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Occupancy of different structural positions in a crystal lattice often seems to play a key role in material prop-erties. Several experimental techniques have been developed to uncover this issue, all of them being mostly bulk sensitive. However, many materials including topological insulators (TIs), which are among the most intriguing modern materials, are intended to be used in devices as thin films, for which the sublattice occupancy may differ from the bulk. One of the possible approaches to occupancy analysis is X-ray Photoelectron Diffraction (XPD), a structural method in surface science with chemical sensitivity. We applied this method in a case study of Sb2(Te1-xSex)3 mixed crystals, which belong to prototypical TIs. We used high-angle annular dark field (HAADF) scanning transmission electron microscopy (STEM) as a reference method to verify our analysis. We revealed that the XPD data for vacuum cleaved bulk crystals are in excellent agreement with the reference ones. Also, we demonstrate that the anion occupancy near a naturally formed surface can be rather different from that of the bulk. The present results are relevant for a wide range of compositions where the system remains a topological phase, as we ultimately show by probing the transiently occupied topological surface state above the Fermi level by ultrafast photoemission.

Topological phases of matter offer exciting possibilities to realize lossless charge and spin information transport on ultrafast time scales. However, this requires detailed knowledge of their nonequilibrium properties. Here, we employ time-, spin- and angle-resolved photoemission to investigate the ultrafast response of the Sb(111) spin-polarized surface state to femtosecond-laser excitation. The surface state exhibits a giant mass enhancement which is observed as a kink structure in its energy-momentum dispersion above the Fermi level. The kink structure, originating from the direct coupling of the surface state to the bulk continuum, is characterized by an abrupt change in the group velocity by ~70%, in agreement with our GW-based band structure calculations. Our observation of this connectivity in the transiently occupied band structure enables the unambiguous experimental verification of the topological nature of the surface state. The influence of bulk-surface coupling is further confirmed by our measurements of the electron dynamics, which show that bulk and surface states behave as a single thermalizing electronic population with distinct contributions from low-k electron-electron and high-k electron-phonon scatterings. These findings are important for future applications of topological semimetals and their excitations in ultrafast spintronics. Understanding the coupling between spin-polarised topological surface states and the bulk provides insight into ultrafast spin dynamics. Here, this coupling is shown to be accompanied by a large mass enhancement in the Sb(111) surface electronic structure, leading to unusual dynamics.

Spin-orbit interaction and structure inversion asymmetry in combination with magnetic ordering is a promising route to novel materials with highly mobile spin-polarized carriers at the surface. Spin-resolved measurements of the photoemission current from the Si-terminated surface of the antiferromagnet TbRh2Si2 and their analysis within an ab initio one-step theory unveil an unusual triple winding of the electron spin along the fourfold-symmetric constant energy contours of the surface states. A two-band k⋅p model is presented that yields the triple winding as a cubic Rashba effect. The curious in-plane spin-momentum locking is remarkably robust and remains intact across a paramagnetic-antiferromagnetic transition in spite of spin-orbit interaction on Rh atoms being considerably weaker than the out-of-plane exchange field due to the Tb 4f moments., This work was supported by the German Research Foundation (Grants No. KR-3831/5-1, No. LA655/20-1, GRK1621, Fermi-NESt No. ANR-16-CE92-0018, and SFB1143, project-id 247310070) and the Spanish Ministry of Science, Innovation, and Universities (Grant Nos. FIS2016-76617-P and MAT-2017-88374-P). We also acknowledge funding from the Department of Education of the Basque government (Grant No. IT1164-19), St. Petersburg State University (Project ID 51126254), and the Russian Foundation for Basic Research (Grant No. 20-32-70127). The SR-ARPES experiments at HiSOR were performed with the approval of the Proposal Assessing Committee of the Hiroshima Synchrotron Radiation Center (Proposal No. 18BG023). We also acknowledge the Impuls-und Vernetzungsfonds der Helmholtz Gemeinschaft (Grant No. HRSF-0067)

Renewed interest in the ferroelectric semi-conductor germanium telluride was recently triggered by the direct observation of a giant Rashba effect and a 30-year-old dream about a functional spin field-effect transistor. In this respect, all-electrical control of the spin texture in this material in combination with ferroelectric properties at the nanoscale would create advanced functionalities in spintronics and data information processing. Here, we investigate the atomic and electronic properties of GeTe bulk single crystals and their (111) surfaces. We succeeded in growing crystals possessing solely inversion domains of similar to 10 nm thickness parallel to each other. Using HAADF-TEM we observe two types of domain boundaries, one of them being similar in structure to the van der Waals gap in layered materials. This structure is responsible for the formation of surface domains with preferential Te-termination (similar to 68%) as we determined using photoelectron diffraction and XPS. The lateral dimensions of the surface domains are in the range of similar to 10-100 nm, and both Ge- and Te-terminations reveal no reconstruction. Using spin-ARPES we establish an intrinsic quantitative relationship between the spin polarization of pure bulk states and the relative contribution of different terminations, a result that is consistent with a reversal of the spin texture of the bulk Rashba bands for opposite configurations of the ferroelectric polarization within individual nanodomains. Our findings are important for potential applications of ferroelectric Rashba semiconductors in nonvolatile spintronic devices with advanced memory and computing capabilities at the nanoscale.

