Magnetic instabilities in Fe3C cementite particles observed with Fe K-edge x-ray circular dichroism under pressure

The ferromagnetic interstitial iron compound Fe(3)C (cementite) is expected to have Invar properties, whereby a high-moment to low-moment transition should occur when the atomic volume is reduced below a critical value. We, therefore, examine the pressure dependence of the Fe K-edge x-ray magnetic circular dichroism in Fe(3)C at ambient temperature and pressures up to 20 GPa. We find clear evidence for a high-moment to low-moment transition around 10 GPa.     

Dynamics of the magnetic and structural alpha-epsilon phase transition in iron

We have studied the high-pressure iron bcc to hcp phase transition by simultaneous x-ray magnetic circular dichroism and x-ray absorption spectroscopy with an x-ray energy dispersive spectrometer. The combination of the two techniques allows us to obtain simultaneously information on both the structure and the magnetic state of iron under pressure. The magnetic and structural transitions simultaneously observed are sharp. Both are of first order in agreement with the theoretical prediction. The pressure domain of the transition observed (2.4+/-0.2 GPa) is narrower than that usually cited in the literature (8 GPa). Our data indicate that the magnetic transition slightly precedes the structural one, suggesting that the origin of the instability of the bcc phase in iron with increasing pressure is to be attributed to the effect of pressure on magnetism as predicted by spin-polarized full-potential total energy calculations.     

Ferrimagnetism in EuFe4Sb12 due to the interplay of f-electron moments and a nearly ferromagnetic host

We combine x-ray magnetic circular dichroism spectroscopy at Fe L2,3 edges, at Eu M4,5 edges, x-ray absorption spectroscopy (XAS) investigation of Eu valence, and local spin density calculations, to show that the filled skutterudite Eu0.95Fe4Sb12 is a ferrimagnet in which the Fe 3d moment and the Eu2+ 4f moment are magnetically ordered with dominant antiferromagnetic coupling. From Eu L3 edge XAS, we find that about 13% of the Eu have a formal valence of 3+. We ascribe the origin of ferrimagnetism at a relatively high transition temperature TC of 85 K in Eu0.95Fe4Sb12 to f-electron interaction with the nearly ferromagnetic [Fe4Sb12]2.2- host lattice.     

Three-dimensional noncollinear antiferromagnetic order in single-crystalline FeMn ultrathin films

We present experimental evidence for a three-dimensional noncollinear antiferromagnetic spin structure in ultrathin single-crystalline fcc Fe50Mn50 layers using magnetic circular dichroism photoelectron emission microscopy and x-ray magnetic linear dichroism. Layer-resolved as-grown domain images of epitaxial trilayers grown on Cu(001) in which FeMn is sandwiched between ferromagnetic layers with different easy axes reveal the presence of antiferromagnetic spin components in the film plane and normal to the film plane. An FeMn spin structure with no collinear order in the film plane is consistent with the absence of x-ray magnetic linear dichroism in Fe L3 absorption in FeMn/Co bilayers.     

Magnetism of the Fe/ZnSe(001) interface

The magnetism of epitaxial ultrathin films of Fe on ZnSe(001) has been investigated by x-ray magnetic circular dichroism down to the submonolayer regime. In contrast to other metallic ferromagnet/semiconductor interfaces, no reduction of the Fe magnetic moment was found at the Fe/ZnSe(001) interface. Furthermore, a significant enhancement of the Fe magnetic moment compared to the bulk value was observed for coverages up to one monolayer in agreement with theoretical predictions. We also demonstrate that the magnetic properties of the Fe/ZnSe(001) interface remain stable against thermal annealing up to 300 degrees C, a prerequisite for the future development of efficient spintronics devices.     

Spin-flop ordering from frustrated ferro- and antiferromagnetic interactions: a combined theoretical and experimental study of a Mn/Fe(100) monolayer

The occurrence of a noncollinear magnetic structure at a Mn monolayer grown epitaxially on Fe(100) is predicted theoretically, using spinor density-functional theory, and observed experimentally, using x-ray magnetic circular dichroism (XMCD) and linear dichroism (XMLD) spectroscopies. The combined use of XMCD and XMLD at the Mn-absorption edge allows us to assess the existence of ferromagnetic and antiferromagnetic order at the interface, and also to determine the moment orientations with element specificity. The experimental results thus obtained are in excellent agreement with the magnetic structure determined theoretically.     

