X-ray Magnetic Circular Dichroism Intensity Research Articles

Direct observation of antiferromagnetic domains and field-induced reversal in Pt/Cr2O3/Pt epitaxial trilayers

Antiferromagnet does not show the net magnetization, whereas the finite uncompensated moment can residue at the surface. On the surface of the magnetoelectric antiferromagnet, the finite boundary magnetization can acquire the magnetic response. In this paper, we address the magnetic response of the boundary magnetization in the Pt/magnetoelectric Cr2O3/Pt epitaxial trilayer based on the anomalous Hall effect (AHE) and the soft x-ray magnetic circular dichroism (XMCD). Decreasing the Cr2O3 thickness down to 15 nm, the film acquired the magnetic responsiveness, which manifested as the rectangular hysteresis in the magnetic field dependence of the AHE. The sizable XMCD intensity and the rectangular magnetic field dependence of the XMCD intensity revealed that the magnetic response was attributed to the interfacial Cr moment. The detailed investigation of AHE and XMCD revealed that the domain wall motion dominated the reversal process of the boundary magnetization, which was directly visualized by the scanning XMCD microscope.

Ferromagnetism induced by hybridization of Fe 3d orbitals with ligand InSb bands in the n -type ferromagnetic semiconductor (In,Fe)Sb

Fe-doped III-V ferromagnetic semiconductor (FMS) (In,Fe)Sb is a promising material for spintronic device applications because of the n-type carrier conduction and the ferromagnetism with high Curie temperature (TC > 300 K). To clarify the mechanism of the high-TC ferromagnetism, we have investigated the electronic structure and magnetic properties of an (In,Fe)Sb thin film by performing x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements at the Fe L2,3 edges. The magnetic-field dependence of the XMCD spectra reveals that there are ferromagnetic-like Fe and paramagnetic-like Fe components in the (In,Fe)Sb thin film. The XAS and XMCD spectra of the ferromagnetic-like and paramagnetic-like Fe components resemble those of other Fe-doped FMSs and extrinsic oxides, respectively. The finite value of the ratio between the orbital and spin magnetic moments estimated by applying the XMCD sum rules indicates that the valence state of the Fe ions substituting for the In sites in (In,Fe)Sb is not purely ionic Fe3+, but intermediate between Fe3+ and Fe2+. The qualitative correspondence between the magnetic-field dependence of the visible-light magnetic circular dichroism intensity and that of the XMCD intensity demonstrates that the Zeeman splitting of the InSb band is proportional to the net magnetization of the doped Fe. These results suggest that the ferromagnetism of (In,Fe)Sb originates from the Fe 3d orbitals hybridized with the host InSb bands.

Probing the tunability of magnetism with external pressure in metastable Sr2NiIrO6 double perovskite

In ${\mathrm{Sr}}_{2}{\mathrm{NiIrO}}_{6}$ long-range Ir-Ir antiferromagnetic exchange interactions have been reported to overcome the ferromagnetic Ni-Ir interactions hampering the otherwise expected ferromagnetic behavior. Prompted by this, a combination of x-ray absorption spectroscopy and x-ray diffraction at high pressure is used here to investigate the interplay between the magnetic structure of the Ir sublattice and lattice degrees of freedom. The compression of ${\mathrm{Sr}}_{2}{\mathrm{NiIrO}}_{6}$ drives an unexpected nonmonotonic change of the x-ray magnetic circular dichroism (XMCD) spectra: The intensity first decreases in the 0- to 18-GPa range, then shows an increase in the 18- to 30-GPa range and again decreases for higher pressures. The XMCD intensity, a measure of the net magnetization in the Ir sublattice, however, is found to remain very low in the whole pressure range so the observed changes do not correspond with a transition from antiferromagnetic to ferromagnetic or ferrimagnetic order. The evolution of the XMCD is better explained in terms of a weakening/strengthening of the long-range antiferromagnetic (AFM) Ir-Ir interaction between ferromagnetic planes associated with the reduction of the lattice parameters. In particular, a correlation can be established between the evolution of the $b$/$a$ ratio and the weakening/strengthening of the AFM interaction.