By measuring the spin polarization of GeTe films as a function of light polarization we observed that the bulk states are fully spin polarized in the initial state, in strong contrast with observations for other systems with a strong spin orbit interaction and the surface derived states in the same system. In agreement with state of the art theory, our experimental results show that fully spin polarized bulk states are an intrinsic property of the ferroelectric Rashba semiconductor amp; 945; GeTe 111 . The fact that the measured spin polarization vector does not change with light polarization can be explained by the absence of a mixing of states with a different total angular momentum J

Topological insulators constitute a new phase of matter protected by symmetries. Time-reversal symmetry protects strong topological insulators of the Z2 class, which possess an odd number of metallic surface states with dispersion of a Dirac cone. Topological crystalline insulators are merely protected by individual crystal symmetries and exist for an even number of Dirac cones. Here, we demonstrate that Bi-doping of Pb1−xSnxSe (111) epilayers induces a quantum phase transition from a topological crystalline insulator to a Z2 topological insulator. This occurs because Bi-doping lifts the fourfold valley degeneracy and induces a gap at \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\bar \Gamma $$\end{document}Γ¯, while the three Dirac cones at the \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${\bar{\rm M}}$$\end{document}M¯ points of the surface Brillouin zone remain intact. We interpret this new phase transition as caused by a lattice distortion. Our findings extend the topological phase diagram enormously and make strong topological insulators switchable by distortions or electric fields., Transitions between topological phases of matter protected by different symmetries remain rare. Here, Mandal et al. report a quantum phase transition from a topological crystalline insulator to a Z2 topological insulator by doping Bi into Pb1-xSnxSe (111) thin films.

To realize spintronic devices based on topological insulators (TIs), well-defined interfaces between magnetic metals and TIs are required. Here, we characterize atomically precisely the interface between the 3d transition metal Fe and the TI Bi2Te3 at different stages of its formation. Using photoelectron diffraction and holography, we show that after deposition of up to 3 monolayers Fe on Bi2Te3 at room temperature, the Fe atoms are ordered at the interface despite the surface disorder revealed by our scanning-tunneling microscopy images. We find that Fe occupies two different sites: a hollow adatom deeply relaxed into the Bi2Te3 quintuple layers and an interstitial atom between the third (Te) and fourth (Bi) atomic layers. For both sites, our core-level photoemission spectra and density-functional theory calculations demonstrate simultaneous chemical bonding of Fe to both Te and Bi atoms. We further show that upon deposition of Fe up to a thickness of 20 nm, the Fe atoms penetrate deeper into the bulk forming a 2-5 nm interface layer containing FeTe. In addition, excessive Bi is pushed down into the bulk of Bi2Te3 leading to the formation of septuple layers of Bi3Te4 within a distance of similar to 25 nm from the interface. Controlling the magnetic properties of the complex interface structures revealed by our work will be of critical importance when optimizing the efficiency of spin injection in TI-based devices.

SmB6 is predicted to be the first member of the intersection of topological insulators and Kondo insulators, strongly correlated materials in which the Fermi level lies in the gap of a many-body resonance that forms by hybridization between localized and itinerant states. While robust, surface-only conductivity at low temperature and the observation of surface states at the expected high symmetry points appear to confirm this prediction, we find both surface states at the (100) surface to be topologically trivial. We find the \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$${\bar{\varGamma }}$$\end{document}Γ¯ state to appear Rashba split and explain the prominent \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\bar X$$\end{document}X¯ state by a surface shift of the many-body resonance. We propose that the latter mechanism, which applies to several crystal terminations, can explain the unusual surface conductivity. While additional, as yet unobserved topological surface states cannot be excluded, our results show that a firm connection between the two material classes is still outstanding., Samarium hexahoride is argued to be a topological Kondo insulator, but this claim remains under debate. Here, Hlawenka et al. provide a topologically trivial explanation for the conducting states at the (100) surface of samarium hexaboride; an explanation based on Rashba splitting and a surface shift of the Kondo resonance.

