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Z. Hu

Publications and source records attributed to Z. Hu.

At least 91 records · Page 5Linked to original sources

Local electronic structure and magnetic properties of LaMn0.5Co0.5O3 studied by x-ray absorption and magnetic circular dichroism spectroscopy

We have studied the local electronic structure of LaMn0.5Co0.5O3 using soft-x-ray absorption spectroscopy at the Co-L_3,2 and Mn-L_3,2 edges. We found a high-spin Co^{2+}--Mn^{4+} valence state for samples with the optimal Curie temperature. We discovered that samples with lower Curie temperatures contain low-spin nonmagnetic Co^{3+} ions. Using soft-x-ray magnetic circular dichroism we established that the Co^{2+} and Mn^{4+} ions are ferromagnetically aligned. We revealed also that the Co^{2+} ions have a large orbital moment: m_orb/m_spin ~ 0.47. Together with model calculations, this suggests the presence of a large magnetocrystalline anisotropy in the material and predicts a non-trivial temperature dependence for the magnetic susceptibility.

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X-ray absorption and x-ray magnetic dichroism study on Ca3CoRhO6 and Ca3FeRhO6

Using x-ray absorption spectroscopy at the Rh-L_2,3, Co-L_2,3, and Fe-L_2,3 edges, we find a valence state of Co^2+/Rh^4+ in Ca3CoRhO6 and of Fe^3+/Rh^3+ in Ca3FeRhO6. X-ray magnetic circular dichroism spectroscopy at the Co-L_2,3 edge of Ca3CoRhO6 reveals a giant orbital moment of about 1.7mu_B, which can be attributed to the occupation of the minority-spin d_0d_2 orbital state of the high-spin Co^2+ (3d^7) ions in trigonal prismatic coordination. This active role of the spin-orbit coupling explains the strong magnetocrystalline anisotropy and Ising-like magnetism of Ca3CoRhO6.

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Direct observation of t2g orbital ordering in magnetite

Using soft-x-ray diffraction at the site-specific resonances in the Fe L23 edge, we find clear evidence for orbital and charge ordering in magnetite below the Verwey transition. The spectra show directly that the (001/2) diffraction peak (in cubic notation) is caused by t2g orbital ordering at octahedral Fe2+ sites and the (001) by a spatial modulation of the t2g occupation.

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Determining the crystal-field ground state in rare earth Heavy Fermion materials using soft-x-ray absorption spectroscopy

We infer that soft-x-ray absorption spectroscopy is a versatile method for the determination of the crystal-field ground state symmetry of rare earth Heavy Fermion systems, complementing neutron scattering. Using realistic and universal parameters, we provide a theoretical mapping between the polarization dependence of Ce $M_{4,5}$ spectra and the charge distribution of the Ce $4f$ states. The experimental resolution can be orders of magnitude larger than the $4f$ crystal field splitting itself. To demonstrate the experimental feasibility of the method, we investigated CePd$_2$Si$_2$, thereby settling an existing disagreement about its crystal-field ground state.

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Insulating state and the importance of the spin-orbit coupling in Ca$_3$CoRhO$_6$

We have carried out a comparative theoretical study of the electronic structure of the novel one-dimensional Ca$_3$CoRhO$_6$ and Ca$_3$FeRhO$_6$ systems. The insulating antiferromagnetic state for the Ca$_3$FeRhO$_6$ can be well explained by band structure calculations with the closed shell high-spin $d^5$ (Fe$^{3+}$) and low-spin $t_{2g}^{6}$ (Rh$^{3+}$) configurations. We found for the Ca$_3$CoRhO$_6$ that the Co has a strong tendency to be $d^7$ (Co$^{2+}$) rather than $d^6$ (Co$^{3+}$), and that there is an orbital degeneracy in the local Co electronic structure. We argue that it is the spin-orbit coupling which will lift this degeneracy thereby enabling local spin density approximation + Hubbard U (LSDA+U) band structure calculations to generate the band gap. We predict that the orbital contribution to the magnetic moment in Ca$_3$CoRhO$_6$ is substantial, i.e. significantly larger than 1 $μ_B$ per formula unit. Moreover, we propose a model for the contrasting intra-chain magnetism in both materials.

