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 present a discussion of published x-ray magnetic circular dichroism (XMCD) measurements performed at the uranium M_4,5 edges of metallic uranium compounds, focusing on the shape of the dichroic signal at the M_5 edge. A well resolved double lobe structure, comprised of a positive and a negative peak, is sometimes observed. Out of the twelve metallic uranium compounds so far investigated by XMCD, six exhibit an intense double-lobe structure at the M_5 edge. This line shape gives information on the empty 5f magnetic density of states with angular quantum number j=7/2. Conclusions about the di…
We have probed the crystalline electric-field ground states of pure $|J = 7/2, J_z = \pm 5/2\rangle$ as well as the anisotropic $c$-$f$ hybridization in both valence fluctuating systems $α$- and $β$-YbAlB$_4$ by linear polarization dependence of angle-resolved core level photoemission spectroscopy. Interestingly, the small but distinct difference between \abyb was found in the polar angle dependence of linear dichroism, indicating the difference in the anisotropy of $c$-$f$ hybridization which may be essential to a heavy Fermi liquid state in $α$-YbAlB$_4$ and a quantum critical state in $β$-Y…
Nonresonant inelastic x-ray scattering (NIXS) has been performed on single crystals of UO$_2$ to study the direction dependence of higher-order-multipole scattering from the uranium $O_{4,5}$ edges (90--110 eV). By comparing the experimental results with theoretical calculations the symmetry of the ground state is confirmed directly as the crystal-field (CF) $Γ_5$ triplet state within the $J$ = 4 manifold. The results also demonstrate that the directional dichroism of the NIXS spectra is sensitive to the CF strength and establish NIXS as a tool for probing CF interactions quantitatively.
Here we present linear and circular polarized soft x-ray absorption spectroscopy (XAS) data at the Ce $M_{4,5}$ edges of the electron (Ir) and hole-doped (Re) Kondo semiconductor CeOs$_2$Al$_{10}$. Both substitutions have a strong impact on the unusual high N$\acute{e}$el temperature, $T_N$=28.5\,K, and also the direction of the ordered moment in case of Ir. The substitution dependence of the linear dichroism is weak thus validating the crystal-field description of CeOs$_2$Al$_{10}$ being representative for the Re and Ir substituted compounds. The impact of electron- and hole-doping on the hyb…
We study the directional dichroic absorption spectra in the x-ray region in a polar ferrimagnet GaFeO_3. The directional dichroism on the absorption spectra at the Fe pre-K-edge arises from the E1-E2 interference process through the hybridization between the 4p and 3d states in the noncentrosymmetric environment of Fe atoms. We perform a microscopic calculation of the spectra on a model of FeO_6 with reasonable parameter values for Coulomb interaction and hybridizations. We obtain the difference in the absorption coefficients when the magnetic field is applied parallel and antiparallel to the …
The orbital and spin magnetic moments, and the X-ray-magnetic circular-dichroism (XMCD) spectra at the $M_{4,5}$ edges of the U atoms in a UAs/Co multilayer and in an $α$-U film are calculated within the framework of the density-functional theory in combination with the local-spin-density approximation (LSDA), the generalized-gradient approximation (GGA) and the LDA+$U$ method. The antiparallel arrangement between the U and Co spin magnetic moments at the interface results in the vanishing of ferromagnetism for the case of very thin Co layers. The U moments decay rapidly with the distance from…
X-ray absorption and resonant X-ray emission measurements at the O 1s edge of the uranium oxides UO2, U3O8 and UO3 are presented. The spectral shapes of the O Kα X-ray emission spectra of UO3 exhibit significant excitation energy dependence, from an asymmetric to a symmetric form, which differs from those of UO2 and U3O8. This energy dependence is attributed to a significant difference in the oxygen-uranium hybridization between two different sites in the crystal structure of UO3. The spectral shapes of UO2 and U3O8 are also found to be different but without significant energy dependence. The …
