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CrI3 is a layered ferromagnetic insulator that has recently attracted enormous interest as it was the first example of a stand-alone monolayer ferromagnet, paving the way towards the study of two-dimensional magnetic materials and their use as building blocks of hybrid van der Waals layered heterostructures. Here we go one step down in the dimensionality ladder and report the synthesis and characterization of a tubular one-dimensional van der Waals heterostructure where CrI3 nanotubes are encapsulated within multiwall carbon nanotubes, integrating a magnetic insulator and a conductor. By means of the capillary filling of multi-wall carbon nanotubes (MWCNT), we obtained single-wall CrI3 nanotubes with diameters ranging between 2 nm and 10 nm, with an average of 5.3 nm. Using aberration corrected electron microscopy in combination with spectroscopic techniques we confirm the structure and chemical composition of the nanotubes. SQUID measurements, combined with element-specific X-ray magnetic circular dichroism (XMCD) indicate unequivocally that the Cr atoms in encapsulated CrI3 nanotubes are magnetic with a collective state compatible with a radial magnetization state predicted both by first-principles calculations and a model Hamiltonian. Our results represent a step forward in establishing 1D van der Waals heterostructures as a playground for the exploration of non-collinear magnetic states arising from the interplay between magnetic anisotropy and curvature in tubular geometries., Comment: 19 pages with 5 figures

Nowadays a wide number of applications based on magnetic materials relies on the properties arising at the interface between different layers in complex heterostructures engineered at the nanoscale. In ferromagnetic/heavy metal multilayers, such as the [Co/Pt]$_N$ and [Co/Pd]$_N$ systems, the magnetic proximity effect was demonstrated to be asymmetric, thus inducing a magnetic moment on the Pt(Pd) layer that is typically higher at the top Co/Pt(Pd) interface. In this work, advanced spectroscopic and imaging techniques were combined with theoretical approaches to clarify the origin of this asymmetry both in Co/Pt trilayers and, for the first time, in multilayer systems that are more relevant for practical applications. The different magnetic moment induced at the Co/Pt interfaces was correlated to the microstructural features, which are in turn affected by the growth processes that induce a different intermixing during the film deposition, thus influencing the interface magnetic profile., Comment: Main paper: 22 pages, 5 figures. Supporting information: 14 pages, 12 figures

CeRh$_2$As$_2$ is a new multiphase superconductor with strong suggestions for an additional itinerant multipolar ordered phase. The modeling of the low temperature properties of this heavy fermion compound requires a quartet Ce$^{3+}$ crystal-field ground state. Here we provide the evidence for the formation of such a quartet state using x-ray spectroscopy. Core-level photoelectron and x-ray absorption spectroscopy confirm the presence of Kondo hybridization in CeRh$_2$As$_2$. The temperature dependence of the linear dichroism unambiguously reveils the impact of Kondo physics for coupling the Kramer's doublets into an effective quasi-quartet. Non-resonant inelastic x-ray scattering data find that the $|\Gamma_7^- \rangle$ state with its lobes along the 110 direction of the tetragonal structure ($xy$ orientation) contributes most to the multi-orbital ground state of CeRh$_2$As$_2$., Comment: 8 pages, 7 figures

The recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ benchmark the (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi$_2$Te$_4$ septuple layers (SL). However, the QAHE realization is complicated in MnBi$_2$Te$_4$ and MnBi$_4$Te$_7$ due to the substantial antiferromagnetic (AFM) coupling between the SL. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SL with an increasing number $n$ of Bi$_2$Te$_3$ layers. However, the mechanisms driving the FM state and the number of necessary QLs are not understood, and the surface magnetism remains obscure. Here, we demonstrate robust FM properties in MnBi$_6$Te$_{10}$ ($n = 2$) with $T_C \approx 12$ K and establish their origin in the Mn/Bi intermixing phenomenon by a combined experimental and theoretical study. Our measurements reveal a magnetically intact surface with a large magnetic moment, and with FM properties similar to the bulk. Our investigation thus consolidates the MnBi$_6$Te$_{10}$ system as perspective for the QAHE at elevated temperatures.

