Bulk spin polarization of magnetite from spin-resolved hard x-ray photoelectron spectroscopy

Physical review / B 104(4), 045129 (1-10) (2021). doi:10.1103/PhysRevB.104.045129

New HAXPES Applications at PETRA III

The application of photoelectron spectroscopy using hard X-rays (HAXPES) is becoming increasingly popular as a powerful spectroscopic tool in materials science. The success of HAXPES lies in the fa...

Hard x-ray photoelectron spectroscopy of buried Heusler compounds

This work reports on high energy photoelectron spectroscopy from the valence band of buried Heusler thin films (Co2MnSi and Co2FeAl0.5Si0.5) excited by photons of about 6?keV energy. The measurements were performed on thin films covered by MgO and SiOx with different thicknesses from 1 to 20?nm of the insulating layer and additional AlOx or Ru protective layers. It is shown that the insulating layer does not affect the high energy spectra of the Heusler compound close to the Fermi energy. The high resolution measurements of the valence band close to the Fermi energy indicate a very large electron mean free path of the electrons through the insulating layer. The spectra of the buried thin fi…

Coexisting electron emission mechanisms in small metal particles observed in fs-laser excited PEEM

Abstract Silver cluster films deposited on Si(1 1 1) were investigated by spectroscopic photoelectron microscopy using fs-laser excitation tuneable between hν = 1.45–1.65 eV and 2.9–3.3 eV. With increasing coverage the films grown as stepped wedges first exhibit clusters of few nanometers diameter with narrow size distributions that later agglomerate forming larger islands up to about 100 nm diameter. The cluster films have been characterized by SEM, AFM and HR-TEM. In the 3.1 eV range the small clusters emit more effectively and the dependence of electron yield on laser power follows a quadratic power law. Microspectroscopy reveals that the Fermi level onset is sharp(

Thermoelectric properties of CoTiSb based compounds

Several CoTiSb based compounds were synthesized and investigated on their thermoelectric properties. The aim was to improve the thermoelectric properties of CoTiSb by the systematic substitution of atoms or the introduction of additional Co into the vacant sublattice. The solid solutions Co1+xTiSb, Co1?yCuyTiSb and CoTiSb1?zBiz were synthesized. X-ray diffraction was used to investigate the crystal structure. The resistivity, the Seebeck coefficient and the thermal conductivity were determined for all compounds in the temperature range from 2 to 400?K. The highest figure of merit for each solid solution is presented. We were able to improve the figure of merit by a factor of approximately s…

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

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…

Correlation of local disorder and electronic properties in the Heusler alloy Co2Cr0.6Fe0.4Al

For the fully ordered Heusler alloy Co2Cr0.6Fe0.4Al half-metallic ferromagnetism has been predicted. Local disorder other than the Al–Cr/Fe (B2)-type disorder is known to destroy the half-metallic bandgap. The usage of appropriate buffer layers improves the structural quality of thin films. We correlate the structural properties of thin magnetron sputtered films determined by x-ray diffraction with details of the x-ray magnetic circular dichroism spectra. From the value of the magnetic moment located at the Cr atom and features of the Co absorption spectra we conclude that the buffer layers lead also to an improvement in the local atomic order. The atomic ordering gradually approaches the l…

Element-specific magnetic moments from core-absorption magnetic circular dichroism of the doped Heusler alloyCo2Cr0.6Fe0.4Al

The magnetic circular dichroism (MCD) of core-level absorption (x-ray absorption spectroscopy, XAS) spectra in the soft x-ray region has been measured for the ferromagnetic Heusler alloy ${\mathrm{Co}}_{2}{\mathrm{Cr}}_{0.6}{\mathrm{Fe}}_{0.4}\mathrm{Al}$ at the Co, Fe, and Cr ${L}_{II,III}$ edges. The comparison of XAS spectra before and after in situ cleaning of polished surfaces revealed a pronounced selective oxidation of Cr in air. For clean surfaces we observed a MCD for all three elements with Fe showing the largest moment per atom. The MCD can be explained by the density of states of the $3d$ unoccupied states, predicted by linear muffin-tin orbital atomic sphere approximation. For …

Charge transfer in the novel donor-acceptor complexes tetra- and hexamethoxypyrene with tetracyanoquinodimethane studied by HAXPES

