Hall effect and electronic structure of films

Abstract Tunneling experiments have shown that in order to retain half-metallicity at room temperature not only a large gap is required but also a Fermi energy considerably distant from the minority band edges. We correlate the position of the Fermi energy in the spin minority gap obtained from band structure calculations to Hall effect experiments. As a model system we chose Co 2 Fe x Mn 1 - x Si , where the Fermi energy was calculated to move from the valence band edge of the minority states to the conduction band edge with increasing x . On high quality laser ablated epitaxial films we observe a sign change of both the normal and the anomalous Hall effect with doping. The experimental da…

Angular-resolved electron spectroscopy from (110) surfaces of ternary Ce-based intermetallics: CePd2Si2 and CeNi2Ge2

Investigations of electronic properties were carried out for the ternary Ce-based intermetallic systems CeT2X2 (T = Ni, Pd; X = Ge, Si). To produce well-ordered and atomically clean surfaces, preparation is carried out in UHV. The polycrystalline substance was evaporated on a W(110) substrate with subsequent annealing. The single-crystalline layers obtained are characterised by MEED (thickness), AES (surface stoichiometry), LEED and SEM (surface structure). For electron-spectroscopic investigations, ARUPS (angle-resolved photoemission spectroscopy) was used. In the photoemission spectra, dispersion effects could be detected by variation of the detection angle.

A spatially resolved investigation of oxygen adsorption on polycrystalline copper and titanium by means of photoemission electron microscopy

Abstract The interaction of oxygen with polycrystalline copper and titanium surfaces was studied by means of photoemission electron microscopy. Variations in the image brightness were used to determine the work function of different Cu crystallites. The change of the work function was monitored during oxygen adsorption on both, Cu and Ti. Those changes are smooth for Cu whereas different Ti crystallites exhibit a rather complicated behavior during oxygen adsorption. The transformation of brightness versus exposure curves into work function versus coverage curves allows to determine the initial dipole moment of the adsorbed oxygen atoms. A value of about 20 mD was found for O on Cu(1 1 0). V…

Half-metallic ferromagnetism with high magnetic moment and high Curie temperature in Co$_2$FeSi

Co$_2$FeSi crystallizes in the ordered L2$_1$ structure as proved by X-ray diffraction and M\"o\ss bauer spectroscopy. The magnetic moment of Co$_2$FeSi was measured to be about $6\mu_B$ at 5K. Magnetic circular dichroism spectra excited by soft X-rays (XMCD) were taken to determine the element specific magnetic moments of Co and Fe. The Curie temperature was measured with different methods to be ($1100\pm20$)K. Co$_2$FeSi was found to be the Heusler compound as well as the half-metallic ferromagnet with the highest magnetic moment and Curie temperature.

Multiphoton photoemission electron microscopy using femtosecond laser radiation

Abstract The interaction of intense, pulsed laser radiation with surfaces results in non-linear optical effects that are responsible for emission of electrons even if the photon energies are below the work function. In the present study, photoelectrons have been excited by means of femtosecond laser pulses from a frequency doubled Ti:sapphire laser with a photon energy of 3.1 eV. The spatial distribution of the photo emitted electrons was imaged using a photoemission electron microscope. All samples exhibit centres of enhanced second or higher order photoemission yield, so called ‘hot spots’. These ‘hot spots’ were preferentially excited with s-polarised light. This behaviour may be explain…

Symmetry of valence states of Heusler compounds explored by linear dichroism in hard-x-ray photoelectron spectroscopy.

This study reports on the linear dichroism in angular-resolved photoemission from the valence band of the Heusler compounds ${\mathrm{NiTi}}_{0.9}{\mathrm{Sc}}_{0.1}\mathrm{Sn}$ and NiMnSb. High-resolution photoelectron spectroscopy was performed with an excitation energy of $h\ensuremath{\nu}=7.938\text{ }\text{ }\mathrm{keV}$. The linear polarization of the photons was changed using an in-vacuum diamond phase retarder. The valence band spectra exhibit the typical structure expected from first-principles calculations of the electronic structure of these compounds. Noticeable linear dichroism is found in the valence band of both materials, and this allows for a symmetry analysis of the cont…

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…

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…

Properties of the quaternary half-metal-type Heusler alloyCo2Mn1−xFexSi

This paper reports on the bulk properties of the quaternary Heusler alloy Co2Mn1�xFexSi with the Fe concentration x =0,1/2,1. All samples, which were prepared by arc melting, exhibit L21 long-range order over the complete range of Fe concentration. The structural and magnetic properties of the Co2Mn1�xFexSi Heusler alloys were investigated by means of x-ray diffraction, high- and low-temperature magnetometry, Mossbauer spectroscopy, and differential scanning calorimetry. The electronic structure was explored by means of highenergy photoemission spectroscopy at about 8 keV photon energy. This ensures true bulk sensitivity of the measurements. The magnetization of the Fe-doped Heusler alloys …

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…

Half-metallic compensated ferrimagnetism with a tunable compensation point over a wide temperature range in the Mn-Fe-V-Al Heusler system

The cubic Heusler compound Mn1.5FeV0.5Al with the L21 Heusler structure is the first fully compensated half-metallic ferrimagnet with 24 valence electrons. The ferrimagnetic state can be tuned by changing the composition such that the compensation point appears at finite temperatures ranging from 0 K up to 226 K, while retaining half-metallicity in the system. In this paper, the structural, magnetic and transport properties of the Mn-Fe-V-Al system are discussed. Magnetic reversal and a change of sign of the anomalous Hall effect were observed at the compensation point, which gives rise to a sublattice spin-crossing. These materials present new possibilities for potential spintronic devices…

Influence of the symmetry on the circular dichroism in angular resolved core-level photoemission

The model for angular resolved photoemission from adsorbed atoms is extended to account for the non-axial symmetry of atoms in a crystal field. In particular, circular dichroism in the angular distribution (CDAD) is theoretically investigated. A special emphasis is put on the case when incident photons are propagating along the principal axis of an atom in Cnv symmetry. The model, although mainly developed for adsorbates, may also be used as a base for emission from solid surfaces. An extension to simple bulk symmetries, like D for hexagonal or O for cubic crystals, is included. The CDAD 6 hh for normal incidence does not vanish in the extended model and reflects the symmetry of the adsorpt…

Quaternary Heusler Compounds without Inversion Symmetry: CoFe 1+ x Ti 1– x Al and CoMn 1+ x V 1– x Al

We report the quaternary Heusler compound derivatives CoFe1+xTi1–xAl and CoMn1+xV1–xAl, which do not have centers of inversion. Classical T2T′M (T, T′ = transition metal, M = main group element) Heusler compounds (prototype: Cu2MnAl) crystallize in the L21 structure, space group Fmm (225) that exhibits a center of inversion. Replacing one of the T2 atoms by another transition element (T″) results in a quaternary TT′T″M compound with F3m symmetry (Y; structure type LiMgPdSn) without center of inversion. In the case of “quasi closed shell” compounds with 24 valence electrons in the primitive cell, one expects the absence of ferromagnetism according to the Slater–Pauling rule. Increasing the n…

Recent progress in photoemission microscopy with emphasis on chemical and magnetic sensitivity

Abstract With the improved access to synchrotron radiation sources photoemission electron microscopy is developing into a versatile analytical tool in surface and materials science. The broad spectral range and the well-defined polarization characteristics of synchrotron light permit a unique combination of topographic, chemical, and even magnetic investigations down to a mesoscopic scale. The potentiality of photoemission electron microscopy is demonstrated by several experiments on surfaces and microstructured thin film systems, which have been carried out with a newly designed instrument. We discuss its different modes of operation with respect to both microscopy and spectroscopy. A comb…

Itinerant half-metallic ferromagnetsCo2TiZ(Z=Si, Ge, Sn):Ab initiocalculations and measurement of the electronic structure and transport properties

This work reports on ab initio calculations and experiments on the half-metallic ferromagnetic Heusler compounds ${\text{Co}}_{2}\text{Ti}Z$ $(Z=\text{Si},\text{ }\text{Ge},\text{ }\text{Sn})$. Aim is a comprehensive study of the electronic-structure and thermoelectric properties. The impact of the variation in the main group element $Z$ on those properties is discussed. X-ray diffraction was performed on the compounds and the lattice parameters are compared to other ${\text{Co}}_{2}$-based compounds. Hard x-ray photoemission measurements were carried out and the results are compared to the calculated electronic structure. The experimentally determined electronic structure, magnetic propert…

Synthesis and characterization of catalytic iridium nanoparticles in imidazolium ionic liquids

Abstract The reduction of [Ir(cod)Cl]2 (cod = 1,5-cyclooctadiene) dissolved in 1-n-butyl-3-methyl tetrafluoroborate, hexafluorophosphate and trifluoromethane sulphonate ionic liquids in the presence of 1-decene by molecular hydrogen produces Ir(0) nanoparticles. The formation of these nanoparticles follows the two-step [A → B, A + B → 2B ( k 1 , k 2 )] autocatalytic mechanism. The same mean diameter values of around 2–3 nm were estimated from in situ TEM and SAXS analyses of the Ir(0) nanoparticles dispersed in the ionic liquids and by XRD of the isolated material. XPS and EXAFS analyses clearly show the interactions of the ionic liquid with the metal surface demonstrating the formation of …

Magnetic Heusler Compounds

Abstract Heusler compounds are a remarkable class of intermetallic materials with 1:1:1 (often called Half-Heusler) or 2:1:1 composition comprising more than 1500 members. New properties and potential fields of applications emerge constantly; the prediction of topological insulators is the most recent example. Surprisingly, the properties of many Heusler compounds can easily be predicted by the valence electron count or within a rigid band approach. The wide range of the multifunctional properties of Heusler compounds is reflected in extraordinary magnetooptical, magnetoelectronic, and magnetocaloric properties. Co 2 -Heusler compounds are predicted and proven half-metallic ferromagnets sho…