Ferromagnetism (FM) is the cornerstone of permanent magnets, data storage and other technologies that directly impact our everyday life by their implementation in standard applications and devices. When downscaling bulk materials into their two-dimensional (2D) magnetic isotropic form, the Mermin-Wagner theorem precludes this collective state mediated by short-range exchange interactions at finite temperatures. Interestingly, this prediction fails when significant magnetic anisotropy is present in the material, as recently demonstrated in single layered van der Waals crystals. Before the latter, single layer metal-organic frameworks (MOFs) grown on metallic supports were one of the earliest candidates for achieving 2D-FM. Such high expectations were based on the chemical and spacing control of the 2D-MOF magnetic centers, the tunability of the organic linkers and the rich self-assembled architectures displayed. However, despite many attempts, extended FM in 2D-MOFs has been experimentally elusive. In this work, we demonstrate that extended, cooperative FM takes place in an atom thick 2D-MOF consisting of 9,10-dicyanoanthracene (DCA) molecules and Fe adatoms grown on Au(111). We show this by means of an experimental multitechnique approach that is endorsed by state-of-the art first-principles calculations. Particularly, this 2D ferromagnet follows a first order transition with TC ~ 35 K, which is driven by exchange interactions mainly through the molecular linkers (J=2 meV) and exhibits an out-of-plane square-like hysteresis loop. The strict periodicity of our 2D-MOF allows us to envision the fabrication of ultra-dense single atom magnetic memories and opens the way to explore periodic magnetic 2D-models that could considerably increase the fundamental superparamagnetic limit., Comment: Main text 18 pages containing 3 figures. Supplementary material 18 pages containing 8 figures

Using light to control transient phases in quantum materials is an emerging route to engineer new properties and functionality, with both thermal and non-thermal phases observed out of equilibrium. Transient phases are expected to be heterogeneous, either through photo-generated domain growth or by generating topological defects, and this impacts the dynamics of the system. However, this nanoscale heterogeneity has not been directly observed. Here we use time- and spectrally resolved coherent X-ray imaging to track the prototypical light induced insulator-to-metal phase transition in vanadium dioxide on the nanoscale with femtosecond time resolution. We show that the early-time dynamics are independent of the initial spatial heterogeneity and observe a 200 fs switch to the metallic phase. A heterogeneous response emerges only after hundreds of picoseconds. Through spectroscopic imaging, we reveal that the transient metallic phase is a highly orthorhombically strained rutile metallic phase, an interpretation that is in contrast to those based on spatially averaged probes. Our results demonstrate the critical importance of spatially and spectrally resolved measurements for understanding and interpreting the transient phases of quantum materials.

Oxygen packaging in transition metal oxides determines the metal-oxygen hybridization and electronic occupation at metal orbitals. Strontium vanadate (SrVO$_3$), having a single electron in a $3d$ orbital, is thought to be the simplest example of strongly correlated metallic oxides. Here, we determine the effects of epitaxial strain on the electronic properties of SrVO$_3$ thin films, where the metal-oxide sublattice is corner-connected. Using x-ray absorption and x-ray linear dichroism at the V $L_{2,3}$ and O $K$-edges, it is observed that tensile or compressive epitaxial strain change the hierarchy of orbitals within the $t_{2g}$ and $e_g$ manifolds. Data show a remarkable $2p-3d$ hybridization, as well as a strain-induced reordering of the V $3d$($t_{2g}$, $e_g$) orbitals. The latter is itself accompanied by a consequent change of hybridization that modulates the hybrid $\pi^*$ and $\sigma^*$ orbitals and the carrier population at the metal ions, challenging a rigid band picture.

Scalable fabrication of magnetic 2D materials and heterostructures constitutes a crucial step for scaling down current spintronic devices and the development of novel spintronic applications. Here, we report on van der Waals (vdW) epitaxy of the layered magnetic metal Fe$_3$GeTe$_2$ - a 2D crystal with highly tunable properties and a high prospect for room temperature ferromagnetism - directly on graphene by employing molecular beam epitaxy. Morphological and structural characterization confirmed the realization of large-area, continuous Fe$_3$GeTe$_2$/graphene heterostructure films with stable interfaces and good crystalline quality. Furthermore, magneto-transport and X-ray magnetic circular dichroism investigations confirmed a robust out-of-plane ferromagnetism in the layers, comparable to state-of-the-art exfoliated flakes from bulk crystals. These results are highly relevant for further research on wafer-scale growth of vdW heterostructures combining Fe$_3$GeTe$_2$ with other layered crystals such as transition metal dichalcogenides for the realization of multifunctional, atomically thin devices.