Abstract The effect of charge transfer (CT) in complexes of the donors tetra - and hexamethoxyprene ( TMP and HMP ) with the classical acceptor tetracyanoquinodimethane ( TCNQ ) was studied using hard X-ray photoemission (HAXPES). Microcrystals of the complex were grown via vapour diffusion from donor–acceptor mixtures. The bulk sensitivity of HAXPES at a photon energy of 6 keV completely eliminates the problem of surface contamination for such delicate organic materials grown from solution. The donor molecules were produced using a novel synthesis route functionalizing polycyclic aromatic hydrocarbons at their periphery. For comparison, spectra were also taken from thin-film samples of the…

Photoemission time-of-flight spectromicroscopy of Ag nanoparticle films on Si(111)

Abstract Time-of-flight photoemission electron microscopy was used to measure spatially resolved energy distribution curves of electrons emitted from Ag nanoparticle films with different mass thicknesses. Two-photon photoemission (2PPE) was induced by femtosecond laser pulse excitation with 3.1 eV photon energy and 200 fs pulse width. Regions of Ag nanoparticles with different average sizes and one region with a continuous 100 nm thick Ag film were deposited as a stepped wedge on a Si(1 1 1) substrate. Upon laser excitation the nanoparticle films exhibit a very high electron emission yield in the images, whereas the uncovered Si surface and the continuous Ag film are dark. The time-of-fligh…

Surface resonance of thin films of the Heusler half-metal Co2MnSi probed by soft x-ray angular resolved photoemission spectroscopy

Heusler compounds are promising materials for spintronics with adjustable electronic properties including 100% spin polarization at the Fermi energy. We investigate the electronic states of AlOx capped epitaxial thin films of the ferromagnetic half-metal Co2MnSi ex situ by soft x-ray angular resolved photoemission spectroscopy (SX-ARPES). Good agreement between the experimental SX-ARPES results and photoemission calculations including surface effects was obtained. In particular, we observed in line with our calculations a large photoemission intensity at the center of the Brillouin zone, which does not originate from bulk states, but from a surface resonance. This provides strong evidence f…

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…

Electronic structure of EuO spin filter tunnel contacts directly on silicon

We present an electronic structure study of a magnetic oxide/ semiconductor model system, EuO on silicon, which is dedicated for efficient spin injection and spin detection in silicon-based spintronics devices. A combined electronic structure analysis of Eu core levels and valence bands using hard X-ray photoemission spectroscopy was performed to quantify the nearly ideal stoichiometry of EuO “spin filter” tunnel barriers directly on silicon, and the absence of silicon oxide at the EuO/Si interface. These results provide evidence for the successful integration of a magnetic oxide tunnel barrier with silicon, paving the way for the future integration of magnetic oxides into functional spintr…

Progress in HAXPES performance combining full-field k-imaging with time-of-flight recording

Journal of synchrotron radiation 26(6), 1996-2012 (2019). doi:10.1107/S1600577519012773

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...

Structure determination of thin CoFe films by anomalous x-ray diffraction

This work reports on the investigation of structure-property relationships in thin CoFe films grown on MgO. Because of the very similar scattering factors of Fe and Co, it is not possible to distinguish the random A2 (W-type) structure from the ordered B2 (CsCl-type) structure with commonly used x-ray sources. Synchrotron radiation based anomalous x-ray diffraction overcomes this problem. It is shown that as grown thin films and 300 K post annealed films exhibit the A2 structure with a random distribution of Co and Fe. In contrast, films annealed at 400 K adopt the ordered B2 structure.

Electronic properties of Co2MnSi thin films studied by hard x-ray photoelectron spectroscopy

This work reports on the electronic properties of thin films of the Heusler compound Co2MnSi studied by means of hard x-ray photoelectron spectroscopy (HAXPES). The results of photoelectron spectroscopy from multilayered thin films excited by photons of 2?8?keV are presented. The measurements were performed on (substrate/buffer layer/Co2MnSi(z)/capping layer) multilayers with a thickness z ranging from 0 to 50?nm. It is shown that high energy spectroscopy is a valuable tool for non-destructive depth profiling. The experimentally determined values of the inelastic electron mean free path in Co2MnSi increase from about 19.5 to 67?? on increasing the kinetic energy from about 1.9 to 6.8?keV. T…

Temperature-Dependent Change of the Electronic Structure in the Kondo Lattice System $YbRh_{2}Si_{2}$

Seminar, Deutschland; Journal of physics / Condensed matter 00(00), 1-20 (2021). doi:10.1088/1361-648X/abe479

Electrical and emission properties of current-carrying silver nanocluster films investigated by emission electron microscopy

Surface resonance of thin films of the Heusler half-metal Co2MnSi probed by soft x-ray angular resolved photoemission spectroscopy