Time-of-flight photoemission electron microscopy – a new way to chemical surface analysis

Abstract The time structure of synchrotron radiation at BESSY I (Berlin) was utilised to operate a photoemission electron microscope in the time-of-flight mode. The electrons that are emitted from the sample surface with different energies are dispersed in a drift tube subsequent to the imaging optics. Two ways of fast image detection have been explored, a fast gated intensified CCD camera (800 ps gate time) and a special counting electronics in combination with a 3D (x,y,t)-resolving delay line detector ( time resolution ps). The latter device has a lateral resolution of about 50 μm in the image plane being equivalent to 1000 pixels along the image diagonal. An energy resolution of 400 meV…

IMAGING OF DICHROISM IN PHOTOEMISSION ELECTRON MICROSCOPY AT NONMAGNETIC MATERIALS USING CIRCULARLY POLARIZED SOFT X-RAYS

A new approach for investigations of circular dichroism in the angular distribution of photoelectrons (CDAD) is presented. The image contrast using a photoemission line of a certain material is combined with imaging of the angular distribution pattern using a photoemission electron microscope (PEEM). CDAD can be used to investigate pure scattering information by means of the same instrument in microscopically selected regions on a surface. The experiment combines angle-resolved XPS imaging with the indirect mapping of the local environment of atoms by means of CDAD holography. In a conventional photoelectron diffraction or photoelectron holography experiment, it is necessary to move the sa…

Completely compensated ferrimagnetism and sublattice spin crossing in the half-metallic Heusler compoundMn1.5FeV0.5Al

The Slater-Pauling rule states that $L{2}_{1}$ Heusler compounds with 24 valence electrons never exhibit a total spin magnetic moment. In the case of strongly localized magnetic moments at one of the atoms (here Mn) they will exhibit a fully compensated half-metallic ferrimagnetic state instead, in particular, when symmetry does not allow for antiferromagnetic order. With the aid of magnetic and anomalous Hall effect measurements, it is experimentally demonstrated that ${\mathrm{Mn}}_{1.5}{\mathrm{V}}_{0.5}\mathrm{FeAl}$ follows such a scenario. The ferrimagnetic state is tuned by the composition. A small residual magnetization, which arises due to a slight mismatch of the magnetic moments …

Dichroism in angular resolved VUV-photoemission from the (0001) surfaces of thin Gd and Nd films epitaxially grown on W(110)

We present investigations of the electronic and magnetic structure of the Rare Earth valence states. In particular, we have examined ultra thin films (≤ 10 ML) of the rare earth metals gadolinium and neodymium epitaxially grown on tungsten (110). Various experiments on dichroism in angular resolved photoemission have been performed using circularly as well as linearly polarised light in the VUV-range with photon energies below 40 eV. A special emphasis was placed on the investigation of the surface state, which was observed for both Gd and Nd. A very small magnetic splitting of about 25 meV was observed for the surface state of ferromagnetic Gd. A magnetic ordering of a Nd-monolayer on a re…

Pressure induced insulator/half-metal/metal transition in a strongly correlatedp-electron system

Mixed-valent Rb${}_{4}$O${}_{6}$ provides an exceptional prototype material for studying the interplay between local correlations (Hubbard $U$) and electron kinetic energy ($W$) in the open $sp$-electron shell. Based on a first-principles calculation we show that depending on $U/W$ ratio, when tuned by external pressure, Rb${}_{4}$O${}_{6}$ exhibits a surprising sequence of phase transitions between strongly correlated antiferromagnetic insulator, ferromagnetic insulator ($U/W\phantom{\rule{-0.16em}{0ex}}\ensuremath{\gg}\phantom{\rule{-0.16em}{0ex}}1$), moderately correlated ferromagnetic half-metal ($U/W\phantom{\rule{-0.16em}{0ex}}\ensuremath{\sim}\phantom{\rule{-0.16em}{0ex}}1$), and fin…

AN EXPERIMENTAL PROOF OF THE BACK-SCATTERING MODEL FOR DICHROIC EFFECTS IN VUV PHOTOEMISSION

The energy dependence of the circular dichroism in the angular distribution of photoelectrons (CDAD) was investigated from the shallow Cs 5p core levels. Cesium was prepared in a hexagonal ordered monolayer on W(110). The results are mainly influenced by scattering of the photoelectrons within the adlayer. At low energies, the behavior observed is described by means of a model that treats only the back-scattering of photoelectrons at the potential step between the adlayer and the substrate. It leads to a simple method determining the position of the monolayer with respect to the substrate. In this approach, the back-scattering model is matched with the measured energy dependence of the CDA…

Challenge of magnetism in strongly correlated open-shell 2p systems.

We report on theoretical investigations of the exotic magnetism in rubidium sesquioxide ${\mathrm{Rb}}_{4}{\mathrm{O}}_{6}$, a model correlated system with an open $2p$ shell. Experimental investigations indicated that ${\mathrm{Rb}}_{4}{\mathrm{O}}_{6}$ is a magnetically frustrated insulator. The frustration is explained here by electronic structure calculations that incorporate the correlation between the oxygen $2p$ electrons and deal with the mixed-valent oxygen. This leads to a physical picture where the symmetry is reduced because one third of the oxygen in ${\mathrm{Rb}}_{4}{\mathrm{O}}_{6}$ is nonmagnetic while the remaining two thirds assemble in antiferromagnetic arrangements. A d…

Spin and Orbital Magnetic Moments of FePt Thin Films

The magnetic moments of disordered and ordered L10 Fe50Pt50 films were investigated using magnetic circular dichroism (MCD) and spin polarized full relativistic Korringa–Kohn–Rostoker (SPRKKR) calculations. The measurements showed that the spin magnetic moments of Fe in both ordered and disordered films were similar with a lower value than that obtained by SPRKKR calculations. Both films however showed larger orbital moments of Fe compared to the calculations. It is suggested that the spin magnetic moment of Fe in FePt thin films was insensitive to L10 ordering.

Tailoring of the electrical and thermal properties using ultra-short period non-symmetric superlattices

Thermoelectric modules based on half-Heusler compounds offer a cheap and clean way to create eco-friendly electrical energy from waste heat. Here we study the impact of the period composition on the electrical and thermal properties in non-symmetric superlattices, where the ratio of components varies according to (TiNiSn)���:(HfNiSn)���������, and 0 ��� n ��� 6 unit cells. The thermal conductivity (��) showed a strong dependence on the material content achieving a minimum value for n = 3, whereas the highest value of the figure of merit ZT was achieved for n = 4. The measured �� can be well modeled using non-symmetric strain relaxation applied to the model of the series of thermal resistanc…

The half-metallic ferromagnet

Abstract Electronic structure calculation were used to predict a new material for spintronic applications. Co 2 Mn 0.5 Fe 0.5 Si is one example which is stable against on-site correlation and disorder effects due to the position of the Fermi energy in the middle of the minority band gap. Experimentally the sample were made exhibiting L 2 1 structure and a high magnetic order.

Ni-based superconductor: Heusler compoundZrNi2Ga

This work reports on the novel Heusler superconductor ZrNi2Ga. Compared to other nickel-based superconductors with Heusler structure, ZrNi2Ga exhibits a relatively high superconducting transition temperature of Tc=2.9 K and an upper critical field of 1.5 T. Electronic structure calculations show that this relatively high transition temperature is caused by a van Hove singularity, which leads to an enhanced density of states at the Fermi energy. The van Hove singularity originates from a higher order valence instability at the L-point in the electronic structure. The enhanced density of states at the Fermi level was confirmed by specific heat and susceptibility measurements. Although many He…

Crystal Structure of New Heusler Compounds

Heusler compounds are promising materials in many fields of contemporary research. The spectrum of their possible applications ranges from magnetic and magneto-mechanical materials over semiconductors and thermoelectrics to superconductors. An important feature of the Heusler compounds is the possibility of controlling the valence electron concentration by partial substitution of elements. On the other hand, the properties also depend on the degree of ordering of the the crystal structure. In general, Heusler compounds crystallize in the Cu2MnAl-type structure but in many cases certain types of disorder are observed. In this paper a detailed description of the different types of disordered …

Electronic transport properties of electron- and hole-doped semiconductingC1bHeusler compounds:NiTi1−xMxSn(M=Sc,V)

The substitutional series of Heusler compounds ${\text{NiTi}}_{1\ensuremath{-}x}{M}_{x}\text{Sn}$ (where $M=\text{Sc},\text{V}$ and $0lx\ensuremath{\le}0.2$) were synthesized and investigated with respect to their electronic structure and transport properties. The results show the possibility to create $n$-type and $p$-type thermoelectrics within one Heusler compound. The electronic structure and transport properties were calculated by all-electron ab initio methods and compared to the measurements. Hard x-ray photoelectron spectroscopy was carried out and the results are compared to the calculated electronic structure. Pure NiTiSn exhibits massive ``in gap'' states containing about 0.1 ele…

Spin-resolved low-energy and hard x-ray photoelectron spectroscopy of off-stoichiometric Co2MnSi Heusler thin films exhibiting a record TMR