Spin state transition in LaCoO3 studied using soft x-ray absorption spectroscopy and magnetic circular dichroism

Using soft x-ray absorption spectroscopy and magnetic circular dichroism at the Co-L(2,3) edge, we reveal that the spin state transition in LaCoO3 can be well described by a low-spin ground state and a triply degenerate high-spin first excited state. From the temperature dependence of the spectral line shapes, we find that LaCoO3 at finite temperatures is an inhomogeneous mixed-spin state system. It is crucial that the magnetic circular dichroism signal in the paramagnetic state carries a large orbital momentum. This directly shows that the currently accepted low- or intermediate-spin picture is at variance. Parameters derived from these spectroscopies fully explain existing magnetic susceptibility, electron spin resonance, and inelastic neutron data.     

First observation of nonreciprocal X-Ray gyrotropy

We report the first observation of a nonreciprocal x-ray linear dichroism caused by the time-reversal odd, real part zeta of the complex gyrotropy tensor zeta(*) which is dominated by electric dipole-electric quadrupole E1E2 interference terms. A nonreciprocal transverse anisotropy was observed in the low temperature insulating phase of a Cr doped V2O3 Mott crystal when a single antiferromagnetic domain was grown by magnetoelectric annealing along the hexagonal c axis. This new element (edge) specific spectroscopy could nicely complement x-ray magnetic circular dichroism which is silent for antiferromagnetic materials.     

Direct observation of a bulklike spin moment at the Fe/GaAs(100)-4x6 interface

We have used x-ray magnetic circular dichroism, which offers a unique capability to give element specific information at submonolayer sensitivity, to determine the spin and orbital magnetic moments at the Fe/GaAs(100) interface. The wedge samples, grown by molecular beam epitaxy at room temperature, consisted of 0.25-1 monolayer (ML) Fe on GaAs(100)-4x6 capped with 9 ML Co and have shown Fe spin moments of (1.84-1.96)micro(B) and a large orbital enhancement. Our results demonstrate unambiguously that the Fe/GaAs(100)-4x6 interface is ferromagnetic with a bulklike spin moment, which is highly promising for spintronics applications.     

Microscopic nature of ferro- and antiferromagnetic interface coupling of uncompensated magnetic moments in exchange bias systems

Exchange bias in layered CoO/Fe structures is investigated by x-ray resonant magnetic reflectivity (XRMR) measurements. Element-specific hysteresis loops are obtained from x-ray magnetic circular dichroism effects in the XRMR spectra. Evidence is provided for the existence of different types of uncompensated moments in the antiferromagnetic material. Explanations are given for the microscopic nature of these moments and the complex exchange interactions that determine the magnetization reversal in exchange bias systems.     

Magnetic and structural properties of FeCr alloys

Synergistic synchrotron x-ray absorption experiments using imaging magnetic microspectroscopy, x-ray magnetic circular dichroism, and ab initio calculations on FeCr alloys reveal that the Cr content strongly influences the ferromagnetic microstructure and the Fe magnetic moments. The Cr local structure resolved by extended x-ray absorption fine structure (EXAFS) is also found to be affected by the alloy's composition. Both EXAFS and ab initio calculations show a change in the Cr local atomic structure above 10 at.% Cr content from the distance contraction of the first two coordination shells around the Cr absorbing atom. These results indicate the strong dependence of magnetic and structural properties of these alloys on Cr concentration.     

Strongly enhanced orbital moment by reduced lattice symmetry and varying composition of Fe1-xCox alloy films

We studied tetragonally distorted Fe(1-x)Co(x) alloy films on Rh(001), which show a strong perpendicular anisotropy in a wide thickness and composition range. Analyzing x-ray magnetic circular dichroism spectra at the L_(3,2) edges we found a dependence of the Co magnetic orbital moment on the chemical composition of the Fe(1-x)Co(x) alloy films, with a maximum at x=0.6. For this composition, we observed an out-of-plane easy axis of magnetization at room temperature for film thickness up to 15 monolayers. Since both the magnetic orbital moment and the anisotropy energy show similar composition dependence, it confirms that both quantities are directly related. Our experiments show that the adjustment of the Fermi level by a proper choice of the alloy composition is decisive for the large magnetic orbital moment and for a large magnetic anisotropy in a tetragonally distorted lattice.     

X-ray magnetic circular dichroism measurements in Ni up to 200 GPa: resistant ferromagnetism

The structural stability of fcc Ni over a very large pressure range offers a unique opportunity to experimentally investigate how magnetism is modified by simple compression. K-edge x-ray magnetic circular dichroism (XMCD) shows that fcc Ni is ferromagnetic up to 200 GPa, contradicting recent predictions of an abrupt transition to a paramagnetic state at 160 GPa. Density functional theory calculations point out that the pressure evolution of the K-edge XMCD closely follows that of the p projected orbital moment rather than that of the total spin moment. The disappearance of magnetism in Ni is predicted to occur above 400 GPa.     