The signature of magnetism without a ferromagnet in a non-magnetic heterostructure is novel as well as fascinating from fundamental research point of view. It has been shown by Al'Mari et al: that magnetism can be induced at the interface of Cu/C60 due to change in density of states. However, the quantification of such interfacial magnetic moment has not been performed yet. In order to quantify the induced magnetic moment in Cu, we have performed X-ray magnetic circular dichroism (XMCD) measurements on Cu/C$_{60}$ multilayers. We have observed room temperature ferromagnetism in Cu/C$_{60}$ stack. Further XMCD measurements show that ~0.01 $\mu_B$/atom magnetic moment has been induced in Cu at the Cu/C$_{60}$ interface., Comment: 5 pages, 5 figures

A combination of theoretical modelling and experiments reveals the origin of the large perpendicular magnetic anisotropy (PMA) that appears in nanometer-thick epitaxial Co films intercalated between graphene (Gr) and a heavy metal (HM) substrate, as a function of the Co thickness. High quality epitaxial Gr/Co\n/HM(111) (HM=Pt,Ir) heterostructures are grown by intercalation below graphene, which acts as a surfactant that kinetically stabilizes the pseudomorphic growth of highly perfect Co face-centered tetragonal ($fct$) films, with a reduced number of stacking faults as the only structural defect observable by high resolution scanning transmission electron microscopy (HR-STEM). Magneto-optic Kerr effect (MOKE) measurements show that such heterostructures present PMA up to large Co critical thicknesses of about 4~nm (20~ML) and 2~nm (10~ML) for Pt and Ir substrates, respectively, while X-ray magnetic circular dichroism (XMCD) measurements show an inverse power law of the anistropy of the orbital moment with Co thickness, reflecting its interfacial nature, that changes sign at about the same critical values. First principles calculations show that, regardless of the presence of graphene, ideal Co $fct$ films on HM buffers do not sustain PMAs beyond around 6~MLs due to the in-plane contribution of the inner bulk-like Co layers. The large experimental critical thicknesses sustaining PMA can only be retrieved by the inclusion of structural defects that promote a local $hcp$ stacking such as twin boundaries or stacking faults. Remarkably, a layer resolved analysis of the orbital momentum anisotropy reproduces its interfacial nature, and reveals that the Gr/Co interface contribution is comparable to that of the Co/Pt(Ir)., Comment: 25 pages, 4 figures, 1 table

The development of high-density magnetic recording media is limited by the superparamagnetism in very small ferromagnetic crystals. Hard magnetic materials with strong perpendicular anisotropy offer stability and high recording density. To overcome the difficulty of writing media with a large coercivity, heat assisted magnetic recording (HAMR) has been developed, rapidly heating the media to the Curie temperature Tc before writing, followed by rapid cooling. Requirements are a suitable Tc, coupled with anisotropic thermal conductivity and hard magnetic properties. Here we introduce Rh2CoSb as a new hard magnet with potential for thin film magnetic recording. A magnetocrystalline anisotropy of 3.6 MJm-3 is combined with a saturation magnetization of {\mu}0Ms = 0.52 T at 2 K (2.2 MJm-3 and 0.44 T at room-temperature). The magnetic hardness parameter of 3.7 at room temperature is the highest observed for any rare-earth free hard magnet. The anisotropy is related to an unquenched orbital moment of 0.42 {\mu}B on Co, which is hybridized with neighbouring Rh atoms with a large spin-orbit interaction. Moreover, the pronounced temperature-dependence of the anisotropy that follows from its Tc of 450 K, together with a high thermal conductivity of 20 Wm-1K-1, makes Rh2CoSb a candidate for development for heat assisted writing with a recording density in excess of 10 Tb/in2.

Long before the recent fascination with two-dimensional materials, the critical behaviour and universality scaling of phase transitions in low-dimensional systems has been a topic of great interest. Particularly intriguing is the case of long-range magnetic order in two dimensions, once considered to be excluded in systems with continuous symmetry by the Hohenberg-Mermin-Wagner theorem. While an out-of-plane anisotropy has been shown to stabilize 2D magnetic order, this proof has remained elusive for a 2D magnet with in-plane rotational symmetry. Here, we construct a nearly ideal easy-plane system, a CrCl3 monolayer grown on Graphene/6H-SiC (0001), and unambiguously demonstrate robust in-plane ferromagnetic ordering with a critical scaling behaviour characteristic of a 2D-XY system. These observations suggest the first realization of a finite-size Berezinskii-Kosterlitz-Thouless (BKT) phase transition in a large-area, quasi-freestanding, van der Waals monolayer magnet with a XY universality class; and further constitute an ideal platform to study exotic phenomena like superfluid spin transport or 2D topological in-plane spin textures -- such as merons.