Half-metallic Co2MnSi-based Heusler compounds have attracted attention because they yield very high tunnelling magnetoresistance (TMR) ratios. Record TMR ratios of 1995% (at 4.2 K) are obtained from off-stoichiometric Co2MnSi-based magnetic tunnel junctions. This work reports on a combination of band structure calculations and spin-resolved and photon-polarisation-dependent photoelectron spectroscopy for off-stoichiometric Heusler thin films with the composition Co2Mn1.30Si0.84. Co and Mn are probed by magnetic dichroism in angle-resolved photoelectron spectroscopy at the 2p core level. In contrast to the delocalised Co 3d states, a pronounced localisation of the Mn 3d states is deduced fro…

Electronic and crystallographic structure, hard x-ray photoemission, and mechanical and transport properties of the half-metallic Heusler compound Co2MnGe

This work reports on the electronic and crystalline structure and the mechanical, magnetic, and transport properties of the polycrystalline Heusler compound Co${}_{2}$MnGe. The crystalline structure was examined in detail by extended x-ray absorption fine-structure spectroscopy and anomalous x-ray diffraction. The compound exhibits a well-ordered $L{2}_{1}$ structure as is typical for Heusler compounds with 2:1:1 stoichiometry. The low-temperature magnetic moment agrees well with the Slater-Pauling rule and indicates a half-metallic ferromagnetic state of the compound, as is predicted by ab initiocalculations. Transport measurements and hard x-ray photoelectron spectroscopy were performed t…

Structural, electronic, and magnetic properties of tetragonalMn3−xGa: Experiments and first-principles calculations

This work reports on the electronic, magnetic, and structural properties of the binary intermetallic compounds ${\mathrm{Mn}}_{3\ensuremath{-}x}\mathrm{Ga}$. The tetragonal ${\mathrm{DO}}_{22}$ phase of the ${\mathrm{Mn}}_{3\ensuremath{-}x}\mathrm{Ga}$ series, with $x$ varying from 0 to 1.0 in steps of $x=0.1$, was successfully synthesized and investigated. It was found that all these materials are hard magnetic, with energy products ranging from $10.1\phantom{\rule{0.3em}{0ex}}\mathrm{kJ}\phantom{\rule{0.2em}{0ex}}{\mathrm{m}}^{\ensuremath{-}3}$ for low Mn content $(x\ensuremath{\rightarrow}1)$ to $61.6\phantom{\rule{0.3em}{0ex}}\mathrm{kJ}\phantom{\rule{0.2em}{0ex}}{\mathrm{m}}^{\ensurema…

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 …

Geometric, electronic, and magnetic structure of Co$_2$FeSi: Curie temperature and magnetic moment measurements and calculations

In this work a simple concept was used for a systematic search for new materials with high spin polarization. It is based on two semi-empirical models. Firstly, the Slater-Pauling rule was used for estimation of the magnetic moment. This model is well supported by electronic structure calculations. The second model was found particularly for Co$_2$ based Heusler compounds when comparing their magnetic properties. It turned out that these compounds exhibit seemingly a linear dependence of the Curie temperature as function of the magnetic moment. Stimulated by these models, Co$_2$FeSi was revisited. The compound was investigated in detail concerning its geometrical and magnetic structure by m…

Using photoelectron emission microscopy with hard-X-rays

We present several successful test cases of using photoelectron emission microscopy (PEEM) for photon energy up to 25 keV. First, the full extended X-ray absorption fine structure analysis was implemented in areas as small as 100 mum(2) for transition-metal K edge absorption spectra and, therefore, demonstrated the feasibility of combining structural and chemical analysis with hard-X-ray absorption spectroscopy with high lateral resolution. We also show that PEEM can be used in a transmission (radiography) mode as an imaging detector for hard-X-ray, This approach again leads to the unprecedented 0.3 mum lateral resolution, particularly critical for the use of coherence-based phase contrast …

Photoelectron-holography using circularly polarized light

Abstract Circular dichroism in the angular distribution of photoelectrons (CDAD) is not only observed from aligned initial states, but also as a consequence of the scattering of photoelectrons at the surrounding atoms in a solid or an adsorbate. Using the analytical result for the CDAD, we show that it is an integral transformation of the product of the angular momentum of the emitted electron and the Fourier-transformed scattering potential of the surrounding atoms. Therefore, we interpret the CDAD pattern as photoelectron-hologram. The real space distribution of atoms can be reconstructed by an inverse integral transformation of the CDAD pattern, which carries the full phase-information. …

Generalization of the atomic random-phase-approximation method for diatomic molecules:N2photoionization cross-section calculations

Partial and total photoionization cross sections of ${\mathrm{N}}_{2}$ molecule are calculated using the generalization of the random-phase approximation (RPA) which earlier has been successfully applied to the description of the atomic photoionization processes. According to this method, at first the Hartree-Fock (HF) ground-state wave functions are calculated in prolate spheroidal coordinates using the fixed-nuclei approximation. With their help the zero order basis set of single particle Hartree-Fock wave functions containing both discrete excited states and continuous spectrum is calculated in the field of a frozen core of a singly charged ion. The calculations are performed for all fou…

Charge transfer and tunable minority band gap at the Fermi energy of a quaternaryCo2(MnxTi1−x)GeHeusler alloy

We investigate the distribution of element-specific magnetic moments and changes in the spin-resolved unoccupied density of states in a series of half-metallic ${\text{Co}}_{2}({\text{Mn}}_{x}{\text{Ti}}_{1\ensuremath{-}x})\text{Ge}$ Heusler alloys using x-ray magnetic circular dichroism. The Co and Mn magnetic moments are oriented parallel while a small Ti moment shows antiparallel to the mean magnetization. The element-specific magnetic moments remain almost independent on the composition. Therefore, a replacement of Ti by Mn results in an increase in magnetization. The increase in magnetization with increasing $x$ follows the Slater-Pauling rule. The Fermi level decreases with respect to…

Correlation in the transition metal based Heusler compounds Co$_2$MnSi and Co$_2$FeSi

Half-metallic ferromagnets like the full Heusler compounds with formula X$_2$YZ are supposed to show an integer value of the spin magnetic moment. Calculations reveal in certain cases of X = Co based compounds non-integer values, in contrast to experiments. In order to explain deviations of the magnetic moment calculated for such compounds, the dependency of the electronic structure on the lattice parameter was studied theoretically. In local density approximation (LDA), the minimum total energy of Co$_2$FeSi is found for the experimental lattice parameter, but the calculated magnetic moment is about 12% too low. Half-metallic ferromagnetism and a magnetic moment equal to the experimental v…

Understanding the trend in the Curie temperatures ofCo2-based Heusler compounds:Ab initiocalculations

The Curie temperatures for the Heusler compounds Co{sub 2}TiAl, Co{sub 2}VGa, Co{sub 2}VSn, Co{sub 2}CrGa, Co{sub 2}CrAl, Co{sub 2}MnAl, Co{sub 2}MnSn, Co{sub 2}MnSi, and Co{sub 2}FeSi are determined ab initio from the electronic structure obtained with the local-density functional approximation and/or the generalized gradient approximation. Frozen spin spirals are used to model the excited states needed to evaluate the spherical approximation for the Curie temperature. The spherical approximation is found to describe the experimental Curie temperatures very well which, for the compounds selected, extend over the range from 95 to 1100 K; as a function of the valence electron count, they sho…

Probing the electronic states of high-TMR off-stoichiometric Co2MnSi thin films by hard x-ray photoelectron spectroscopy

The tunnel magnetoresistance ratio (TMR) of fully epitaxial magnetic tunnel junctions with an off-stoichiometric Co${}_{2}$MnSi Heusler alloy has been shown to exhibit a systematic dependence on Mn content, reaching 1135% at 4.2 K for Co${}_{2}$Mn${}_{1.29}$Si. In this paper, we explain the behavior of the observed TMR ratio using ab initio calculations and hard x-ray photoelectron spectroscopy (HAXPES). For the Mn-deficient samples, we show that the the drop of the TMR is caused by Co antisite atoms, which impose extra states into the minority-spin band gap. On the other hand, Mn-excess composition shows nearly half-metallic behavior. This result can be intuitively understood since both Co…

Electronic and structural properties of palladium-based Heusler superconductors

Abstract This work reports on superconductivity in the Heusler compounds Pd2ZrAl and Pd2HfAl. Magnetisation and resistance measurements were carried out to verify their superconducting states. The compounds exhibit transition temperatures of 3.2 K (Zr) and 3.4 K (Hf). From their behaviour in external magnetic fields, it was determined that both compounds are type II superconductors. Similar to the half-metallic ferromagnets, the superconducting Heusler compounds follow an electron counting scheme based on theoretical considerations. As found from ab initio calculations, the superconductivity can be explained by a valence instability at the L -point, that has been used as design criterion.