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Valence, spin, and orbital state of the Co ions in the one-dimensional Ca3Co2O6: an x-ray absorption and magnetic circular dichroism study

We have investigated the valence, spin, and orbital state of the Co ions in the one-dimensional cobaltate Ca3Co2O6 using x-ray absorption and x-ray magnetic circular dichroism at the Co-L2,3 edges. The Co ions at both the octahedral Co_oct and trigonal Co_trig sites are found to be in a 3+ state. From the analysis of the dichroism we established a low-spin state for the Co_oct and a high-spin state with an anomalously large orbital moment of 1.7 muB at the Co3+ trig ions. This large orbital moment along the c-axis chain and the unusually large magnetocrystalline anisotropy can be traced back to the double occupancy of the d2 orbital in trigonal crystal field.

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The spin state transition in LaCoO$_{3}$; revising a revision

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 LaCoO$_{3}$ 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 lineshapes we find that LaCoO$_{3}$ at finite temperatures is an inhomogeneous mixed-spin-state system. Crucial is that the magnetic circular dichroism signal in the paramagnetic state carries a large orbital momentum. This directly shows that the currently accepted low-/intermediate-spin picture is at variance. Parameters derived from these spectroscopies fully explain existing magnetic susceptibility, electron spin resonance and inelastic neutron data.

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Nitrogen based magnetic semiconductors

We describe a possible pathway to new magnetic materials with no conventional magnetic elements present. The substitution of Nitrogen for Oxygen in simple non magnetic oxides leads to holes in N 2$p$ states which form local magnetic moments. Because of the very large Hund's rule coupling of Nitrogen and O 2$p$ electrons and the rather extended spatial extend of the wave functions these materials are predicted to be ferromagnetic metals or small band gap insulators. Experimental studies support the theoretical calculations with regard to the basic electronic structure and the formation of local magnetic moments. It remains to be seen if these materials are magnetically ordered and if so below what temperature.

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Evolution of the $E(1/2^+_1)-E(3/2^+_1)$ energy spacing in odd-mass K, Cl and P isotopes for $N=20-28$

The energy of the first excited state in the neutron-rich N=28 nucleus 45Cl has been established via in-beam gamma-ray spectroscopy following proton removal. This energy value completes the systematics of the E(1/2^+_1)-E(3/2^+_1) level spacing in odd-mass K, Cl and P isotopes for N=20-28. The results are discussed in the framework of shell-model calculations in the sd-fp model space. The contribution of the central, spin-orbit and tensor components is discussed from a calculation based on a proton single-hole spectrum from G-matrix and pi + rho meson exchange potentials. A composite model for the proton 0d_{3/2}-1s_{1/2} single-particle energy shift is presented.

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Orbitally driven spin-singlet dimerization in $S$=1 La$_{4}$Ru$_{2}$O$_{10}$

Using x-ray absorption spectroscopy at the Ru-$L_{2,3}$ edge we reveal that the Ru$^{4+}$ ions remain in the $S$=1 spin state across the rare 4d-orbital ordering transition and spin-gap formation. We find using local spin density approximation + Hubbard U (LSDA+U) band structure calculations that the crystal fields in the low temperature phase are not strong enough to stabilize the $S$=0 state. Instead, we identify a distinct orbital ordering with a significant anisotropy of the antiferromagnetic exchange couplings. We conclude that La$_{4}$Ru$_{2}$O$_{10}$ appears to be a novel material in which the orbital physics drives the formation of spin-singlet dimers in a quasi 2-dimensional $S$=1 system.

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Variation with mass of $\boldmath{B(E3; 0_1^+ \to 3_1^-)}$ transition rates in $A=124-134$ even-mass xenon nuclei

$B(E3; 0_1^+ \to 3_1^-)$ transition matrix elements have been measured for even-mass $^{124-134}$Xe nuclei using sub-barrier Coulomb excitation in inverse kinematics. The trends in energy $E(3^-)$ and $B(E3; 0_1^+ \to 3_1^-)$ excitation strengths are well reproduced using phenomenological models based on a strong coupling picture with a soft quadrupole mode and an increasing occupation of the intruder $h_{11/2}$ orbital.

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Soft x-ray magnetic circular dichroism study on Gd-doped EuO thin films

We report on the growth and characterization of ferromagnetic Gd-doped EuO thin films. We prepared samples with Gd concentrations up to 11% by means of molecular beam epitaxy under distillation conditions, which allows a very precise control of the doping concentration and oxygen stoichiometry. Using soft x-ray magnetic circular dichroism at the Eu and Gd M4,5 edges, we found that the Curie temperature ranged from 69 K for pure stoichiometric EuO to about 170 K for the film with the optimal Gd doping of around 4%. We also show that the Gd magnetic moment couples ferromagnetically to that of Eu.

