Strain-induced magnetic anisotropies in Co films on Mo(110)

Giant magnetic anisotropy energy and coercivity in Fe island and atomic wire on W(110)

We have directly investigated the giant magnetic anisotropy energy and coercivity of monolayer (ML) Fe islands and stripes on flat and stepped W(110) surfaces using x-ray magnetic circular dichroism. Both for islands and stripes, the magnetic anisotropy energy is $\ensuremath{\sim}$1.0 meV/atom, independent of the coverage below 0.5 ML. On the contrary, the coercive field of the islands rapidly drops from 4.3 T at 0.25 ML to 1.9 T at 0.50 ML, while that of the stripes moderately degrades from 3.5 T at 0.15 ML ($\ensuremath{\sim}$3 atom rows) to 3.0 T at 0.50 ML. We explain the contrastive behavior for the islands and stripes by different nucleation and remagnetization processes. Considering…

Evidence for eight node mixed-symmetry superconductivity in a correlated organic metal

We report a combined theoretical and experimental investigation of the superconducting state in the quasi-two-dimensional organic superconductor $\kappa$-(ET)$_2$Cu[N(CN)$_2$]Br. Applying spin-fluctuation theory to a low-energy material-specific Hamiltonian derived from ab initio density functional theory we calculate the quasiparticle density of states in the superconducting state. We find a distinct three-peak structure that results from a strongly anisotropic mixed-symmetry superconducting gap with eight nodes and twofold rotational symmetry. This theoretical prediction is supported by low-temperature scanning tunneling spectroscopy on in situ cleaved single crystals of $\kappa$-(ET)$_2$…

Magnetization dynamics in polycrystalline Permalloy and epitaxial Co platelets observed by time-resolved photoemission electron microscopy

We studied the dynamic magnetization response in rectangular polycrystalline Permalloy and also epitaxial Co structures (lateral sizes comprised tens of microns at a thickness of tens of nanometers) during the action of a magnetic field pulse, using time-resolved X-ray photoemission electron microscopy with a time resolution of 10 ps. In the case of Permalloy platelets the restoring torque that is necessary for the stroboscopic image acquisition is provided by the Landau flux closure structure representing a minimum of the free energy. We investigated the dynamic response of 90° Neel domain walls. The main results are: the maximum velocity of the domain wall is 1.5 × 104 m/s, the intrinsic …

Space-, time- and spin-resolved photoemission

Journal of electron spectroscopy and related phenomena 200, 94 - 118 (2015). doi:10.1016/j.elspec.2015.05.016

Magnetization dynamics in microscopic spin-valve elements: Shortcomings of the macrospin picture

We have studied ultrafast magnetodynamics in micropatterned spin-valve structures using time-resolved x-ray photoemission electron microscopy combined with x-ray magnetic circular dichroism. Exciting the system with ultrafast field pulses of $250\phantom{\rule{0.3em}{0ex}}\mathrm{ps}$ width, we find the dynamic response of the free layer to fall into two distinctly different contributions. On the one hand, it exhibits localized spin wave modes that strongly depend on the shape of the micropattern. A field pulse applied perpendicular to the exchange bias field along the diagonal of a square pattern leads to the excitation of a standing spin wave mode with two nodes along the field direction.…

Anomalous transport properties of the half-metallic ferromagnets Co 2 TiSi, Co 2 TiGe and Co 2 TiSn

In this work the theoretical and experimental investigations of Co2TiZ (Z = Si, Ge, or Sn) compounds are reported. Half-metallic ferromagnetism is predicted for all three compounds with only two bands crossing the Fermi energy in the majority channel. The magnetic moments fulfill the Slater-Pauling rule and the Curie temperatures are well above room temperature. All compounds show a metallic like resistivity for low temperatures up to their Curie temperature, above the resistivity changes to semiconducting like behavior. A large negative magnetoresistance of 55% is observed for Co2TiSn at room temperature in an applied magnetic field of 4T which is comparable to the large negative magnetore…

Momentum Distribution of Electrons Emitted from Resonantly Excited Individual Gold Nanorods.

Electron emission by femtosecond laser pulses from individual Au nanorods is studied with a time-of-flight momentum resolving photoemission electron microscope (ToF k-PEEM). The Au nanorods adhere to a transparent indium–tin oxide substrate, allowing for illumination from the rear side at normal incidence. Localized plasmon polaritons are resonantly excited at 800 nm with 100 fs long pulses. The momentum distribution of emitted electrons reveals two distinct emission mechanisms: a coherent multiphoton photoemission process from the optically heated electron gas leads to an isotropic emission distribution. In contrast, an additional emission process resulting from the optical field enhanceme…

Morphological and magnetic analysis of Fe nanostructures on W(110) by using scanning tunneling microscopy and Lorentz microscopy

Abstract We investigated morphological features and magnetic properties of epitaxial Fe nanostructures (films, stripes and nanoparticles) on a W(110) surface with monoatomic steps preferentially along the direction. The nanostructures were prepared in ultra-high vacuum by using electron-beam evaporation and subsequent annealing at different temperatures. Scanning tunneling microscopy measurements in-situ revealed elongated Fe nanostructures with aspect ratios of up to . The observable shape and orientation (along or perpendicular to the monoatomic steps of the substrate) of the nanostructures depended substantially on the preparation parameters. By capping the system with 7 monolayers of Pt…

Thermomagnetic Materials: Thermomagnetic Properties Improved by Self-Organized Flower-Like Phase Separation of Ferromagnetic Co2Dy0.5Mn0.5Sn (Adv. Funct. Mater. 9/2012)

Specular reflection of spin-polarized electrons from the W(001) spin-filter crystal in a large range of scattering energies and angles

Extending previous work on the imaging spin-filter technique based on electron diffraction from W(001) in the specular (00)-LEED (low-energy electron diffraction) spot, we studied the scattering-energy and angle-of-incidence landscape of spin sensitivity $S$ and reflectivity ${I/I}_{0}$. The setup includes a spin-polarized GaAs electron source and a rotatable delay-line detector for spatially resolving detection. We measured the intensity and spin asymmetry of the specularly reflected beam for energies between 14 and 37 eV and angles of incidence between ${30}^{\ensuremath{\circ}}$ and ${60}^{\ensuremath{\circ}}$. Resulting energy-angular landscapes show rather good agreement with theory [r…

Disorder-induced gap in the normal density of states of the organic superconductorκ-(BEDT-TTF)2Cu[N(CN)2]Br

The local density of states (DOS) of the organic superconductor κ-(BEDT-TTF)2Cu[N(CN)2]Br, measured by scanning tunneling spectroscopy on in situ cleaved surfaces, reveals a logarithmic suppression near the Fermi edge persisting above the critical temperature T(c). The experimentally observed suppression of the DOS is in excellent agreement with a soft Hubbard gap as predicted by the Anderson-Hubbard model for systems with disorder. The electronic disorder also explains the diminished coherence peaks of the quasi-particle DOS below T(c).

Temperature-induced martensite in magnetic shape memory Fe2MnGa observed by photoemission electron microscopy

The magnetic domain structure in single crystals of a Heusler shape memory compound near the composition Fe2MnGa was observed during phase transition by photoelectron emission microscopy at Beamline 11.0.1.1 of the Advanced Light Source. The behavior is comparable with recent observations of an adaptive martensite phase in prototype Ni2MnGa, although the pinning in the recent work is an epitaxial interface and in this work the effective pinning plane is a boundary between martensitic variants that transform in a self-accommodating way from the single crystal austenite phase present at high temperatures. Temperature dependent observations of the twinning structure give information as to the …

Spin-Polarized Scanning Tunnelling Microscopy of Ultrathin Films

Using low temperature spin-polarized scanning tunneling microscopy we have studied the morphology and magnetic properties of ultrathin Fe(0.5 ML)Au(0.5 ML) nanowires prepared on a Mo(110) single crystal. The Fe nanostripes grown by step flow on a Mo(110) at 700 K were covered by Au at RT, and subsequently annealed at 700 K. Differences in the morphology of Au on Fe(110)/Mo(110) and clean Mo(110) surfaces are observed and discussed. After annealing, the Mo is covered by a homogeneous FeAu ML alloy with several iron enriched islands which reveal an out-of-plane magnetic contrast. Direct lateral exchange coupling has been observed for these islands.

Exchange bias in epitaxial Mn2Au (0 0 1)/Fe (0 0 1) bilayers

Spinovo rozlisena time-of-flight k-reozlisena fotoemissia Ir-- Kompletny fotoemissny experiment.