Superconductivity in palladium-based Heusler compounds

This work reports on four more Heusler superconductors: ${\text{Pd}}_{2}\text{ZrAl}$, ${\text{Pd}}_{2}\text{HfAl}$, ${\text{Pd}}_{2}\text{ZrIn}$, and ${\text{Pd}}_{2}\text{HfIn}$. These compounds exhibit superconducting transition temperatures ranging from 2.4--3.8 K as determined by resistivity measurements. According to their behavior in an external magnetic field, all compounds are type II bulk superconductors. The occurrence of superconductivity was predicted for these compounds using electronic structure calculations. The electronic structures exhibit van Hove singularities (saddle points) at the $L$ point. These lead to a maximum in the corresponding density of states and superconduct…

Co2CrIn: A further magnetic Heusler compound

Summary and Outlook In summary, this work presents the synthesis andcharacterisation of the Heusler compound Co 2 CrIn.The compound is L2 1 ordered and shows no major an-tisite disorder. Co 2 CrIn turns out to be a ferrimagnetwith a magnetic moment of 1.18 µ B at 5 K. In addi-tion, the hysterisis curve reveals a soft magnetic be-haviour. A measurement of the site specific magneticmomentsis highlydesirableas it might leadto a deeperunderstanding of the magnetic properties of Co 2 CrIn.Furthermore, the measured magnetic moment is not aninteger number, as expected for a half-metallic ferro-magnet. Thus, Co 2 CrIn can not be a half-metallic fer-romagnet, as most of the other Co 2 YZ Heusler com-…

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…

Circular dichroism in angular resolved photoemission from pure and Rb-doped C60 and C22H14 layers on platinum and tungsten

Abstract Polycrystalline C60 and Pentacene films grown on W(110) and Pt(111) have been studied in valence band photoemission using circularly polarised synchrotron radiation from BESSY with special emphasis on circular dichroism in photoemission. For thin films of C60, dichroic asymmetries of about 10% occur independent of the temperature and the substrate hinting that the rotation of the topmost layer is hindered even at room temperature. For Pentacene we found asymmetries up to 50% in the region of the σ-electrons. Moreover, we found for this molecule a dichroic asymmetry in normal emission, that is a forbidden geometry. This hints on adsorption with the molecules perpendicularly oriented…

Investigation of Co$_2$FeSi: The Heusler compound with Highest Curie Temperature and Magnetic Moment

This work reports on structural and magnetic investigations of the Heusler compound Co$_2$FeSi. X-Ray diffraction and M\"o\ss bauer spectrometry indicate an ordered $L2_1$ structure. Magnetic measurements by means of X-ray magnetic circular dichroism and magnetometry revealed that this compound is, currently, the material with the highest magnetic moment ($6 \mu_B$) and Curie-temperature (1100K) in the classes of Heusler compounds as well as half-metallic ferromagnets.

Properties of Co/sub 2/YZ Heusler compounds

Heusler compounds of Co/sub 2/XY composition (Co/sub 2/Cr/sub 0.6/Fe/sub 0.4/Al, Co/sub 2/FeSi) offer a variety of half-metallic ferromagnetic materials. These were prepared by arc melting and comprehensively characterized by means of X-ray diffraction ( XRD), Mossbauer spectroscopy, magnetic X-ray circular dichroism spectroscopy (MXCD), superconducting quantum interference device (SQUID) magnetometry, electron spectroscopy for chemical analysis (ESCA), extended X-ray absorption fine structure (EXAFS) and Auger electron spectroscopy (AES) depth profiling. Structural disorder phenomena, magnetic hysteresis, magnetic moments, magnetic transition temperatures and Curie temperature were obtaine…

Temperature-dependent angular resolved UV-photoemission spectroscopy from CeNi2Ge2

Abstract Pronounced temperature effects in angular resolved ultraviolet photoelectron spectroscopy from the (001) surface of the ternary heavy fermion compound CeNi 2 Ge 2 are presented. The measurements were performed on atomically clean and well-ordered thin films grown on a W(110) substrate. A strongly enhanced intensity at the Fermi edge ( ϵ F ) is observed at low-temperatures if the spectra are excited by means of HeI light ( hν =21.2 eV). In addition, the work function is dramatically increased with temperature, exhibiting an unusually high positive temperature coefficient of about 0.65 meV/K. The observed temperature dependency suggests a strong redistribution of the states near the …

Preparation of thin films of the ternary heavy fermion system CeNi 2 Ge 2

Ge2 layers on W(110). In order to produce well-ordered and atomically clean surfaces of the Ce-based intermetallic system the growth was performed under UHV conditions (p<2×10-11 mbar). Both the polycrystalline CeNi2Ge2 compound and the individual elements Ce, Ni, and Ge were used as evaporants. The characterisation of the layers was made with LEED, SEM, and XPS. We find a significant influence of the substrate temperature and the evaporation power on the growth characteristics. The compound material CeNi2Ge2 exhibits complicated behaviour when evaporated. Under carefully selected growth conditions we obtain well-ordered films with a stoichiometry of Ce:Ni:Ge=1:2:2 and a (001) oriented surf…

Clean and ordered surfaces of CeNi 2 Ge 2 layers on W(110)

Investigations of the geometric and electronic properties of ternary Ce-based heavy fermion systems CeT2X2 (T : Ni,Pd,Rh; X : Ge,Si) were carried out by means of electron spectroscopic methods. The main problem for these surface-sensitive techniques is the preparation of well-ordered and atomically clean surfaces. The ternary substance CeNi2Ge2 was grown on a W(110) substrate by MBE with subsequent annealing. A nearly layer-by-layer growth mode was detected using MEED. The annealed layers are ordered, but show small Ni2Ge crystalline islands. The composition was characterised by means of AES in dependence of the substrate as well as the annealing temperature. Electronic properties are inves…

Correlation in Heusler compounds YSi(Y=3d transition metal)

Abstract Ferromagnetic Co 2 -based Heusler compounds have generated increasing interest over the last few years because of their peculiar electronic structure. They exhibit a band gap for the electrons of one direction and are metallic for the other. Further, they cover a very wide range of magnetic moments and Curie temperatures. Despite lot of efforts in theory and experiment to describe bulk materials and thin films, there are some marked discrepancies between observed and predicted properties of these materials. These discrepancies appear not only across but also within synthesis methods as well as in the theoretical predictions. In this contribution, the electronic structure of Co 2 YS…

Electronic, structural, and magnetic properties of the half-metallic ferromagnetic quaternary Heusler compounds CoFeMnZ(Z=Al, Ga, Si, Ge)

The quaternary intermetallic Heusler compounds CoFeMn$Z$ ($Z=\text{Al}$, Ga, Si, or Ge) with $1:1:1:1$ stoichiometry were predicted to exhibit half-metallic ferromagnetism by ab initio electronic structure calculations. The compounds were synthesized using an arc-melting technique and the crystal structures were analyzed using x-ray powder diffraction. The electronic properties were investigated using hard x-ray photoelectron spectroscopy. The low-temperature magnetic moments, as determined from magnetization measurements, follow the Slater-Pauling rule, confirming the proposed high spin polarizations. All compounds have high Curie temperatures, allowing for applications at room temperature…

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…

Unraveling the Formation of Core−Shell Structures in Nanoparticles by S-XPS

The combination of the surface sensitivity of X-ray photoelectron spectroscopy (XPS) with the high flux and variable photon energy excitation of Synchrotron radiation (S-XPS) is used to probe the atomic distribution of bimetallic nanoparticles. Based on the energy dependence of the photoemission differential cross section of core level photoelectrons, we propose a methodology to monitor the formation and to evaluate sizes of the core−shell structure. We have successfully applied it to unveil the mechanism involved in the atomic rearrangement of thermally treated Pt0.7Pd0.3 nanoparticles.

Angular and temperature dependence of the magnetic circular dichroism in4dcore-level photoemission from Gd(0001)

We present experimental and theoretical results for the angular and temperature dependence of magnetic circular dichroism in Gd $4d$ core-level photoelectron emission from a Gd(0001) surface in both normal and off-normal directions and with azimuthal variation. Two theoretical approaches are used to model this data: a single electron theory with full multiple scattering of the outgoing photoelectron and a full-relativistic many-electron theory with single scattering only. Thermal effects due to atomic vibrations and the excitation of initial-state multiplets are also included. For normal emission, we find smooth free-atom-like angular variations in emission intensity, while for off-normal e…

Co2CrIn: A Further Magnetic Heusler Compound

Summary and Outlook In summary, this work presents the synthesis andcharacterisation of the Heusler compound Co 2 CrIn.The compound is L2 1 ordered and shows no major an-tisite disorder. Co 2 CrIn turns out to be a ferrimagnetwith a magnetic moment of 1.18 µ B at 5 K. In addi-tion, the hysterisis curve reveals a soft magnetic be-haviour. A measurement of the site specific magneticmomentsis highlydesirableas it might leadto a deeperunderstanding of the magnetic properties of Co 2 CrIn.Furthermore, the measured magnetic moment is not aninteger number, as expected for a half-metallic ferro-magnet. Thus, Co 2 CrIn can not be a half-metallic fer-romagnet, as most of the other Co 2 YZ Heusler com-…

Charakterisierung von dotierten Heusler-Verbindungen: Co2Cr1−xFexAl

Electronic structure, localization, and spin-state transition in Cu-substitutedFeSe:Fe1−xCuxSe

We report density-functional studies of the ${\text{Fe}}_{1\ensuremath{-}x}{\text{Cu}}_{x}\text{Se}$ alloy done using supercell and coherent-potential approximation methods. Magnetic behavior was investigated using the disordered local moment approach. We find that Cu occurs in a nominal ${d}^{10}$ configuration and is highly disruptive to the electronic structure of the Fe sheets. This would be consistent with a metal-insulator transition due to Anderson localization. We further find a strong crossover from a weak moment itinerant system to a local moment magnet at $x\ensuremath{\approx}0.12$. We associate this with the experimentally observed jump near this concentration. Our results are …

The dependence of circular dichroism in photoemission on the optical properties of Cs monolayers on Pt(111)

We report on the dependence of dichroic photoemission excited by circularly polarised light on the angle of photon incidence. We measured the difference in the angle-resolved photoemission intensities from Cs 5p semi-core levels excited by photons of opposite helicity, which is known as CDAD. We found that the dependence of the measured differences on the angle of light incidence deviates strongly from the model of CDAD for free atoms, as expected. Using the Fresnel equations and a complex index of refraction, one finds that not only the third component but also the second component of the Stokes vector is responsible for the excitation process. Both Stokes components change sign if the ini…

Photoabsorption and MXCD in Photoemission Microscopy for Characterization of Advanced Materials

We used imaging spectromicroscopy to characterise micro-patterned thin films of magnetic materials like FeNi alloys on Silicon. To investigate devices built from complex materials we applied element-sensitive photoelectron emission microscopy (PEEM). Information about the chemical composition of the imaged sample can be obtained by PEEM via tuning the photon energy to X-ray absorption edges. One aim of our work was to observe oxygen related defects and changes in the composition effecting the physical properties of the materials. The use of circularly polarised photons allows us to image magnetic domains by making use of the magnetic circular dichroism (MXCD).

