produce unconventional electronic effects in solids.

Long-lifetime spin excitations near domain walls in 1T-TaS2.

SignificanceThere is an intense ongoing search for two-level quantum systems with long lifetimes for applications in quantum communication and computation. Much research has been focused on studying isolated spins in semiconductors or band insulators. Mott insulators provide an interesting alternative platform but have been far less explored. In this work we use a technique capable of resolving individual spins at atomic length scales, to measure the two-level switching of spin states in 1T-TaS2. We find quasi-1D chains of spin-1/2 electrons embedded in 1T-TaS2 which have exceptionally long lifetimes. The discovery of long-lived spin states in a tractable van der Waal material opens doors to using Mott systems in future quantum information applications.

Topological spin/structure couplings in layered chiral magnet Cr1/3TaS2: The discovery of spiral magnetic superstructure.

Chiral magnets have recently emerged as hosts for topological spin textures and related transport phenomena, which can find use in next-generation spintronic devices. The coupling between structural chirality and noncollinear magnetism is crucial for the stabilization of complex spin structures such as magnetic skyrmions. Most studies have been focused on the physical properties in homochiral states favored by crystal growth and the absence of long-ranged interactions between domains of opposite chirality. Therefore, effects of the high density of chiral domains and domain boundaries on magnetic states have been rarely explored so far. Herein, we report layered heterochiral Cr1/3TaS2, exhibiting numerous chiral domains forming topological defects and a nanometer-scale helimagnetic order interlocked with the structural chirality. Tuning the chiral domain density, we discovered a macroscopic topological magnetic texture inside each chiral domain that has an appearance of a spiral magnetic superstructure composed of quasiperiodic Néel domain walls. The spirality of this object can have either sign and is decoupled from the structural chirality. In weak, in-plane magnetic fields, it transforms into a nonspiral array of concentric ring domains. Numerical simulations suggest that this magnetic superstructure is stabilized by strains in the heterochiral state favoring noncollinear spins. Our results unveil topological structure/spin couplings in a wide range of different length scales and highly tunable spin textures in heterochiral magnets.

Ferrorotational Selectivity in Ilmenites.

Unlike what happens in conventional ferroics, the ferrorotational (FR) domain manipulation and visualization in FR materials are nontrivial as they are invariant under both space-inversion and time-reversal operations. FR domains have recently been observed by using the linear electrogyration (EG) effect and X-ray diffraction (XRD) diffraction mapping. However, ferrorotational selectivity, such as the selective processing of the FR domains and direct visualization of the FR domains, e.g., under an optical microscope, would be the next step to study the FR domains and their possible applications in technology. Unexpectedly, we discovered that the microscopic FR structural distortions in ilmenite crystals can be directly coupled with macroscopic mechanical rotations in such a way that FR domains can be visualized under an optical microscope after innovative rotational polishing, a combined ion milling with a specific rotational polishing, or a twisting-induced fracturing process. Thus, the FR domains could be a unique medium to register the memory of a rotational mechanical process due to a novel selective coupling between its microscopic structural rotations and an external macroscopic rotation. Analogous to the important enantioselectivity in modern chemistry and the pharmaceutical industry, this newly discovered ferrorotational selectivity opens up opportunities for FR manipulation and new FR functionality-based applications.

Tunable Single-Atomic Charges on a Cleaved Intercalated Transition Metal Dichalcogenide.

Control of a single ionic charge state by altering the number of bound electrons has been considered as an ultimate testbed for atomic charge-induced interactions and manipulations, and such subject has been studied in artificially deposited objects on thin insulating layers. We demonstrate that an entire layer of controllable atomic charges on a periodic lattice can be obtained by cleaving metallic Co1/3NbS2, an intercalated transition metal dichalcogenide. We identified a metastable charge state of Co with a different valence and manipulated atomic charges to form a linear chain of the metastable charge state. Density functional theory investigation reveals that the charge state is stable due to a modified crystal field at the surface despite the coupling between NbS2 and Co via a1g orbitals. The idea can be generalized to other combinations of intercalants and base matrices, suggesting that they can be a new platform to explore single-atom-operational 2D electronics/spintronics.

Linking emergent phenomena and broken symmetries through one-dimensional objects and their dot/cross products.