Ultramicroscopy 183, 19 - 29 (2017). doi:10.1016/j.ultramic.2017.06.025

Structure and electronic properties of ultrathin Co films on W(110)

Abstract The structure and electronic properties of ultrathin Co films on W(1 1 0) grown by molecular beam epitaxy in UHV were investigated by low energy electron diffraction (LEED) and scanning tunneling microscopy and spectroscopy (STM and STS). For coverages above 0.7 ML the pseudomorphic (ps) monolayer is transformed gradually into close-packed (cp-) monolayer areas, showing up as separated islands that increase in size with coverage until the cp-monolayer is complete. Two different structures of the cp-monolayer were observed by atomically resolved STM, both leading to a 8 × 1 superstructure in the LEED pattern. Higher coverages continue to grow in the Stransky–Krastanov growth mode fo…

Optical magnetic circular dichroism in threshold photoemission from a magnetite thin film

Threshold photoemission excited by polarization-modulated ultraviolet femtosecond laser light is exploited for phase-sensitive detection of magnetic circular dichroism (MCD) for a magnetite thin film. Magnetite (Fe(3)O(4)) shows a magnetic circular dichroism of ∼(4.5 ± 0.3) × 10(-3) for perpendicularly incident circularly polarized light and a magnetization vector switched parallel and antiparallel to the helicity vector by an external magnetic field. The asymmetry in threshold photoemission is discussed in comparison to the magneto-optical Kerr effect. The optical MCD contrast in threshold photoemission will provide a basis for future laboratory photoemission studies on magnetic surfaces.

Suppression of the vacuum space-charge effect in fs-photoemission by a retarding electrostatic front lens

Review of scientific instruments 92(5), 053703 (2021). doi:10.1063/5.0046567

Energy- and angle-dependent threshold photoemission magnetic circular dichroism from an ultrathin Co/Pt(111) film

Threshold photoemission magnetic circular dichroism (TPMCD) in one-photon photoemission (1PPE) and two-photon photoemission (2PPE) is measured at an ultrathin Co film grown on Pt(111). Energy-dependent measurements reveal maximum asymmetries directly at the photoemission threshold (1.90% for 1PPE and 11.7% for 2PPE) which weakly decrease with increasing photon energy. The measured TPMCD asymmetries are discussed in two excitation models on the basis of spin-resolved band-structure calculations. For the model of direct band-to-band transitions in other k directions than the direction of observation (Gamma-L) ab initio calculations for 1PPE and 2PPE are performed. The theory is in reasonable …

Magnetic surface anisotropies in NiFe-alloy films: separation of intrinsic Néel-type from strain relaxation contributions

Abstract Magnetic surface anisotropies (MSA) in NiFe/Cu(1 1 1) films were investigated experimentally, for varying compositions of the NiFe alloy. By restricting the measurements to the pseudomorphic range, the pure intrinsic Neel-type anisotropy could be isolated without strain relaxation contributions. The intrinsic MSA of the xNi(1−x)Fe/Cu(1 1 1) interface varies linearly with composition x between easy plane for pure Ni to perpendicular for x=60 and 48%. It vanishes near the permalloy composition x=80%.

Reconstructed bcc Co films on the surface

Abstract Ultrathin epitaxial Co films on Cr ( 1 1 0 ) are examined by scanning tunneling microscopy and spectroscopy (STM and STS). At room temperature Co grows as pseudomorphic bcc layers for the first two monolayers and forms close-packed Co layers with stacking faults for thicker coverages. A periodic lattice distortion appears in two equivalent (3 × 1) reconstruction domains in combination with a regular lattice of dislocation lines oriented along the in-plane close-packed row directions bcc [ 1 1 ¯ 1 ] and bcc [ 1 ¯ 1 1 ] . The reconstruction and the occurrence of dislocation lines are caused by the epitaxial strain. The local density-of-states function is mapped by scanning tunneling …

Direct observation of half-metallicity in the Heusler compound $Co_{2}MnSi$

Ferromagnetic thin films of Heusler compounds are highly relevant for spintronic applications owing to their predicted half-metallicity, that is, 100% spin polarization at the Fermi energy. However, experimental evidence for this property is scarce. Here we investigate epitaxial thin films of the compound Co2MnSi in situ by ultraviolet-photoemission spectroscopy, taking advantage of a novel multi-channel spin filter. By this surface sensitive method, an exceptionally large spin polarization of () % at room temperature is observed directly. As a more bulk sensitive method, additional ex situ spin-integrated high energy X-ray photoemission spectroscopy experiments are performed. All experimen…

Nano-holes vs nano-cracks in thin gold films: What causes anomalous THz transmission?

Nano-structuring materials can change their properties extraordinarily, but so can defects caused by manufacturing. We study the effect of capacitive defects on terahertz transmission in golden nanomeshes, and find their influence crucial.

Self-Trapping of Magnetic Oscillation Modes in Landau Flux-Closure Structures

We investigated the magnetodynamics in rectangular Permalloy platelets by means of time-resolved x-ray photoemission microscopy. 10 nm thick platelets of size 16 x 32 microm were excited by an oscillatory field along the short side of the sample with a fundamental frequency of 500 MHz and considerable contributions of higher harmonics. Under the influence of the oscillatory field, the Néel wall in the initial classical Landau pattern shifts away from the center, corresponding to an induced magnetic moment perpendicular to the exciting field. This phenomenon is explained by a self-trapping effect of the dominating spin-wave mode when the system is excited just below the resonance frequency. …

Rashba splitting of the Tamm surface state on Re(0001) observed by spin-resolved photoemission and scanning tunneling spectroscopy

Physical review research 2(1), 013296 (2020). doi:10.1103/PhysRevResearch.2.013296

Temperature-driven spin reorientation transition inFe∕Mo(110)nanostructures

Using low-temperature spin polarized scanning tunneling microscopy and spectroscopy, we observed a temperature-driven spin-reorientation transition (SRT) in Fe double layer (DL) nanostructures grown by step-flow growth on Mo(110). Magnetization components along the vertical and horizontal directions were detected with $4∕16$ ML Co∕10 ML $\mathrm{Au}∕\mathrm{W}(110)$ tips with out-of-plane (4 ML Co) and in-plane (16 ML Co) magnetic sensitivities. The magnetic easy axis of the Fe DL nanostructures continuously rotates from the vertical direction at $5\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ to an in-plane direction at $20\phantom{\rule{0.3em}{0ex}}\mathrm{K}$. The rotation angle is independent …

New Materials with High Spin Polarization Investigated by X-Ray Magnetic Circular Dichroism

We investigate element-specific spin and orbital magnetic moments of polycrystalline bulk Heusler alloys that are predicted to be half-metallic with composition Co2YZ (Y = Ti, Cr, Mn, Fe and Z = Al, Ga, Si, Ge, Sn, Sb) using magnetic circular dichroism in X-ray absorption spectroscopy (XAS/XMCD). In addition to stoichiometric compounds we also investigate composition series with partly replaced elements on the Y-site (Co2Fe x Cr1−x Si, Co2Mn x Ti1−x Si and Co2Mn x Ti1−x Ge) and on the Z-site (Co2MnGa1−x Ge x ) promising a tailoring of the Fermi level with respect to the minority band gap. We compare experimental results with theoretical predictions elucidating the influence of local disorde…

Threshold photoemission magnetic circular dichroism at the spin-reorientation transition of ultrathin epitaxial Pt/Co/Pt(111)/W(110) films

X-ray magnetic circular dichroism (MCD) is nowadays widely used for the investigation of magnetic properties of surfaces and thin films. Recently, similarly large effects have been observed for UV-VIS MCD effects both in single [1] and two-photon photoemission [2-3]. This threshold MCD effect is directly related to spin-orbit effects present at the Fermi edge. We report on the observation of threshold photoemission magnetic circular dichroism (TPMCD) in one-photon and two-photon photoemission (1PPE and 2PPE) at a Pt-capped ultrathin Co wedge grown on Pt(111)/W(110) using femtosecond laser light. TPMCD measurements result in asymmetries continuously increasing with the sample thickness. This…

Determination of surface and interface magnetic properties for the multiferroic heterostructure Co/BaTiO3using spleed and arpes

Co/BaTiO$_3$(001) is one of the most interesting multiferroic heterostructures as it combines different ferroic phases, setting this way the fundamentals for innovative technical applications. Various theoretical approaches have been applied to investigate the electronic and magnetic properties of Co/BaTiO$_3$(001). Here we determine the magnetic properties of 3 ML Co/BaTiO$_3$ by calculating spin-polarized electron diffraction as well as angle-resolved photoemission spectra, with both methods being well established as surface sensitive techniques. Furthermore, we discuss the impact of altering the BaTiO$_3$ polarization on the spectra and ascribe the observed changes to characteristic deta…