Rapid development of experimental techniques has enabled real time studies of solid gas reactions at the level reaching the atomic scale. In the present paper, we focus on a combination of atomic resolution STEM/EDX, which visualizes the reaction zone, and near ambient pressure (NAP) XPS, which collects information for a surface layer of variable thickness under reaction conditions. We compare the behavior of two affined topological insulators, Bi2Te3 and Sb2Te3. We used a simple reaction with molecular oxygen occurring at 298 K, which is of practical importance to avoid material degradation. Despite certain limitations, a combination of in situ XPS and ex situ cross-sectional STEM/EDX allowed us to obtain a self-consistent picture of the solid gas reaction mechanism for oxidation of Sb2Te3 and Bi2Te3 crystals, which includes component redistribution between the oxide and the subsurface layer and Te segregation with formation of a thin ordered layer at the interface. The process is multistep in case of both compounds. At the very beginning of the oxidation process the reactivity is determined by the energy benefit of the corresponding element oxygen bond formation. Further in the oxidation process, the behavior of these two compounds becomes similar and features component redistribution between the oxide and the subsurface layer.

Magnetic doping is expected to open a band gap at the Dirac point of topological insulators by breaking time-reversal symmetry and to enable novel topological phases. Epitaxial (Bi$_{1-x}$Mn$_{x}$)$_{2}$Se$_{3}$ is a prototypical magnetic topological insulator with a pronounced surface band gap of $\sim100$ meV. We show that this gap is neither due to ferromagnetic order in the bulk or at the surface nor to the local magnetic moment of the Mn, making the system unsuitable for realizing the novel phases. We further show that Mn doping does not affect the inverted bulk band gap and the system remains topologically nontrivial. We suggest that strong resonant scattering processes cause the gap at the Dirac point and support this by the observation of in-gap states using resonant photoemission. Our findings establish a novel mechanism for gap opening in topological surface states which challenges the currently known conditions for topological protection., 26 pages, 7 figures

Topological materials promise new functionalities, which are revealed with the help of angle resolved photoemission. Herein, the search for the magnetic bandgap at the Dirac point as a precondition for the quantum anomalous Hall effect is reviewed and its opening for the topological insulator heterostructure MnBi2Te4 Bi2Te3 is demonstrated. Essential preconditions are explained and the reasons why nonmagnetic gaps occur when Se replaces Te. Angle resolved photoelectron spectroscopy ARPES probes the quantum mechanical final state, and this allows investigation of spin manipulation by light using spin resolved ARPES and the dependence of the charge carrier lifetime on the peculiar spin texture of topological states. It is shown that ARPES data do not support SmB6 as the first strongly correlated topological insulator and an alternative, trivial explanation for the results of ARPES and electrical transport experiments is formulated. Epitaxially grown topological crystalline insulators are, due to their dependence on crystal symmetries, more versatile in the control of individual bulk band inversions. It is shown that this leads to topological quantum phase transitions and associated novel functionalities. Finally, the surface and bulk band connectivity of a type II 3D Weyl semimetal is investigated and an outlook is given for the scientific field

The authors investigate the electronic and spin structure of topological surface states across a topological quantum phase transition. They find a surface band gap opening at the Dirac point of the topological surface states, giving rise to massive fermions with nonzero spin polarization on both sides of the phase transition. A mechanism of bulk-mediated scattering processes that increase with decreasing spin-orbit coupling strength is proposed as an explanation for the problem of the unconventional transformation between spin Dirac phases.

Using high-resolution angle-resolved photoemission, we observe a strong spin-dependent renormalization and lifetime broadening of the quasiparticle excitations in the electronic band structure of Ni(111) in an energy window of $\sim$0.3 eV below the Fermi level. We derive a quantitative result for the spin-dependent lifetime broadening by comparing the scattering rates of majority and minority $d$ states, and further show that spin-dependent electron correlations are instead negligible for $sp$ states. From our analysis we experimentally determine the effective on-site Coulomb interaction $U$ caused by Stoner-like interband transitions between majority and minority $d$ states. The present results unambiguously demonstrate the remarkable impact of spin-dependent electron correlation effects originating from single-particle excitations in a prototypical 3$d$ transition metal, paving the way for further refinement of current many-body theoretical approaches., 5 pages, 4 figures, submitted on 24.05.2018

