Rashba-like Spin Textures in Graphene Promoted by Ferromagnet-Mediated Electronic Hybridization with a Heavy Metal.

Epitaxial graphene/ferromagnetic metal (Gr/FM) heterostructures deposited onto heavy metals have been proposed for the realization of spintronic devices because of their perpendicular magnetic anisotropy and sizable Dzyaloshinskii-Moriya interaction (DMI), allowing for both enhanced thermal stability and stabilization of chiral spin textures. However, establishing routes toward this goal requires the fundamental understanding of the microscopic origin of their unusual properties. Here, we elucidate the nature of the induced spin-orbit coupling (SOC) at Gr/Co interfaces on Ir. Through spin- and angle-resolved photoemission spectroscopy along with density functional theory, we show that the interaction of the heavy metals with the Gr layer via hybridization with the FM is the source of strong SOC in the Gr layer. Furthermore, our studies on ultrathin Co films underneath Gr reveal an energy splitting of ∼100 meV for in-plane and negligible for out-of-plane spin polarized Gr π-bands, consistent with a Rashba-SOC at the Gr/Co interface, which is either the fingerprint or the origin of the DMI. This mechanism vanishes at large Co thicknesses, where neither in-plane nor out-of-plane spin-orbit splitting is observed, indicating that Gr π-states are electronically decoupled from the heavy metal. The present findings are important for future applications of Gr-based heterostructures in spintronic devices.

Atomic Diffusion-Induced Polarization and Superconductivity in Topological Insulator-Based Heterostructures.

The proximity effect at a highly transparent interface of an s-wave superconductor (S) and a topological insulator (TI) provides a promising platform to create Majorana zero modes in artificially designed heterostructures. However, structural and chemical issues pertinent to such interfaces have been poorly explored so far. Here, we report the discovery of Pd diffusion-induced polarization at interfaces between superconductive Pd1+x(Bi0.4Te0.6)2 (xPBT, 0 ≤ x ≤ 1) and Pd-intercalated Bi2Te3 by using atomic-resolution scanning transmission electron microscopy. Our quantitative image analysis reveals that nanoscale lattice strain and QL polarity synergistically suppress and promote Pd diffusion at the normal and parallel interfaces, formed between Te-Pd-Bi triple layers (TLs) and Te-Bi-Te-Bi-Te quintuple layers (QLs), respectively. Further, our first-principles calculations unveil that the superconductivity of the xPBT phase and topological nature of the Pd-intercalated Bi2Te3 phase are robust against the broken inversion symmetry. These findings point out the necessity of considering the coexistence of electric polarization with superconductivity and topology in such S-TI systems.

Hopfion rings in a cubic chiral magnet.

Magnetic skyrmions and hopfions are topological solitons1-well-localized field configurations that have gained considerable attention over the past decade owing to their unique particle-like properties, which make them promising objects for spintronic applications. Skyrmions2,3 are two-dimensional solitons resembling vortex-like string structures that can penetrate an entire sample. Hopfions4-9 are three-dimensional solitons confined within a magnetic sample volume and can be considered as closed twisted skyrmion strings that take the shape of a ring in the simplest case. Despite extensive research on magnetic skyrmions, the direct observation of magnetic hopfions is challenging10 and has only been reported in a synthetic material11. Here we present direct observations of hopfions in crystals. In our experiment, we use transmission electron microscopy to observe hopfions forming coupled states with skyrmion strings in B20-type FeGe plates. We provide a protocol for nucleating such hopfion rings, which we verify using Lorentz imaging and electron holography. Our results are highly reproducible and in full agreement with micromagnetic simulations. We provide a unified skyrmion-hopfion homotopy classification and offer insight into the diversity of topological solitons in three-dimensional chiral magnets.

Optical Properties of MoSe2 Monolayer Implanted with Ultra-Low-Energy Cr Ions.