Spin-polarized Low Energy Electron Diffraction

We review recent progress in the understanding of the physics of ultrathin ferromagnetic films and surfaces that has been made using elastic spin-polarized low-energy electron diffraction (SPLEED). Further development of the experimental technique including high efficient electron sources, spin manipulation and imaging allows a wide range of applications. We report on a quantitative comparison of relativistic dynamical scattering calculations with SPLEED experiments on Fe(110) surfaces and Fe(100)/W(100) thin films leading to an understanding of the spatial distribution of spin densities. Exploiting the surface sensitivity in combination with the large asymmetry of SPLEED, it becomes feasib…

Electronic structure of the austenitic and martensitic state of magnetocaloric Ni-Mn-In Heusler alloy films

Changes of the electronic and magnetic structure near the martensitic phase transition of Ni-Mn-In Heusler alloys doped with Co are investigated by experiment and theory. The nonstoichiometric Ni${}_{48}$Co${}_{5}$Mn${}_{35}$In${}_{12}$ epitaxial film undergoes a transition from a weakly magnetic martensitic phase below ${T}_{m}=350$ K to a ferromagnetic austenitic phase above ${T}_{m}$. Element-specific magnetic moments and the unoccupied density of states function is investigated using x-ray magnetic circular dichroism. We find an antiparallel alignment of Mn and Ni/Co magnetic moments in both phases. The electronic structure is calculated using the SPR-KKR Green's function approach consi…

Energy- and k -resolved mapping of the magnetic circular dichroism in threshold photoemission from Co films on Pt(111)

The magnetic circular dichroism in threshold photoemission (TPMCD) for perpendicularly magnetized fcc Co films on Pt(111) has been revisited. A complete mapping of the spectral function $I({E}_{B},{k}_{x},{k}_{y})$ (binding energy ${E}_{B}$, momentum parallel to surface ${k}_{x}$, ${k}_{y}$) and the corresponding TPMCD asymmetry distribution ${A}_{\mathrm{MCD}}({E}_{B},{k}_{x},{k}_{y})$ has been performed for one-photon and two-photon photoemission using time-of-flight momentum microscopy. The experimental results allow distinguishing direct from indirect transitions. The measurements reveal clear band features of direct transitions from bulk bands that show a nontrivial asymmetry pattern. …

Spin texture of time-reversal symmetry invariant surface states on W(110)

AbstractWe find in the case of W(110) previously overlooked anomalous surface states having their spin locked at right angle to their momentum using spin-resolved momentum microscopy. In addition to the well known Dirac-like surface state with Rashba spin texture near the "Equation missing"-point, we observe a tilted Dirac cone with circularly shaped cross section and a Dirac crossing at 0.28 × "Equation missing" "Equation missing" within the projected bulk band gap of tungsten. This state has eye-catching similarities to the spin-locked surface state of a topological insulator. The experiments are fortified by a one-step photoemission calculation in its density-matrix formulation.

Effect of annealing on Co2FeAl0.5Si0.5thin films: A magneto-optical and x-ray absorption study

A series of Al and MgO-capped Co${}_{2}$FeAl${}_{0.5}$Si${}_{0.5}$ epitaxial thin films grown on MgO with various levels of L2${}_{1}$ ordering was obtained by in situ annealing. The films were studied by means of x-ray absorption spectroscopy, x-ray magnetic circular dichroism (XMCD), magneto-optical Kerr effect magnetometry, and Brillouin light scattering. We find the anisotropy constants decrease, while the spin wave stiffness increases as the samples are annealed to higher temperatures. The magnetization as determined by Brillouin light scattering reveals a maximum value at intermediate annealing temperatures. Surprisingly, the orbital-to-spin-moment ratio (as seen from XMCD) is essenti…

Femtosecond time-resolved photoemission electron microscopy operated at sample illumination from the rear side

We present an advanced experimental setup for time-resolved photoemission electron microscopy (PEEM) with sub-20 fs resolution, which allows for normal incidence and highly local sample excitation with ultrashort laser pulses. The scheme makes use of a sample rear side illumination geometry that enables us to confine the sample illumination spot to a diameter as small as 6 μm. We demonstrate an operation mode in which the spatiotemporal dynamics following a highly local excitation of the sample is globally probed with a laser pulse illuminating the sample from the front side. Furthermore, we show that the scheme can also be operated in a time-resolved normal incidence two-photon PEEM mode w…

Relation between spin–orbit induced spin polarization, Fano-effect and circular dichroism in soft x-ray photoemission

A Feynman diagram analysis of photoemission probabilities suggests a relation between two final-state spin polarization effects, the optical spin-orientation originating from the interaction with circularly polarized light ([Formula: see text], Fano effect) and the spin polarization induced by the spin-orbit scattering ([Formula: see text], Mott effect). The analysis predicts that [Formula: see text] is proportional to the product of [Formula: see text] and the circular dichroism in the angular distribution (CDAD) of photoelectrons. To confirm this prediction, the spin polarization of photoelectrons excited by soft x-ray radiation from initial spin-degenerate bulk states of tungsten using t…

Magnetic moment investigations of epitaxial magnetite thin films

In this report, we provide an x-ray magnetic circular dichroism (XMCD) study for 100nm thick epitaxial magnetite (Fe3O4) films on MgO (001) and Al2O3 (0001) substrates. For XMCD, we recorded the surface sensitive total electron yield and the bulk sensitive transmission spectra. From the analysis of the XMCD data, we find an increased Fe spin moment (10% larger) at the surface of the film on MgO (100) with respect to the corresponding bulk value of the film. Surface and bulk spin moments of the film on Al2O3(0001) are almost equal. For both films, the bulk orbital to spin moments ratio increases from zero at 70K to 0.03–0.04 at 300K. For Fe3O4∕MgO (001), the surface orbital to spin moment ra…

Magnetization states in ultrathin films with laterally modulated anisotropies

Abstract Micromagnetic theory has been applied to a model system for ultrathin films with laterally modulated anisotropies, consisting of a periodic array of stripes with alternating uniaxial anisotropies. Despite of the discontinuous change of anisotropy, the magnetization direction only changes on a lateral scale given by the exchange length. If the width of one of the two alternating stripes is reduced below a critical value, the magnetization will switch into a uniform state. The variation of the critical width with period, anisotropy constants, exchange constant, and film thickness has been determined using an analytic approach. Non-uniform magnetization states and the magnetization re…

Transient spatio-temporal domain patterns in permalloy microstructures induced by fast magnetic field pulses

The response of multidomain flux-closure structures (Landau states) in micrometer-scale magnetic thin-film elements upon fast magnetic field pulses leads to the excitation of magnetic eigenmodes and to short-lived domain patterns that do not occur in quasi-static remagnetisation. Such transient spatio-temporal patterns and particular detail features are discussed. Examples are presented for permalloy platelets of various shapes and sizes. Dynamic series of domain patterns with variable delay between field pulse and photon pulse (synchrotron radiation) have been taken using stroboscopic XMCD-PEEM. Precessional remagnetisation starts at the domain boundaries. The damped precessional motion pr…

Structural and Magnetic Properties of Co-Fe Binary Alloy Monolayers on W(110)

We present an experimental investigation of ${\mathrm{C}\mathrm{o}}_{x}{\mathrm{F}\mathrm{e}}_{1\ensuremath{-}x}$ monolayers grown on flat and stepped W(110) surfaces. Atomically resolved scanning tunneling microscopy and low energy electron diffraction reveal continuous miscibility and pseudomorphic growth of Co and Fe for $0\ensuremath{\le}xl0.6$. We observe short range ordered ${\mathrm{C}\mathrm{o}\mathrm{F}\mathrm{e}}_{3}$-$p(2\ifmmode\times\else\texttimes\fi{}2)$ and CoFe-$c(2\ifmmode\times\else\texttimes\fi{}2)$ structures in the pseudomorphic monolayer. High Co concentrations lead to a phase separation. The Curie temperature and the ferromagnetic Kerr signal at low temperatures decr…

Microscopic origin of the charge transfer in single crystals based on thiophene derivatives: A combined NEXAFS and density functional theory approach

We have investigated the charge transfer mechanism in single crystals of DTBDT-TCNQ and DTBDT-F4TCNQ (where DTBDT is dithieno[2,3-d;2',3'-d'] benzo[1,2-b;4,5-b']dithiophene) using a combination of near-edge X-ray absorption spectroscopy (NEXAFS) and density functional theory calculations (DFT) including final state effects beyond the sudden state approximation. In particular, we find that a description that considers the partial screening of the electron-hole Coulomb correlation on a static level as well as the rearrangement of electronic density shows excellent agreement with experiment and allows to uncover the details of the charge transfer mechanism in DTBDT-TCNQ and DTBDT-F4 TCNQ, as w…

Evidence of Spatially Inhomogeneous Electron Temperature in a Resonantly Excited Array of Bow-Tie Nanoantennas

We studied the excitation of large-area Au bow-tie nanoantenna arrays, which we have fabricated on indium-tin-oxide (ITO)-coated glass substrates using colloidal lithography with nanoscale polystyr...