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Nature of magnetism in Ca$_3$Co$_2$O$_6$

We find using LSDA+U band structure calculations that the novel one-dimensional cobaltate Ca$_3$Co$_2$O$_6$ is not a ferromagnetic half-metal but a Mott insulator. Both the octahedral and the trigonal Co ions are formally trivalent, with the octahedral being in the low-spin and the trigonal in the high-spin state. The inclusion of the spin-orbit coupling leads to the occupation of the minority-spin $d_{2}$ orbital for the unusually coordinated trigonal Co, producing a giant orbital moment (1.57 $μ_{B}$). It also results in an anomalously large magnetocrystalline anisotropy (of order 70 meV), elucidating why the magnetism is highly Ising-like. The role of the oxygen holes, carrying an induced magnetic moment of 0.13 $μ_{B}$ per oxygen, for the exchange interactions is discussed.

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Orbital-assisted metal-insulator transition in VO$_{2}$

We found direct experimental evidence for an orbital switching in the V 3d states across the metal-insulator transition in VO$_{2}$. We have used soft-x-ray absorption spectroscopy at the V $L_{2,3}$ edges as a sensitive local probe, and have determined quantitatively the orbital polarizations. These results strongly suggest that, in going from the metallic to the insulating state, the orbital occupation changes in a manner that charge fluctuations and effective band widths are reduced, that the system becomes more 1-dimensional and more susceptible to a Peierls-like transition, and that the required massive orbital switching can only be made if the system is close to a Mott insulating regime.

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Controlling orbital moment and spin orientation in CoO layers by strain

We have observed that CoO films grown on different substrates show dramatic differences in their magnetic properties. Using polarization dependent x-ray absorption spectroscopy at the Co L$_{2,3}$ edges, we revealed that the magnitude and orientation of the magnetic moments strongly depend on the strain in the films induced by the substrate. We presented a quantitative model to explain how strain together with the spin-orbit interaction determine the 3d orbital occupation, the magnetic anisotropy, as well as the spin and orbital contributions to the magnetic moments. Control over the sign and direction of the strain may therefore open new opportunities for applications in the field of exchange bias in multilayered magnetic films.

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Spectroscopy of stripe order in La1.8Sr0.2NiO4 using resonant soft x-ray diffraction

Strong resonant enhancements of the charge-order and spin-order superstructure-diffraction intensities in La1.8Sr0.2NiO4 are observed when x-ray energies in the vicinity of the Ni L2,3 absorption edges are used. The pronounced photon-energy and polarization dependences of these diffraction intensities allow for a critical determination of the local symmetry of the ordered spin and charge carriers. We found that not only the antiferromagnetic order but also the charge-order superstructure resides within the NiO2 layers; the holes are mainly located on in-plane oxygens surrounding a Ni2+ site with the spins coupled antiparallel in close analogy to Zhang-Rice singlets in the cuprates.

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Determination of the orbital moment and crystal field splitting in LaTiO$_{3}$

Utilizing a sum-rule in a spin-resolved photoelectron spectroscopic experiment with circularly polarized light, we show that the orbital moment in LaTiO$_3$ is strongly reduced both below and above the Néel temperature. Using Ti $L_{2,3}$ x-ray absorption spectroscopy as a local probe, we found that the crystal field splitting in the $t_{2g}$ subshell is about 0.12-0.30 eV. This large splitting does not facilitate the formation of an orbital liquid.

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Magnetic versus crystal field linear dichroism in NiO thin films

We have detected strong dichroism in the Ni $L_{2,3}$ x-ray absorption spectra of monolayer NiO films. The dichroic signal appears to be very similar to the magnetic linear dichroism observed for thicker antiferromagnetic NiO films. A detailed experimental and theoretical analysis reveals, however, that the dichroism is caused by crystal field effects in the monolayer films, which is a non trivial effect because the high spin Ni $3d^{8}$ ground state is not split by low symmetry crystal fields. We present a practical experimental method for identifying the independent magnetic and crystal field contributions to the linear dichroic signal in spectra of NiO films with arbitrary thicknesses and lattice strains. Our findings are also directly relevant for high spin $3d^{5}$ and $3d^{3}$ systems such as LaFeO$_{3}$, Fe$_{2}$O$_{3}$, VO, LaCrO$_{3}$, Cr$_{2}$O$_{3}$, and Mn$^{4+}$ manganate thin films.

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