X-ray magnetic circular dichroism imaging with hard X-rays

X-ray polarization-contrast images resulting from X-ray magnetic circular dichroism (XMCD) in the hard X-ray region have been successfully recorded for the first time. The apparatus used consisted of an X-ray polarizer, double X-ray phase retarders, and a high-spatial-resolution X-ray charge-coupled-device detector. The sample used was a hexagonal-close-packed cobalt polycrystal foil having a thickness of about 4 microns. The X-ray polarization-contrast image resulting from XMCD was observed at a photon energy of 10 eV above the cobalt K-absorption edge (7709 eV). The observed contrast in the image was reversed by inversion of the magnetic field. Furthermore, the contrast was reversed again at a photon energy of 32 eV above the cobalt K-absorption edge.     

Laser induced threshold photoemission magnetic circular dichroism and its application to photoelectron microscope

This work enlightens the threshold photoemission magnetic circular dichroism (MCD) and its adaption on photoemission electron microscopy (PEEM) using lasers. MCD is a simple and efficient way to investigate magnetic properties since it does not need any spin analyzers with low efficiency, and thus the MCD related techniques have developed to observe magnetic domains. Usually, MCD in a total yield measurement in the valence band with weak spin–orbit coupling (SOC) excited by low photon energy (hν≤ 6 eV) does not compete with the X-ray magnetic circular dichroism (XMCD) with strong SOC. XMCD PEEM observation of magnetic domains has been successfully established while MCD PEEM derived from valence bands has not been. However, using angle and energy resolved photoelectron, valence band MCD provides large asymmetry similar to that by XMCD. Threshold measurement of photoelectron in a total electron yield procedure can take advantage of the measurement of photoelectrons with a limited angle and energy mode. This restriction of the photoelectron makes the threshold MCD technique an efficient way to get magnetic information and gives more than 10% asymmetry for Ni/Cu(0 0 1), which is comparable to that obtained by angle resolved photoemission. Thus the threshold MCD technique is a suitable method to observe magnetic domains by PEEM. For threshold MCD, incident angle dependence and high sensitivity to out-of-plane magnetized films compared with in-plane ones are discussed. Ultrashort pulse lasers make it feasible to measure two photon photoemission MCD combined with PEEM, where resonant excitation has a possibility to enhance dichroic asymmetry. Recent results for valence band magnetic dichroism PEEM are presented.     

ODE: a new beam line for high-pressure XAS and XMCD studies at SOLEIL

X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) under pressure are probes of local order and microscopic magnetic properties. XMCD is a selective probe that has access to a large variety of elements. The dispersive extended X-ray absorption fine structure (EXAFS) station at SOLEIL (ODE beam line) provides the possibility to perform numerous pressure XAS and XMCD experiments with an excellent statistic. The main advantages of dispersive XAFS are the focusing optics, the short acquisition time (few μs) and great stability during the measurements due to the absence of any mechanical movement. These advantages allow the study of small samples, 70 μm at SOLEIL, which is mandatory in the case of high-pressure studies. We present the new ODE beam line at SOLEIL and its first high-pressure XMCD results.     

XMCD study of the local magnetic and structural properties of microcrystalline NdFeB-based alloys

X-ray Magnetic Circular Dichroism (XMCD) technique was used to investigate local magnetic properties of microcrystalline Nd_10.4Zr_4.0Fe_79.2B_6.4 samples, oriented along either easy or hard magnetization direction. The Nd L _2,3 and Fe K edge XMCD spectra were measured at room temperature under a magnetic field of T. A very strong dependence of XMCD spectra on the sample orientation has been observed at the NdL _2,3-edges, whereas the Fe K-edge XMCD spectra are found to be practically isotropic. This result indicates that magnetic anisotropy of NdFeB-based alloys originates from the Nd sublattice. In addition, element selective magnetization curves have been recorded by measuring the intensity of XMCD signals as a function of an applied magnetic field up to T. To find a correlation between local and macroscopic magnetic properties of studied samples we compared these data with magnetization curves, measured by vibrating sample magnetometer up to T. Results are important for understanding the origin of high-coercivity state in NdFeB-based intermetallic compounds.     

X-ray circular magnetic dichroism in the presence of strong spin fluctuations

The use of X-ray magnetic circular dichroism (XMCD) spectra for determininghe t magnitude of atomic magnetic moments in compounds of rare-earth and transition elements is discussed. The standard sum rule approach often yields a magnitude of moments that is often smaller than values obtained from magnetic measurements. We attribute this to strong spin fluctuations in the surface layers in which XMCD signals form. A way of determining the values of local magnetic moments in the presence of strong fluctuations is proposed and tested.     