Ultrafast dynamics in three-dimensional topological insulators (TIs) opens new routes for increasing the speed of information transport up to frequencies thousand times faster than in modern electronics. However, up to date, disentangling the exact contributions from bulk and surface transport to the subpicosecond dynamics of these materials remains a difficult challenge. Here, using time- and angle-resolved photoemission, we demonstrate that driving a TI from the bulk-conducting into the bulk-insulating transport regime allows to selectively switch on and off the emergent channels of ultrafast transport between the surface and the bulk. We thus establish that ultrafast transport is one of the main driving mechanisms responsible for the decay of excited electrons in prototypical TIs following laser excitation. We further show how ultrafast transport strongly affects the thermalization and scattering dynamics of the excited states up to high energies above the Fermi level. In particular, we observe how inhibiting the transport channels leads to a thermalization bottleneck that substantially slows down electron-hole recombination via electron-electron scatterings. Our results pave the way for exploiting ultrafast transport to control thermalization time scales in TI-based optoelectronic applications, and expand the capabilities of TIs as intrinsic solar cells., Comment: 10 pages, 5 figures

The behavior of ternary mixed crystals or solid solutions and its correlation with the properties of their binary constituents is of fundamental interest. Due to their unique potential for application in future information technology, mixed crystals of topological insulators with the spin-locked, gapless states on their surfaces attract huge attention of physicists, chemists and material scientists. (Bi1−xSbx)2Te3 solid solutions are among the best candidates for spintronic applications since the bulk carrier concentration can be tuned by varying x to obtain truly bulk-insulating samples, where the topological surface states largely contribute to the transport and the realization of the surface quantum Hall effect. As this ternary compound will be evidently used in the form of thin-film devices its chemical stability is an important practical issue. Based on the atomic resolution HAADF-TEM and EDX data together with the XPS results obtained both ex situ and in situ, we propose an atomistic picture of the mixed crystal reactivity compared to that of its binary constituents. We find that the surface reactivity is determined by the probability of oxygen attack on the Te–Sb bonds, which is directly proportional to the number of Te atoms bonded to at least one Sb atom. The oxidation mechanism includes formation of an amorphous antimony oxide at the very surface due to Sb diffusion from the first two quintuple layers, electron tunneling from the Fermi level of the crystal to oxygen, oxygen ion diffusion to the crystal, and finally, slow Te oxidation to the +4 oxidation state. The oxide layer thickness is limited by the electron transport, and the overall process resembles the Cabrera–Mott mechanism in metals. These observations are critical not only for current understanding of the chemical reactivity of complex crystals, but also to improve the performance of future spintronic devices based on topological materials.

Negative longitudinal magnetoresistance (NLMR) is shown to occur in topological materials in the extreme quantum limit, when a magnetic field is applied parallel to the excitation current. We perform pulsed and DC field measurements on Pb1-xSnxSe epilayers where the topological state can be chemically tuned. The NLMR is observed in the topological state, but is suppressed and becomes positive when the system becomes trivial. In a topological material, the lowest N=0 conduction Landau level disperses down in energy as a function of increasing magnetic field, while the N=0 valence Landau level disperses upwards. This anomalous behavior is shown to be responsible for the observed NLMR. Our work provides an explanation of the outstanding question of NLMR in topological insulators and establishes this effect as a possible hallmark of bulk conduction in topological matter., Comment: Accepted in Physical Review Letters

Helically spin-polarized Dirac fermions (HSDF) in protected topological surface states (TSS) are of high interest as a new state of quantum matter. In three-dimensional (3D) materials with TSS, electronic bulk states often mask the transport properties of HSDF. Recently, the high-field Hall resistance and low-field magnetoresistance indicate that the TSS may coexist with a layered two-dimensional electronic system (2DES). Here, we demonstrate quantum oscillations of the Hall resistance at temperatures up to 50 K in nominally undoped bulk Bi2Se3 with a high electron density n of about 2·1019 cm−3. From the angular and temperature dependence of the Hall resistance and the Shubnikov-de Haas oscillations we identify 3D and 2D contributions to transport. Angular resolved photoemission spectroscopy proves the existence of TSS. We present a model for Bi2Se3 and suggest that the coexistence of TSS and 2D layered transport stabilizes the quantum oscillations of the Hall resistance.

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin–orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized G W +Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron–electron and electron–phonon scatterings. Taking the prototypical insulator Bi 2 Te 3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron–electron and electron–phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials.

Topologically nontrivial states reveal themselves in strongly spin-orbit coupled systems by Dirac cones. However, their appearance is not a sufficient criterion for a topological phase. In topological insulators, where these states protect surface metallicity, they are straightforwardly assigned based on bulk-boundary correspondence. On metals, where these states are suspected to have tremendous impact as well, e.g., in catalysis, their topological protection is difficult to assess due to the lacking band gap and the frequent assignment to topological properties appears unjustified. Here, we discover by angle-resolved photoemission a state with the dispersion of a Dirac cone at a low-symmetry point of W(110). Our ab initio calculations predict this feature with a linear band crossing and high spin polarization. However, instead of being born by topology, the states arise from Rashba split bands and do not fundamentally depend on the opening of a spin-orbit gap. On the other hand, we find that the [001] mirror plane protects the band crossing point and renormalizes the dispersion towards a Dirac-cone shape. In this sense, the discovered state is the metal counterpart of the surface state of a topological crystalline insulator. The Dirac cone is tilted due to its origin in an accidental band crossing away from high symmetry points. Tilted Dirac cones have recently been predicted for two- and three-dimensional materials and were observed in three-dimensional Weyl semimetals. Accordingly, the protection and renormalization by mirror symmetry uncovered here are a potentially much wider spread phenomenon which does not require topological properties. Our results also indicate why the massive gapless crossing predicted for topological crystalline insulators has never been observed.