Controlling interfacial interactions in magnetic/topological insulator heterostructures is a major challenge for the emergence of novel spin-dependent electronic phenomena. As for any rational design of heterostructures that rely on proximity effects, one should ideally retain the overall properties of each component while tuning interactions at the interface. However, in most inorganic interfaces interactions are too strong, consequently perturbing, and even quenching, both the magnetic moment and the topological surface states at each side of the interface. Here we show that these properties can be preserved by using ligand chemistry to tune the interaction of magnetic ions with the surface states. By depositing Co-based porphyrin and phthalocyanine monolayers on the surface of Bi$_2$Te$_3$ thin films, robust interfaces are formed that preserve undoped topological surface states as well as the pristine magnetic moment of the divalent Co ions. The selected ligands allow us to tune the interfacial hybridization within this weak interaction regime. These results, which are in stark contrast with the observed suppression of the surface state at the first quintuple layer of Bi$_2$Se$_3$ induced by the interaction with Co phthalocyanines, demonstrate the capability of planar metal-organic molecules to span interactions from the strong to the weak limit.

Room-temperature ferrimagnetism was discovered for the anti-site-disordered perovskite Ca2MnOsO6 with Tc = 305 K. Ca2MnOsO6 crystallizes into an orthorhombic structure with a space group of Pnma, in which Mn and Os share the oxygen-coordinated-octahedral site at an equal ratio without a noticeable ordered arrangement. The material is electrically semiconducting with variable-range-hopping behavior. X-ray absorption spectroscopy confirmed the trivalent state of the Mn and the pentavalent state of the Os. X-ray magnetic circular dichroism spectroscopy reveals that the Mn and Os magnetic moments are aligned antiferromagnetically, thereby classifying the material as a ferrimagnet which is in accordance with band structure calculations. It is intriguing that the magnetic signal of the Os is very weak, and that the observed total magnetic moment is primarily due to the Mn. The Tc = 305 K is the second highest in the material category of so-called disordered ferromagnets such as CaRu1-xMnxO3, SrRu1-xCrxO3, and CaIr1-xMnxO3, and hence, may support the development of spintronic oxides with relaxed requirements concerning the anti-site disorder of the magnetic ions.

Since the discovery of the quantum anomalous Hall effect in the magnetically doped topological insulators (MTI) Cr:(Bi,Sb)$_2$Te$_3$ and V:(Bi,Sb)$_2$Te$_3$, the search for the exchange coupling mechanisms underlying the onset of ferromagnetism has been a central issue, and a variety of different scenarios have been put forward. By combining resonant photoemission, X-ray magnetic dichroism and multiplet ligand field theory, we determine the local electronic and magnetic configurations of V and Cr impurities in (Bi,Sb)$_2$Te$_3$. While strong pd hybridisation is found for both dopant types, their 3d densities of states show pronounced differences. State-of-the-art first-principles calculations show how these impurity states mediate characteristic short-range pd exchange interactions, whose strength sensitively varies with the position of the 3d states relative to the Fermi level. Measurements on films with varying host stoichiometry support this trend. Our results establish the essential role of impurity-state mediated exchange interactions in the magnetism of MTI.

The fast spin dynamics provide many opportunities for the future communication and memory technologies. One of the most promising examples is the domain wall (DW) racetrack memory. To achieve fast device performances, the high-speed motion of DWs is naturally demanded that leaves antiferromagnets (AFMs) and compensated ferrimagnets (FIMs) as the promising materials. While controlling and probing the dynamics of DWs in AFMs remains challenging, the fast motion of DWs with velocities around 1500 m/s has been demonstrated in metallic FIMs. The velocity of DWs in metallic FIMs is, however, suppressed by the magnetic damping of conduction electrons, which motivates us to explore how fast DWs can move in insulating FIMs where the conduction electron is absent. In this work, through synthesizing compensated FIM insulator Gd3Fe5O12 thin films with a perpendicular magnetic anisotropy, we demonstrate that the spin-orbit torque (SOT) induced motion of DWs along the Gd3Fe5O12/Pt racetrack can approach 6000 m/s. Our results show that the exceptionally fast motion of DWs can be achieved in compensated FIM insulators owing to small damping inherent to magnetic insulators, which could potentially facilitate the emerging ultrahigh-speed spintronic logics and racetrack memories by introducing insulating compensated FIMs as a new material platform., Comment: All comments are welcome

