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L H Tjeng

Publications and source records attributed to L H Tjeng.

15 recordsLinked to original sources
PubMed2006

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.

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PubMed2006

Transfer of spectral weight and symmetry across the metal-insulator transition in VO(2).

We present a detailed study of the valence and conduction bands of VO2 across the metal-insulator transition using bulk-sensitive photoelectron and O K x-ray absorption spectroscopies. We observe a giant transfer of spectral weight with distinct features that require an explanation which goes beyond the Peierls transition model as well as the standard single-band Hubbard model. Analysis of the symmetry and energies of the bands reveals the decisive role of the V 3d orbital degrees of freedom. Comparison to recent realistic many body calculations shows that much of the k dependence of the self-energy correction can be cast within a dimer model.

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PubMed2006

Orbitally driven spin-singlet dimerization in S=1 La4Ru2O10.

Using x-ray absorption spectroscopy at the Ru-L2,3 edge we reveal that the Ru4+ 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 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 La4Ru2O10 appears to be a novel material in which the orbital physics drives the formation of spin-singlet dimers in a quasi-two-dimensional S=1 system.

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PubMed2005

Orbital-assisted metal-insulator transition in VO2.

We found direct experimental evidence for an orbital switching in the V 3d states across the metal-insulator transition in VO2. We have used soft-x-ray absorption spectroscopy at the V L2,3 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 bandwidths are reduced, that the system becomes more one 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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PubMed2005

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 L2,3 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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PubMed2005

Nature of magnetism in Ca3Co2O6.

We find using local spin density approximation + Hubbard U band structure calculations that the novel one-dimensional cobaltate Ca3Co2O6 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 d2 orbital for the unusually coordinated trigonal Co, producing a giant orbital moment (1.57 microB). 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 microB per oxygen, for the exchange interactions is discussed.

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PubMed2005

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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PubMed2005

Determination of the orbital moment and crystal-field splitting in LaTiO3.

Utilizing a sum rule in a spin-resolved photoelectron spectroscopic experiment with circularly polarized light, we show that the orbital moment in LaTiO3 is strongly reduced from its ionic value, both below and above the Ne el temperature. Using Ti L2,3 x-ray absorption spectroscopy as a local probe, we found that the crystal-field splitting in the t2g subshell is about 0.12-0.30 eV. This large splitting does not facilitate the formation of an orbital liquid.

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PubMed2004

Different look at the spin state of Co(3+) ions in a CoO(5) pyramidal coordination.

Using soft-x-ray absorption spectroscopy at the Co L(2,3) and O K edges, we demonstrate that the Co3+ ions with the CoO5 pyramidal coordination in the layered Sr2CoO3Cl compound are unambiguously in the high spin state. Our result questions the reliability of the spin state assignments made so far for the recently synthesized layered cobalt perovskites and calls for a reexamination of the modeling for the complex and fascinating properties of these new materials.

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PubMed2003

Crossing the gap from p- to n-type doping: nature of the states near the chemical potential in La(2)-(x)Sr(x)CuO(4) and Nd(2-x)Ce(x)CuO(4-delta).

We report on an x-ray absorption and resonant photoemission study on single crystals of the high-T(c) cuprates La2-xSrxCuO4 and Nd(2-x)Ce(x)CuO(4-delta). Using an intrinsic energy reference, we find that the chemical potential of La2-xSrxCuO4 lies near the top of the La2CuO4 valence band whereas in Nd(2-x)Ce(x)CuO(4-delta) it is situated near the bottom of the Nd2CuO4 conduction band. The data clearly establish that the introduction of Ce in Nd2CuO4 results in electrons being doped into the CuO2 planes. We infer that the states closest to the chemical potential have a Cu 3d(10) singlet origin in Nd(2-x)Ce(x)CuO(4-delta) and a 3d(9)L singlet origin in La2-xSrxCuO4.

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PubMed2002

Exchange splitting and charge carrier spin polarization in EuO.

High quality thin films of the ferromagnetic semiconductor EuO have been prepared and were studied using a new form of spin-resolved spectroscopy. We observed large changes in the electronic structure across the Curie and metal-insulator transition temperature. We found that these are caused by the exchange splitting of the conduction band in the ferromagnetic state, which is as large as 0.6 eV. We also present strong evidence that the bottom of the conduction band consists mainly of majority spins. This implies that doped charge carriers in EuO are practically fully spin polarized.

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PubMed2001

Detection of Zhang-Rice singlets using spin-polarized photoemission.

From a spin-resolved photoemission study on the Bi(2)Sr(2)CaCu(2)O(8+delta) superconductor, we show experimentally that the first ionization state is of nearly pure singlet character. This is true both above and below the superconducting transition and in the presence of doping and band formation. This provides direct support for the existence and stability of Zhang-Rice singlets in high-temperature superconductors, justifying the ansatz of single-band models. Moreover, we establish this technique as an important probe for a wide range of cuprates and strongly correlated materials.

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PubMed2001

Spin-orbit coupling in the Mott insulator Ca(2)RuO(4).

O 1s x-ray absorption study of the Mott insulator Ca(2)RuO(4) shows that the orbital population of the 4d t(2g) band dramatically changes with temperature. In addition, spin-resolved circularly polarized photoemission study of Ca(2)RuO(4) shows that a substantial orbital angular momentum is induced in the Ru 4d t(2g) band. Based on the experimental results and model Hartree-Fock calculations, we argue that the cooperation between the strong spin-orbit coupling in the Ru 4d t(2g) band and the small distortion of the RuO(6) octahedra causes the interesting changeover of the spin and orbital anisotropy as a function of temperature.

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PubMed1993

Soft x-ray magnetic circular dichroism: a probe for studying paramagnetic bioinorganic systems.

Soft x-ray magnetic circular dichroism was used to study a paramagnetic bioinogranic system. We measured the Fe L edges of Pyrococcus furiosus rubredoxin, using circularly polarized synchrotron radiation, a split-coil super-conducting magnet, low sample temperatures, and fluorescence detection. The observed dichroism effect is strong (30%) and in general agreement with the calculation. The method is element- and oxidation state-specific, and the data can be interpreted by established theoretical procedures. Soft x-ray magnetic circular dichroism demonstrates enormous potential as a probe for studying paramagnetic systems in biology, chemistry, and material science.

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