Spin Polarimetry and Magnetic Dichroism on a Buried Magnetic Layer Using Hard X-ray Photoelectron Spectroscopy

The spin-resolved electronic structure of buried magnetic layers is studied by hard X-ray photoelectron spectroscopy (HAXPES) using a spin polarimeter in combination with a high-energy hemispherical electron analyzer at the high-brilliance BL47XU beamline (SPring-8, Japan). Spin-resolved photoelectron spectra are analyzed in comparison with the results of magnetic linear and circular dichroism in photoelectron emission in the case of buried Co2FeAl0.5Si0.5 layers. The relatively large inelastic mean free path (up to 20 nm) of fast photoelectrons enables us to extend the HAXPES technique with electron-spin polarimetry and to develop spin analysis techniques for buried magnetic multilayers a…

Improving thermoelectric performance of TiNiSn by mixing MnNiSb in the half-Heusler structure

The thermoelectric properties of n type semiconductor, TiNiSn is optimized by partial substitution with metallic, MnNiSb in the half Heusler structure. Herein, we study the transport properties and intrinsic phase separation in the system. The Ti1-xMnxNiSn1-xSbx alloys were prepared by arc-melting and were annealed at temperatures obtained from differential thermal analysis and differential scanning calorimetry results. The phases were characterized using powder X-ray diffraction patterns, energy dispersive X-ray spectroscopy, and differential scanning calorimetry. After annealing the majority phase was TiNiSn with some Ni rich sites and the minority phases was majorly Ti6Sn5, Sn, and MnSn2…

Challenging the Prediction of Anionogenic Ferromagnetism for Rb4O6

It has been suggested that Rb4O6 should be a half-metallic ferromagnet with the magnetic moment carried by the hyperoxide anions and a Curie temperature above room temperature. In the present work,...

Electronic structure calculations in ordered and disordered solids with spiral magnetic order

A scheme to calculate the electronic structure of systems having a spiral magnetic structure is presented. The approach is based on the Korringa-Kohn-Rostoker Green's function formalism which allows, in combination with the coherent potential approximation alloy theory, dealing with chemically disordered materials. It is applied to the magnetic random alloys Fe${}_{x}$Ni${}_{1\ensuremath{-}x}$, Fe${}_{x}$Co${}_{1\ensuremath{-}x}$, and Fe${}_{x}$Mn${}_{1\ensuremath{-}x}$. For these systems the stability of their magnetic structure was analyzed. For Fe${}_{x}$Ni${}_{1\ensuremath{-}x}$ the spin stiffness for was determined as a function of concentration that was found in satisfying agreement w…

New Heusler Compounds and Their Properties

Spintronics is a multidisciplinary field and a new research area. New materials must be found for satisfying the different types of requirement. The search for stable half-metallic ferromagnets and ferromagnetic semiconductors with Curie temperatures higher than room temperature is still a challenge for solid state scientists. A general understanding of how structures are related to properties is a necessary prerequisite for material design. Computational simulations are an important tool for a rational design of new materials. The new developments in this new field are reported from the point of view of material scientists.

Theoretical study of new acceptor and donor molecules based on polycyclic aromatic hydrocarbons

Functionalized polcyclic aromatic hydrocarbons (PAHs) are an interesting class of molecules in which the electronic state of the graphene-like hydrocarbon part is tuned by the functional group. Searching for new types of donor and acceptor molecules, a set of new PAHs has recently been investigated experimentally using ultraviolet photoelectron spectroscopy (UPS). In this work, the electronic structure of the PAHs is studied numerically with the help of B3LYP hybrid density functionals. Using the DELTA-SCF method, electron binding energies have been determined which affirm, specify and complement the UPS data. Symmetry properties of molecular orbitals are analyzed for a categorization and a…

Bulk sensitive photo emission spectroscopy of compounds

This work reports about bulk-sensitive, high energy photoelectron spectroscopy from the valence band of CoTiSb excited by photons from 1.2 to 5 keV energy. The high energy photoelectron spectra were taken at the KMC-1 high energy beamline of BESSY II employing the recently developed Phoibos 225 HV analyser. The measurements show a good agreement to calculations of the electronic structure using the LDA scheme. It is shown that the high energy spectra reveal the bulk electronic structure better compared to low energy XPS spectra.

Exotic magnetism in the alkali sesquioxidesRb4O6andCs4O6

Among the various alkali oxides the sesquioxides ${\text{Rb}}_{4}{\text{O}}_{6}$ and ${\text{Cs}}_{4}{\text{O}}_{6}$ are of special interest. Electronic-structure calculations using the local spin-density approximation predicted that ${\text{Rb}}_{4}{\text{O}}_{6}$ should be a half-metallic ferromagnet, which was later contradicted when an experimental investigation of the temperature-dependent magnetization of ${\text{Rb}}_{4}{\text{O}}_{6}$ showed a low-temperature magnetic transition and differences between zero-field-cooled and field-cooled measurements. Such behavior is known from spin glasses and frustrated systems. ${\text{Rb}}_{4}{\text{O}}_{6}$ and ${\text{Cs}}_{4}{\text{O}}_{6}$ c…

Electronic structure calculations forZnFe2O4

Local density approximation was applied to scrutinize the electronic structure and magnetic properties of the spinel ferrite ${\mathrm{ZnFe}}_{2}{\mathrm{O}}_{4}$. Various cation distributions were established to obtain the ground state for the system. In magnetic crystals, the position of the atoms is not enough for symmetry determination. A structure prediction by decreasing the octahedral point group symmetry ${\mathrm{O}}_{h}$ of Fe to ${\mathrm{D}}_{4h}$, ${\mathrm{C}}_{4v}$, and ${\mathrm{C}}_{3v}$ was carried out. The effect of the exchange and correlation terms on the band structure of ${\mathrm{ZnFe}}_{2}{\mathrm{O}}_{4}$ was studied by the generalized gradient approximation $+$ th…

Photoabsorption and MXCD in photoemission microscopy for characterisation of advanced materials

Abstract We applied chemical and magnetic sensitive photoemission electron microscopy (PEEM) to investigate surfaces of advanced materials. PEEM at low photon energies provides a high spatial resolution, but suffers from the lack of information about the chemical composition of the imaged surface. Such information can be obtained by PEEM via tuning the photon energy to X-ray absorption edges. To apply spectromicroscopy we acquired and subtracted microscopic images using photon energies just below and at the edges. The resulting difference gives a micro-image of the lateral distribution of a specific element. Microspectroscopy is performed by recording the intensity of secondary electrons in…

EXAFS-Messungen an dotierten Heusler-Verbindungen

Spintronik: eine Herausforderung für Materialwissenschaften und Festkörperchemie

Spintronik ist ein multidisziplinares Forschungsfeld zwischen Physik, Material- und Ingenieurwissenschaften, aber auch ein neuer Forschungsbereich der Festkorperforschung. Fur die verschiedensten Anforderungen mussen unterschiedlichste Materialien gefunden werden. Die Suche nach ferromagnetischen Halbleitern und stabilen halbmetallischen Ferromagneten mit Curie-Temperaturen hoher als Raumtemperatur ist immer noch eine zentrale Aufgabe fur die Festkorperchemie. Ein allgemeines Verstandnis der Struktur-Eigenschafts-Beziehungen ist eine notwendige Voraussetzung fur das Design neuer Materialien. In diesem Aufsatz werden die wichtigsten Entwicklungen im Bereich der Spintronik aus der Perspektive…

A Ni-based Superconductor: the Heusler Compound ZrNi$_2$Ga

This work reports on the novel Heusler superconductor ZrNi2Ga. Compared to other nickel-based superconductors with Heusler structure, ZrNi2Ga exhibits a relatively high superconducting transition temperature of Tc=2.9 K and an upper critical field of 1.5 T. Electronic structure calculations show that this relatively high transition temperature is caused by a van Hove singularity, which leads to an enhanced density of states at the Fermi energy. The van Hove singularity originates from a higher order valence instability at the L-point in the electronic structure. The enhanced density of states at the Fermi level was confirmed by specific heat and susceptibility measurements. Although many He…

Fabrication and characterization of semiconducting half Heusler YPtSb thin films

The semiconducting half Heusler compound YPtSb was predicted theoretically to be capable of changing into topological insulator under proper strain. In this work, p type semiconducting half-Heusler YPtSb thin films were prepared by magnetron co-sputtering method from a specially designed target for the first time. Textured structure with (111) plane paralleling with (001) of MgO substrate was observed when YPtSb thin films were grown on MgO (100) substrate at 600{\deg}C.Electrical measurements show that the resistivity of YPtSb films decreases with increasing temperature, indicating a semiconductor-like behavior. The carrier density is as high as 1.15 X 10^21 cm-3 at 300 K. The band gap of …

Structural and magnetic properties of Fe2CoGa Heusler nanoparticles

Abstract Fe2CoGa Heusler nanoparticles are synthesized by a chemical method. The structure and magnetic properties of Fe2CoGa Heusler nanoparticles are investigated by x-ray diffraction, extended x-ray absorption fine structure and Mössbauer spectroscopy. The crystal structure of Fe2CoGa nanoparticles is described by the X-type structure (prototype: Li2AgSb). Magnetic measurements reveal the presence of small Fe2CoGa nanoparticles and lower magnetic moments compared with the theoretically predicted values.