Direct observation of the magnetic ordering process in the ferromagnetic semiconductor Ga1−xMnxAs via soft x-ray magnetic circular dichroism

In order to understand the mechanism of the ferromagnetism in the ferromagnetic semiconductor Ga1−xMnxAs [(Ga,Mn)As], we have investigated the magnetic behavior on a microscopic level through systematic temperature (T)- and magnetic field (H)-dependent soft x-ray magnetic circular dichroism (XMCD) experiments at the Mn L2,3 absorption edges. The T and H dependences of XMCD intensities have been analyzed using a model consisting of the ferromagnetic (FM), paramagnetic, and superparamagnetic (SPM) components. Intriguingly, we have found a common behavior for the ferromagnetic ordering process in (Ga,Mn)As samples with different Mn concentrations (4% and 10.8%) and different Curie temperature (TC) values (65, 120, and 164 K). In particular, the SPM component develops well above TC, indicating that local FM regions are formed well above TC. The present findings indicate that the onset of ferromagnetic ordering is triggered by local electronic states around the substitutional Mn ions rather than uniform electronic states considered by mean-field theories. Insight into the most representative ferromagnetic semiconductor, (Ga,Mn)As, provided by the present study will be an important step in understanding the mechanism of ferromagnetic ordering in various ferromagnetic semiconductor families.

Mechanism of L2,3-edge x-ray magnetic circular dichroism intensity from quantum chemical calculations and experiment-A case study on V(IV)/V(III) complexes.

In this work, we present a combined experimental and theoretical study on the V L2,3-edge x-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectra of VIVO(acac)2 and VIII(acac)3 prototype complexes. The recorded V L2,3-edge XAS and XMCD spectra are richly featured in both V L3 and L2 spectral regions. In an effort to predict and interpret the nature of the experimentally observed spectral features, a first-principles approach for the simultaneous prediction of XAS and XMCD spectra in the framework of wavefunction based ab initio methods is presented. The theory used here has previously been formulated for predicting optical absorption and MCD spectra. In the present context, it is applied to the prediction of the V L2,3-edge XAS and XMCD spectra of the VIVO(acac)2 and VIII(acac)3 complexes. In this approach, the spin-free Hamiltonian is computed on the basis of the complete active space configuration interaction (CASCI) in conjunction with second order N-electron valence state perturbation theory (NEVPT2) as well as the density functional theory (DFT)/restricted open configuration interaction with singles configuration state functions based on a ground state Kohn-Sham determinant (ROCIS/DFT). Quasi-degenerate perturbation theory is then used to treat the spin-orbit coupling (SOC) operator variationally at the many particle level. The XAS and XMCD transitions are computed between the relativistic many particle states, considering their respective Boltzmann populations. These states are obtained from the diagonalization of the SOC operator along with the spin and orbital Zeeman operators. Upon averaging over all possible magnetic field orientations, the XAS and XMCD spectra of randomly oriented samples are obtained. This approach does not rely on the validity of low-order perturbation theory and provides simultaneous access to the calculation of XMCD A, B, and C terms. The ability of the method to predict the XMCD C-term signs and provide access to the XMCD intensity mechanism is demonstrated on the basis of a generalized state coupling mechanism based on the type of the excitations dominating the relativistically corrected states. In the second step, the performance of CASCI, CASCI/NEVPT2, and ROCIS/DFT is evaluated. The very good agreement between theory and experiment has allowed us to unravel the complicated XMCD C-term mechanism on the basis of the SOC interaction between the various multiplets with spin S' = S, S ± 1. In the last step, it is shown that the commonly used spin and orbital sum rules are inadequate in interpreting the intensity mechanism of the XAS and XMCD spectra of the VIVO(acac)2 and VIII(acac)3 complexes as they breakdown when they are employed to predict their magneto-optical properties. This conclusion is expected to hold more generally.