This paper explores the optical properties of an exfoliated MoSe2 monolayer implanted with Cr+ ions, accelerated to 25 eV. Photoluminescence of the implanted MoSe2 reveals an emission line from Cr-related defects that is present only under weak electron doping. Unlike band-to-band transition, the Cr-introduced emission is characterized by nonzero activation energy, long lifetimes, and weak response to the magnetic field. To rationalize the experimental results and get insights into the atomic structure of the defects, we modeled the Cr-ion irradiation process using ab initio molecular dynamics simulations followed by the electronic structure calculations of the system with defects. The experimental and theoretical results suggest that the recombination of electrons on the acceptors, which could be introduced by the Cr implantation-induced defects, with the valence band holes is the most likely origin of the low-energy emission. Our results demonstrate the potential of low-energy ion implantation as a tool to tailor the properties of two-dimensional (2D) materials by doping.

Long-Range Orbital Torque by Momentum-Space Hotspots.

While it is often assumed that the orbital response is suppressed and short ranged due to strong crystal field potential and orbital quenching, we show that the orbital response can be remarkably long ranged in ferromagnets. In a bilayer consisting of a nonmagnet and a ferromagnet, spin injection from the interface results in spin accumulation and torque in the ferromagnet, which rapidly oscillate and decay by spin dephasing. In contrast, even when an external electric field is applied only on the nonmagnet, we find substantially long-ranged induced orbital angular momentum in the ferromagnet, which can go far beyond the spin dephasing length. This unusual feature is attributed to nearly degenerate orbital characters imposed by the crystal symmetry, which form hotspots for the intrinsic orbital response. Because only the states near the hotspots contribute dominantly, the induced orbital angular momentum does not exhibit destructive interference among states with different momentum as in the case of the spin dephasing. This gives rise to a distinct type of orbital torque on the magnetization, increasing with the thickness of the ferromagnet. Such behavior may serve as critical long-sought evidence of orbital transport to be directly tested in experiments. Our findings open the possibility of using long-range orbital response in orbitronic device applications.

Inducing Single Spin-Polarized Flat Bands in Monolayer Graphene.

Due to the fundamental and technological implications in driving the appearance of non-trivial, exotic topological spin textures and emerging symmetry-broken phases, flat electronic bands in 2D materials, including graphene, are nowadays a relevant topic in the field of spintronics. Here, via europium doping, single spin-polarized bands are generated in monolayer graphene supported by the Co(0001) surface. The doping is controlled by Eu positioning, allowing for the formation of a K ¯ $\bar{\mathrm{K}}$ -valley localized single spin-polarized low-dispersive parabolic band close to the Fermi energy when Eu is on top, and of a π* flat band with single spin character when Eu is intercalated underneath graphene. In the latter case, Eu also induces a bandgap opening at the Dirac point while the Eu 4f states act as a spin filter, splitting the π band into two spin-polarized branches. The generation of flat bands with single spin character, as revealed by the spin- and angle-resolved photoemission spectroscopy (ARPES) experiments, complemented by density functional theory (DFT) calculations, opens up new pathways toward the realization of spintronic devices exploiting such novel exotic electronic and magnetic states.

Geometry-Induced Spin Filtering in Photoemission Maps from WTe_{2} Surface States.

We demonstrate that an important quantum material WTe_{2} exhibits a new type of geometry-induced spin filtering effect in photoemission, stemming from low symmetry that is responsible for its exotic transport properties. Through the laser-driven spin-polarized angle-resolved photoemission Fermi surface mapping, we showcase highly asymmetric spin textures of electrons photoemitted from the surface states of WTe_{2}. Such asymmetries are not present in the initial state spin textures, which are bound by the time-reversal and crystal lattice mirror plane symmetries. The findings are reproduced qualitatively by theoretical modeling within the one-step model photoemission formalism. The effect could be understood within the free-electron final state model as an interference due to emission from different atomic sites. The observed effect is a manifestation of time-reversal symmetry breaking of the initial state in the photoemission process, and as such it cannot be eliminated, but only its magnitude influenced, by special experimental geometries.