Are AuPdTM (T = Sc, Y and M = Al, Ga, In), Heusler Compounds Superconductors without Inversion Symmetry?

Heusler compounds with 2:1:1 stoichiometry either have a centrosymmetric Cu 2 MnAl structure or an Li 2 AgSb structure without a centre of inversion. The centrosymmetry is always lost in quaternary Heusler compounds with 1:1:1:1 stoichiometry and LiMgPdSn structure. This presents the possibility of realizing non-centrosymmetric superconductors in the family of Heusler compounds. The objective of this study is to search for and investigate such quaternary derivatives of Heusler compounds, particularly with respect to superconductivity. Several compounds were identified by carrying out calculations from first principles and superconductivity was observed in experiments conducted on AuPdScAl a…

Completely compensated ferrimagnetism and sublattice spin crossing in the half-metallic Heusler compound Mn1.5FeV0.5Al

The Slater-Pauling rule states that L21 Heusler compounds with 24 valence electrons do never exhibit a total spin magnetic moment. In case of strongly localized magnetic moments at one of the atoms (here Mn) they will exhibit a fully compensated half-metallic ferrimagnetic state instead, in particular, when symmetry does not allow for antiferromagnetic order. With aid of magnetic and anomalous Hall effect measurements it is experimentally demonstrated that Mn1.5V0.5FeAl follows such a scenario. The ferrimagnetic state is tuned by the composition. A small residual magnetization, that arises due to a slight mismatch of the magnetic moments in the different sublattices results in a pronounced …

Magnetic dichroism in angular-resolved hard X-ray photoelectron spectroscopy from buried layers

This work reports the measurement of magnetic dichroism in angular-resolved photoemission from in-plane magnetized buried thin films. The high bulk sensitivity of hard X-ray photoelectron spectroscopy (HAXPES) in combination with circularly polarized radiation enables the investigation of the magnetic properties of buried layers. HAXPES experiments with an excitation energy of 8 keV were performed on exchange-biased magnetic layers covered by thin oxide films. Two types of structures were investigated with the IrMn exchange-biasing layer either above or below the ferromagnetic layer: one with a CoFe layer on top and another with a Co$_2$FeAl layer buried beneath the IrMn layer. A pronounced…

Design Scheme of New Tetragonal Heusler Compounds for Spin-Transfer Torque Applications and its Experimental Realization

Band Jahn-Teller type structural instabilities of cubic Mn(2)YZ Heusler compounds causing tetragonal distortions can be predicted by ab initio band-structure calculations. This allows for identification of new Heusler materials with tunable magnetic and structural properties that can satisfy the demands for spintronic applications, such as in spin-transfer torque-based devices.

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…

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…

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…

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…

Characterisation of structured thin films made from complex materials by photoabsorption spectromicroscopy

Al3 and YBa2Cu3O7/PrBa2Cu3O7. To investigate devices built from these complex materials we applied element-sensitive photoemission electron microscopy (PEEM). Information about the chemical composition of the imaged sample can be obtained by PEEM via tuning the photon energy to X-ray absorption edges. To apply spectromicroscopy we acquired microscopic images using photon energies near and at the edges. Such images give the lateral distribution of a specific element. Microspectroscopy is performed by recording the intensity of the true secondary electrons in selected spots during a sweep of the photon energy. The main aim of our work was to observe oxygen-related defects and changes in the c…

Magnetic dichroism in angle-resolved hard x-ray photoemission from buried layers

This work reports the measurement of magnetic dichroism in angular-resolved photoemission from in-plane magnetized buried thin films. The high bulk sensitivity of hard x-ray photoelectron spectroscopy (HAXPES) in combination with circularly polarized radiation enables the investigation of the magnetic properties of buried layers. HAXPES experiments with an excitation energy of 8 keV were performed on exchange-biased magnetic layers covered by thin oxide films. Two types of structures were investigated with the IrMn exchange-biasing layer either above or below the ferromagnetic layer: one with a CoFe layer on top and another with a Co${}_{2}$FeAl layer buried beneath the IrMn layer. A pronou…

Selective Hydrogenation of 1,3-Butadiene to 1-Butene by Pd(0) Nanoparticles Embedded in Imidazolium Ionic Liquids

The reduction of Pd(acac)2 (acac=acetylacetonate), dissolved in 1-n-butyl-3-methylimidazolium hexafluorophosphate (BMI⋅PF6) or tetrafluoroborate (BMI⋅BF4) ionic liquids, by molecular hydrogen (4 atm) at 75 °C affords stable, nanoscale Pd(0) particles with sizes of 4.9±0.8 nm. Inasmuch as 1,3-butadiene is at least four times more soluble in the BMI⋅BF4 than butenes, the selective partial hydrogenation could be performed by Pd(0) nanoparticles embedded in the ionic liquid. Thus, the isolated nanoparticles promote the hydrogenation of 1,3-butadiene to butenes under solventless or multiphase conditions. Selectivities up to 97% in butenes were observed in the hydrogenation of 1,3-butadiene by Pd…

Electronic Properties, Band Structure, and Fermi Surface Instabilities ofNi1+/Ni2+NickelateLa3Ni2O6, Isoelectronic with Superconducting Cuprates

Electronic structure calculations were performed for the mixed-valent Ni(1+)/Ni(2+) nickelate La3Ni2O6, which exhibits electronic instabilities of the Fermi surface similar to that of the isostructural superconducting La2CaCu2O6 cuprate. La3Ni2O6 shows activated hopping, which fits to Mott's variable-range-hopping model with localized states near the Fermi level. However, a simple local spin density approximation calculation leads to a metallic ground state. The calculations including local density approximation+Hubbard U and hybrid functionals indicate a multiply degenerate magnetic ground state. For electron-doped La2ZrNi2O6, which is isoelectronic with La2CaCu2O6, an antiferromagnetic in…

Half-Heusler materials as model systems for phase-separated thermoelectrics

Semiconducting half-Heusler compounds based on NiSn and CoSb have attracted attention because of their good performance as thermoelectric materials. Nanostructuring of the materials was experimentally established through phase separation in (T1−x′Tx″)T(M1−yMy′) alloys when mixing different transition metals (T, T′, T″) or main group elements (M, M′). The electric transport properties of such alloys depend not only on their micro- or nanostructure but also on the atomic-scale electronic structure. In the present work, the influence of the band structure and density of states on the electronic transport and thermoelectric properties is investigated in detail for the constituents of phase-sepa…

A nondestructive analysis of the B diffusion in Ta–CoFeB–MgO–CoFeB–Ta magnetic tunnel junctions by hard x-ray photoemission

This work reports on hard x-ray photoelectron spectroscopy (HAXPES) of CoFeB based tunnel junctions. Aim is to explain the role of the boron diffusion for the observed improvement of the tunneling magnetoresistance ratio with increasing annealing temperature. The high bulk sensitivity of HAXPES was used as a nondestructive technique to analyze CoFeB–MgO–CoFeB magnetic tunnel junctions. The investigated samples were processed at different annealing temperatures from 523 to 923 K. Hard x-ray core level spectroscopy reveals an enforced diffusion of boron from the CoFeB into the adjacent Ta layer with increasing annealing temperature. The dependence of the tunneling magnetoresistance on the ann…

Determining the optical properties of adsorbate covered surfaces by dichroism in VUV-photoemission

The dichroic effects of photoemission excited by polarised light depend on the angle of photon incidence. Measurements of the difference in the angle-resolved photoemission intensities from Cs 5p semi-corelevels excited by photons of opposite helicity, or of orthogonal linear polarisation are reported. It was thought that the dependence of dichroism on the angle of incidence cannot be described using equations omitting metal optics. A complete consideration of the vector potential of the exciting light is needed, including the phase shift between it's parallel and perpendicular components. The phase shift is produced by the complex index of refraction. Using the Fresnel equations for struct…

Fast elemental mapping and magnetic imaging with high lateral resolution using a novel photoemission microscope

Abstract Using tunable soft X-ray synchrotron radiation and a new-generation photoemission electron microscope with integral sample stage and microarea selector, elemental images and local XANES spectra have been measured. Given the present conditions (PM3 at BESSY), the lateral resolution was in the range of 130 nm with the potential of considerable improvement with high-brilliance sources (a base resolution of 25 nm was obtained in threshold photoemission). Measurements at the oxygen K-edge demonstrate that differences in the local chemical environment of the emitter atom are clearly revealed and can thus be used as a fingerprint technique for its chemical state and geometrical surroundin…

The dependence of dichroism in VUV-photoemission on the optical properties of adsorbates: Cs-monolayer on W(110)

Abstract We report on the dependence of dichroic photoemission excited by polarised light on the angle of photon incidence. We measured the difference in the angle-resolved photoemission intensities from Cs-5p semi-corelevels excited by photons of opposite helicity, known as CDAD and of orthogonal linear polarisation—LDAD. We found that the dependence of dichroism on the angle of incidence can not be described by the equations used in the photoemission model for free atomic states. A complex consideration of the parallel and perpendicular components of the vector potential of the exciting light is needed, including the phase shift between these components. The phase shift is produced by the…

Quaternary half-metallic Heusler ferromagnets for spintronics applications

This work reports on three quaternary Heusler compounds NiFeMnGa, NiCoMnGa, and CuCoMnGa. In contrast to their ternary relatives, quaternary Heusler compounds are still rarely investigated. A very large pool of interesting materials lies thus idle waiting for exploration. The difficulty consists in choosing prospective compositions, and trial and error is elaborate and expensive. We have identified several candidates employing ab initioelectronic-structure calculations. The compounds were synthesized, and the structural and magnetic properties were investigated experimentally. CuCoMnGa is a quaternary Heusler compound; NiFeMnGa and NiCoMnGa are unreported half-metallic ferromagnetic materia…

k-resolved electronic properties of ternary heavy fermion systems

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…

Bulk sensitive photo emission spectroscopy of C1b compounds

This work reports about bulk-sensitive, high energy photoelectron spectroscopy from the valence band of CoTiSb excited by photons from 1.2 to 5 keV energy. The high energy photoelectron spectra were taken at the KMC-1 high energy beamline of BESSY II employing the recently developed Phoibos 225 HV analyser. The measurements show a good agreement to calculations of the electronic structure using the LDA scheme. It is shown that the high energy spectra reveal the bulk electronic structure better compared to low energy XPS spectra.