The symmetry of the whole experimental setups, including specific sample environments and measurables, can be compared with that of specimens for observable physical phenomena. We, first, focus on one-dimensional (1D) experimental setups, independent from any spatial rotation around one direction, and show that eight kinds of 1D objects (four; vector-like, the other four; director-like), defined in terms of symmetry, and their dot and cross products are an effective way for the symmetry consideration. The dot products form a Z2× Z2× Z2group with Abelian additive operation, and the cross products form a Z2× Z2group with Abelian additive operation or Q8, a non-Abelian group of order eight, depending on their signs. Those 1D objects are associated with characteristic physical phenomena. When a 3D specimen has symmetry operational similarity (SOS) with (identical or lower, but not higher, symmetries than) an 1D object with a particular phenomenon, the 3D specimen can exhibit the phenomenon. This SOS approach can be a transformative and unconventional avenue for symmetry-guided materials designs and discoveries.

Low-Loss Tunable Infrared Plasmons in the High-Mobility Perovskite (Ba,La)SnO3.

BaSnO3 exhibits the highest carrier mobility among perovskite oxides, making it ideal for oxide electronics. Collective charge carrier oscillations known as plasmons are expected to arise in this material, thus providing a tool to control the nanoscale optical field for optoelectronics applications. Here, the existence of relatively long-lived plasmons supported by high-mobility charge carriers in La-doped BaSnO3 (BLSO) is demonstrated. By exploiting the high spatial and energy resolution of electron energy-loss spectroscopy with a focused beam in a scanning transmission electron microscope, the dispersion, confinement ratio, and damping of infrared localized surface plasmons (LSPs) in BLSO nanoparticles are systematically investigated. It is found that LSPs in BLSO exhibit a high degree of spatial confinement compared to those sustained by noble metals and have relatively low losses and high quality factors with respect to other doped oxides. Further analysis clarifies the relation between plasmon damping and carrier mobility in BLSO. The results support the use of nanostructured degenerate semiconductors for plasmonic applications in the infrared region and establish a solid alternative to more traditional plasmonic materials.

Kinetically stabilized ferroelectricity in bulk single-crystalline HfO2:Y.

HfO2, a simple binary oxide, exhibits ultra-scalable ferroelectricity integrable into silicon technology. This material has a polymorphic nature, with the polar orthorhombic (Pbc21) form in ultrathin films regarded as the plausible cause of ferroelectricity but thought not to be attainable in bulk crystals. Here, using a state-of-the-art laser-diode-heated floating zone technique, we report the Pbc21 phase and ferroelectricity in bulk single-crystalline HfO2:Y as well as the presence of the antipolar Pbca phase at different Y concentrations. Neutron diffraction and atomic imaging demonstrate (anti)polar crystallographic signatures and abundant 90°/180° ferroelectric domains in addition to switchable polarization with negligible wake-up effects. Density-functional-theory calculations indicate that the yttrium doping and rapid cooling are the key factors for stabilization of the desired phase in bulk. Our observations provide insights into the polymorphic nature and phase control of HfO2, remove the upper size limit for ferroelectricity and suggest directions towards next-generation ferroelectric devices.

Charge Density Wave Vortex Lattice Observed in Graphene-Passivated 1T-TaS2 by Ambient Scanning Tunneling Microscopy.

The nearly commensurate charge density wave (CDW) excitations native to the transition-metal dichalcogenide crystal, 1T-TaS2, under ambient conditions are revealed by scanning tunneling microscopy (STM) and spectroscopy (STS) measurements of a graphene/TaS2 heterostructure. Surface potential measurements show that the graphene passivation layer prevents oxidation of the air-sensitive 1T-TaS2 surface. The graphene protective layer does not however interfere with probing the native electronic properties of 1T-TaS2 by STM/STS, which revealed that nearly commensurate CDW hosts an array of vortex-like topological defects. We find that these topological defects organize themselves to form a lattice with quasi-long-range order, analogous to the vortex Bragg glass in type-II superconductors but accessible in ambient conditions.

Excitations of Intercalated Metal Monolayers in Transition Metal Dichalcogenides.