Magnetic Circular Dichroism in Two-Photon Photoemission

We report the observation of magnetic circular dichroism (MCD) in two-photon photoemission (2PPE). The Heusler alloys Ni2MnGa and Co2FeSi were investigated by excitation with femtosecond laser light, showing MCD asymmetries of A=(3.5+/-0.5)x10;{-3} for Ni2MnGa and of A=(2.1+/-1.0)x10;{-3} for Co2FeSi, respectively. A theoretical explanation is provided based on local spin-density calculations for the magnetic dichroic response; the computed 2PPE MCD agrees well with the experiment. The observed 2PPE magnetic contrast represents an interesting alternative for future time-resolved photoemission studies on surface magnetism practicable in the laboratory.

Characterization and magnetic properties of nanoparticles based on FePt solid solution with an oxide shell

Abstract We present the results of magnetic properties investigations of ferromagnetic nanoparticles which ensembled with ferromagnetic shell. The aim of this work is to study the connection of structure–phase composition and thermal treatment with the magnetic properties, partially, with the coercive force and the exchange bias field in a two-dimension spin system of core–shell type. It is found that the exchange bias field increases with the growth of the oxide shell thickness. This is realized by annealing in a dosed oxygen flow. The decrease of the coercive force with the increase of annealing temperature is connected with the concentration effect (the concentration of ferromagnetic par…

Investigating spintronics thin film systems with synchrotron radiation

Abstract Spintronics is a research field involving a wide variety of different magnetic materials. Synchrotron radiation in the VUV and soft X-ray regime is ideally suited to investigate the relationships between magnetic properties and electronic structure of spintronics thin film stacks. Complex layered structures and nanomagnets are the main building blocks for current and future spintronics applications. In this contribution we describe the study of spintronics model systems with respect to the static and dynamic behavior with an emphasis on interfaces.

Thermomagnetic Properties Improved by Self-Organized Flower-Like Phase Separation of Ferromagnetic Co2Dy0.5Mn0.5Sn

A thermodynamically stable phase separation of Co2Dy0.5Mn0.5Sn into the Heusler compound Co2MnSn and Co8Dy3Sn4 is induced by rapid cooling from the liquid phase. The phase separation forms an ordered flower-like structure on the microscale. The increased scattering of phonons at the phase boundaries reduces the thermal conductivity and thus improves thermoelectric and spincaloric properties.

Investigation of a novel material for magnetoelectronics: Co2Cr0.6Fe0.4Al

Heusler compounds are promising candidates for future spintronics device applications. The electronic and magnetic properties of Co2Cr0.6Fe0.4Al, an electron-doped derivative of Co2CrAl, are investigated using circularly polarized synchrotron radiation and photoemission electron microscopy (PEEM). Element specific imaging reveals needle shaped Cr rich phases in a homogeneous bulk of the Heusler compound. The ferromagnetic domain structure is investigated on an element-resolved basis using x-ray magnetic circular dichroism (XMCD) contrast in PEEM. The structure is characterized by micrometre-size domains with a superimposed fine ripple structure; the lateral resolution in these images is abo…

Orbital-Resolved Partial Charge Transfer from the Methoxy Groups of Substituted Pyrenes in Complexes with Tetracyanoquinodimethane—A NEXAFS Study

It is demonstrated that the near-edge X-ray absorption fine structure (NEXAFS) provides a powerful local probe of functional groups in novel charge transfer (CT) compounds and their electronic properties. Microcrystals of tetra-/hexamethoxypyrene as donors with the strong acceptor tetracyano-p-quinodimethane (TMP/HMP-TCNQ) were grown by vapor diffusion. The oxygen and nitrogen K-edge spectra are spectroscopic fingerprints of the functional groups in the donor and acceptor moieties, respectively. The orbital selectivity of the NEXAFS pre-edge resonances allows us to precisely elucidate the participation of specific orbitals in the charge transfer process. Upon complex formation, the intensit…

Band structure tuning of Heusler compounds: Spin- and momentum-resolved electronic structure analysis of compounds with different band filling

Physical review / B 103(5), 054407 (2021). doi:10.1103/PhysRevB.103.054407

Martensite transition and microscopic magnetism of epitaxial Ni2MnGa films

AbstractA magnetically induced shape memory effect in Ni2MnGa results in huge magnetostrictive effects of several percent. Using x-ray absorption spectroscopy (XAS) and magnetic circular dichroism (XMCD) we investigated element specific magnetic moments and electronic structure of single crystalline, (110) oriented Ni2MnGa films on a-plane Al2O3 substrates in the austenite and martensite state. The structural phase transition of the samples is evident from temperature dependent x-ray diffraction and magnetization measurements. The Ni XAS differ significantly for temperatures above and below the martensite transition in agreement with published ab-initio calculations. Using XAS in transmissi…

Single-Hemisphere Photoelectron Momentum Microscope With Time-of-Flight Recording

Photoelectron momentum microscopy is an emerging powerful method for angle-resolved photoelectron spectroscopy (ARPES), especially in combination with imaging spin filters. These instruments record kx-ky images, typically exceeding a full Brillouin zone. As energy filters double-hemispherical or time-of-flight (ToF) devices are in use. Here we present a new approach for momentum mapping of the full half-space, based on a single hemispherical analyzer (path radius 225 mm). Excitation by an unfocused He lamp yielded an energy resolution of 7.7 meV. The performance is demonstrated by k-imaging of quantum-well states in Au and Xe multilayers. The alpha-square-aberration term (alpha: entrance an…

Multi-MHz time-of-flight electronic bandstructure imaging of graphene on Ir(111)

In the quest for detailed spectroscopic insight into the electronic structure at solid surfaces in a large momentum range, we have developed an advanced experimental approach. It combines the 3D detection scheme of a time-of-flight momentum microscope with an optimized filling pattern of the BESSY II storage ring. Here, comprehensive data sets covering the full surface Brillouin zone have been used to study faint substrate-film hybridization effects in the electronic structure of graphene on Ir(111), revealed by a pronounced linear dichroism in angular distribution. The method paves the way to 3D electronic bandmapping with unprecedented data recording efficiency.

Element-Specific Magnetic and Electronic Properties of Epitaxial Heusler Films

X-ray magnetic circular dichroism (XMCD) provides an experimental access to element-specific electronic properties of thin epitaxial films of Heusler alloys. The combination of bulk-sensitive transmission and surface-sensitive electron yield methods reveals quantitative information on bulk and interface properties. Extreme cases of magnetically dead and life layers at interfaces illustrate the high potential of XMCD. The dependence of XMCD on disorder, structure and composition is discussed as well as dynamic properties investigated by a combination of ferromagnetic resonance and XMCD. Examples are shown where spectroscopic information provided by XMCD is exploited to discuss subtle changes…

Mapováni spinů povrchových a bulkových Rashba stavů v tenkých vrstvách feroelektrického α-GeTe(111)

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…

Néel Vector Induced Manipulation of Valence States in the Collinear Antiferromagnet Mn 2 Au

The coupling of real and momentum space is utilized to tailor electronic properties of the collinear metallic antiferromagnet Mn2Au by aligning the real space Neel vector indicating the direction o...

NanoESCA: imaging UPS and XPS with high energy resolution

Abstract A novel imaging electron spectrometer has been used for laterally resolved ultraviolet photoelectron spectroscopy (UPS) and X-ray photoelectron spectroscopy (XPS) in the soft X-ray range. The instrument is based on a high-resolution emission microscope optics using a cathode lens and an imaging dispersive analyser. The analyser is corrected for the leading aberration term ( α 2 -term) by means of two hemispherical analysers in antisymmetric configuration with an appropriate transfer lens. Small-area spectra as well as energy-filtered images have been taken in the soft X-ray range for a meteorite sample and in the range of the d-band of a Cu polycrystal. An energy resolution of 106 …

Atomic-scale magnetic domain walls in quasi-one-dimensional Fe nanostripes.

Fe nanostripes on W(110) are investigated by Kerr magnetometry and spin-polarized scanning tunneling microscopy (SP-STM). An Arrhenius law is observed for the temperature dependent magnetic susceptibility indicating a one-dimensional magnetic behavior. The activation energy for creating antiparallel spin blocks indicates extremely narrow domain walls with a width on a length scale of the lattice constant. This is confirmed by imaging the domain wall by SP-STM. This information allows the quantification of the exchange stiffness and the anisotropy constant.