Oxygen packaging in transition metal oxides determines the metal-oxygen hybridization and electronic occupation at metal orbitals. Strontium vanadate (SrVO$_3$), having a single electron in a $3d$ orbital, is thought to be the simplest example of strongly correlated metallic oxides. Here, we determine the effects of epitaxial strain on the electronic properties of SrVO$_3$ thin films, where the metal-oxide sublattice is corner-connected. Using x-ray absorption and x-ray linear dichroism at the V $L_{2,3}$ and O $K$-edges, it is observed that tensile or compressive epitaxial strain change the h…
X-ray magnetic circular dichroism (XMCD) at the Eu L-edge (2p->5d) in two compounds exhibiting valence fluctuation, namely EuNi2(Si0.18Ge0.82)2 and EuNi2P2, has been investigated at pulsed high magnetic fields of up to 40 T. A distinct XMCD peak corresponding to the trivalent state (Eu3+; f6), whose ground state is nonmagnetic (J=0), was observed in addition to the main XMCD peak corresponding to the magnetic (J=7/2) divalent state (Eu2+; f7). This result indicates that the 5d electrons belonging to both valence states are magnetically polarized. It was also found that the ratio P5d(3+)/P5d(2+…
The coexisting magnetic and ferroelectric orders in multiferroic materials give rise to a handful of novel magnetoelectric phenomena, such as the absorption difference for the opposite propagation directions of light called the non-reciprocal directional dichroism (NDD). Usually these effects are restricted to low temperature, where the multiferroic phase develops. In this paper we report the observation of NDD in the paramagnetic phase of Sr2CoSi2O7 up to temperatures more than ten times higher than its Néel temperature (7 K) and in fields up to 30 T. The magnetically induced polarization and…
We use x-ray absorption spectroscopy as well as its linear and circular magnetic dichroisms to characterize relevant interactions and energy scales in the surface intermetallic CePt$_5$/Pt(111). The experiments provide insight into crystal field splitting, effective paramagnetic moments, their Kondo screening and mutual interactions and thus into many aspects which typically determine the low temperature behavior of correlated rare earth compounds. Exploiting the tuneability of Ce valence through the thickness dependent epitaxial strain at the CePt$_5$/Pt(111) interface, we are able to systema…
The Fermi surface (FS) nesting properties of URu$_2$Si$_2$ are analyzed with particular focus on their implication for the mysterious hidden order phase. We show that there exist two Fermi surfaces that exhibit a strong nesting at the antiferromagnetic wavevector, $\boldsymbol{Q}_0$=(0,\,0,\,1). The corresponding energy dispersions fulfill the relation $ε_{1}(\boldsymbol{k})$=$- ε_{2} (\boldsymbol{k}\pm \boldsymbol{Q}_0)$ at eight FS hotspot lines. The spin-orbital characters of the involved $5f$ states are {\it distinct} ($j_z$=$\pm$5/2 {\it vs.} $\pm$3/2) and hence the degenerate Dirac cross…
The origin of x-ray magnetic circular dichroism (XMCD) at the Cu L2,3 edge in YBa2Cu3O7/La(1-x)Ca(x)MnO3 superlattices is revealed by performing first-principle electronic structure calculation using fully-relativistic spin-polarized linear muffin-tin orbital and projected augmented plane wave methods. We show that the XMCD spectra at the Cu L2,3 edges are proportional to the difference of the densities of majority- and minority-spin Cu 3z2-1 states. Although the Cu 3z2-1 states lie well below the Fermi level, a small number of majority-spin 3z2-1 holes is created by the Cu 3z2-1 - O p_z - Mn …
We report on microscopic study of the ferromagnetism enhancement in the Ru doped ferromagnetic superconductor (FM SC) UCoGe. For that purpose, two single crystals with composition UCo0.97Ru0.03Ge and UCo0.88Ru0.12Ge were prepared. Both single crystals were investigated by polarized neutron diffraction (PND) at low temperatures in magnetic fields and the latter one also by the soft X-ray magnetic circular dichroism (XMCD) method. UCo0.96Ru0.03Ge and UCo0.88Ru0.12Ge have been found ordering ferromagnetically below the Curie temperature TC = 6 K and 8.5 K, respectively, which are considerable hig…
We report a combined study for the electronic structures of ferromagnetic CeAgSb$_2$ using soft X-ray absorption (XAS), magnetic circular dichroism (XMCD), and angle-resolved photoemission (ARPES) spectroscopies. The Ce $M_{4, 5}$ XAS spectra show very small satellite structures, reflecting a strongly localized character of the Ce $4f$ electrons. The linear dichroism effects in the Ce $M_{4, 5}$ XAS spectra demonstrate the ground state Ce $4f$ symmetry of $Γ{_6}$, the spatial distribution of which is directed along the $c$-axis. The XMCD results give support to the picture of local-moment magn…