We combine Raman scattering spectroscopy and lattice dynamics calculations to reveal the fundamental excitations of the intercalated metal monolayers in the FexTaS2 (x = 1/4, 1/3) family of materials. Both in- and out-of-plane modes are identified, each of which has trends that depend upon the metal-metal distance, the size of the van der Waals gap, and the metal-to-chalcogenide slab mass ratio. We test these trends against the response of similar systems, including Cr-intercalated NbS2 and RbFe(SO4)2, and demonstrate that the metal monolayer excitations are both coherent and tunable. We discuss the consequences of intercalated metal monolayer excitations for material properties and developing applications.

Ultrafast Modulations and Detection of a Ferro-Rotational Charge Density Wave Using Time-Resolved Electric Quadrupole Second Harmonic Generation.

We show the ferro-rotational nature of the commensurate charge density wave (CCDW) in 1T-TaS_{2} and track its dynamic modulations by temperature-dependent and time-resolved electric quadrupole rotation anisotropy-second harmonic generation (EQ RA-SHG), respectively. The ultrafast modulations manifest as the breathing and the rotation of the EQ RA-SHG patterns at three frequencies around the reported single CCDW amplitude mode frequency. A sudden shift of the triplet frequencies and a dramatic increase in the breathing and rotation magnitude further reveal a photoinduced transient CDW phase across a critical pump fluence of ∼0.5 mJ/cm^{2}.

Nature and evolution of incommensurate charge order in manganites visualized with cryogenic scanning transmission electron microscopy.

Incommensurate charge order in hole-doped oxides is intertwined with exotic phenomena such as colossal magnetoresistance, high-temperature superconductivity, and electronic nematicity. Here, we map, at atomic resolution, the nature of incommensurate charge-lattice order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature ([Formula: see text]93 K). In diffraction, the ordering wave vector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the ordered state forms lattice-locked regions over a few wavelengths interspersed with phase defects and changing periodicity. The cations undergo picometer-scale ([Formula: see text]6 pm to 11 pm) transverse displacements, suggesting that charge-lattice coupling is strong. We further unearth phase inhomogeneity in the periodic lattice displacements at room temperature, and emergent phase coherence at 93 K. Such local phase variations govern the long-range correlations of the charge-ordered state and locally change the periodicity of the modulations, resulting in wave vector shifts in reciprocal space. These atomically resolved observations underscore the importance of lattice coupling and phase inhomogeneity, and provide a microscopic explanation for putative "incommensurate" order in hole-doped oxides.

Atomic-Scale Observation of Topological Vortices in the Incommensurate Charge Density Wave of 2H-TaSe2.

It has been only recently realized that topological vortices associated with structural distortions or ordered spins are rather common in numerous materials where long-range interactions are not dominant. Incommensurate modulations that frequently occur in charge density wave (CDW) materials are often understood in terms of discommensurations with a periodic phase shift. The accumulation of a one-dimensional (1D) phase shift can result in, for example, CDW dislocations in 2H-TaSe2 with incommensurate CDW (I-CDW). Since any atomic-scale experimental investigation of CDW dislocations in 2H-TaSe2 has been lacking, we have performed the atomic-scale observation of 2H-TaSe2 with I-CDW, stabilized with Pd intercalation or strain, with scanning probe microscopy, and unveiled the existence of topological Z6 or Z4 vortices with topologically protected 2D winding movements of atomic displacement vectors. The discovery opens the ubiquitous nature of topological vortex domains and a new avenue to explore new facets of various incommensurate modulations or discommensurations.

Honeycomb-Lattice Mott Insulator on Tantalum Disulphide.

Effects of electron many-body interactions amplify in an electronic system with a narrow bandwidth opening a way to exotic physics. A narrow band in a two-dimensional (2D) honeycomb lattice is particularly intriguing as combined with Dirac bands and topological properties but the material realization of a strongly interacting honeycomb lattice described by the Kane-Mele-Hubbard model has not been identified. Here we report a novel approach to realize a 2D honeycomb-lattice narrow-band system with strongly interacting 5d electrons. We engineer a well-known triangular lattice 2D Mott insulator 1T-TaS_{2} into a honeycomb lattice utilizing an adsorbate superstructure. Potassium (K) adatoms at an optimum coverage deplete one-third of the unpaired d electrons and the remaining electrons form a honeycomb lattice with a very small hopping. Ab initio calculations show extremely narrow Z_{2} topological bands mimicking the Kane-Mele model. Electron spectroscopy detects an order of magnitude bigger charge gap confirming the substantial electron correlation as confirmed by dynamical mean field theory. It could be the first artificial Mott insulator with a finite spin Chern number.