One of the most promising platforms for spintronics and topological quantum computation is the two-dimensional electron gas (2DEG) with strong spin-orbit interaction and out-of-plane ferromagnetism. In proximity to an s-wave superconductor, such 2DEG may be driven into a topologically non-Trivial superconducting phase, predicted to support zero-energy Majorana fermion modes. Using angle-resolved photoemission spectroscopy and ab initio calculations, we study the 2DEG at the surface of the vanadium-doped polar semiconductor with a giant Rashba-Type splitting, BiTeI. We show that the vanadium-induced magnetization in the 2DEG breaks time-reversal symmetry, lifting Kramers degeneracy of the Rashba-split surface state at the Brillouin zone center via formation of a huge gap of about 90 meV. As a result, the constant energy contour inside the gap consists of only one circle with spin-momentum locking. These findings reveal a great potential of the magnetically-doped semiconductors with a giant Rashba-Type splitting for realization of novel states of matter., The work was partially supported by grant of Saint Petersburg State University for scientific investigations (N. 15.61.202.2015). This study was supported by the Russian Science Foundation (project N. 17-12-01047, in part of crystal growth, structural characterization and ARPES measurements (Figs 1, 2)). The funding by the University of the Basque Country (Grant Nos GIC07IT36607 and IT-756-13), the Spanish Ministry of Science and Innovation (Grant Nos FIS2013-48286-C02-02-P, FIS2013-48286-C02-01-P, and FIS2016-75862-P) and Tomsk State University Academic D.I. Mendeleev Fund Program in 2015 (research grant N 8.1.05.2015) are also gratefully acknowledged. The authors also acknowledge support from the Russian-German laboratory at BESSY II, the “German-Russian Interdisciplinary Science Center”(G-RISC) program and the Impuls- und Vernetzungsfonds der Helmholtz-Gemeinschaft (Grant No. HRJRG-408).

Using time-, spin- and angle-resolved photoemission, we investigate the ultrafast spin dynamics of hot electrons on the surface of the topological insulator Bi$_2$Te$_3$ following optical excitation by fs-infrared pulses. We observe two surface-resonance states above the Fermi level coexisting with a transient population of Dirac fermions that relax in about $\sim$2 ps. One state is located below $\sim$0.4 eV just above the bulk continuum, the other one at $\sim$0.8 eV inside a projected bulk band gap. At the onset of the excitation, both states exhibit a reversed spin texture with respect to that of the transient Dirac bands, in agreement with our one-step photoemission calculations. Our data reveal that the high-energy state undergoes spin relaxation within $\sim$0.5 ps, a process that triggers the subsequent spin dynamics of both the Dirac cone and the low-energy state, which behave as two dynamically-locked electron populations. We discuss the origin of this behavior by comparing the relaxation times observed for electrons with opposite spins to the ones obtained from a microscopic Boltzmann model of ultrafast band cooling introduced into the photoemission calculations. Our results demonstrate that the nonequilibrium surface dynamics is governed by electron-electron rather than electron-phonon scattering, with a characteristic time scale unambiguously determined by the complex spin texture of excited states above the Fermi level. Our findings reveal the critical importance of detecting momentum and energy-resolved spin textures with fs resolution to fully understand the sub-ps dynamics of transient electrons on the surface of topological insulators., 10 pages, 5 figures

In this Rapid Communication we investigate the coupling between excited electrons and phonons in the highly anisotropic electronic structure of the prototypical topological insulator Bi$_2$Te$_3$. Using time- and angle-resolved photoemission spectroscopy we are able to identify the emergence and ultrafast temporal evolution of the longitudinal-optical A$_{1g}$ coherent-phonon mode in Bi$_2$Te$_3$. We observe an antiphase behavior in the onset of the coherent-phonon oscillations between the $\overline{\Gamma K}$ and the $\overline{\Gamma M}$ high-symmetry directions that is consistent with warping. The qualitative agreement between our density-functional theory calculations and the experimental results reveals the critical role of the anisotropic coupling between Dirac fermions and phonon modes in the topological insulator Bi$_2$Te$_3$.