Electronic and Magnetic States of Pr and Mn in the Pr1–xSrxMnO3 Films Studied by XANES and XMCD Spectroscopy

The spectral dependences of X-ray absorption near-edge spectroscopy (XANES) and X-ray magnetic circular dichroism (XMCD) and the field dependences of XMCD near the K edge of Mn and the L2,3 edges of Pr in the Pr0.8Sr0.2MnO3 and Pr0.6Sr0.4MnO3 films at T = 90 K are studied. The spectral dependences point to a mixed valence state of Mn and Pr in the films. It is found that, as compared to XANES, XMCD is more sensitive to the valence state of Pr4+. The field dependences of XMCD point to ferromagnetic behavior of Mn ions and the Van Vleck paramagnetism of Pr ions, which makes a significant contribution to the total magnetization of the films. It is shown that as the Sr concentration increases, the XMCD intensity at the K edge of Mn increases, which indicates a growth of the total magnetic moment of the film due to an increase in the 4p–3d hybridization.

Iron L2,3-Edge X-ray Absorption and X-ray Magnetic Circular Dichroism Studies of Molecular Iron Complexes with Relevance to the FeMoco and FeVco Active Sites of Nitrogenase.

Herein, a systematic study of a series of molecular iron model complexes has been carried out using Fe L2,3-edge X-ray absorption (XAS) and X-ray magnetic circular dichroism (XMCD) spectroscopies. This series spans iron complexes of increasing complexity, starting from ferric and ferrous tetrachlorides ([FeCl4]−/2–), to ferric and ferrous tetrathiolates ([Fe(SR)4]−/2–), to diferric and mixed-valent iron–sulfur complexes [Fe2S2R4]2–/3–. This test set of compounds is used to evaluate the sensitivity of both Fe L2,3-edge XAS and XMCD spectroscopy to oxidation state and ligation changes. It is demonstrated that the energy shift and intensity of the L2,3-edge XAS spectra depends on both the oxidation state and covalency of the system; however, the quantitative information that can be extracted from these data is limited. On the other hand, analysis of the Fe XMCD shows distinct changes in the intensity at both L3 and L2 edges, depending on the oxidation state of the system. It is also demonstrated that the XMCD intensity is modulated by the covalency of the system. For mononuclear systems, the experimental data are correlated with atomic multiplet calculations in order to provide insights into the experimental observations. Finally, XMCD is applied to the tetranuclear heterometal–iron–sulfur clusters [MFe3S4]3+/2+ (M = Mo, V), which serve as structural analogues of the FeMoco and FeVco active sites of nitrogenase. It is demonstrated that the XMCD data can be utilized to obtain information on the oxidation state distribution in complex clusters that is not readily accessible for the Fe L2,3-edge XAS data alone. The advantages of XMCD relative to standard K-edge and L2,3-edge XAS are highlighted. This study provides an important foundation for future XMCD studies on complex (bio)inorganic systems.

Detection of induced paramagnetic moments in Pt onY3Fe5O12via x-ray magnetic circular dichroism

Magnetic moments in an ultra-thin Pt film on a ferrimagnetic insulator Y$_3$Fe$_5$O$_{12}$ (YIG) have been investigated at high magnetic fields and low temperatures by means of X-ray magnetic circular dichroism (XMCD). We observed an XMCD signal due to the magnetic moments in a Pt film at the Pt $L_{3}$- and $L_{2}$-edges. By means of the element-specific magnetometry, we found that the XMCD signal at the Pt $L_{3}$-edge gradually increases with increasing the magnetic field even when the field is much greater than the saturation field of YIG. Importantly, the observed XMCD intensity was found to be much greater than the intensity expected from the Pauli paramagnetism of Pt when the Pt film is attached to YIG. These results imply the emergence of induced paramagnetic moments in Pt on YIG and explain the characteristics of the unconventional Hall effect in Pt/YIG systems.

