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Register a new userX-ray magnetic circular dichroism experiments and theory of transuranium Laves phase compounds
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The actinide cubic Laves compounds NpAl2, NpOs2, NpFe2, and PuFe2 have been examined by X-ray magnetic circular dichroism (XMCD) at the actinide M4,5 absorption edges and Os L2,3 absorption edges. The XMCD experiments performed at the M4,5 absorption edges of Np and Pu allow us to determine the spectroscopic branching ratio, which gives information on the coupling scheme in these materials. In all materials the intermediate coupling scheme is found appropriate. Comparison with the SQUID data for NpOs2 and PuFe2 allows a determination of the individual orbital and spin magnetic moments and the magnetic dipole contribution mmd. The resulting orbital and spin magnetic moments are in good agreement with earlier values determined by neutron diffraction, and the values of mmd are non-negligible, and close to those predicted for intermediate coupling. There is a comparatively large induced moment on the Os atom in NpOs2 such that the Os contribution to the total moment per formula unit is ~30% of the total. The spin and orbital moments at the Os site are parallel, in contrast to the anti-parallel configuration of Os impurities in 3d ferromagnetic transition metals. Calculations using the LDA+U technique are reported. The ab initio computed XMCD spectra show good agreement with experimental spectra for small values (0-1eV) of the Hubbard U parameter, which underpins that 5f electrons in these compounds are relatively delocalized.
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X-ray absorption (XAS) and x-ray magnetic circular dichroism (XMCD) spectra at the L$_{2,3}$ edges of Mn in (Ge,Mn) compounds have been measured and are compared to the results of first principles calculation. Early textit{ab initio} studies show that the Density Functional Theory (DFT) can very well describe the valence band electronic properties but fails to reproduce a characteristic change of sign in the L$_{3}$ XMCD spectrum of Mn in Ge$_3$Mn$_5$, which is observed in experiments. In this work we demonstrate that this disagreement is partially related to an underestimation of the exchange splitting of Mn 2$p$ core states within the local density approximation. It is shown that the change in sign experimentally observed is reproduced if the exchange splitting is accurately calculated within the Hartree-Fock approximation, while the final states can be still described by the DFT. This approach is further used to calculate the XMCD in different (Ge,Mn) compounds. It demonstrates that the agreement between experimental and theoretical spectra can be improved by combining state of the art calculations for the core and valence states respectively.
We study the spin-dependent electronic structure of UTe and UT_{2}Si_{2} (T=Cu and Mn) compounds with a combination of x-ray magnetic circular dichroism measurements and first principle calculations. By exploiting the presence of sizable quadrupolar and dipolar contributions to the U L_{2,3}-edge x-ray absorption cross section we are able to provide unique information on the extent of hybridization between 5f and 6d/3d electronic states, a key parameter regulating the physical properties of all actinide materials. Since this information is hardly accessible to other probes, the new methodology opens up new venues for investigating this important class of materials.
We have measured X-ray magnetic circular dichroism (XMCD) spectra at the Pu $M_{4,5}$ absorption edges from a newly-prepared high-quality single crystal of the heavy fermion superconductor $^{242}$PuCoGa$_{5}$, exhibiting a critical temperature $T_{c} = 18.7~{rm K}$. The experiment probes the vortex phase below $T_{c}$ and shows that an external magnetic field induces a Pu 5$f$ magnetic moment at 2 K equal to the temperature-independent moment measured in the normal phase up to 300 K by a SQUID device. This observation is in agreement with theoretical models claiming that the Pu atoms in PuCoGa$_{5}$ have a nonmagnetic singlet ground state resulting from the hybridization of the conduction electrons with the intermediate-valence 5$f$ electronic shell. Unexpectedly, XMCD spectra show that the orbital component of the $5f$ magnetic moment increases significantly between 30 and 2 K; the antiparallel spin component increases as well, leaving the total moment practically constant. We suggest that this indicates a low-temperature breakdown of the complete Kondo-like screening of the local 5$f$ moment.
Ca_1-xSr_xRuO_3, which is ferromagnetic for Sr concentration x > 0.3, has been studied by x-ray magnetic circular dichroism (XMCD) in Ru 3p and O 1s core-level x-ray absorption. XMCD signals appear at x ~ 0.3 and monotonically increases with x in the ferromagnetic phase. While the monotonic increase of the XMCD signals with x is of a typical Stoner-type, the absence of appreciable change in the spectral line shapes of both the Ru 3p and O 1s XMCD spectra indicate that the itinerant-electron ferromagnetism in Ca_1-xSr_xRuO_3 is influenced by strong electron correlation.
The ferromagnetic superconductor UCoGe has been investigated by high field X-ray magnetic circular dichroism (XMCD) at the U-M$_{4,5}$ and Co/Ge-K edges. The analysis of the branching ratio and XMCD at the U-M$_{4,5}$ edges reveals that the U-5$f$ electrons count is close to 3. The orbital ($sim0.70,mu_B$) and spin ($sim-0.30,mu_B$) moments of U at 2.1K and 17T (H//c) have been determined. Their ratio ($sim-2.3$) suggests a significant delocalization of the 5$f$ electron states. The similar field dependences of the local U/Co and the macroscopic magnetization indicate that the Co moment is induced by the U moment. The XMCD at the Co/Ge-K edges reveal the presence of small Co-4$p$ and Ge-4$p$ orbital moments parallel to the macroscopic magnetization. In addition, the Co-3$d$ moment is estimated to be at most of the order of 0.1$mu_B$ at 17T. Our results rule out the possibility of an unusual polarisability of the U and Co moments as well as their antiparallel coupling. We conclude that the magnetism which mediates the superconductivity in UCoGe is driven by U.
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