Heat-assisted magnetic recording (HAMR) uses the tiny hot spot of a laser to flip bit states, and suitable materials are needed to enable this technology. The authors show that antidots of a ferrimagnetic alloy arrayed atop nonmagnetic holes present an effective bit size of 45 nm, and four magnetic states at room temperature. Key here is the antidots' magnetic-anisotropy reorientation at just 350 K, whereas a typical HAMR material must be heated above its Curie temperature (~750 K, or higher) to work. These $f\phantom{\rule{0}{0ex}}e\phantom{\rule{0}{0ex}}r\phantom{\rule{0}{0ex}}r\phantom{\rule{0}{0ex}}i\phantom{\rule{0}{0ex}}m\phantom{\rule{0}{0ex}}a\phantom{\rule{0}{0ex}}g\phantom{\rule{0}{0ex}}n\phantom{\rule{0}{0ex}}e\phantom{\rule{0}{0ex}}t\phantom{\rule{0}{0ex}}i\phantom{\rule{0}{0ex}}c$ nanostructures do not suffer from a superparamagnetic limit, and seem promising for ultrahigh-density data storage.

Three-dimensional topological insulators (TIs) are characterized by spin-polarized Dirac-cone surface states that are protected from backscattering by time-reversal symmetry. Control of the spin polarization of topological surface states (TSSs) using femtosecond light pulses opens novel perspectives for the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Using time-, spin-, and angle-resolved spectroscopy, we directly monitor for the first time the ultrafast response of the spin polarization of photoexcited TSSs to circularly-polarized femtosecond pulses of infrared light. We achieve all-optical switching of the transient out-of-plane spin polarization, which relaxes in about 1.2 ps. Our observations establish the feasibility of ultrafast optical control of spin-polarized Dirac fermions in TIs and pave the way for novel optospintronic applications at ultimate speeds., Comment: 9 pages, 4 figures

We perform ultrahigh-resolution angle-resolved photoemission experiments at a temperature $T=0.8$ K on the type-II Weyl semimetal candidate ${\mathrm{WTe}}_{2}$. We find a surface Fermi arc connecting the bulk electron and hole pockets on the (001) surface. Our results show that the surface Fermi arc connectivity to the bulk bands is strongly mediated by distinct surface resonances dispersing near the border of the surface-projected bulk band gap. By comparing the experimental results to first-principles calculations, we argue that the coupling to these surface resonances, which are topologically trivial, is compatible with the classification of ${\mathrm{WTe}}_{2}$ as a type-II Weyl semimetal hosting topological Fermi arcs. We further support our conclusion by a systematic characterization of the bulk and surface character of the different bands and discuss the similarity of our findings to the case of topological insulators.

Rozbíjení inverzní symetrie ve fereeleRashba efekt; Fotoemisse; DFTktrickém polovodiči způsobuje děleni stavů, tzv Rashba efekt. V tomto článku ukazujeme kompletně mapování spinové polarizace těchto Rashba stavů za pomoci spinovo rozlišené fotoemisse. The breaking of bulk inversion symmetry in ferroelectric semiconductors causes a Rashba-type spin splitting of electronic bulk bands. This is shown by a comprehensive mapping of the spin polarization of the electronic bands in ferroelectric α- GeTe(111) films using a time-of-flight momentum microscope equipped with an imaging spin filter that enables a simultaneous measurement of more than 10 000 data points. The experiment reveals an opposite spin helicity of the inner and outer Rashba bands with a different spin polarization in agreement with theoretical predictions, confirming a complex spin texture of bulk Rashba states. The outer band has about twice larger spin polarization than the inner one, giving evidence of a spin-orbit effect being related to the orbital composition of the band states. The switchable inner electric field of GeTe implies new functionalities for spintronic devices.

The interface of graphene with ferromagnets is highly relevant for spintronics, because graphene on Co(0001) shows a largely intact Dirac cone and strong hybridization with Co $3d$ states breaking the sublattice symmetry that had been considered mutually exclusive. Here we show by spin- and angle-resolved photoemission that the Dirac cone and Dirac point are also highly spin polarized $(\ensuremath{\sim}\ensuremath{-}25%)$, which reinforces the puzzling issue of a strong graphene-substrate interaction. The problem is solved by our ab initio calculations which show that (i) the upper and lower halves of the Dirac cone belong to different sublattices and (ii) one half is spin polarized by spin-dependent hybridization because it is situated at the edge of a minority-spin band gap of the Co substrate.