Quantitative microscopy of magnetic domains in Fe(100) by core-level x-ray photoelectron spectroscopy

We present an experimental technique for imaging of magnetic domain patterns based on element-specific core-level photoemission using polarized soft-x-ray radiation. It is applied to the measurement of domain patterns at the Fe(100) surface and at the surface of polycrystalline Fe. Different from well established imaging techniques that use a photoemission electron microscope to measure the secondary electron intensity at the Fe absorption threshold, we have investigated the photoemission intensity contrast on the the Fe $2{p}_{3∕2}$ core level using circularly polarized x-ray light. The linear and circular dichroism characteristics of the identical domain pattern are extracted by linear co…

Quasiparticle interference of spin momentum locked surface states at step edges on Re(0001)

Quasiparticle interference patterns formed by a surface state on the Re(0001) surface were investigated using scanning tunneling spectroscopy. The energy dispersion is inferred from Fourier-transformed differential conductivity maps for occupied and unoccupied states. The band dispersion for occupied states agrees with earlier published results obtained by angle-resolved photoemission spectroscopy. An analysis of the phase of interference patterns at step edges reveals a drastic change in the effective energy barrier for backscattering above and below the Fermi level. The attenuation of the interference pattern with increasing distance indicates interband scattering is the dominant scatteri…

Dominance of the first excitation step for magnetic circular dichroism in near-threshold two-photon photoemission

Magnetic circular dichroism (MCD) in near-threshold photoemission is measured for a perpendicularly magnetized Cs/Co/Pt(111) film with work function adjusted by Cs adsorption. For one-photon photoe ...

Back Cover: Mobilization upon Cooling (Angew. Chem. Int. Ed. 35/2021)

Site-specific atomic order and band structure tailoring in the diluted magnetic semiconductor (In,Ga,Mn)As

Physical review / B 103(7), 075107 (1-13) (2021). doi:10.1103/PhysRevB.103.075107

Mobilization upon Cooling

Abstract Phase transitions between different aggregate states are omnipresent in nature and technology. Conventionally, a crystalline phase melts upon heating as we use ice to cool a drink. Already in 1903, Gustav Tammann speculated about the opposite process, namely melting upon cooling. So far, evidence for such “inverse” transitions in real materials is rare and limited to few systems or extreme conditions. Here, we demonstrate an inverse phase transition for molecules adsorbed on a surface. Molybdenum tetraacetate on copper(111) forms an ordered structure at room temperature, which dissolves upon cooling. This transition is mediated by molecules becoming mobile, i.e., by mobilization up…

Morphology and electronic structure of bcc Co(110) and fcc/hcp Co(111) on Fe(110) investigated by STM and STS

Abstract We report on the growth of ultrathin epitaxial Co films on Fe(1 1 0) examined by scanning tunneling microscopy and spectroscopy (STM and STS). At room temperature Co forms pseudomorphic, ideally ordered body-centered cubic (bcc) layers for the first two monolayers as confirmed by atomically resolved STM images. This is in contrast to the related case of Co/Cr(1 1 0) where a superstructure occurs in the second layer. The third monolayer forms a close-packed structure and causes a transformation of the buried second monolayer into a close-packed structure. The Fe(1 1 0) substrate strongly influences the electronic structure of the first Co monolayer as concluded from the dI / dU spec…

Formation of an intermolecular charge-transfer compound in UHV codeposited tetramethoxypyrene and tetracyanoquinodimethane

Ultrahigh vacuum (UHV)-deposited films of the mixed phase of tetramethoxypyrene and tetracyanoquinodimethane $({\text{TMP}}_{1}{\text{-TCNQ}}_{1})$ on gold have been studied using ultraviolet photoelectron spectroscopy (UPS), x-ray diffraction (XRD), infrared (IR) spectroscopy, and scanning tunneling spectroscopy (STS). The formation of an intermolecular charge-transfer (CT) compound is evident from the appearance of new reflexes in XRD (${d}_{1}=0.894\text{ }\text{nm}$ and ${d}_{2}=0.677\text{ }\text{nm}$). A softening of the CN stretching vibration (redshift by $7\text{ }{\text{cm}}^{\ensuremath{-}1}$) of TCNQ is visible in the IR spectra, being indicative of a CT on the order of $0.3e$ f…

Magneto-optical linear dichroism in threshold photoemission electron microscopy of polycrystalline Fe films.

Magnetic linear dichroism in threshold photoemission has been exploited to obtain magnetic contrast in a photoemission electron microscope using a mercury arc lamp. The dichroism at threshold can be described similar to the magneto-optical Kerr effect in the region of visible light. The asymmetry of electron intensity observed for a 100 nm polycrystalline Fe film on silicon is A=(0.37+/-0.05)%. The asymmetry occurs for the geometry of the transverse Kerr effect. For unpolarized light the asymmetry was about half the value observed for linearly polarized light. Threshold photoemission microscopy has a large potential for high resolution magnetic domain imaging with fast data acquisition.

Dirakův kužel a pseudogapped hustota stavů v topologické polovině Heuslerovy sloučeniny YPtBi

Topologické izolátory (Tis) jsou zajímavé materiály, které vykazují nebývalé vlastnosti. . Zde jsme prozkoumali sloučeniny YPtBi jako příklad ze třídy polovu-Heuslerových materiálů. Topological insulators (TIs) are exciting materials, which exhibit unprecedented properties, such as helical spinmomentum locking, which leads to large torques for magnetic switching and highly efficient spin current detection. Here we explore the compound YPtBi, an example from the class of half-Heusler materials, for which the typical band inversion of topological insulators was predicted. We prepared this material as thin films by conventional cosputtering from elementary targets. By in situ time-of-flight mo…

Microwave properties and structure of La–Ti–Si–B–O glass-ceramics for applications in GHz electronics

Abstract A dielectric bulk glass-ceramic of the La 2 O 3 –TiO 2 –SiO 2 –B 2 O 3 system is developed which is able to fulfill the requirements for dielectric loading-based mobile communication technologies. It is shown that the given dielectric requirements can be fulfilled by glass-ceramic materials without being dependent on ceramic processing techniques. The material exhibited permittivity values of 20  ɛ r Qf τ f τ f material with a Qf value of 9500 GHz and ɛ r  = 21.4 could be achieved at a ceramming temperature T cer  = 870 °C. The material is aimed to provide an alternative to existing, commercially used sintered ceramic materials. Further focus is laid on the investigation of the dom…

Investigation of Many‐Body Effects in the Quasi‐Two‐Dimensional Electronic System of Organic Charge‐Transfer Salts

Magnetic Anisotropies and Coupling Mechanisms inFe/Mo(110)Nanostripes

Using low-temperature (5 K) spin-polarized scanning tunneling microscopy, we have studied the morphology and magnetic properties of monolayer (ML) and double layer (DL) thick Fe nanowires grown by step flow on a Mo(110) single crystal. Magnetic contrast has been obtained using tungsten tips covered by Au/Co thin films. We find that the DL Fe nanowires, similarly to ML Fe nanowires, are perpendicularly magnetized. Because of the dipolar coupling, separated DL Fe nanowires are antiferromagnetically coupled. DL wires that are touching at step edges are ferromagnetically ordered due to direct exchange coupling. We measured the widths of the magnetic domain walls in the ML and DL Fe nanowires. T…

Field Emission of Electrons Generated by the Near Field of Strongly Coupled Plasmons

Field emission of electrons is generated solely by the ultrastrong near-field of strongly coupled plasmons without the help of a noticeable dc field. Strongly coupled plasmons are excited at Au nanoparticles in subnanometer distance to a Au film by femtosecond laser pulses. Field-emitted electrons from individual nanoparticles are detected by means of photoelectron emission microscopy and spectroscopy. The dependence of total electron yield and kinetic energy on the laser power proves that field emission is the underlying emission process. We derive a dynamic version of the Fowler-Nordheim equation that yields perfect agreement with the experiment.

Imaging spin filter for electrons based on specular reflection from iridium (001)

Abstract As Stern–Gerlach type spin filters do not work with electrons, spin analysis of electron beams is accomplished by spin-dependent scattering processes based on spin–orbit or exchange interaction. Existing polarimeters are single-channel devices characterized by an inherently low figure of merit (FoM) of typically 10 −4 –10 −3 . This single-channel approach is not compatible with parallel imaging microscopes and also not with modern electron spectrometers that acquire a certain energy and angular interval simultaneously. We present a novel type of polarimeter that can transport a full image by making use of k -parallel conservation in low-energy electron diffraction. We studied specul…

Magnetic and Electronic Properties of Heusler Alloy Films Investigated by X-Ray Magnetic Circular Dichroism

We have investigated the magnetic properties of epitaxial Heusler alloy films using x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism∈dex{x-ray!magnetic circular dichroism} (XMCD) in the transmission (TM) and in the surface sensitive total electron yield (TEY) mode. We have investigated Ni_2MnGa based shape memory alloys and half-metallic Co2Cro.6Feo.4 films. Single crystalline Ni2MnGa(110)/Al2O3(1120) and Ni2MnGa(100)/MgO(100) films show a martensitic transition from a cubic high temperature phase to a martensitic low-temperature phase at 250–275 K as concluded from magnetometry and x-ray diffraction. The martensitic transition of this Heusler compound is shifted in…

4D texture of circular dichroism in soft-x-ray photoemission from tungsten

Brief treatment and crisis intervention 21(1), 013017 (2019). doi:10.1088/1367-2630/aaf4cd

Beyond the Heisenberg Model: Anisotropic Exchange Interaction between a Cu-Tetraazaporphyrin Monolayer andFe3O4(100)

The exchange coupling of a single spin localized at the central ion of Cu-tetraazaporphyrin on a magnetite(100) surface has been studied using x-ray magnetic circular dichroism (XMCD). Sum rule analysis of the XMCD spectra results in Cu spin and orbital magnetic moments as a function of the applied external field at low temperatures (20 K). The exchange coupling is positive for magnetization direction perpendicular to the surface (ferromagnetic) while it is negative for in-plane magnetization direction (antiferromagnetic). We attribute the anisotropy of the Heisenberg exchange coupling to an orbitally dependent exchange Hamiltonian.