Stabilization of Competing Ferroelectric Phases of HfO_{2} under Epitaxial Strain.

Hafnia (HfO_{2})-based thin films have promising applications in nanoscale electronic devices due to their robust ferroelectricity and integration with silicon. Identifying and stabilizing the ferroelectric phases of HfO_{2} have attracted intensive research interest in recent years. In this work, first-principles calculations on (111)-oriented HfO_{2} are used to discover that imposing an in-plane shear strain on the metastable tetragonal phase drives it to a polar phase. This in-plane-shear-induced polar phase is shown to be an epitaxial-strain-induced distortion of a previously proposed metastable ferroelectric Pnm2_{1} phase of HfO_{2}. This ferroelectric Pnm2_{1} phase can account for the recently observed ferroelectricity in (111)-oriented HfO_{2}-based thin films on a SrTiO_{3} (STO) (001) substrate [Nat. Mater. 17, 1095 (2018)NMAACR1476-112210.1038/s41563-018-0196-0]. Further investigation of this alternative ferroelectric phase of HfO_{2} could potentially improve the performances of HfO_{2}-based films in logic and memory devices.

Single-Crystal Growth and Room-Temperature Magnetocaloric Effect of X-Type Hexaferrite Sr2Co2Fe28O46.

X-type hexaferrites have been receiving considerable attention due to their promising applications in many magnetic-electronic fields. However, the growth of single-crystal X-type hexaferrite is still a challenge. Herein we reported, for the first time, the preparation of single crystal X-type hexaferrite Sr2Co2Fe28O46 (Sr2Co2X) with high-quality and large size using floating-zone method with laser as the heating source. The crystals show rhombohedral symmetry with space group of R-3m (No. 166, a = 5.8935(1) Å and c = 83.7438(17) Å). Co2+ and Fe3+ oxidation states were confirmed by the X-ray absorption near-edge spectroscopy. The prepared Sr2Co2X exhibits a spin reorientation transition from easy-cone to easy-axis at T2 of 343 K and a ferrimagnetism-paramagnetism transition at Curie temperature (TC) of ∼743 K. The spin reorientation transition was accompanied by magnetocaloric effect (MCE). Both conventional and inverse MCEs were observed near T2 with a magnetic field applied along the c-axis. The maximum value of the magnetic entropy change along the c-axis was evaluated to be 1.1 J/kg·K for a magnetic field change of 5 T.

Record High-Proximity-Induced Anomalous Hall Effect in (BixSb1-x)2Te3 Thin Film Grown on CrGeTe3 Substrate.

Quantum anomalous Hall effect (QAHE) can only be realized at extremely low temperatures in magnetically doped topological insulators (TIs) due to limitations inherent with the doping process. In an effort to boost the quantization temperature of QAHE, the magnetic proximity effect in magnetic insulator/TI heterostructures has been extensively investigated. However, the observed anomalous Hall resistance has never been more than several ohms, presumably owing to the interfacial disorders caused by the structural and chemical mismatch. Here, we show that, by growing (BixSb1-x)2Te3 (BST) thin films on structurally and chemically well-matched, ferromagnetic-insulating CrGeTe3 (CGT) substrates, the proximity-induced anomalous Hall resistance can be enhanced by more than an order of magnitude. This sheds light on the importance of structural and chemical matches for magnetic insulator/TI proximity systems.

Giant Magnetic Anisotropy Induced by Ligand LS Coupling in Layered Cr Compounds.

We propose a novel origin of magnetic anisotropy to explain the unusual magnetic behaviors of layered ferromagnetic Cr compounds (3d^{3}) wherein the anisotropy field varies from ≲0.01 to ∼3 T on changing the ligand atom in a common hexagonal structure. The effect of the ligand p orbital spin-orbit (LS) coupling on the magnetic anisotropy is explored by using four-site full multiplet cluster model calculations for energies involving the superexchange interaction at different spin axes. Our calculation shows that the anisotropy energy, which is the energy difference for different spin axes, is strongly affected not only by the LS coupling strength but also by the degree of p-d covalency in the layered geometry. This anisotropy energy involving the superexchange appears to dominate the magnetic anisotropy and even explains the giant magnetic anisotropy as large as 3 T observed in CrI_{3}.