Relativistic multiple scattering theory of K-edge X-ray magnetic circular dichroism

We discuss the angular dependent K-edge X-ray magnetic circular dichroism (XMCD) spectra based on the non-relativistic Green’s function expansion of the relativistic 4×4 Green’s function developed by Gesztesy et al. [Ann. Inst. Henri Poincaré 40 (1984) 159]. For the core functions we use the Dirac equation solutions whereas the relativistic effects for photoelectrons are automatically taken into account in the Gesztesy expansion. Analyses of the angular anisotropy provides us useful information on local symmetry violation around X-ray absorbing atoms even though we include relativistic effects. We explicitly show three different types of the symmetry which give rise to the suppression of the sin β-dependence in XMCD spectra. We also present explicit formulas of XMCD for randomly oriented and spatially fixed systems. Discussion on Debye–Waller factors is given in the present theoretical framework. Some illustrative calculations are also shown to understand the relativistic effects on the XMCD. The results are given for the Gd L₁-edge and Fe K-edge XMCD.     

Sum rules for X-ray magnetic circular dichroism spectra in strongly correlated ferromagnets

It is proven that the sum rules for X-ray magnetic dichroism (XMCD) spectra that are used to separate spin and orbital contributions to the magnetic moment are formally correct for an arbitrary strength of electron-electron interactions. However, their practical application for strongly correlated systems can become complicated due to the spectral density weight spreading over a broad energy interval. Relevance of incoherent spectral density for the XMCD sum rules is illustrated by a simple model of a ferromagnet with orbital degrees of freedom.     

A new ultra‐high‐vacuum variable temperature and high‐magnetic‐field X‐ray magnetic circular dichroism facility at LNLS

X‐ray magnetic circular dichroism (XMCD) is one of the most powerful tools for investigating the magnetic properties of different types of materials that display ferromagnetic behavior. Compared with other magnetic‐sensitive techniques, XMCD has the advantage of being element specific and is capable of separating the spin and magnetic moment contributions associated with each element in the sample. In samples involving, for example, buried atoms, clusters on surfaces or at interfaces, ultrathin films, nanoparticles and nanostructures, three experimental conditions must be present to perform state‐of‐the‐art XMCD measurements: high magnetic fields, low temperatures and an ultra‐high‐vacuum environment. This paper describes a new apparatus that can be easily installed at different X‐ray and UV beamlines at the Brazilian Synchrotron Light Laboratory (LNLS). The apparatus combines the three characteristics described above and different methods to measure the absorption signal. It also permits in situ sample preparation and transfer to another chamber for measurement by conventional surface science techniques such as low‐energy electron diffraction (LEED), reflection high‐energy electron diffraction (RHEED), X‐ray photoelectron spectroscopy (XPS) and X‐ray photoelectron diffraction (XPD). Examples are given of XMCD measurements performed with this set‐up on different materials.     

X-ray magnetic circular dichroism sum rule correction for the light transition metals

Distinguishable L₂ and L₃ edges and a clear separation into j _3/2 and j _1/2 excitations are necessary for the application of L_2,3 edge X-ray magnetic circular dichroism (XMCD) sum rules, which provide element-specific information about spin and orbital magnetic moments. This separation is present for the heavy transition metals (TM), like Co and Ni, due to their large L_2,3 spin–orbit splitting. However, for the light TM, the 2p spin–orbit splitting is strongly reduced and quantum mechanical mixing of j _3/2 and j _1/2 excitations is present. This mixing reduces the observed XMCD related spin and magnetic dipole term contributions and prevents the direct application of XMCD spin sum rules. A large number of 2p?→?3d absorption spectra have been fitted nearly perfectly by a simple and phenomenological model, which takes into account lifetime effects and provides quantitative information about jj-mixing at the light TMs. On the basis of this mixing coefficient, sum rule correction factors have been determined. The proposed model results in renormalized magnetic projected XMCD spin moments, verified for different compounds of V, Cr, and Mn. A comparison with complementary methods gives consistent results. This or a similar fitting procedure and the estimated correction factors can be used in the future as a light element XMCD spin renormalization technique.     

Element-specific hard X-ray micro-magnetometry of magnetic modifications in Co–Pt dots fabricated by ion etching

We developed a micro-magnetometry with a 2.5 μm spatial resolution based on micro X-ray magnetic circular dichroism (XMCD) technique in order to study magnetic properties of dot arrays for bit-patterned media. This micro-magnetometer was applied to the magnetic characterization of Co–Pt dot arrays fabricated by ion beam etching. As the dot size became small, the intensity of XMCD drastically decreased for dots fabricated by Ga-focused ion beam. This suggested that the dot edges were damaged magnetically by implantation of Ga ions. The damaged width of the dot edge was estimated to be about 13 nm from the decrease in XMCD intensities. This damaged edge width agreed with the ion-implanted area estimated by Monte-Carlo simulation. The less-damaged effect of Ar ion etching was verified by the XMCD measurement of Co–Pt dots with diameter of 20 and 70 nm. It was concluded that ions with inertness, lower energy and smaller atomic number should be used to fabricate dot arrays with an areal density of 1 Tbit/in².     