Heusler compounds are promising materials for spintronics with adjustable electronic properties including 100% spin polarization at the Fermi energy. We investigate the electronic states of ${\mathrm{AlO}}_{x}$ capped epitaxial thin films of the ferromagnetic half-metal ${\mathrm{Co}}_{2}\mathrm{MnSi}$ ex situ by soft x-ray angular resolved photoemission spectroscopy (SX-ARPES). Good agreement between the experimental SX-ARPES results and photoemission calculations including surface effects was obtained. In particular, we observed in line with our calculations a large photoemission intensity at the center of the Brillouin zone, which does not originate from bulk states, but from a surface r…

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…

Photoemission Electron Microscopy as a tool for the investigation of optical near fields

Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiO$_{x}$). Photoemission was induced by illumination with a Hg UV-lamp (photon energy cutoff $\hbar\omega_{UV}=5.0$ eV, wavelength $\lambda_{UV}=250$ nm) and with a Ti:Sapphire femtosecond laser ($\hbar\omega_{l}=3.1$ eV, $\lambda_{l}=400$ nm, pulse width below 200 fs), respectively. While homogeneous photoelectron emission from the metal is observed upon illumination at energies above the silver plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signat…

Magnetometry of buried layers—Linear magnetic dichroism and spin detection in angular resolved hard X-ray photoelectron spectroscopy

Abstract The electronic properties of buried magnetic nano-layers were studied using the linear magnetic dichroism in the angular distribution of photoemitted Fe, Co, and Mn 2p electrons from a CoFe–Ir78Mn22 multi-layered sample. The buried layers were probed using hard X-ray photoelectron spectroscopy, HAXPES, at the undulator beamline P09 of the 3rd generation storage ring PETRA III. The results demonstrate that this magnetometry technique can be used as a sensitive element specific probe for magnetic properties suitable for application to buried ferromagnetic and antiferromagnetic magnetic materials and multilayered spintronics devices. Using the same instrument, spin-resolved Fe 2p HAXP…

Orbital character variation of the Fermi surface and doping dependent changes of the dimensionality inBaFe2−xCoxAs2from angle-resolved photoemission spectroscopy

From a combination of high resolution angle-resolved photoemission spectroscopy and density functional calculations, we derive information on the dimensionality and the orbital character of the electronic states of ${\text{BaFe}}_{2\ensuremath{-}x}{\text{Co}}_{x}{\text{As}}_{2}$. Upon increasing Co doping, the electronic states in the vicinity of the Fermi level take on increasingly three-dimensional character. Both the orbital variation with ${k}_{z}$ and the more three-dimensional nature of the doped compounds have important consequences for the nesting conditions and thus possibly also for the appearance of antiferromagnetic and superconducting phases.

Electronic structure and optical, mechanical, and transport properties of the pure, electron-doped, and hole-doped Heusler compound CoTiSb

The Heusler compound CoTiSb was synthesized and investigated theoretically and experimentally with respect to electronic structure and optical, mechanical, and vibrational properties. The optical properties were investigated in a wide spectral range from 10 meV to 6.5 eV and compared with ab initio calculations. The optical spectra confirm the semiconducting nature of CoTiSb, with a strong exciton absorption at 1.83 eV. The calculated phonon dispersion as well as elastic constants verify the mechanical stability of CoTiSb in the cubic $C{1}_{b}$ system. Furthermore, solid solution series of CoTi${}_{1\ensuremath{-}x}$${M}_{x}$Sb ($M=\text{Sc}$, V and $0\ensuremath{\leqslant}x\ensuremath{\le…

Magnetic and Structural Properties of Heusler Compounds with 27.8 Valence Electrons 

Co2-based Heusler compounds with 27.8 valence electrons exhibit an exceptional electronic structure that makes them interesting materials for the application in spintronics. Co2Cr0.6Fe0.4Al is the most prominent example of this particular family of compounds. In this article new materials of this class are tested with respect to their structural and magnetic properties. X-ray diffraction, Mossbauer spectroscopy, energy dispersive X-ray spectroscopy, and SQUID magnetometry were carried out to characterize the compounds. The use of Co2Fe0.45Ti0.55Ge as a new material in spintronic devices is suggested.

Electronic structure of delta-doped $La:SrTiO_{3}$ layers by hard X-ray photoelectron spectroscopy

We have employed hard x-ray photoemission (HAXPES) to study a delta-doped SrTiO3 layer that consisted of a 3-nm thickness of La-doped SrTiO3 with 6% La embedded in a SrTiO3 film. Results are compared to a thick, uniformily doped La:SrTiO3 layer. We find no indication of a band offset for the delta-doped layer, but evidence of the presence of Ti3+ in both the thick sample and the delta-layer, and indications of a density of states increase near the Fermi energy in the delta-doped layer. These results further demonstrate that HAXPES is a powerful tool for the non-destructive investigation of deeply buried doped layers.