Tailoring the electronic structure of half-metallic Heusler alloys

We investigated element-specific magnetic moments and the spin-resolved unoccupied density of states (DOS) of polycrystalline ${\text{Co}}_{2}\text{Ti}Z$ $(Z=\text{Si},\text{ }\text{Ge},\text{ }\text{Sn},\text{ }\text{Sb})$, ${\text{Co}}_{2}{\text{Mn}}_{x}{\text{Ti}}_{1\ensuremath{-}x}\text{Si}$ and ${\text{Co}}_{2}{\text{MnGa}}_{1\ensuremath{-}x}{\text{Ge}}_{x}$ Heusler alloys using circular dichroism in x-ray absorption spectroscopy (XMCD). We find a small $(l0.03{\ensuremath{\mu}}_{B})$ Ti moment oriented antiparallel and a large $(g3{\ensuremath{\mu}}_{B})$ Mn moment oriented parallel to the Co moment of approximately $1{\ensuremath{\mu}}_{B}$ per atom in the investigated compounds. Orb…

Stroboscopic XMCD-PEEM Imaging

Abstract This article summarizes recent results on magnetization dynamics obtained with time-resolved photoemission electron microscopy (PEEM) using X-ray magnetic circular dichroism as contrast mechanism. Time resolution is performed by a stroboscopic technique that is exclusively sensitive to reversible processes, but offers a very high time resolution only limited by the X-ray pulse width. A time resolution of 20 ps in combination with a lateral resolution of 100 nm has been achieved.

Structure and Microscopic Magnetism of Epitaxial Ni-Mn-Ga Films

We report on the structural and magnetic properties of epitaxial thin films of the ferromagnetic shape memory material Ni–Mn–Ga prepared by DC magnetron sputter deposition. Different substrate materials, i.e., MgO(100) and Al2O3(11−20) allow for a tailored epitaxial growth. Using a sacrificial chromium buffer layer freestanding epitaxial films are obtained. In combination with photolithography partially freestanding structures such as microbridges are fabricated. The complex martensite crystal structure in substrate-constrained and freestanding films is studied by means of X-ray diffraction. The identified asymmetric twin variant configuration is associated with a macroscopic surface patter…

Element-specific magnetic moments and spin-resolved density of states in CoFeMnZ(Z=Al, Ga; Si, Ge)

Using circular dichroism in x-ray-absorption spectroscopy (XAS/XMCD), we determined element-specific magnetic moments and spin-resolved unoccupied densities of states (DOS) for Co, Fe, and Mn in the quaternary Heusler compounds CoFeMn$Z$ ($Z=\text{Al}$, Ga; Si, Ge). These compounds belong to a class of highly spin-polarized materials with cubic LiMgPdSn-type structure. Different structure models for the sublattice occupation leading to similar average magnetization values can be distinguished by comparison of element-specific moments with theory. We find that the compounds form similar structures, where Co, Fe, Mn, and $Z$ occupy the $X$, ${X}^{\ensuremath{'}}$, $Y$, and $Z$ sublattice of t…

Modification of the charge and magnetic order of a low dimensional ferromagnet by molecule-surface bonding

The ability to design and control the spin and charge order of low dimensional materials on the molecular scale offers an intriguing pathway towards the miniaturization of spintronic technology towards the nanometer scale. In this work, we focus on the adsorption induced modifications of the magnetic and electronic properties of a low dimensional ferromagnetic surface alloy after the adsorption of the prototypical organic molecule perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA). For this metal-organic interface, we observe the formation of a localized $\sigma$-like bond between the functional molecular groups and the surface alloy atoms. This strong chemical bonding coincides with a l…

Analyzing the enforcement of a high-spin ground state for a metallacrown single-molecule magnet

We have studied element-selective magnetic properties of the hetero- and homometallic metallacrowns $\mathrm{Cu}{(\mathrm{II})}_{2}[12\ensuremath{-}{\mathrm{MC}}_{YN(Shi)}\ensuremath{-}4]$ ($Y=\text{Cu}$, Fe, in short ${\mathrm{CuCu}}_{4}$ and ${\mathrm{CuFe}}_{4}$). These metallacrowns comprise four Fe or Cu ions surrounding a central Cu ion. Using x-ray magnetic circular dichroism we have probed local symmetries, electronic configuration, orbital and spin magnetic moments of the magnetic ions. The ratio between the Cu and Fe moment of $\ensuremath{-}0.11$ is independent of temperature in the range of 15 K to 90 K. The Cu moment shows antiparallel to the Fe moment. For ${\mathrm{CuCu}}_{4}…

Temperature Dependence of Electronic and Magnetic Properties of (DOEO)<sub>4</sub>[HgBr<sub>4</sub>]·TCE Single Crystals

The temperature dependence of electronic and magnetic properties of the organic charge-transfer salt (DOEO)4[HgBr4]·TCE was investigated using magnetometry. The magnetic susceptibility shows a maximum at 40 K followed by an onset of a pronounced increase at 70 K and a constant behavior above 120 K. Implications on the charge carrier density are discussed. Combining the magnetometry with resistivity and ESR measurements we propose a sequence of insulating, metallic and semiconducting behavior with increasing temperature. Our results indicate that (DOEO)4[HgBr4]·TCE is close to the boundary between an insulating and conducting ground state.

Stroboscopic XMCD–PEEM imaging of standing and propagating spinwave modes in permalloy thin-film structures

Abstract Using synchrotron-based stroboscopic photoemission electron microscopy with X-ray circular dichroism as contrast method, we have investigated the high-frequency response of permalloy thin-film structures. Standing precessional modes have been studied in rectangular elements (16 × 32 μm 2 , 10 nm thick) with a high time resolution of about 15 ps in the low- α mode of BESSY. With increasing amplitude of the applied magnetic AC field the particle is driven from an initial symmetric Landau flux-closure state into an asymmetric state and finally into a single-domain state magnetized perpendicular to the applied field H AC . The electromagnetic microwave field thus can induces a net magn…

Sub-nanosecond resolution x-ray magnetic circular dichroism photoemission electron microscopy of magnetization processes in a permalloy ring

Fast magnetization processes in a microstructured permalloy ring with 80 µm o.d. and 30 nm thickness have been observed by photoemission electron microscopy exploiting x-ray magnetic circular dichroism as the magnetic contrast mechanism. As a high speed probe we employed synchrotron radiation pulses at the ESRF (Grenoble) operated in 16-bunch mode, yielding photon pulses of 105 ps FWHM with a period of 176 ns. Fast magnetic field pulses have been generated by means of current pulses through coplanar waveguides with the magnetic structure being lithographically prepared on their surface. A stroboscopic pump–probe set-up with a variable time delay between the field pulse and photon pulse allo…

Anomalous d-like surface resonances on Mo(110) analyzed by time-of-flight momentum microscopy.

The electronic surface states on Mo(110) have been investigated using time-of-flight momentum microscopy with synchrotron radiation (hν=35 eV). This novel angle-resolved photoemission approach yields a simultaneous acquisition of the E-vs-k spectral function in the full surface Brillouin zone and several eV energy interval. (kx,ky,EB)-maps with 3.4 A(-1) diameter reveal a rich structure of d-like surface resonances in the spin-orbit induced partial band gap. Calculations using the one-step model in its density matrix formulation predict an anomalous state with Dirac-like signature and Rashba spin texture crossing the bandgap at Γ¯ and EB=1.2 eV. The experiment shows that the linear dispersi…

Lateral indirect exchange coupling in a two-dimensional nanostripe array

We observe a lateral indirect exchange coupling in a multistripe system of parallel Fe nanostripes grown by self-organized growth on a vicinal single-crystal W(110) surface. The width and the distance between the stripes of monolayer height were modified via the total amount of deposited Fe. The easy axis of the magnetization lies perpendicular to the stripe edges and in the surface plane, thus resulting in a ferromagnetic dipolar coupling. In addition to the dipolar coupling we observe an antiferromagnetic indirect exchange coupling for the nanostripe system covered by Au. The coupling causes a superferromagnetic phase transition in the nanostripe array.