Structural and magnetic characterization of soft-magnetic FeCo alloy nanoparticles

Soft-magnetic FeCo alloy nanoparticles with diameters less than 100 nm are prepared by ball milling. X-ray photoemission spectroscopy (XPS) and X-ray magnetic circular dichroism (XMCD) are used to characterize these particles. While the XPS spectrum from the as-prepared sample clearly shows Co photoemission peaks, no sign of Fe is observed in the same spectrum. However, Fe photoemission peaks appear after 1 h of Ar ion sputtering. A quantitative analysis of the XPS spectra shows an increase of Fe concentration versus sputtering time until the Fe:Co ratio of the bulk alloy is reached. In addition, the narrow scan Fe and Co 2p XPS spectra show that Co is more oxidized than Fe. All these measurements indicate that the nanoparticles have a Co shell and an Fe-rich core. They further demonstrate the usefulness of XPS combined with depth-profiling via sputtering to obtain element- and chemically-sensitive structural information on nanoparticles. XMCD as an element-specific magnetic analysis tool further reveals that Fe and Co are ferromagnetically coupled in these particles. The information obtained is useful for establishing a structure–property relation for the studied material that is expected to have applications as a soft magnetic material at high temperatures.     

Disentanglement of magnetic contributions in multi‐component systems by using X‐ray magnetic circular dichroism at a single absorption edge

X‐ray magnetic circular dichroism (XMCD) has become in recent years an outstanding tool for studying magnetism. Its element specificity, inherent to core‐level spectroscopy, combined with the application of magneto‐optical sum rules allows quantitative magnetic measurements at the atomic level. These capabilities are now incorporated as a standard tool for studying the localized magnetism in many systems. However, the application of XMCD to the study of the conduction‐band magnetism is not so straightforward. Here, it is shown that the atomic selectivity is not lost when XMCD probes the delocalized states. On the contrary, it provides a direct way of disentangling the magnetic contributions to the conduction band coming from the different elements in the material. This is demonstrated by monitoring the temperature dependence of the XMCD spectra recorded at the rare‐earth L₂‐edge in the case of RT₂ (R = rare‐earth, T = 3d transition metal) materials. These results open the possibility of performing element‐specific magnetometry by using a single X‐ray absorption edge.     

Nature of magnetic coupling between Mn ions in As-grown Ga1-xMnxAs studied by X-ray magnetic circular dichroism

The magnetic properties of as-grown Ga1-xMnxAs have been investigated by the systematic measurements of temperature and magnetic field dependent soft x-ray magnetic circular dichroism (XMCD). The intrinsic XMCD intensity at high temperatures obeys the Curie-Weiss law, but a residual spin magnetic moment appears already around 100 K, significantly above the Curie temperature (T_{C}), suggesting that short-range ferromagnetic correlations are developed above T_{C}. The present results also suggest that the antiferromagnetic interaction between the substitutional and interstitial Mn (Mn_{int}) ions exists and that the amount of the Mn_{int} affects T_{C}.     

New scientific opportunities for high pressure research by energy-dispersive XMCD

ABSTRACT

XMCD under pressure is used to study the magnetic properties of the transition metal (TM) systems for over 15 years. We present the technique and how it has been developed. The energy dispersive XAS spectrometer is particularly suited for these studies. The effect of pressure on TM magnetism is discussed. Recent studies performed at different edges illustrate the information that can be obtained through XMCD. Finally, some results obtained on TMs are presented, either at the L_II,III edges of 5d metals or at the K edge of 3d metals, which correspond to the energy ranges that can be probed when using diamond anvil cells for high pressure. Different cases are treated: pure 3d metals, alloys, magnetic insulator and inorganic compounds.     

Soft X-ray magnetic circular dichroism of Cr-doped GaN

Soft X-ray magnetic circular dichroism (XMCD) have been measured for the Ga_0.97Cr_0.03N film grown by NH₃-assisted molecular beam epitaxy. Temperature dependence of the XMCD intensity was well described by the Curie–Weiss law. Although the sample showed ferromagnetic behavior at least up to room temperature, the ferromagnetic component could not be detected by the XMCD measurement.     