Charge order in LuFe2O4: an unlikely route to ferroelectricity

We present the refinement of the crystal structure of charge-ordered LuFe2O4, based on single-crystal x-ray diffraction data. The arrangement of the different Fe-valence states, determined with bond-valence-sum analysis, corresponds to a stacking of charged Fe bilayers, in contrast with the polar bilayers previously suggested. This arrangement is supported by an analysis of x-ray magnetic circular dichroism spectra, which also evidences a strong charge-spin coupling. The nonpolar bilayers are inconsistent with charge order based ferroelectricity.     

Cycloidal order of 4f moments as a probe of chiral domains in DyMnO₃

Using soft x-ray diffraction at the Dy-M? resonance, pronounced circular dichroism in the ferroelectric phase of DyMnO? is observed in connection with sizable b and c components of the Dy-4f magnetic moments. This provides strong evidence for cycloidal order of the 4f moments, corroborating that inversion-symmetry breaking in this material is not accomplished by the Mn spins alone. The 4f circular dichroism allows us to image multiferroic domains that are imprinted on the surface of DyMnO? using the local charging by the x-ray beam via the photoelectric effect.     

Spin and orbital magnetic moments of Fe3O4

We present measurements of the spin and orbital magnetic moments of Fe3O4 by using SQUID and magnetic circular dichroism in soft x-ray absorption. The measurements show that Fe3O4 has a noninteger spin moment, in contrast to its predicted half-metallic feature. Fe3O4 also exhibits a large unquenched orbital moment. Calculations using the local density approximation including the Hubbard U method and the configuration interaction cluster-model suggest that strong correlations and spin-orbit interaction of the 3d electrons result in the noninteger spin and large orbital moments of Fe3O4.     

Symmetry-breaking induced exchange bias in ferromagnetic Ni-Cu-Co and Ni-Fe-Co sandwiches grown on a vicinal Cu(001) surface

Ferromagnetic Ni-Cu-Co and Ni-Fe-Co sandwiches were grown epitaxially onto a vicinal Cu(001) substrate and investigated using magneto-optical Kerr effect and x-ray magnetic circular dichroism techniques. We find that the atomic steps of the vicinal surface break the magnetic reversal symmetry to induce an exchange bias in the Ni perpendicular magnetic hysteresis loop. The Ni exchange bias direction can be switched by changing the direction of the in-plane Co magnetization. In addition, the exchange bias can be tailored by changing the Cu or Fe spacer layer thickness.     

Nature of Ho magnetism in multiferroic HoMnO3

Using x-ray resonant magnetic scattering and x-ray magnetic circular dichroism, techniques that are element specific, we have elucidated the role of Ho3+ in multiferroic HoMnO3. In zero field, Ho3+ orders antiferromagnetically with moments aligned along the hexagonal c direction below 40 K, and undergoes a transition to another magnetic structure below 4.5 K. In applied electric fields of up to 1 x 10(7) V/m, the magnetic structure of Ho3+ remains unchanged.     

X-ray absorption and magnetic circular dichroism characterization of Mo1–xFexO2 (x = 0–0.05) thin films grown by pulsed laser ablation

The electronic and magnetic properties of well characterized Mo_1???xFe_xO₂ (x = 0–0.5) thin films that show ferromagnetism at room temperature (RT) have been investigated by the means of near edge x-ray absorption fine structure (NEXAFS) and x-ray magnetic circular dichroism (XMCD) experiments at the O K-, Fe L-, and Mo M-edges. The NEXAFS spectra at O K- and Mo M_3,2 -edges show a strong hybridization of O 2p-4d Mo orbitals, and Mo ions change their symmetry with the substitution of Fe ions into MoO₂ matrix. The Fe 2p NEXAFS/XMCD spectra exhibit multiple absorption peaks and an appreciable XMCD signal that persists even at RT. These results demonstrate that Fe is in a mixed valence state of Fe^2?+?–Fe^3?+?, substituting at the Mo site and that the Fe^2?+?/3?+? ions are ferromagnetically polarized.     

Orbital and bonding anisotropy in a half-filled GaFeO3 magnetoelectric ferrimagnet

We investigated the orbital anisotropy of GaFeO3 using the Fe L2,3-edge x-ray magnetic circular dichroism and the polarization dependent O K-edge x-ray absorption spectroscopy. We found that the system shows a considerably large orbital momentum and anisotropic Fe-O bonding, which are unexpected in a half-filled d5 system such as GaFeO3. The orbital and bonding anisotropies, which turn out to be induced by the lattice distortions with exotic off-centering site movements, contribute the large magnetocrystalline energy and magnetoelasticity. These results provide critical clues on the microscopic understanding of the magnetoelectricity.