arXiv subjects

L. H. Tjeng

Publications and source records attributed to L. H. Tjeng.

At least 91 records · Page 5Linked to original sources

arXiv2009

Crystal-field ground state of the non-centrosymmetric superconductor CePt3Si: a combined polarized soft X-ray absorption and polarized neutron study

We determined the crystal-field split Hund's rule ground state of the non-centrosymmetric heavy fermion superconductor CePt3Si with polarization dependent soft X-ray absorption spectroscopy (XAS) and polarized neutron scattering. We are also able to give the sequence of the crystal-field states from the temperature evolution of the linear dichroic signal in the XAS. The quantitative analysis of the XAS temperature dependence together with the neutron transition energies complete the identification of the crystal-field level scheme.

cond-mat.str-el↗

arXiv2009

Static and fluctuating stripe order observed by resonant soft x-ray diffraction in La1.8Sr0.2NiO4

We studied the stripe phase of La1.8Sr0.2NiO4 using neutron diffraction, resonant soft x-ray diffraction (RSXD) at the Ni L2,3 edges, and resonant x-ray diffraction (RXD) at the Ni K threshold. Differences in the q-space resolution of the different techniques have to be taken into account for a proper evaluation of diffraction intensities associated with the spin and charge order superstructures. We find that in the RSXD experiment the spin and charge order peaks show the same temperature dependence. In the neutron experiment by contrast, the spin and charge signals follow quite different temperature behaviors. We infer that fluctuating magnetic order contributes considerably to the magnetic RSXD signal and we suggest that this result may open an interesting experimental approach to search for fluctuating order in other systems by comparing RSXD and neutron diffraction data.

cond-mat.str-el↗

arXiv2009

Spin blockade, orbital occupation and charge ordering in La_(1.5)Sr_(0.5)CoO4

Using Co-L_(2,3) and O-K x-ray absorption spectroscopy, we reveal that the charge ordering in La_(1.5)Sr_(0.5)CoO4 involves high spin (S=3/2) Co^2+ and low spin (S=0) Co^3+ ions. This provides evidence for the spin blockade phenomenon as a source for the extremely insulating nature of the La_(2-x)Sr_(x)CoO4 series. The associated e_g^2 and e_g^0 orbital occupation accounts for the large contrast in the Co-O bond lengths, and in turn, the high charge ordering temperature. Yet, the low magnetic ordering temperature is naturally explained by the presence of the non-magnetic (S=0) Co^3+ ions. From the identification of the bands we infer that La_(1.5)Sr_(0.5)CoO4 is a narrow band material.

cond-mat.str-el↗

arXiv2008

Ising magnetism and ferroelectricity in Ca$_3$CoMnO$_6$

The origin of both the Ising chain magnetism and ferroelectricity in Ca$_3$CoMnO$_6$ is studied by $ab$ $initio$ electronic structure calculations and x-ray absorption spectroscopy. We find that Ca$_3$CoMnO$_6$ has the alternate trigonal prismatic Co$^{2+}$ and octahedral Mn$^{4+}$ sites in the spin chain. Both the Co$^{2+}$ and Mn$^{4+}$ are in the high spin state. In addition, the Co$^{2+}$ has a huge orbital moment of 1.7 $μ_B$ which is responsible for the significant Ising magnetism. The centrosymmetric crystal structure known so far is calculated to be unstable with respect to exchange striction in the experimentally observed $\uparrow\uparrow\downarrow\downarrow$ antiferromagnetic structure for the Ising chain. The calculated inequivalence of the Co-Mn distances accounts for the ferroelectricity.

cond-mat.mtrl-sci↗

arXiv2008

Low energy excitations in CoO studied by temperature dependent x-ray absorption spectroscopy

We have measured the intricate temperature dependence of the Co L2,3 x-ray absorption spectra (2p-3d excitations) of CoO. To allow for accurate total electron yield measurements, the material has been grown in thin film form on a metallic substrate in order to avoid charging problems usually encountered during electron spectroscopic studies on bulk CoO samples. The changes in spectra due to temperature are in good agreement with detailed ligand-field calculations indicating that these changes are mostly due to thermal population of closely lying excited states, originating from degenerate t2g levels lifted by the spin-orbit coupling. Magnetic coupling in the ordered phase, modeled as a mean-field exchange field, mixes in excited states inducing a tetragonal charge density. The spin-orbit coupling induced splitting of the low energy states results in a non-trivial temperature dependence for the magnetic susceptibility.

cond-mat.str-el↗

arXiv2008

Crystal-field level inversion in lightly Mn-doped Sr3Ru2O7

Sr3(Ru1-xMnx)2O7, in which 4d-Ru is substituted by the more localized 3d-Mn, is studied by x-ray dichroism and spin-resolved density functional theory. We find that Mn impurities do not exhibit the same 4+ valence of Ru, but act as 3+ acceptors; the extra eg electron occupies the in-plane 3dx2-y2 orbital instead of the expected out-of-plane 3d3z2-r2. We propose that the 3d-4d interplay, via the ligand oxygen orbitals, is responsible for this crystal-field level inversion and the material's transition to an antiferromagnetic, possibly orbitally-ordered, low-temperature state.