Replacing a magnetic atom by a spinless atom in a heavy fermion compound generates a quantum state often referred to as a 'Kondo-hole'. No experimental imaging has been achieved of the atomic-scale electronic structure of a Kondo-hole, or of their destructive impact (Lawrence JM, et al. (1996) Kondo hole behavior in Ce0. 97La0. 03Pd3. Phys Rev B 53:12559-12562; Bauer ED, et al. (2011) Electronic inhomogeneity in a Kondo lattice. Proc Natl Acad Sci. 108:6857-6861) on the hybridization process between conduction and localized electrons which generates the heavy fermion state. Here we report visu…
Artificially fabricated 3$d$/5$d$ superlattices (SLs) involve both strong electron correlation and spin-orbit coupling in one material by means of interfacial 3$d$-5$d$ coupling, whose mechanism remains mostly unexplored. In this work we investigated the mechanism of interfacial coupling in LaMnO$_3$/SrIrO$_3$ SLs by several spectroscopic approaches. Hard x-ray absorption, magnetic circular dichroism and photoemission spectra evidence the systematic change of the Ir ferromagnetism and the electronic structure with the change of the SL repetition period. First-principles calculations further re…
We investigate magnetic excitations in an $S=3/2$ Heisenberg model representing two-dimensional antiferromagnet ${\rm Ba_2CoGe_2O_7}$. In terahertz absorption experiment of the compound, Goldstone mode as well as novel magnetic excitations, conventional magnetic resonance at 2 meV and both electric- and magnetic-active excitation at 4 meV, have been observed. By introducing a hard uniaxial anisotropy term $Λ(S^z)^2$, three modes can be explained naturally. We also indicate that, via the spin-dependent metal-ligand hybridization mechanism, the 4 meV excitation is an electric-active mode through…
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 PuCo…
In heavy-fermion compounds, f electrons show both itinerant and localized behaviour depending on the external conditions, and the hybridization between localized f electrons and itinerant conduction bands gives rise to their exotic properties like heavy-fermions, magnetic orders and unconventional superconductivity. Duo to the risk of handling radioactive actinide materials, the direct experimental evidence of the band structure evolution across the localized-itinerant and magnetic transitions for 5f electrons is lacking. Here, by using angle-resolved photoelectron spectroscopy, we revealed th…
We investigated the Ru 4d and O 2p electronic structure and magnetic properties of an ultra-high-quality SrRuO3 film on SrTiO3 grown by machine-learning-assisted molecular beam epitaxy. The high itinerancy and long quantum lifetimes of the quasiparticles in the Ru 4d t2g-O 2p hybridized valence band are confirmed by observing the prominent well-screened peak in the Ru 3d core-level photoemission spectrum, the coherent peak near the Fermi energy in the valence band spectrum, and quantum oscillations in the resistivity. The element-specific magnetic properties and the hybridization between the R…
Fe$_5$GeTe$_2$ is a van der Waals (vdW)-coupled unconventional ferromagnetic metal with a high Curie temperature ($T_C$) exceeding 300 K. The formation of an anomalous ground state significantly below $T_C$ has received considerable attention, resulting in increased interest in understanding the spin-polarized electronic state evolution near the Fermi energy ($E_F$) as a function of temperature. Despite recent extensive studies, a microscopic understanding of the spin-polarized electronic structure around $E_F$ has not yet been established owing to the intrinsic complexity of both the crystal …
Magnetic circular dichroism (MCD) in the x-ray absorption spectroscopy (XAS) at the L2,3 edges for almost entire series of rare-earth (RE) elements in RE2Fe14B, is studied experimentally and theoretically. By a quantitative comparison of the complicated MCD spectral shapes, we find that (i) the 4f-5d intra-atomic exchange interaction not only induces the spin and orbital polarization of the 5d states, which is vital for the MCD spectra of the electric dipole transition from the 2p core states to the empty 5d conduction band, but also it accompanies a contraction of the radial part of the 5d wa…
The Kondo effect in ferromagnetic quantum critical CeRh$_6$Ge$_4$
Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Deutsches Elektronen-Synchrotron DESY（德国电子同步辐射中心）；Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室）；National Yang Ming Chiao Tung University（国立阳明交通大学）；National Synchrotron Radiation Research Center（国家同步辐射研究中心）；Technische Universität Braunschweig（布伦瑞克工业大学）
Relocalization of Uranium 5f Electrons in Antiferromagnetic Heavy Fermion Superconductor UPd$_2$Al$_3$: Insights from Angle-Resolved Photoemission Spectroscopy
We report x-ray absorption and x-ray linear dichroism measurements at the Fe L2,3 edges of the geometrically frustrated systems of potassium and hydronium iron jarosite. Comparison with simulated spectra, involving ligand-field multiplet calculations modelling the 3d-2p hybridization between the iron ion and the oxygen ligands, has yielded accurate estimates for the ligand metal-ion hybridization and the resulting single-ion crystal field anisotropy energy. Using this method we provide an experimentally verified scenario for the appearance of a single-ion anisotropy in this nominally high-spin…
Nature of the field-induced charge ordered phase (phase II) of SmRu$_4$P$_{12}$ has been investigated by resonant x-ray diffraction (RXD) and polarized neutron diffraction (PND), focusing on the relationship between the atomic displacements and the antiferromagnetic (AFM) moments of Sm. From the analysis of the interference between the non-resonant Thomson scattering and the resonant magnetic scattering, combined with the spectral function obtained from x-ray magnetic circular dichroism, it is shown that the AFM moment of Sm prefers to be parallel to the field ($m_{\text{AF}} \parallel H$), gi…
In intermetallic compounds with zero-orbital momentum ($L=0$) the magnetic anisotropy and the electronic band structure are interconnected. Here, we investigate this connection on divalent Eu and trivalent Gd intermetallic compounds. We find by X-ray magnetic circular dichroism an out-of-plane easy magetization axis in 2D atom-thick EuAu$_2$. Angle-resolved photoemission and density-functional theory prove that this is due to strong $f-d$ band hybridization and Eu$^{2+}$ valence. In contrast, the easy in-plane magnetization of the structurally-equivalent GdAu$_2$ is ruled by spin-orbit-split $…
Magnetism in Ni-Mn-Z (Z = Ga,In,Sn,Sb) Heusler alloys has so far been predominantly attributed to Rudermann-Kittel-Kasuya-Yoshida type interactions between Mn atoms. We investigate magnetic interactions in one such alloy, Ni$_{2}$Mn$_{1.4}$In$_{0.6}$ and attempt to explain the origin of antiferromagnetic (AFM) interactions that coexist with ferromagnetic ones. Through the combination of x-ray absorption spectroscopy and x-ray magnetic circular dichroism (XMCD), we find that Ni plays an important role along with Mn in the overall magnetism. A significant hybridization that develops between Mn a…
The critical behavior of dc magnetization in the uranium ferromagnet URhAl with the hexagonal ZrNiAl-type crystal structure has been studied around the ferromagnetic transition temperature T_C. The critical exponent beta for the temperature dependence of the spontaneous magnetization below T_C, gamma for the magnetic susceptibility, and delta for the magnetic isotherm at T_C have been obtained with a modified Arrott plot, a Kouvel-Fisher plot, the critical isotherm analysis and the scaling analysis. We have determined the critical exponents as beta = 0.287 +- 0.005, gamma = 1.47 +- 0.02, and d…
A partial disorder on a layered triangular lattice is theoretically investigated from a viewpoint of toroidal ordering and magnetoelectric effects. We consider an extended periodic Anderson model including a site-dependent antisymmetric spin-orbit coupling between conduction and localized electrons. We show that, by the mean-field approximation, the model exhibits a coplanar vortex-lattice-type magnetic order as observed in a hexagonal uranium compound UNi4B, in the parameter region with intermediate hybridization and electron correlation. This peculiar state accommodates a toroidal order, whi…
We measured geometric and magnetic properties of Co films on the Pd(111) surface by x-ray photoelectron diffraction (XPD), x-ray magnetic circular dichroism (MCD) at the Co L_{2,3} edge, and the surface magneto-optical Kerr effect (SMOKE) measurements. Co thin films are found to grow incoherently with fcc island structure on the smooth Pd(111) substrate. Comparison of MCD and SMOKE measurements of Co thin films grown on rough and smooth Pd(111) surfaces suggests that perpendicular remanent magnetization and Co orbital moment are enhanced by the rough interface. Pd capping layer also induces pe…