Pressure effect on the magnetism of the diluted magnetic semiconductor(Ba1−xKx)(Zn1−yMny)2As2with independent spin and charge doping

We used x-ray magnetic circular dichroism (XMCD) to probe the ferromagnetic properties of As $p$-symmetric ($4p$) states in the recently synthesized diluted magnetic semiconductor $(\mathrm{B}{\mathrm{a}}_{1\ensuremath{-}x}{\mathrm{K}}_{x}){(\mathrm{Z}{\mathrm{n}}_{1\ensuremath{-}y}\mathrm{M}{\mathrm{n}}_{y})}_{2}\mathrm{A}{\mathrm{s}}_{2}$ system under ambient- and high-pressure conditions. The As $K$-edge XMCD signal scales with the sample magnetization (dominated by Mn) and scales with the ferromagnetic ordering temperature $T\mathrm{c}$, and hence it is representative of the bulk magnetization. The XMCD intensity gradually decreases upon compression and vanishes at around 25 GPa, indicating quenching of ferromagnetism at this pressure. Transport measurements show a concomitant increase in conductivity with pressure, leading to a nearly metallic state at about the same pressure where magnetic order collapses. High-pressure x-ray diffraction shows an absence of structural transitions to 40 GPa. The results indicate that the mobility of doped holes, probed by both transport and x-ray absorption spectroscopy ($4p$ band broadening), is intimately connected with the mechanism of magnetic ordering in this class of compounds and that its control using external pressure provides an alternative route for tuning the magnetic properties in diluted magnetic semiconductor materials.

Magnetization Measurements and XMCD Studies on Ion Irradiated Iron Oxide and Core-Shell Iron/Iron-Oxide Nanomaterials

Magnetite (Fe <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">4</sub> ) and core-shell iron/iron-oxide (Fe/FexOy) nanomaterials prepared by a cluster deposition system were irradiated with 5.5 MeV Si <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2+</sup> ions and the structures determined by X-ray diffraction as consisting of 100% magnetite and 36/64 wt% Fe/FeO, respectively. However, X-ray magnetic circular dichroism (XMCD) indicates similar surfaces in the two samples, slightly oxidized and so having more Fe <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3+</sup> than the expected magnetite structure, with XMCD intensity much lower for the irradiated core-shell samples indicating weaker magnetism. X-ray absorption spectroscopy (XAS) data lack a strong signature for FeO, but the irradiated core-shell system consists of Fe-cores with ~13 nm of separating oxide crystallite, so it is likely that most FeO (octahedral Fe <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2+</sup> ) exists deeper than the probe depth of the XAS (~5 nm). Exchange bias (Hex) for both samples becomes increasingly negative as temperature is lowered, but the irradiated Fe <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">4</sub> sample shows greater sensitivity of cooling field on Hex. Loop asymmetries and Hex sensitivities of the irradiated Fe <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> O <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">4</sub> sample are due to interfaces and interactions between grains, which were not present in samples before irradiation, as well as surface oxidation. Asymmetries in the hysteresis curves of the irradiated core/shell sample are related to the reversal mechanism of the antiferromagnetic FeO and possibly some near surface oxidation.

Equilibrium surface magnetization of α-Cr2O3 studied through interfacial chromium magnetization in Co/α-Cr2O3 layered structures

We show experimental evidence of the equilibrium surface magnetization of α-Cr2O3(0001) by studying chromium magnetization at the Co(111)/α-Cr2O3(0001) interface. The soft X-ray magnetic circular dichroism intensity from uncompensated Cr spins was found to be almost independent of the interface roughness and exchange anisotropy energy. Moreover, no exchange bias training effect was found, except in the transition temperature regime, suggesting that the antiferromagnetic spin structure, including the interface spin arrangement, is in equilibrium. Furthermore, the exchange bias polarity was switched by magnetoelectric field cooling, which is also a salient feature of the surface magnetization of α-Cr2O3(0001).