Phase separation in the quaternary Heusler compound CoTi(1−x)MnxSb – A reduction in the thermal conductivity for thermoelectric applications

We investigate the phase separation of the solid solution CoTi(1−x)MnxSb into the two Heusler compounds CoTiSb and CoMnSb. Energy-dispersive X-ray spectroscopy measurements on the two-phase material reveal the presence of size- and shape-tunable CoTiSb regions in a CoMnSb matrix. We demonstrate that the formed phase and grain boundaries have a considerable influence on the phonon scattering processes, which leads to a reduction in the thermal conductivity by a factor of three compared to single-phase CoTiSb.

Robustness of plasmonic angular momentum confinement in cross resonant optical antennas

Using a combination of photoemission electron microscopy and numerical simulations, we investigated the angular moment transfer in strongly enhanced optical near-fields of artificially fabricated optical antennas. The polarization dependence of the optical near-field enhancement has been measured in a maximum symmetric geometry, i.e., excitation by a normal incident planar wave. Finite-difference time-domain simulations for the realistic antenna geometries as determined by high-resolution electron microscopy reveal a very good agreement with experimental data. The agreement confirms that the geometrical asymmetries and inhomogeneities due to the nanoscale fabrication process preserve the ci…

Spin-polarized photoelectrons resonantly excited by circularly polarized light from a fractional Ag film on GaAs(100)

We demonstrate a finite spin polarization of photoelectrons emitted from GaAs(100) covered by a fractional Ag film. The photoemission yield shows a sharp maximum for intermediate coverage and the spin polarization increases with increasing laser intensity. Photoelectrons are excited by circularly polarized 100 fs laser pulses of 800 nm wavelength. We recorded the photoemitted electrons using a photoemission electron microscope combined with a Mott spin polarimeter. The spin polarization is analyzed in dependence on the excitation frequency and intensity and on the average thickness of the silver film. The results are explained by a model combining multiphoton photoemission and optical field…

Direct 3D mapping of the Fermi surface and Fermi velocity.

Time-of-flight momentum microscopy is developed. It enables direct three-dimensional mapping of the topology of the Fermi surface, identification of electron and hole pockets, and quantification of Fermi velocity as a function of wavevector.

Von geordneten zu mobilen Molekülen durch Kühlen

Phasenübergänge zwischen unterschiedlichen Aggregatzuständen sind in Natur und Technik allgegenwärtig. Üblicherweise schmilzt ein Kristall, wenn er erwärmt wird. Daher nutzen wir Eis, um einen Drink zu kühlen. Bereits im Jahre 1903 spekulierte Gustav Tammann über den umgekehrten Prozess des Schmelzens durch Kühlen. Bisher gibt es allerdings nur sehr wenige Beispiele für solche “inversen” Phasenübergänge, die meist auch auf extreme Bedingungen beschränkt sind. Hier zeigen wir einen inversen Phasenübergang von adsorbierten Molekülen auf einer Oberfläche. Molybdänacetat bildet bei Zimmertemperatur eine geordnete Struktur auf der (111)-Oberfläche von Kupfer, die sich beim Kühlen auflöst. Dieser…

Domain wall energy in quasi-one-dimensional Fe/W(110) nanostripes

The magnetic susceptibility in Fe/W(110) nanostripes decreases exponentially with increasing temperature according to an Arrhenius law which indicates a quasi-one-dimensional behavior. The interface energy of the Arrhenius law corresponds to the domain wall energy of a domain wall across a single stripe, separating fluctuating regions of homogeneous magnetization. The domain wall energy increases linearly with the width of the stripes, revealing a negative offset which we attribute to boundary effects. Domain wall energies have been determined for Fe/W(110) nanostripes coated with Au and Pd and are compared to values for uncoated Fe/W(110) nanostripes in ultrahigh vacuum.

Tip-induced mobilization upon cooling of Ni monolayers on Re(0001)

Usually, cooling a metal sample down to cryogenic temperatures leads to immobilization of the surface atoms. In this study, we demonstrate a movement of Ni adatoms at $4.6\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ on Ni films grown on a Re(0001) single crystal, while the surface is rigid at room temperature. The mobility is observed from 2 to 20 atomic-layer-thick films. Measurements at intermediate temperatures reveal an increasing mobility with decreasing temperature. The observed velocity of advancing steps is consistent with a model considering a sudden release of material, eventually triggered by the tip, followed by free diffusion. According to the model, an increasing length scale for t…

Dipolar superferromagnetism in monolayer nanostripes of Fe(110) on vicinal W(110) surfaces

By epitaxial growth of Fe on a vicinal W~110! substrate, densely spaced and continuous monolayer stripes of Fe~110! were prepared, directed along @001#. They exhibit a sharp phase transition to ferromagnetic order, free from relaxations. The magnetic easy axis is in the plane, but along @110# that means across the stripes. This cross magnetization induces ferromagnetic dipolar coupling between the spin blocks in adjacent stripes, which are preformed by exchange interactions. The resulting superferromagnetic phase transition is therefore driven by dipolar interactions. @S0163-1829~98!52002-4#

Detekcia vektora spinovej polarizácie vo viackanálovej spinovo rozlýšenej fotoemissie za použitia spinového filtra založeného na Ir(001)

Physical review / B 95(10), 104423 (2017). doi:10.1103/PhysRevB.95.104423

Spin-polarized scanning tunneling microscopy and spectroscopy of ultrathinFe∕Mo(110)films usingW∕Au∕Cotips

We report on magnetic contrast observed in low-temperature spin-polarized scanning tunneling microscopy (SP-STM) of Fe nanowires deposited on Mo(110) using tungsten tips covered by $\mathrm{Au}∕\mathrm{Co}$ thin films. Due to the spin reorientation transition of Co films on Au an out-of-plane magnetic sensitivity is obtained for tips with thin cobalt films (up to 8 monolayers of Co), while for thicker Co coverages an in-plane magnetization component can be probed. Using $\mathrm{W}∕\mathrm{Au}∕\mathrm{Co}$ tips with out-of-plane magnetic sensitivity we show that the one (ML) and two (DL) atomic layers thick Fe nanowires prepared using step flow growth on a Mo(110) crystal are perpendicularl…

Structural, electronic, and magnetic properties of pseudomorphic CrFe nanostripes on W(110)

We have grown pseudomorphic binary ${\mathrm{Cr}}_{1\ensuremath{-}x}{\mathrm{Fe}}_{x}$ alloy monolayers and sequences of Cr and Fe nanostripes on W(110) by molecular-beam epitaxy in ultrahigh vacuum. By coadsorption of Cr and Fe a pseudomorphic random CrFe alloy grows on the W(110) substrate. At a substrate temperature of $700\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ the CrFe alloy forms monolayer stripes in the step flow growth mode. We have measured magnetic properties of the monolayer alloy for $0.75\ensuremath{\leqslant}x\ensuremath{\leqslant}1$ using Kerr magnetometry. At a constant relative temperature $t=T∕{T}_{C}$ the saturation value of the Kerr rotation shows a maximum at $x=0.95$ an…

Rücktitelbild: Von geordneten zu mobilen Molekülen durch Kühlen (Angew. Chem. 35/2021)

Highly efficient multichannel spin-polarization detection.

Since the original work by Mott, the low efficiency of electron spin polarimeters, remaining orders of magnitude behind optical polarimeters, has prohibited many fundamental experiments. Here we report a solution to this problem using a novel concept of multichannel spin-polarization analysis that provides a stunning increase in efficiency by 4 orders of magnitude. This improvement was demonstrated in a setup using a hemispherical electron energy analyzer. An imaging setup proved the principal capability of resolving more than ${10}^{5}$ data points in parallel.