Topological insulators are characterized by Dirac-cone surface states with electron spins locked perpendicular to their linear momenta. Recent theoretical and experimental work implied that this specific spin texture should enable control of photoelectron spins by circularly polarized light. However, these reports questioned the so far accepted interpretation of spin-resolved photoelectron spectroscopy. We solve this puzzle and show that vacuum ultraviolet photons (50-70 eV) with linear or circular polarization indeed probe the initial-state spin texture of Bi2Se3 while circularly polarized 6-eV low-energy photons flip the electron spins out of plane and reverse their spin polarization, with its sign determined by the light helicity. Our photoemission calculations, taking into account the interplay between the varying probing depth, dipole-selection rules, and spin-dependent scattering effects involving initial and final states, explain these findings and reveal proper conditions for light-induced spin manipulation. Our results pave the way for future applications of topological insulators in optospintronic devices.

The new journal of physics 15, 115009 (2013). doi:10.1088/1367-2630/15/11/115009, Published by IOP Publ. [u.a.], London

The appearance of massless Dirac fermions in graphene requires two equivalent carbon sublattices of trigonal shape. While the generation of an effective mass and a band gap at the Dirac point remains an unresolved problem for freestanding extended graphene, it is well established by breaking translational symmetry by confinement and by breaking sublattice symmetry by interaction with a substrate. One of the strongest sublattice symmetry breaking interactions with predicted and measured band gaps ranging from 400 meV to more than 3 eV has been attributed to the interfaces of graphene with Ni and Co, which are also promising spin filter interfaces. Here, we apply angle resolved photoemission to epitaxial graphene on Ni 111 and Co 0001 to show the presence of intact Dirac cones 2.8 eV below the Fermi level. Our results challenge the common belief that the breaking of sublattice symmetry by a substrate and the opening of the band gap at the Dirac energy are in a straightforward relation. A simple effective model of a biased bilayer structure composed of graphene and a sublattice symmetry broken layer, corroborated by densityfunctional theory calculations, demonstrates the general validity of our conclusions

The helical Dirac fermions at the surface of topological insulators show a strong circular dichroism which has been explained as being due to either the initial-state spin angular momentum, the initial-state orbital angular momentum, or the handedness of the experimental setup. All of these interpretations conflict with our data from Bi2Te3 which depend on the photon energy and show several sign changes. Our one-step photoemission calculations coupled to ab initio theory confirm the sign change and assign the dichroism to a final-state effect. The spin polarization of the photoelectrons, instead, remains a reliable probe for the spin in the initial state., 16 pages, 4 figures; submitted to Physical Review Letters

We have investigated the spin-dependent quasiparticle lifetimes and the strength of electron correlation effects in the ferromagnetic 3$d$ transition metals Fe, Co, and Ni by means of spin- and angle-resolved photoemission spectroscopy. The experimental data are accompanied by state-of-the-art many-body calculations within the dynamical mean-field theory and the three-body scattering approximation, including fully relativistic calculations of the photoemission process within the one-step model. Our quantitative analysis reveals that inclusion of local many-body Coulomb interactions are of ultimate importance for a realistic description of correlation effects in ferromagnetic 3$d$ transition metals. However, we found that more sophisticated many-body calculations with larger modifications in the case of Fe and Co are still needed to improve the quantitative agreement between experiment and theory. In general, it turned out that not only the dispersion behavior of energetic structures should be affected by nonlocal correlations but also the line widths of most of the photoemission peaks are underestimated by the current theoretical approaches. The increasing values of the on-site Coulomb interaction parameter $U$ and the band narrowing of majority spin states obtained when moving from Fe to Ni indicate that the effect of nonlocal correlations becomes weaker with increasing atomic number, whereas correlation effects tend to be stronger.

Understanding and control of spin degrees of freedom on the surfaces of topological materials are key to future applications as well as for realizing novel physics such as the axion electrodynamics associated with time-reversal (TR) symmetry breaking on the surface. We experimentally demonstrate magnetically induced spin reorientation phenomena simultaneous with a Dirac-metal to gapped-insulator transition on the surfaces of manganese-doped Bi2Se3 thin films. The resulting electronic groundstate exhibits unique hedgehog-like spin textures at low energies, which directly demonstrate the mechanics of TR symmetry breaking on the surface. We further show that an insulating gap induced by quantum tunnelling between surfaces exhibits spin texture modulation at low energies but respects TR invariance. These spin phenomena and the control of their Fermi surface geometrical phase first demonstrated in our experiments pave the way for the future realization of many predicted exotic magnetic phenomena of topological origin., Comment: 38 pages, 18 Figures, Includes new text, additional datasets and interpretation beyond arXiv:1206.2090, for the final published version see Nature Physics (2012)

We report on a quantitative investigation of the spin-dependent quasiparticle lifetimes and electron correlation effects in ferromagnetic hcp Co(0001) by means of spin- and angle-resolved photoemission spectroscopies. The experimental spectra are compared in detail to state-of-the-art many-body calculations within the dynamical mean-field theory and the three-body scattering approximation, including a full calculation of the one-step photoemission process. From this comparison we conclude that although strong local many-body Coulomb interactions are of major importance for the qualitative description of correlation effects in Co, more sophisticated many-body calculations are needed in order to improve the quantitative agreement between theory and experiment, in particular, concerning the linewidths. The quality of the overall agreement obtained for Co indicates that the effect of nonlocal correlations becomes weaker with increasing atomic number.