cond-mat.str-el↗

arXiv2008

Aligning spins in antiferromagnetic films using antiferromagnets

We have explored the possibility to orient spins in antiferromagnetic thin films with low magnetocrystalline anisotropy via the exchange coupling to adjacent antiferromagnetic films with high magnetocrystalline anisotropy. We have used MnO as a prototype for a system with negligible single-ion anisotropy. We were able to control its spin direction very effectively by growing it as a film on antiferromagnetic CoO films with different predetermined spin orientations. This result may pave the way for tailoring antiferromagnets with low magnetocrystalline anistropy for applications in exchange bias systems. Very detailed information concerning the exchange coupling and strain effects was obtained from the Mn $L_{2,3}$ soft x-ray absorption spectroscopy.

cond-mat.str-el↗

arXiv2008

Image charge screening: a new approach to enhance magnetic ordering temperatures

We have tested the concept of image charge screening as a new approach to enhance magnetic ordering temperatures and superexchange interactions in ultra thin films. Using a 3 monolayer NiO(100) film grown on Ag(100) and an identically thin film on MgO(100) as model systems, we observed that the Neel temperature of the NiO film on the highly polarizable metal substrate is 390 K while that of the film on the poorly polarizable insulator substrate is below 40 K. This demonstrates that screening by highly polarizable media may point to a practical way towards designing strongly correlated oxide nanostructures with greatly improved magnetic properties.

cond-mat.mtrl-sci↗

arXiv2008

Atomic multiplet calculation of 3d_{5/2} -> 4f resonant x-ray diffraction from Ho metal

We compare for Ho metal the x-ray absorption spectrum and the resonant soft x-ray diffraction spectra obtained at the $3d_{5/2} \to 4f$ ($M_5$) resonance for the magnetic 1st and 2nd order diffraction peaks $(0,0,τ)$ and $(0,0,2τ)$ with the result of an atomic multiplet calculation. We find a good agreement between experiment and simulation giving evidence that this kind of simulation is well suited to quantitatively analyze resonant soft x-ray diffraction data from correlated electron systems.

cond-mat.str-el↗

arXiv2008

Resonant soft x-ray scattering from stepped surfaces of SrTiO3

We studied the resonant diffraction signal from stepped surfaces of SrTiO3 at the Ti 2p -> 3d (L2,3) resonance in comparison with x-ray absorption (XAS) and specular reflectivity data. The steps on the surface form an artificial superstructure suited as a model system for resonant soft x-ray diffraction. A small step density on the surface is sufficient to produce a well defined diffraction peak, showing the high sensitivity of the method. At larger incidence angles, the resonant diffraction spectrum from the steps on the surface resembles the spectrum for specular reflectivity. Both deviate from the XAS data in the relative peak intensities and positions of the peak maxima. We determined the optical parameters of the sample across the resonance and found that the differences between the XAS and scattering spectra reflect the different quantities probed in the different signals. When recorded at low incidence or detection angles, XAS and specular reflectivity spectra are distorted by the changes of the angle of total reflection with energy. Also the step peak spectra, though less affected, show an energy shift of the peak maxima in grazing incidence geometry.

cond-mat.str-el↗

arXiv2008

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.

cond-mat.str-el↗

arXiv2008

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.

cond-mat.str-el↗

arXiv2008

Strong spin-orbit coupling effects on the Fermi surface of Sr2RuO4 and Sr2RhO4

We present a first-principle study of spin-orbit coupling effects on the Fermi surface of Sr2RuO4 and Sr2RhO4. For nearly degenerate bands, spin-orbit coupling leads to a dramatic change of the Fermi surface with respect to non-relativistic calculations; as evidenced by the comparison with experiments on Sr2RhO4, it cannot be disregarded. For Sr2RuO4, the Fermi surface modifications are more subtle but equally dramatic in the detail: spin-orbit coupling induces a strong momentum dependence, normal to the RuO2 planes, for both orbital and spin character of the low-energy electronic states. These findings have profound implications for the understanding of unconventional superconductivity in Sr2RuO4.

cond-mat.str-el↗

arXiv2008

Magnetic coupling in highly-ordered NiO/Fe3O4(110): Ultrasharp magnetic interfaces vs. long-range magnetoelastic interactions

We present a laterally resolved X-ray magnetic dichroism study of the magnetic proximity effect in a highly ordered oxide system, i.e. NiO films on Fe3O4(110). We found that the magnetic interface shows an ultrasharp electronic, magnetic and structural transition from the ferrimagnet to the antiferromagnet. The monolayer which forms the interface reconstructs to NiFe2O4 and exhibits an enhanced Fe and Ni orbital moment, possibly caused by bonding anisotropy or electronic interaction between Fe and Ni cations. The absence of spin-flop coupling for this crystallographic orientation can be explained by a structurally uncompensated interface and additional magnetoelastic effects.

cond-mat.mtrl-sci↗

arXiv2007

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.

cond-mat.str-el↗

arXiv2007

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.

cond-mat.str-el↗

arXiv2007

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.

cond-mat.str-el↗

arXiv2007

Non-resonant inelastic x-ray scattering involving excitonic excitations

In a recent publication Larson \textit{et al.} reported remarkably clear $d$-$d$ excitations for NiO and CoO measured with x-ray energies well below the transition metal $K$ edge. In this letter we demonstrate that we can obtain an accurate quantitative description based on a local many body approach. We find that the magnitude of $\vec{q}$ can be tuned for maximum sensitivity for dipole, quadrupole, etc. excitations. We also find that the direction of $\vec{q}$ with respect to the crystal axes can be used as an equivalent to polarization similar to electron energy loss spectroscopy, allowing for a determination of the local symmetry of the initial and final state based on selection rules. This method is more generally applicable and combined with the high resolution available, could be a powerful tool for the study of local distortions and symmetries in transition metal compounds including also buried interfaces.

cond-mat.str-el↗