Spin and orbital magnetic moments of Fe in the n-type ferromagnetic semiconductor (In,Fe)As

The electronic and magnetic properties of Fe atoms in the ferromagnetic semiconductor (In,Fe)As codoped with Be have been studied by x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) at the Fe L2,3 edge. The XAS and XMCD spectra showed simple spectral line shapes similar to Fe metal, but the ratio of the orbital and spin magnetic moments (Morb/Mspin) estimated using the XMCD sum rules was significantly larger than that of Fe metal, indicating a significant orbital moment of Fe 3d electrons in (In,Fe)As:Be. The positive value of Morb/Mspin implies that the Fe 3d shell is more than half-filled, which arises from the hybridization of the Fe3+ (d5) state with the charge-transfer d6L¯ states, where L¯ is a ligand hole in the host valence band. The XMCD intensity as a function of magnetic field indicated hysteretic behavior of the superparamagnetic-like component due to discrete ferromagnetic domains.

Simultaneous Pressure-Induced Magnetic and Valence Transitions in Type-I Clathrate Eu8Ga16Ge30

We have performed X-ray magnetic circular dichroism (XMCD) and X-ray absorption spectroscopy (XAS) measurements at pressures up to 17 GPa for the clathrate Eu8Ga16Ge30 (Curie temperature TC = 36 K). The temperature dependence of the XMCD spectra agrees well with that of the DC magnetization at ambient pressure. The TC is gradually enhanced with increasing pressures up to 13.3 GPa, and the divalent state of the Eu ions with J = 7/2 remains stable, but at 17 GPa the XMCD intensity is strongly suppressed and a spectral weight corresponding to the trivalent state of Eu ions (with no magnetic moment) appears in the XAS spectrum. The concurrent change from the type-I clathrate structure to an amorphous phase has been observed by X-ray diffraction experiment. We conclude that the amorphization of this compound induces the mixed valence state, which collapses the ferromagnetism.

Pressure-induced amorphization and collapse of magnetic order in the type-I clathrate Eu8Ga16Ge30

We investigate the low temperature structural and electronic properties of the type-I clathrate Eu8Ga16Ge30 under pressure using x-ray powder diffraction (XRD), x-ray absorption near-edge structure (XANES) and x-ray magnetic circular dichroism (XMCD) techniques. The XRD measurements reveal a transition to an amorphous phase above 18 GPa. Unlike previous reports on other clathrate compounds, no volume-collapse is observed prior to the crystalline-amorphous phase transition which takes place when the unit cell volume is reduced to 81% of its ambient pressure value. Fits of the pressure-dependent relative volume to a Murnaghan equation of state (EOS) yield a bulk modulus B0 = 65+-3 GPa and a pressure derivative B'0 = 3.3+-0.5. The Eu L2-edge XMCD data shows quenching of the magnetic order at the crystalline-amorphous phase transition. The XANES spectra indicate the persistence of Eu2+ valency state up to 22 GPa, therefore the suppression of XMCD intensity is due to the loss of magnetic order as a result of frustrated exchange interactions in the amorphous phase, and not due to quenching of local moments. When compared with other clathrates, the results point to the importance of guest ion-cage interactions in determining the mechanical stability of the framework structure and the critical pressure for amorphization. Finally, the crystalline structure is not found to recover after pressure release, resulting in a novel amorphous material that is at least metastable at ambient pressure and temperature.

Phase diagram of Ca1−xCexMnO3 thin films studied by X-ray magnetic circular dichroism

In the perovskite-type Ca1−xCexMnO3 (CCMO), one can control the transport and magnetic properties through varying Ce content. In the case of thin films, the properties can also be controlled by epitaxial strain from the substrate through changing it such as YAlO3 (YAO), NdAlO3 (NAO), and LaSrAlO4 (LSAO). However, one cannot measure the magnetization of thin films on NAO substrates by conventional magnetization measurements because of the strong paramagnetic signals from the Nd3+ ions. In order to eliminate the influence of Nd3+ and to identify magnetic phases of the CCMO thin films, we have performed element-selective X-ray magnetic circular dichroism (XMCD) measurements of the Mn 2p core level. By studying the anisotropy of the XMCD intensity, we could unambiguously determine the magnetic phase diagram of the CCMO thin films.