High-resolution resonant inelastic X-ray scattering (RIXS) at the oxygen K-edge has been used to study the orbital excitations of Ca2RuO4 and Sr2RuO4. In combination with linear dichroism X-ray absorption spectroscopy, the ruthenium 4d-orbital occupation and excitations were probed through their hybridization with the oxygen p-orbitals. These results are described within a minimal model, taking into account crystal field splitting and a spin-orbit coupling λ_{so}=200~meV. The effects of spin-orbit interaction on the electronic structure and implications for the Mott and superconducting ground …
We investigated the electronic and magnetic properties of fully oxidized BaFeO3 thin films, which show ferromagnetic-insulating properties with cubic crystal structure, by hard x-ray photoemission spectroscopy (HAXPES), x-ray absorption spectroscopy (XAS) and soft x-ray magnetic circular dichroism (XMCD). We analyzed the results with configuration-interaction (CI) cluster-model calculations for Fe4+, which showed good agreement with the experimental results. We also studied SrFeO3 thin films, which have an Fe4+ ion helical magnetism in cubic crystal structure, but are metallic at all temperatu…
The electronic structure and numerous magnetic properties of MnBi magnetic systems are investigated using local spin density approximation (LSDA) with on-cite Coulomb correlations (LSDA+$U$) included. We show that the inclusion of Coulomb correlations provides a much better description of equilibrium magnetic moments on Mn atom as well as the magnetic anisotropy energy (MAE) behavior with temperature and magneto-optical effects. We found that the inversion of the anisotropic pairwise exchange interaction between Bi atoms is responsible for the observed spin reorientation transition at 90 K. Th…
The electronic structure of the Cr ions in the diluted ferromagnetic semiconductor Zn$_{1-x}$Cr$_x$Te ($x=0.03$ and 0.15) thin films has been investigated using x-ray magnetic circular dichroism (XMCD) and photoemission spectroscopy (PES). Magnetic-field ($H$) and temperature ($T$) dependences of the Cr $2p$ XMCD spectra well correspond to the magnetization measured by a SQUID magnetometer. The line shape of the Cr $2p$ XMCD spectra is independent of $H$, $T$, and $x$, indicating that the ferromagnetism is originated from the same electronic states of the Cr ion. Cluster-model analysis indicat…
Pressure-induced self-doping and Fermi surface reconstruction in UAs2
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Institute of Quantum Materials and Physics, Henan Academy of Sciences（河南省科学院量子物质与物理研究所）；University of Chinese Academy of Sciences（中国科学院大学）
We investigate near-Fermi-energy (EF) element-specific electronic and spin states of ferromagnetic van der Waals (vdW) metal Fe5GeTe2. The soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) measurement provides spectroscopic evidence of localized Fe 3d band. We also find prominent hybridization between the localized Fe 3d band and the delocalized Ge/Te p bands. This picture is strongly supported from direct observation of the remarkable spin polarization of the ligand p bands near EF, using x-ray magnetic circular dichroism (XMCD) measurements. The strength of XMCD signal from lig…
The magnetism in the ferromagnetic superconductor UCoGe has been studied using a combination of magnetic Compton scattering, bulk magnetization, X-ray magnetic circular dichroism and electronic structure calculations, in order to determine the spin and orbital moments. The experimentally observed total spin moment, $M_s$, was found to be -0.24 $\pm$ 0.05~$μ_B$ at 5~T. By comparison with the total moment of 0.16 $\pm$ 0.01~$μ_B$, the orbital moment, $M_l$, was determined to be 0.40 $\pm$ 0.05~$μ_B$. The U and Co spin moments were determined to be antiparallel. We find that the U 5\textit{f} ele…
Field-rigid Ising antiferromagnetism with giant spin-flip fields in Van der Waals UOTe
Washington University in St. Louis（圣路易斯华盛顿大学）；National High Magnetic Field Laboratory, Los Alamos National Laboratory（洛斯阿拉莫斯国家实验室国家高磁场实验室）；Neutron Scattering Division, Oak Ridge National Laboratory（橡树岭国家实验室中子散射部）；Harvard University（哈佛大学）；National High Magnetic Field Laboratory, Florida State University（佛罗里达州立大学国家高磁场实验室）