Emergence of zero-field non-synthetic single and interchained antiferromagnetic skyrmions in thin films.

Antiferromagnetic (AFM) skyrmions are envisioned as ideal localized topological magnetic bits in future information technologies. In contrast to ferromagnetic (FM) skyrmions, they are immune to the skyrmion Hall effect, might offer potential terahertz dynamics while being insensitive to external magnetic fields and dipolar interactions. Although observed in synthetic AFM structures and as complex meronic textures in intrinsic AFM bulk materials, their realization in non-synthetic AFM films, of crucial importance in racetrack concepts, has been elusive. Here, we unveil their presence in a row-wise AFM Cr film deposited on PdFe bilayer grown on fcc Ir(111) surface. Using first principles, we demonstrate the emergence of single and strikingly interpenetrating chains of AFM skyrmions, which can co-exist with the rich inhomogeneous exchange field, including that of FM skyrmions, hosted by PdFe. Besides the identification of an ideal platform of materials for intrinsic AFM skyrmions, we anticipate the uncovered knotted solitons to be promising building blocks in AFM spintronics.

Fabrication and Imaging Monatomic Ni Kagome Lattice on Superconducting Pb(111).

Artificial fabrication of a monolayer Kagome material can offer a promising opportunity to explore exceptional quantum states and phenomena in low dimensionality. Here, we have systematically studied a monatomic Ni Kagome lattice grown on Pb(111) by scanning tunneling microscopy/spectroscopy (STM/STS) and density functional theory (DFT). Sawtooth edge structures with distinct heights due to subsurface Ni atoms have been revealed, leading to asymmetric edge scattering of surface electrons on Pb(111). In addition, a local maximum at about -0.2 eV in tunneling spectra represents a manifestation of characteristic phase-destructive flat bands. Although charge transfer from underlying Pb(111) substrate results in a vanishing magnetic moment of Ni atoms, the proximity-induced superconducting gap is slightly enhanced on the Ni Kagome lattice. In light of single-atomic-layer Ni Kagome lattice on superconducting Pb(111) substrate, it could serve as an ideal platform to investigate the interplay between Kagome physics and superconductivity down to the two-dimensional limit.

Quasiparticle Self-Consistent GW Study of Simple Metals.

The GW method is a standard method to calculate the electronic band structure from first principles. It has been applied to a large variety of semiconductors and insulators but less often to metallic systems, in particular, with respect to a self-consistent employment of the method. In this work, we take a look at all-electron quasiparticle self-consistent GW (QSGW) calculations for simple metals (alkali and alkaline earth metals) based on the full-potential linearized augmented-plane-wave approach and compare the results to single-shot (i.e., non-selfconsistent) G0W0 calculations, density-functional theory (DFT) calculations in the local-density approximation, and experimental measurements. We show that, while DFT overestimates the bandwidth of most of the materials, the GW quasiparticle renormalization corrects the bandwidths in the right direction, but a full self-consistent calculation is needed to consistently achieve good agreement with photoemission data. The results mainly confirm the common belief that simple metals can be regarded as nearly free electron gases with weak electronic correlation. The finding is particularly important in light of a recent debate in which this seemingly established view has been contested.

Spanning Fermi arcs in a two-dimensional magnet.

The discovery of topological states of matter has led to a revolution in materials research. When external or intrinsic parameters break symmetries, global properties of topological materials change drastically. A paramount example is the emergence of Weyl nodes under broken inversion symmetry. While a rich variety of non-trivial quantum phases could in principle also originate from broken time-reversal symmetry, realizing systems that combine magnetism with complex topological properties is remarkably elusive. Here, we demonstrate that giant open Fermi arcs are created at the surface of ultrathin hybrid magnets where the Fermi-surface topology is substantially modified by hybridization with a heavy-metal substrate. The interplay between magnetism and topology allows us to control the shape and the location of the Fermi arcs by tuning the magnetization direction. The hybridization points in the Fermi surface can be attributed to a non-trivial mixed topology and induce hot-spots in the Berry curvature, dominating spin and charge transport as well as magneto-electric coupling effects.