Separation of magnetic properties at uranium and cobalt sites in UCoAl using soft x-ray magnetic circular dichroism

Temperature ($T$) and magnetic field ($H$) dependence of the magnetic properties in metamagnetic UCoAl have been investigated using a soft x-ray magnetic circular dichroism (XMCD). In order to extract element-specific magnetic properties at the U and Co sites, the XMCD experiment has been performed at the U 4$d$-5$f$ (${N}_{4},5$) and Co 2$p$-3$d$ (${L}_{2},3$) absorption edges, respectively. Directions of magnetic moments at the U and Co sites have been determined from shapes of the XMCD spectra. The directions of the total magnetic moments at the U and Co sites are parallel to the $H$ direction ($c$ axis), but the direction of the spin magnetic moment at the U site is opposite to that at the Co site. The XMCD intensities at both the U and Co sites at $T=5.5$ K increase steeply at $H=0.77$ T (${H}_{\mathrm{m}}$), corresponding to the metamagnetic transition. The XMCD intensities do not saturate, even in the field-induced ferromagnetic state above ${H}_{\mathrm{m}}$. In addition, the ratio of the increase of the XMCD intensity at the Co site is smaller than that at the U site. From comparison of the $H$ dependence of the XMCD intensities at $T=25$ and 5.5 K, we found that the magnetic behavior of the Co atom has a stronger $T$ dependence than that of the U atom.

Ferromagnetism of cobalt-doped anatase TiO2 studied by bulk- and surface-sensitive soft x-ray magnetic circular dichroism

We have studied magnetism in anatase Ti1−xCoxO2−δ (x = 0.05) thin films with various electron carrier densities, by soft x-ray magnetic circular dichroism (XMCD) measurements at the Co L2,3 absorption edges. For electrically conducting samples, the magnetic moment estimated by XMCD was &amp;lt;0.3 μB/Co using the surface-sensitive total electron yield mode, while it was 0.3–2.4 μB/Co using the bulk-sensitive total fluorescence yield mode. The latter value is in the same range as the saturation magnetization 0.6–2.1 μB/Co deduced by SQUID measurement. The magnetization and the XMCD intensity increased with carrier density, consistent with the carrier-induced origin of the ferromagnetism.

X-ray magnetic circular dichroism of ferromagnetic Co4N epitaxial films on SrTiO3(001) substrates grown by molecular beam epitaxy

5-nm thick Co4N layers capped with 3-nm thick Au layers were grown epitaxially on SrTiO3(001) substrates by molecular beam epitaxy using solid Co and a radio-frequency NH3 plasma. Spin and orbital magnetic moments of the Co4N layers were estimated using x-ray magnetic circular dichroism (XMCD) measurements at 300 K. The site-averaged Co 3d spin magnetic moment is evaluated to be about 1.4 μB, which is smaller than that predicted theoretically (1.58 μB). The element-specific XMCD intensities for the Co L3 edge and N K edge show that the magnetic moment is induced at the N atoms.

Ferromagnetic interaction between Cu ions in the bulk region of Cu-doped ZnO nanowires

We have studied the electronic structure and the magnetism of Cu-doped ZnO nanowires, which have been reported to show ferromagnetism at room temperature [G. Z. Xing ${et}$ ${al}$., Adv. Mater. {\bf 20}, 3521 (2008).], by x-ray photoemission spectroscopy (XPS), x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD). From the XPS and XAS results, we find that the Cu atoms are in the "Cu$^{3+}$" state with mixture of Cu$^{2+}$ in the bulk region ($\sim$ 100 nm), and that "Cu$^{3+}$" ions are dominant in the surface region ($\sim$ 5 nm), i.e., the surface electronic structure of the surface region differs from the bulk one. From the magnetic field and temperature dependences of the XMCD intensity, we conclude that the ferromagnetic interaction in ZnO:Cu NWs comes from the Cu$^{2+}$ and "Cu$^{3+}$" states in the bulk region, and that most of the doped Cu ions are magnetically inactive probably because they are antiferromagnetically coupled with each other.

Crystal field effect on X-ray magnetic circular dichroism spectra at the L2,3 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 L2,3 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 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.