Seebeck coefficients of half-metallic ferromagnets

In this report the Co2 based Heusler compounds are discussed as potential materials for spin voltage generation. The compounds were synthesized by arcmelting and consequent annealing. Band structure calculations were performed and revealed the compounds to be half-metallic ferromagnets. Magnetometry was performed on the samples and the Curie temperatures and the magnetic moments were determined. The Seebeck coefficients were measured from low to ambient temperatures for all compounds. For selected compounds high temperature measurements up to 900 K were performed.

Magnetic properties of Co2Mn1−xFexSi Heusler alloys

Co2Mn1−xFexSi Heusler alloys with Fe concentration x = 0–0.4 as prepared by arc melting show a L21 long range order for all Fe concentrations. Magnetic properties of Co2Mn1−xFexSi Heusler alloys were investigated by magnetometry and circular magnetic dichroism. The magnetization of the Fe doped Heusler alloys is in agreement with the Slater–Pauling values expected for half-metallic ferromagnets. Element specific magnetic moments as determined by x-ray absorption using the total electron yield method are in disagreement with theoretical predictions for x = 0 but approach the predicted values as the Fe concentration increases. Surprisingly small Fe concentration increases the magnetic moments…

Microanalysis of the surfaces of natural iron-based minerals by means of synchrotron radiation based experimental techniques

We investigated the surfaces of natural iron-based minerals that are magnetite, hematite, goethite, pyrite, pyrrhotite, chalcopyrite, bornite and vivianite, using synchrotron radiation based techniques. Most iron chalkogenides are very suitable for photoemission microscopy studies due to their low resistivity, which prevents from surface charging. The local compositions were studied employing photoemission microscopy in combination with X-ray absorption spectroscopy. Imaging of the sample in the near-edge region of the absorption edges was used to visualise the spatial distributions of the chemical phases on the surface. Distributions of trace elements are imaged with high chemical and late…

The spatial distribution of non-linear effects in multi-photon photoemission from metallic adsorbates on Si(1 1 1)

Multi-photon excitations from thin metallic films on silicon substrates have been observed utilising photoemission electron microscopy. The photoelectrons have been excited by means of high power femtosecond laser pulses with a photon energy below the work function threshold. The strong spatial variations of the non-linear effects became directly visible in electron emission from the adsorbed thin films. Centres of enhanced photoelectron yield, so-called hot spots, were observed on the surfaces of various samples. The multi-photon electron yield of the metallic films (permalloy and lead) depends strongly on the sample topography and the photon polarisation.

Spintronics: a challenge for materials science and solid-state chemistry.

Spintronics is a multidisciplinary field involving physics, chemistry, and engineering, and is a new research area for solid-state scientists. A variety of new materials must be found to satisfy different demands. The search for ferromagnetic semiconductors and stable half-metallic ferromagnets with Curie temperatures higher than room temperature remains a priority for solid-state chemistry. A general understanding of structure-property relationships is a necessary prerequisite for the design of new materials. In this Review, the most important developments in the field of spintronics are described from the point of view of materials science.

Magnetic dichroism in photoemission with unpolarized light.

A magnetic dichroism in photoemission from ferromagnets induced by unpolarized light is observed for the first time in the valence band region as well as for surface states. The study was carried out with magnetized Fe(110), Co(0001), and Gd(0001) films grown epitaxially on W(110). This phenomenon leads to an intensity asymmetry for opposite directions of the sample magnetization. It can be easily used for a routine laboratory diagnostic of magnetic behavior. A simple theoretical interpretation of the phenomenon based on the atomic model is given.

Probing the Size Effect of Co2FeGa-SiO2@C Nanocomposite Particles Prepared by a Chemical Approach

In this contribution, we report the chemical synthesis of carbon coated, silica supported Co2FeGa (Co2FeGa-SiO2@C) nanocomposite particles. The particle size of Co2FeGa particles can be tuned by varying the amount of silica supports. The dependences of the crystal structure and magnetic properties on particle size have been investigated by synchrotron radiation based X-ray diffraction (XRD), X-ray absorption fine structure (XAFS) spectroscopy, transmission electron microscope (TEM), 57Fe Mossbauer spectroscopy, and superconducting quantum interference device (SQUID). The superparamagnetic critical size of Co2FeGa Heusler nanoparticles is found to be ∼17 nm by correlating the TEM derived par…

Field dependence of spin and orbital moments of Fe in L10 FePt magnetic thin films

Abstract The field dependence of spin and orbital magnetic moments of Fe in L10 FePt magnetic thin films was investigated using X-ray magnetic circular dichroism (XMCD). The spin and orbital moments were calculated using the sum rules; it was found that the spin and orbital moment of Fe in L10 FePt films are ∼2.5 and 0.2 μB, respectively. The relative XMCD asymmetry at Fe L3 peak on the dependence of applied field suggested that the majority magnetic moment of L10 FePt films resulted from Fe.

Geometric, electronic, and magnetic structure ofCo2FeSi: Curie temperature and magnetic moment measurements and calculations

In this work a simple concept was used for a systematic search for materials with high spin polarization. It is based on two semiempirical models. First, the Slater-Pauling rule was used for estimation of the magnetic moment. This model is well supported by electronic structure calculations. The second model was found particularly for ${\mathrm{Co}}_{2}$ based Heusler compounds when comparing their magnetic properties. It turned out that these compounds exhibit seemingly a linear dependence of the Curie temperature as function of the magnetic moment. Stimulated by these models, ${\mathrm{Co}}_{2}\mathrm{FeSi}$ was revisited. The compound was investigated in detail concerning its geometrical…

Spin polarisation and dichroism in ARUPS from thin rare earth films

Abstract In the present study, spin polarisation and dichroism were investigated in angular resolved VUV photoemission ARUPS from magnetised as well as paramagnetic rare earth surfaces. Thin Gd(0001) films were prepared epitaxially on W(110). The photoelectrons were excited by polarised synchrotron radiation from the BESSY I synchrotron radiation source. A SPLEED detector attached to an electron spectrometer mounted on a single axis goniometer was used for angular resolved spin analysis. The main part of this work focused on the characteristic surface state of Gd(0001) which shows a splitting, as previously observed by linear magnetic dichroism and spin polarised photoemission. The spin ana…

Electronic structure and transport properties of the Heusler compound Co2TiAl

The properties of the Heusler compound Co2TiAl were investigated in detail by experimental techniques and theoretical methods. X-ray diffraction measurements indicate that as-cast samples of the compound exhibit the L21 structure with a small amount of B2-type disorder. This leads to a reduced saturation magnetization per formula unit of 0.747 μB. The Curie temperature is approximately 120 K. The transport properties are influenced by the change in the electronic structure at the Curie temperature, as revealed experimentally by conductivity, thermal transport and specific heat measurements. Different theoretical models based on ab initio calculations of the electronic structure are used to …

Photoemission microscopy with microspot-XPS by use of undulator radiation and a high-throughput multilayer monochromator at BESSY

We present a new experiment for photoelectron microspectroscopy by use of undulator radiation, which has been set up at the beamline U2 at the Berlin electron storage ring BESSY 1. This approach employs a non-imaging simulated hemispherical electron energy analyser attached to an imaging photoemission electron microscope (FOCUS IS-PEEM) with integrated microarea selector. The photoemission microscope exhibits a lateral resolution of 25 nm (with 4.9 eV UV-excitation), while the resolution with incident synchrotron radiation in the soft X-ray range is about 100-120 nm (mainly due to chromatic aberrations). Photoemission microscopy as well as photoelectron microspectroscopy of selected areas o…

Rational design of new materials for spintronics: Co2FeZ (Z=Al, Ga, Si, Ge)

Spintronic is a multidisciplinary field and a new research area. New materials must be found for satisfying the different types of demands. The search for stable half-metallic ferromagnets and ferromagnetic semiconductors with Curie temperatures higher than room temperature is still a challenge for solid state scientists. A general understanding of how structures are related to properties is a necessary prerequisite for material design. Computational simulations are an important tool for a rational design of new materials. The new developments in this new field are reported from the point of view of material scientists. The development of magnetic Heusler compounds specifically designed as …

Enhanced orbital magnetic moments in the Heusler compounds ,,

Abstract Using the magnetic circular dichroism in X-ray absorption at the L2,3-edges of the 3d-transition metals, we determined the element specific ratio between orbital and spin magnetic moment of the Heusler compounds Co 2 CrAl , Co 2 Cr 0.6 Fe 0.4 Al and Co2FeAl. The orbital magnetic moment per spin is large (0.1–0.2) compared to bulk values of Fe and Co metals.