Noncollinear Spin Current for Switching of Chiral Magnetic Textures.

We propose a concept of noncollinear spin current, whose spin polarization varies in space even in nonmagnetic crystals. While it is commonly assumed that the spin polarization of the spin Hall current is uniform, asymmetric local crystal potential generally allows the spin polarization to be noncollinear in space. Based on microscopic considerations, we demonstrate that such noncollinear spin Hall currents can be observed, for example, in layered Kagome Mn_{3}X (X=Ge, Sn) compounds. Moreover, by referring to atomistic spin dynamics simulations we show that noncollinear spin currents can be used to switch the chiral spin texture of Mn_{3}X in a deterministic way even in the absence of an external magnetic field. Our theoretical prediction can be readily tested in experiments, which will open a novel route toward electric control of complex spin structures in noncollinear antiferromagnets.

Is There a Polaron Signature in Angle-Resolved Photoemission of CsPbBr_{3}?

The formation of large polarons has been proposed as reason for the high defect tolerance, low mobility, low charge carrier trapping, and low nonradiative recombination rates of lead halide perovskites. Recently, direct evidence for large-polaron formation has been reported from a 50% effective mass enhancement in angle-resolved photoemission of CsPbBr_{3} over theory for the orthorhombic structure. We present in-depth band dispersion measurements of CsPbBr_{3} and GW calculations, which lead to similar effective masses at the valence band maximum of 0.203±0.016 m_{0} in experiment and 0.226 m_{0} in orthorhombic theory. We argue that the effective mass can be explained solely on the basis of electron-electron correlation and large-polaron formation cannot be concluded from photoemission data.

Fermi-Surface Origin of Skyrmion Lattices in Centrosymmetric Rare-Earth Intermetallics.

We show from first principles that barrel-shaped structures within the Fermi surface of the centrosymmetric intermetallic compounds GdRu_{2}Si_{2} and Gd_{2}PdSi_{3} give rise to Fermi surface nesting, which determines the strength and sign of quasi-two-dimensional Ruderman-Kittel-Kasuya-Yosida pairwise exchange interactions between the Gd moments. This is the principal mechanism leading to their helical single-q spin-spiral ground states, providing transition temperatures and magnetic periods in good agreement with experiment. Using atomistic spin-dynamic simulations, we draw a direct line between the subtleties of the three-dimensional Fermi surface topology and the stabilization of a square skyrmion lattice in GdRu_{2}Si_{2} at applied magnetic fields as observed in experiment.

Spin-orbit enabled all-electrical readout of chiral spin-textures.

Chirality and topology are intimately related fundamental concepts, which are heavily explored to establish spin-textures as potential magnetic bits in information technology. However, this ambition is inhibited since the electrical reading of chiral attributes is highly non-trivial with conventional current perpendicular-to-plane (CPP) sensing devices. Here we demonstrate from extensive first-principles simulations and multiple scattering expansion the emergence of the chiral spin-mixing magnetoresistance (C-XMR) enabling highly efficient all-electrical readout of the chirality and helicity of respectively one- and two-dimensional magnetic states of matter. It is linear with spin-orbit coupling in contrast to the quadratic dependence associated with the unveiled non-local spin-mixing anisotropic MR (X-AMR). Such transport effects are systematized on various non-collinear magnetic states - spin-spirals and skyrmions - and compared to the uncovered spin-orbit-independent multi-site magnetoresistances. Owing to their simple implementation in readily available reading devices, the proposed magnetoresistances offer exciting and decisive ingredients to explore with all-electrical means the rich physics of topological and chiral magnetic objects.

Theory of unidirectional magnetoresistance and nonlinear Hall effect.