Emission Electron Microscopy of Nanoparticles in Strong fs Laser Fields

Full Tunability of Strain along the fcc-bcc Bain Path in Epitaxial Films and Consequences for Magnetic Properties

Strained coherent film growth is commonly either limited to ultrathin films or low strains. Here, we present an approach to achieve high strains in thicker films, by using materials with inherent structural instabilities. As an example, 50 nm thick epitaxial films of the ${\mathrm{Fe}}_{70}{\mathrm{Pd}}_{30}$ magnetic shape memory alloy are examined. Strained coherent growth on various substrates allows us to adjust the tetragonal distortion from $c/{a}_{\mathrm{bct}}=1.09$ to 1.39, covering most of the Bain transformation path from fcc to bcc crystal structure. Magnetometry and x-ray circular dichroism measurements show that the Curie temperature, orbital magnetic moment, and magnetocrysta…

Spin scattering and spin-polarized hybrid interface states at a metal-organic interface

Spin scattering at the interface formed between metallic Fe and Cu-phthalocyanine molecules is investigated by spin-polarized scanning tunneling spectroscopy and spin-resolved photoemission. The results are interpreted using first-principles electronic structure theory. The combination of experimental and theoretical techniques allows us to shed light on the role of hybrid interface states for the spin scattering. We show that Cu-phthalocyanine acts, via hybrid interface states, as a local spin filter up to room temperature both below and above the Fermi energy, ${E}_{\mathrm{F}}$. At the same time, the molecule behaves as a featureless scattering barrier in a region of about 1 eV around ${…

Emitter-site specificity of hard x-ray photoelectron Kikuchi-diffraction

New journal of physics 22(10), 103002 (1-13) (2020). doi:10.1088/1367-2630/abb68b

High-pass energy-filtered photoemission electron microscopy imaging of dopants in silicon.

Differently doped areas in silicon can show strong electron-optical contrast in dependence on the dopant concentration and surface conditions. Photoemission electron microscopy is a powerful surface-sensitive technique suitable for fast imaging of doping-induced contrast in semiconductors. We report on the observation of Si (100) samples with n- and p-type doped patterns (with the dopant concentration varied from 10(16) to 10(19) cm(-3)) on a p- and n-type substrate (doped to 10(15) cm(-3)), respectively. A high-pass energy filter of the entire image enabled us to obtain spectroscopic information, i.e. quantified photo threshold and related photoyield differences depending on the doping lev…

Test of band structure calculations for Heusler compounds by spin-resolved photoemission spectroscopy

The electronic density of states of epitaxial thin films of the Heusler compound Co${}_{2}$MnGa is probed in situ by spin-resolved ultraviolet photoemission spectroscopy. The experiments reveal several characteristic features in the intensity spectrum and a clear Fermi edge signature. A high spin polarization of $\ensuremath{\simeq}\phantom{\rule{-0.16em}{0ex}}55%$ at the Fermi edge is followed by a sign change at the binding energy of $\ensuremath{\simeq}$0.8 eV. Corresponding calculations of the band structure and the photoemission spectrum were performed employing a spin-polarized relativistic Korringa-Kohn-Rostoker code. Good agreement between the experimental data and calculations was …

Heteroepitaxial growth of Co on W(110) investigated by scanning tunneling microscopy

We investigated the growth of Co submonolayers on bcc W(110) by scanning tunneling microscopy. Due to the strong Co-W bonding, monolayers of Co grow in equilibrium pseudomorphically on W(110) until the monolayer is almost completed. When excess atoms are deposited atop the pseudomorphic monolayer, it transforms to a close-packed (cp) monolayer with misfit dislocation lines parallel to $[11\ifmmode\bar\else\textasciimacron\fi{}0]$ (Nishiyama-Wassermann orientation). The structure of the cp monolayer, as concluded from atomically resolved STM images, deviates from the rigid hard-sphere model of a cp (111) layer. Details of the structure are compared to a structure model previously proposed by…

The Properties of Co2Cr1-xFexAl Heusler Compounds

The classical concept of band structure tuning as used for semiconductors by partly replacing one atom by a chemical neighbor without altering the structure is applied examplarily to the half-metallic ferromagnetic Heusler compound Co 2 Cr 1 - x Fe x Al. Band structure calculations are presented for ordered and disordered compounds. We present experimental and theoretical results. The connection between specific site disorder and the band structure is shown explicitly with particular emphasis on the half-metallic properties. Experimentally observed deviations from the ideal Heusler structure and from the simple Slater-Pauling rule for the magnetization are discussed in close relation to the…

Phase-separation-induced changes in the magnetic and transport properties of the quaternary Heusler alloyCo2Mn1−xTixSn

The quaternary Heusler compound ${\text{Co}}_{2}{\text{Mn}}_{1\ensuremath{-}x}{\text{Ti}}_{x}\text{Sn}$ with $x=0$, 0.2, 0.4, 0.5, 0.6, 0.8, and 1 shows a phase separation into the two Heusler compounds, ${\text{Co}}_{2}\text{MnSn}$ and ${\text{Co}}_{2}\text{TiSn}$. Only at the edges of the composition range a slight admixture of Mn and Ti to the respective other phase is observed. This phase separation leads to a distinct microstructure which can be altered by the composition of the material. Pronounced changes in the magnetic and electronic properties take place with varying composition. Two magnetic transitions occur which indicate different Curie temperatures for both phases. The reduct…

Spin-resolved unoccupied density of states in epitaxial Heusler-alloy films

We investigate the electronic properties of epitaxial ${\text{Co}}_{2}({\text{Fe}}_{x}{\text{Mn}}_{1\ensuremath{-}x})\text{Si}$, ${\text{Co}}_{2}\text{Fe}({\text{Al}}_{1\ensuremath{-}x}{\text{Si}}_{x})$, and ${\text{Co}}_{2}({\text{Cr}}_{0.6}{\text{Fe}}_{0.4})\text{Al}$ films on MgO(100) substrates using circular dichroism in x-ray absorption spectroscopy (XMCD). Considering final-state electron correlations, the spin-resolved partial density of states at the Co atom can be extracted from XMCD data. The experimental results corroborate the predicted half-metallic ferromagnetic properties of these alloys and reveal a compositional dependence of the Fermi energy position within the minority b…

Element-specific ferromagnetic resonance in epitaxial Heusler spin valve systems

Time-resolved x-ray magnetic circular dichroism was used to investigate epitaxial MgO(100)/Co2Cr0.6Fe0.4Al and MgO(100)/Co2Cr0.6Fe0.4Al/Cr/CoFe films. The precessional motion of the individual sublattice magnetization, excited by continuous microwave excitation in the range 2–10 GHz, was detected by tuning the x-ray photon energy to the L 3 absorption edges of Cr, Fe and Co. The relative phase angle of the sublattice magnetization's response is smaller than the detection limit of 2°. A weakly antiferromagnetically coupled CoFe layer causes an increase in the ferromagnetic resonance linewidth consisting of a constant offset and a component linearly increasing with frequency that we partly at…

Periodic unmixing of a binary metallic vapor

We report on a type of surface structuring after short pulse laser ablation of a binary alloy. We observe the emergence of a concentric ring structure with changing elemental composition. The composition changes are interpreted by condensation of the ambient ablation vapor due to stress wave excitations in the ablation spot.

Near Field of Strongly Coupled Plasmons: Uncovering Dark Modes

Strongly coupled plasmons in a system of individual gold nanoparticles placed at subnanometer distance to a gold film (nanoparticle-on-plane, NPOP) are investigated using two complementary single particle spectroscopy techniques. Optical scattering spectroscopy exclusively detects plasmon modes that couple to the far field via their dipole moment (bright modes). By using photoemission electron microscopy (PEEM), we detect in the identical NPOPs near-field modes that do not couple to the scattered far field (dark modes) and are characterized by a strongly enhanced nonlinear electron emission process. To our knowledge, this is the first time that both far- and near-field spectroscopy are carr…

Ferromagnetism at the summit: A perspective on: “Spin polarized field emission from Fe and co-coated W tips” by Y.R. Niu and M.S. Altman

PEEM with high time resolution—imaging of transient processes and novel concepts of chromatic and spherical aberration correction

The potential of time-resolved photoemission electron microscopy (PEEM) for imaging ultrafast processes and for aberration correction in full-field imaging is discussed. In particular, we focus on stroboscopic imaging of precessional magnetic excitations via XMCD-PEEM exploiting the time structure of synchrotron radiation (magnetic field pulse pump–X-ray probe). In a special bunch-compression mode at BESSY, a time resolution of about 15 ps has been obtained. Further, we discuss an all-optical pump–probe technique using femtosecond laser excitation. A highly promising alternative to stroboscopic imaging is an approach using time-resolved image detection. As a second application of time-resol…

Development of hard x-ray photoelectron SPLEED-based spectrometer applicable for probing of buried magnetic layer valence states

Abstract A novel design of high-voltage compatible polarimeter for spin-resolved hard X-ray photoelectron spectroscopy (Spin-HAXPES) went into operation at beamline BL09XU of SPring-8 in Hyogo, Japan. The detector is based on the well-established principle of electron diffraction from a W(001) single-crystal at a scattering energy of 103.5 eV. It's special feature is that it can be operated at a high negative bias potential up to 10 kV, necessary to access the HAXPES range. The polarimeter is operated behind a large hemispherical analyzer (Scienta R-4000). It was optimized for high transmission of the transfer optics. A delay-line detector (20 mm dia.) is positioned at the exit plane of the…