MAGNETIC COUPLING OF ALKALI AND RARE-GAS FILMS ADSORBED ON A FERROMAGNETIC SURFACE

The observation of magnetic circular dichroism in the angular distribution of photoelectrons (MCDAD) from alkali and rare-gas films adsorbed on a thin remanently magnetized Co layer is reported. The observation of an antisymmetric MCDAD near normal emission for Co(0001)–Cs 5p semi core level is shown. The reversed magnetization leads to a mirror-image-like distribution. The second system under investigation, physisorbed Co(0001)–Xe 5p, does not give such an but shows significant differences in the MCDAD signal for both directions of magnetization, in particular in the |mj| substates of the p3/2 level. A magnetic coupling between Xe and Co is evident when we take results of spin-resolved ph…

Image enhancement in photoemission electron microscopy by means of imaging time-of-flight analysis

Abstract Photoemission electron microscopy (PEEM) is widely used in combination with synchrotron sources as a powerful tool to observe chemical and magnetic properties of metal and semiconductor surfaces. Presently, the resolution limit of these instruments using soft-X-ray excitation is limited to about 50 nm, because of the chromatic aberation of the electron optics used. Various sophisticated approaches have thus been reported for enhancing the spatial resolution in photoemission electron microscopy. This work demonstrates the use of a simple imaging energy filter based on electron time-of-flight (ToF) selection. The spatial resolution could be improved dramatically, even though the inst…

Electron-spectroscopic investigations on ternary HFS: CeT2X2

Investigations of the electronic properties were carried out for ternary Ce-based heavy fermion systems. The well-ordered surfaces of HFS were prepared by MBE on W (110) with subsequent annealing. The layers are characterised by MEED, LEED, AES and XPS. For the electron-spectroscopic investigations, ARUPS and SPEELS were used. In the photoemission spectra, dispersion effects could be detected. By means of SPEELS, the dipole-forbidden Ce f-f transitions could be observed. The comparison of the energy loss spectra above and below the characteristic temperature T∗ reveals differences in the energy losses as well as in the asymmetries.

Quaternary Heusler compounds Co(2-x)Rh(x)MnZ (Z = Ga, Sn, Sb): crystal structure, electronic structure, and magnetic properties.

Within the huge family of Heusler compounds only a few quaternary derivatives are known that crystallize in the F43m space group. In this work, the yet unreported compounds CoRhMnZ (Z = Ga, Sn, Sb) and the alloy Co(0.5)Rh(1.5)MnSb were investigated in detail by experimental techniques and theoretical methods. The ab initio calculations predict the CoRhMnZ compounds to be half-metallic ferromagnets or to be close to the half-metallic ferromagnetic state. Calculations of the elastic constants show that the cubic structure is stable in compounds containing Mn. Both calculations and experiment reveal that Mn cannot be exchanged by Fe (CoRhFeGa). The low temperature magnetization of the compound…

Structural properties of the quaternary Heusler compound Co2 Cr1−x Fex Al

Abstract The structural and chemical properties of the quaternary Heusler compound Co2 Cr1−x Fex Al were investigated comparing powder and bulk samples. The long range order was determined by means of X-ray diffraction, while the site specific (short range) order was proved by the extended X-ray absorption fine structure method (EXAFS). The chemical composition was analysed by means of X-ray photo emission spectroscopy (XPS) combined with Auger electron spectroscopy (AES) depth profiling. The results from these methods are compared to get a detailed idea about the differences between surface and bulk properties and appearance of disorder in such alloys.

Emission Electron Microscopy of Nanoparticles in Strong fs Laser Fields

Heusler compounds as ternary intermetallic nanoparticles: Co2FeGa

This work describes the preparation of ternary nanoparticles based on the Heusler compound Co2FeGa. Nanoparticles with sizes of about 20?nm were synthesized by reducing a methanol impregnated mixture of CoCl2 ? 6H2O, Fe(NO3)3 ? 9H2O and Ga(NO3)3 ? xH2O after loading on fumed silica. The dried samples were heated under pure H2 gas at 900??C. The obtained nanoparticles?embedded in silica?were investigated by means of x-ray diffraction (XRD), transmission electron microscopy, temperature dependent magnetometry and M??bauer spectroscopy. All methods clearly revealed the Heusler-type L21 structure of the nanoparticles. In particular, anomalous XRD data demonstrate the correct composition in addi…

Dichroism in VUV photoemission from the (0001)-surfaces of ultrathin Gd and Nd films on W(110)

Abstract Ultrathin layers of Gd and Nd epitaxially grown on W(110) have been investigated using linearly and circularly polarised light at the 6.5 m NIM beamline at the BESSY storage ring in Berlin. The high quality of the films was monitored by the sharp and dispersionless surface state just below the Fermi energy. The CDAD (circular dichroism in the angular distribution of photoelectrons) measurements showed strong effects in the surface states as well as in the valence bands. The LMDAD (linear magnetic dichroism in…) from Gd(0001) showed a small, but significant splitting of the surface state. This splitting can be reproduced by numerical one-step calculations based on spin-dependent sur…

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…

Tunable multifunctional topological insulators in ternary Heusler compounds

Recently the Quantum Spin Hall effect (QSH) was theoretically predicted and experimentally realized in a quantum wells based on binary semiconductor HgTe[1-3]. QSH state and topological insulators are the new states of quantum matter interesting both for fundamental condensed matter physics and material science[1-11]. Many of Heusler compounds with C1b structure are ternary semiconductors which are structurally and electronically related to the binary semiconductors. The diversity of Heusler materials opens wide possibilities for tuning the band gap and setting the desired band inversion by choosing compounds with appropriate hybridization strength (by lattice parameter) and the magnitude o…

Probing the chemical interaction between iridium nanoparticles and ionic liquid by XPS analysis

Abstract In situ X-ray photoelectron spectroscopy analysis of Ir(0) nanoparticles (1.6 ± 0.3 nm) dispersed in imidazolium ionic liquid (EMI.EtSO4) shows evidences of the effective interaction between the metallic clusters and the surrounding liquid. By monitoring the C 1s signal of the ionic liquid one observes a change of the binding energy in one of its components (C2) when in the presence of Ir nanoparticles. This result was corroborated by isotope labeling experiments.

Influence of nanoscale order–disorder transitions on the magnetic properties of Heusler compounds for spintronics

Modifications in nanoscale chemical order are used to tune the magnetic properties, namely T-C, of Co2FeSixAl1-x (0 < x < 1). High-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) with Z-contrast reveals nanoscale regions of L2(1) order within a B2 matrix in the off-stoichiometry samples. Perhaps surprisingly, the latter, more chemically disordered structure, exhibits a higher T-C. Upon annealing, the off-stoichiometry samples become more homogeneous with the fraction of L2(1) order decreasing. The short-range order was also investigated using X-ray absorption fine structure (XAFS) measurements at the Co and Fe K edges. Since the local atomic environments of C…

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…

Structural properties of the quaternary Heusler alloy Co2Cr1−xFexAl

The quarternary substitutional series Co2Cr1?xFexAl was investigated by means of surface and bulk sensitive techniques in order to exploit its structural and compositional properties. Both bulk and powder samples of the alloy series were investigated to obtain specific information about this material.The long range order was determined by means of x-ray diffraction and neutron diffraction, while the site specific (short range) order was proved by extended x-ray absorption fine structure spectroscopy. The magnetic structure was investigated by M?ssbauer spectroscopy in transmission and scattering modes in order to compare and separate powder and bulk properties. The chemical composition was …

Chemical microimaging and microspectroscopy of surfaces with a photoemission microscope

We applied element sensitive photoemission electron microscopy (PEEM) to investigate surfaces of devices built from complex materials. Conventional PEEM suffers from lack of information about the chemical composition of the imaged surface. Such information can be obtained by PEEM via tuning the photon energy to X-ray absorption edges. To apply spectromicroscopy we acquired and subtracted microscopic images using photon energies just below and at the edges. The resulting difference gives a micro-image of the lateral distribution of a specific element. Microspectroscopy is performed by recording the intensity of secondary electrons in selected spots during a sweep of the photon energy. We app…

Correlation in the transition-metal-based Heusler compoundsCo2MnSiandCo2FeSi

Half-metallic ferromagnets, such as the Heusler compounds with formula ${X}_{2}YZ$, are expected to show an integer value for the spin magnetic moment. In contrast to experiments, calculations give noninteger values in certain cases where the compounds are based on $X=\mathrm{Co}$. In order to explain deviations of the magnetic moment calculated for such compounds, the dependence of the electronic structure on the lattice parameter was studied theoretically. In the local density approximation (LDA), the minimum total energy of ${\mathrm{Co}}_{2}\mathrm{FeSi}$ is found for the experimental lattice parameter, but the calculated magnetic moment is approximately 12% too low. In addition, half-m…

Superconductivity in the Heusler Family of Intermetallics

Several physical properties of the superconducting Heusler compounds, focusing on two systems (Y, Lu, Sc)Pd2Sn and APd2M, where A=Hf, Zr and M=Al, In, are summarized and compared. The analysis of the data shows the importance of the electron-phonon coupling for superconductivity in this family. We report the superconducting parameters of YPd2Sn, which has the highest Tc among all known Heusler superconductors.

Electronic, magnetic, and structural properties of the ferrimagnet Mn2CoSn

The magnetic ground state of the Heusler compound Mn${}_{2}$CoSn was predicted to be nearly half-metallic ferrimagnetic with a high spin polarization by ab initio electronic structure calculations. Mn${}_{2}$CoSn was synthesized, and the magnetic behavior of the compound was studied using a superconducting quantum interference device and x-ray magnetic circular dichroism. The experimental values were found to be in fair accordance with the theoretical predictions. The electronic structure and the crystal structure of Mn${}_{2}$CoSn were characterized comprehensively using x-ray powder diffraction, $^{119}\mathrm{Sn}$ M\"ossbauer spectroscopy, nuclear magnetic resonance, and hard x-ray photo…