We study the unidirectional magnetoresistance (UMR) and the nonlinear Hall effect (NLHE) in the ferromagnetic Rashba model. For this purpose we derive expressions to describe the response of the electric current quadratic in the applied electric field. We compare two different formalisms, namely the standard Keldysh nonequilibrium formalism and the Moyal-Keldysh formalism, to derive the nonlinear conductivities of UMR and NLHE. We find that both formalisms lead to identical numerical results when applied to the ferromagnetic Rashba model. The UMR and the NLHE nonlinear conductivities tend to be comparable in magnitude according to our calculations. Additionally, their dependencies on the Rashba parameter and on the quasiparticle broadening are similar. The nonlinear zero-frequency response considered here is several orders of magnitude higher than the one at optical frequencies that describes the photocurrent generation in the ferromagnetic Rashba model. Additionally, we compare our Keldysh nonequilibrium expression in the independent-particle approximation to literature expressions of the UMR that have been obtained within the constant relaxation time approximation of the Boltzmann formalism. We find that both formalisms converge to the same analytical formula in the limit of infinite relaxation time. However, remarkably, we find that the Boltzmann result does not correspond to the intraband term of the Keldysh expression. Instead, the Boltzmann result corresponds to the sum of the intraband term and an interband term that can be brought into the form of an effective intraband term due to thef-sum rule.

Magnetic skyrmion braids.

Skyrmions are vortex-like spin textures that form strings in magnetic crystals. Due to the analogy to elastic strings, skyrmion strings are naturally expected to braid and form complex three-dimensional patterns, but this phenomenon has not been explored yet. We found that skyrmion strings can form braids in cubic crystals of chiral magnets. This finding is confirmed by direct observations of skyrmion braids in B20-type FeGe using transmission electron microscopy. The theoretical analysis predicts that the discovered phenomenon is general for a wide family of chiral magnets. These findings have important implications for skyrmionics and propose a solid-state framework for applications of the mathematical theory of braids.

Ordering of Oxygen Vacancies and Related Ferroelectric Properties in HfO_{2-δ}.

Using density functional theory combined with an evolutionary algorithm, we investigate ferroelectricity in substoichiometric HfO_{2-δ} with fixed composition δ=0.25. We find that oxygen vacancies tend to cluster in the form of two-dimensional extended defects, revealing several patterns of local relative arrangements within an energy range of 100 meV per Hf atom. Two lowest-energy patterns result in polar monoclinic structures with different transformation properties. The lowest one elastically transforms to the ferroelectric orthorhombic structure via a shear deformation, overcoming an energy barrier, which is more than twice lower than in the stoichiometric hafnia. The second-lowest structure transforms at smaller volumes to a nonpolar tetragonal one. We discuss the experimentally observed wake-up effect, fatigue, and imprint in HfO_{2}-based ferroelectrics in terms of different local ordering of oxygen-vacancy extended defects, which favor specific crystallographic phases.

Topological magnon insulators in two-dimensional van der Waals ferromagnets CrSiTe3 and CrGeTe3: Toward intrinsic gap-tunability.

The bosonic analogs of topological insulators have been proposed in numerous theoretical works, but their experimental realization is still very rare, especially for spin systems. Recently, two-dimensional (2D) honeycomb van der Waals ferromagnets have emerged as a new platform for topological spin excitations. Here, via a comprehensive inelastic neutron scattering study and theoretical analysis of the spin-wave excitations, we report the realization of topological magnon insulators in CrXTe3 (X = Si, Ge) compounds. The nontrivial nature and intrinsic tunability of the gap opening at the magnon band-crossing Dirac points are confirmed, while the emergence of the corresponding in-gap topological edge states is demonstrated theoretically. The realization of topological magnon insulators with intrinsic gap-unability in this class of remarkable 2D materials will undoubtedly lead to new and fascinating technological applications in the domain of magnonics and topological spintronics.