Epitaxy and magnetic properties of surfactant-mediated growth of bcc cobalt

High resolution core level photoemission spectroscopy, photoelectron diffraction, and x-ray magnetic circular dicroism (XMCD) have been used to characterize the structural and magnetic properties of bcc-cobalt films grown on GaAs(110) substrates by using Sb as a surfactant. We have unambiguously disentangled the surfactant role played by the Sb which improves the crystallinity and reduces the lattice distortion of the metallic films as well as changes the interdiffusion process at the interface compared to the Co/GaAs(110) system. As a consequence of these combined effects, an improvement on the magnetic response of the grown Co thin films has been observed by XMCD measurements.     

EXAFS and XMCD studies of correlations of atoms and magnetic moments in the disordered nanocrystalline alloys Fe with sp-elements (Al, Si, Sn)

The results of the studies of an extended X-ray absorption fine structure (EXAFS, at the Fe and Sn K edges) and X-ray magnetic circular dichroism (XMCD, at the Fe K edge) of binary nanocrystaline oversaturated solid solutions of Fe with sp-elements Al, Si, and Sn containing an sp-element up to 50 at % are presented. The parameters of the obtained partial pair correlation functions demonstrate an increase in the short-range chemical order as the concentration of the sp-element increases and with a high degree of local static distortions of the crystal lattice. A considerable change in the XMCD signal observed for Fe-Al and Fe-Sn alloys as the sp-element content increases can be qualitatively explained using a model of local magnetic moments corresponding to the case of the Mattis magnet.     

Comment on the analysis of angle-dependent X-ray magnetic circular dichroism in systems with reduced dimensionality

The magnetic dipole term T appearing in the X-ray magnetic circular dichroism (XMCD) spin sum rule can be eliminated from the analysis within the spin sum rule by angle-dependent XMCD spectroscopy if the effects of spin–orbit coupling are small so that T_x+T_y+T_z≈0. It is shown by the ab initio electron theory for the extreme case of a low-dimensional system, i.e., for a free-standing monatomic Co wire that this relation is strongly violated, indicating that the determination of T by the angle-dependent XMCD is possibly not very reliable for low-dimensional magnetic systems.     

Ground-State-Moment-Analysis: A quantitative tool for X-ray magnetic circular dichroism analysis for <Emphasis Type="Italic">3d</Emphasis> transition metals

By the use of sum rules and X-ray magnetic circular dichroism (XMCD) integral spectral values, experimentally determined element specific spin- and orbital-magnetic moments could be extracted. Therefore, sum rules neglect all additional spectral shape information. On the basis of so called ground state moments and their spectral representations, XMCD spectra could be fitted. The gain of information due to this method is directly related to the analysis of the spectral shape. Simple and complex spectra, with many different observable spectral features, could be quantitatively analyzed. Different unoccupied parts of the bandstructure have been resolved and intuitively interpreted by the moment analysis procedure. Focusing on this fitting method, we will review recent applications to Iron-Garnets and CrO₂ and show new results for Fe-, Mn-, and V-L_2,3 XMCD spectra. In addition, spectral overlap between the L₂ and L₃ edges at the light transition metal site could be handled by this method, and quantitative magnetic moments have been extracted from the spectra. This is the basis for a possible future element specific renormalization technique, used for the whole series of the transition metals, which is very important at the light transition metal site. PACS 87.64.Ni; 75.70.-i; 75.50.Cc; 75.70.Ak     

Crystal field effect on X-ray magnetic circular dichroism spectra at the L<Subscript>2,3</Subscript> absorption edges of mixed-valence Ce and Yb compounds in high magnetic fields

A theoretical study is presented, with an extended single impurity Anderson model, for the crystal field effect on the X-ray magnetic circular dichroism (XMCD) spectra at L_2,3 edges of mixed-valence Ce and Yb compounds in high magnetic fields. The crystal field acting on the 4f electrons is assumed to have cubic symmetry. Due to the competition among the effects of crystal field, mixed valency, and external magnetic field, the magnetic-field-dependence of XMCD spectra exhibits a variety of features; for instance, the branching ratio, R(L₂/L₃), of L₂ and L₃ XMCD intensities of Ce compounds can take R(L₂/L₃) > 1.0 and <1.0, and that of Yb compounds can take R(L₂/L₃) > 0 and <0. It is shown that the magnetic-field-dependence of the total XMCD intensity I(L₂ + L₃) is proportional to the magnetization curve, but that of R(L₂/L₃) gives more precise information on the ground state wavefunction in magnetic fields. A new and useful method to correlate the XMCD spectra, the 4f magnetization and the ground state wavefunction is proposed and used to discuss the relation between I(L₂ + L₃) and the magnetization curve and that between R(L₂/L₃) and the ground state wavefunction.