A quantum cavity for spin is created using a tungsten crystal as substrate of high nuclear charge and breaking the structural inversion symmetry through deposition of a gold quantum film. Spin- and angle-resolved photoelectron spectroscopy shows directly that quantum-well states and the ``matrioshka'' or Russian nested doll Fermi surface of the gold film are spin polarized and spin-orbit split up to a thickness of at least nine atomic layers. Ferromagnetic materials or external magnetic fields are not required, and the quantum film does not need to possess a high atomic number as analogous results with silver show.

Graphene is considered a candidate material for spintronics. Recently, graphene grown on Ni(111) has been reported to show a Rashba effect which depends on the magnetization. By spin- and angle-resolved photoelectron spectroscopy, we investigate the preconditions for such an effect for graphene on Ni as well as on Co which has a $\ensuremath{\sim}3\ifmmode\times\else\texttimes\fi{}$ larger $3d$ magnetic moment: (i) spin polarization or (ii) exchange splitting of graphene $\ensuremath{\pi}$ states in normal emission geometry, and (iii) Rashba-type spin-orbit splitting off normal. As none of these are found to be of considerable size, the reported effect is neither Rashba-type, nor due to the spin-orbit coupling, nor involving the electron spin.

For the purpose of recovering the intriguing electronic properties of freestanding graphene at a solid surface, graphene self-organized on a Au monolayer on Ni(111) is prepared and characterized by scanning tunneling microscopy. Angle-resolved photoemission reveals a gapless linear $\ensuremath{\pi}$-band dispersion near $\overline{K}$ as a fingerprint of strictly monolayer graphene and a Dirac crossing energy equal to the Fermi energy (${E}_{F}$) within 25 meV meaning charge neutrality. Spin resolution shows a Rashba effect on the $\ensuremath{\pi}$ states with a large ($\ensuremath{\sim}13\text{ }\text{ }\mathrm{meV}$) spin-orbit splitting up to ${E}_{F}$ which is independent of $\mathbf{k}$.

The paper sums up a theoretical and experimental investigation of the influence of the spin–orbit coupling in W(110) on the spin structure of electronic states in deposited Au and Cu monolayers. Angle-resolved photoemission spectroscopy reveals that in the case of monolayers of Au and Cu spin–orbit split bands are formed in a surface-projected gap of W(110). Spin resolution shows that these states are spin polarized and that, therefore, the spin–orbit splitting is of Rashba type. The states evolve from hybridization of W 5d, 6p-derived states with the s, p states of the deposited metal. Interaction with Au and Cu shifts the original W 5d-derived states from the edges toward the center of the surface-projected gap. The size of the spin–orbit splitting of the formed states does not correlate with the atomic number of the deposited metal and is even higher for Cu than for Au. These states can be described as W-derived surface resonances modified by hybridization with the p, d states of the adsorbed metal. Our electronic structure calculations performed in the framework of the density functional theory correlate well with the experiment and demonstrate the crucial role of the W top layer for the spin–orbit splitting. It is shown that the contributions of the spin–orbit interaction from W and Au act in opposite directions which leads to a decrease of the resulting spin–orbit splitting in the Au monolayer on W(110). For the Cu monolayer with lower spin–orbit interaction the resulting spin splitting is higher and mainly determined by the W.

The magnetic interlayer coupling of Fe19Ni81/Cu/Co trilayered microstructures has been studied by means of x-ray magnetic circular dichroism in combination with photoelectron emission microscopy (XMCD-PEEM). We find that a parallel coupling between magnetic domains coexists with a non-parallel coupling between magnetic domain walls (DWs) of each ferromagnetic layer. We attribute the non-parallel coupling of the two magnetic layers to local magnetic stray fields arising at DWs in the magnetically harder Co layer. In the magnetically softer FeNi layer, non-ordinary DWs, such as 270° and 90° DWs with overshoot of the magnetization either inwards or outwards relative to the turning direction of the Co magnetization, are identified. Micromagnetic simulations reveal that in the absence of magnetic anisotropy, both types of overshooting DWs are energetically equivalent. However, if a uniaxial in-plane anisotropy is present, the relative orientation of the DWs with respect to the anisotropy axis determines which of these DWs is energetically favorable.