A spatially resolved investigation of the local, micro-magnetic domain structure of single and polycrystalline Co2FeSi

The Heusler compound Co2FeSi is a promising material for magneto-electronic devices. With a Curie temperature of 1100?K and a saturation magnetization of 6?Bohr magnetons and a high spin polarization at the Fermi edge it fulfils the essential requirements for magnetic sensors or spin valve structures. An essential feature for such devices is the micro-magnetic domain structure. X-ray magnetic circular dichroism?photo emission electron microscopy has been used for a direct observation of the domain structure of single- and polycrystalline samples. The polycrystalline material exhibits a micro-magnetic ripple structure, as it is well known for pure Co and other polycrystalline Heusler compoun…

Investigation of the Thermoelectric Properties of the Series TiCo1-xNixSnxSb1-x

The effect of the simultaneous substitution of cobalt by nickel and antimony by tin in the solid solution TiCo1–xNixSnxSb1–x was systematically investigated. The number of valence electrons does not change by this substitution and therefore the resistivity stays semimetallic or semiconducting. The series were synthesized by arcmelting and the thermoelectric properties were determined. It was found out that the substitution of cobalt and antimony by nickel and tin reduces the thermal conductivity to 2 W·m–1·K–1 at 400 K. The reduction is caused by titanium rich prolate micro structures that were found by energy dispersive X-ray spectroscopy investigations. The Seebeck coefficient and the res…

Electronic Structure Changes across the Metamagnetic Transition in FeRh via Hard X-Ray Photoemission

International audience; Stoichiometric FeRh undergoes a temperature-induced antiferromagnetic (AFM) to ferromagnetic (FM) transition at similar to 350 K. In this Letter, changes in the electronic structure accompanying this transition are investigated in epitaxial FeRh thin films via bulk-sensitive valence-band and core-level hard x-ray photoelectron spectroscopy with a photon energy of 5.95 keV. Clear differences between the AFM and FM states are observed across the entire valence-band spectrum and these are well reproduced using density-functional theory. Changes in the 2p core levels of Fe are also observed and interpreted using Anderson impurity model calculations. These results indicat…

Emission Electron Microscopy of Nanoparticles in Strong fs Laser Fields

Doped semiconductors as half-metallic materials: Experiments and first-principles calculations ofCoTi1−xMxSb(M=Sc, V, Cr, Mn, Fe)

This work reports experiments and first-principles calculations on the substitutional semiconducting $C{1}_{b}$ compound $\mathrm{Co}{\mathrm{Ti}}_{1\ensuremath{-}x}{M}_{x}\mathrm{Sb}$. Diluted magnetic semiconductors have been prepared by substituting titanium in the semiconducting compound CoTiSb by other $3d$ transition elements $M$. Self-consistent calculations of the electronic structure predict some of the materials to be half-metallic ferromagnets. The structural, electronic, electric, and magnetic properties of the pure and substituted materials have been investigated. It is found from the experiments that substitution of up to 10% Ti by Fe, Mn, Cr, and V does not affect the crystal…

Optimum Carrier Concentration in n-Type PbTe Thermoelectrics

Taking La- and I-doped PbTe as an example, the current work shows the effects of optimizing the thermoelectric figure of merit, zT, by controlling the doping level. The high doping effectiveness allows the carrier concentration to be precisely designed and prepared to control the Fermi level. In addition to the Fermi energy tuning, La-doping modifies the conduction band, leading to an increase in the density of states effective mass that is confirmed by transport, infrared reflectance and hard X-ray photoelectron spectroscopy measurements. Taking such a band structure modification effect into account, the electrical transport properties can then be well-described by a self-consistent single…

Chemical stability of the magnetic oxide EuO directly on silicon observed by hard x-ray photoemission spectroscopy

We present a detailed study of the electronic structure and chemical state of high-quality stoichiometric EuO and O-rich ${\mathrm{Eu}}_{1}{\mathrm{O}}_{1+x}$ thin films grown directly on silicon without any buffer layer using hard x-ray photoemission spectroscopy (HAXPES). We determine the EuO oxidation state from a consistent quantitative peak analysis of $4f$ valence band and $3d$ core-level spectra. The results prove that nearly ideal, stoichiometric, and homogeneous EuO thin films can be grown on silicon, with a uniform depth distribution of divalent Eu cations. Furthermore, we identify the chemical stability of the EuO/silicon interface from Si $2p$ core-level photoemission. This work…