Combinations of non-trivial band topology and long-range magnetic order hold promise for realizations of novel spintronic phenomena, such as the quantum anomalous Hall effect and the topological magnetoelectric effect. Following theoretical advances material candidates are emerging. Yet, a compound with a band-inverted electronic structure and an intrinsic net magnetization remains unrealized. MnBi$_2$Te$_4$ is a candidate for the first antiferromagnetic topological insulator and the progenitor of a modular (Bi$_2$Te$_3$)$_n$(MnBi$_2$Te$_4$) series. For $n$ = 1, we confirm a non-stoichiometric composition proximate to MnBi$_4$Te$_7$ and establish an antiferromagnetic state below 13 K followed by a state with net magnetization and ferromagnetic-like hysteresis below 5 K. Angle-resolved photoemission experiments and density-functional calculations reveal a topological surface state on the MnBi$_4$Te$_7$(0001) surface, analogous to the non-magnetic parent compound Bi$_2$Te$_3$. Our results render MnBi$_4$Te$_7$ as a band-inverted material with an intrinsic net magnetization and a complex magnetic phase diagram providing a versatile platform for the realization of different topological phases., Comment: Accepted to Phys. Rev. X

A major challenge for future spintronics is to develop suitable spin transport channels with long spin lifetime and propagation length. Graphene can meet these requirements, even at room temperature. On the other side, taking advantage of the fast motion of chiral textures, i.e., N\'eel-type domain walls and magnetic skyrmions, can satisfy the demands for high-density data storage, low power consumption and high processing speed. We have engineered epitaxial structures where an epitaxial ferromagnetic Co layer is sandwiched between an epitaxial Pt(111) buffer grown in turn onto MgO(111) substrates and a graphene layer. We provide evidence of a graphene-induced enhancement of the perpendicular magnetic anisotropy up to 4 nm thick Co films, and of the existence of chiral left-handed N\'eel-type domain walls stabilized by the effective Dzyaloshinskii-Moriya interaction (DMI) in the stack. The experiments show evidence of a sizeable DMI at the gr/Co interface, which is described in terms of a conduction electron mediated Rashba-DMI mechanism and points opposite to the Spin Orbit Coupling-induced DMI at the Co/Pt interface. In addition, the presence of graphene results in: i) a surfactant action for the Co growth, producing an intercalated, flat, highly perfect fcc film, pseudomorphic with Pt and ii) an efficient protection from oxidation. The magnetic chiral texture is stable at room temperature and grown on insulating substrate. Our findings open new routes to control chiral spin structures using interfacial engineering in graphene-based systems for future spin-orbitronics devices fully integrated on oxide substrates., Comment: 10 pages, 6 figures

Pure spin currents hold promises for an energy-friendlier spintronics. They can be generated by a flow of charge along a non-magnetic metal having a large spin-orbit coupling. It produces a spin accumulation at its surfaces, controllable by the magnetization of an adjacent ferromagnetic layer. Paramagnetic metals typically used are close to a ferromagnetic instability and thus magnetic proximity effects can contribute to the observed angular-dependent magnetoresistance (ADMR). As interface phenomena govern the spin conductance across the metal/ferromagnetic-insulator heterostructures, unraveling these distinct contributions is pivotal to full understanding of spin current conductance. We report here x-ray absorption and magnetic circular dichroism (XMCD) at Pt-M and (Co,Fe)-L absorption edges and atomically-resolved energy loss electron spectroscopy (EELS) data of Pt/CoFe2O4 bilayers where CoFe2O4 layers have been capped by Pt grown at different temperatures. It turns out that the ADMR differs dramatically, being either dominated by spin Hall magnetoresistance (SMR) associated to spin Hall effect or anisotropic magnetoresistance (AMR). The XMCD and EELS data indicate that the Pt layer grown at room temperature does not display any magnetic moment, whereas when grown at higher temperature it is magnetic due to interfacial Pt-(Co,Fe) alloying. These results allow disentangling spin accumulation from interfacial chemical reconstructions and for tailoring the angular dependent magnetoresistance., Comment: ACS Applied Materials & Interfaces, 2018 (under revision)