arXiv subjects

H. H. Hsieh

Publications and source records attributed to H. H. Hsieh.

33 records · Page 2Linked to original sources

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

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↗

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↗

arXiv2006

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.

cond-mat.str-el↗

arXiv2006

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.

cond-mat.str-el↗

arXiv2006

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.

cond-mat.str-el↗

arXiv2005

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.

cond-mat.str-el↗

arXiv2005

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.

cond-mat.str-el↗

arXiv2005

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.

cond-mat.str-el↗

arXiv2004

A Universal Intrinsic Scale of Hole Concentration for High-Tc Cuprates

We have measured thermoelectric power (TEP) as a function of hole concentration per CuO2 layer, Ppl, in Y1-xCaxBa2Cu3O6 (Ppl = x/2) with no oxygen in the Cu-O chain layer. The room-temperature TEP as a function of Ppl, S290(Ppl), of Y1-xCaxBa2Cu3O6 behaves identically to that of La2-zSrzCuO4 (Ppl = z). We argue that S290(Ppl) represents a measure of the intrinsic equilibrium electronic states of doped holes and, therefore, can be used as a common scale for the carrier concentrations of layered cuprates. We shows that the Ppl determined by this new universal scale is consistent with both hole concentration microscopically determined by NQR and the hole concentration macroscopically determined by the Cu valency. We find two characteristic scaling temperatures, TS* and TS2*, in the TEP vs. temperature curves that change systematically with doping. Based on the universal scale, we uncover a universal phase diagram in which almost all the experimentally determined pseudogap temperatures as a function of Ppl fall on two common curves; upper pseudogap temperature defined by the TS* versus Ppl curve and lower pseudogap temperature defined by the TS2* versus Ppl curve. We find that while pseudogaps are intrinsic properties of doped holes of a single CuO2 layer for all high-Tc cuprates, Tc depends on the number of layers, therefore the inter-layer coupling, in each individual system.

cond-mat.supr-con↗

arXiv2004

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.

cond-mat.str-el↗

arXiv2003

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.

cond-mat.str-el↗

arXiv2003

A different look at the spin state of Co$^{3+}$ ions in CoO$_{5}$ pyramidal coordination

Using soft-x-ray absorption spectroscopy at the Co-$L_{2,3}$ and O-$K$ edges, we demonstrate that the Co$^{3+}$ ions with the CoO$_{5}$ pyramidal coordination in the layered Sr$_2$CoO$_3$Cl 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 re-examination of the modeling for the complex and fascinating properties of these new materials.

cond-mat.str-el↗

arXiv2003

Growth and properties of strained VOx thin films with controlled stoichiometry

We have succeeded in growing epitaxial films of rocksalt VOx on MgO(001) substrates. The oxygen content as a function of oxygen flux was determined using 18O2-RBS and the vanadium valence using XAS. The upper and lower stoichiometry limits found are similar to the ones known for bulk material (0.8<x<1.3). From the RHEED oscillation period a large number of vacancies for both vanadium and oxygen were deduced, i.e. ~16% for stoichiometric VO. These numbers are, surprisingly, very similar to those for bulk material and consequently quite strain-insensitive. XAS measurements reveal that the vacancies give rise to strong low symmetry ligand fields to be present. The electrical conductivity of the films is much lower than the conductivity of bulk samples which we attribute to a decrease in the direct overlap between t2g orbitals in the coherently strained layers. The temperature dependence of the conductivity is consistent with a variable range hopping mechanism.

cond-mat.str-el↗

arXiv2002

Direct observation of electron doping in La0.7Ce0.3MnO3 using x-ray absorption spectroscopy

We report on a X-ray absorption spectroscopic (XAS) study on a thin film of La0.7Ce0.3MnO3, a manganite which was previously only speculated to be an electron doped system. The measurements clearly show that the cerium is in the Ce(IV) valence state and that the manganese is present in a mixture of Mn2+ and Mn3+ valence states. These data unambiguously demonstrate that La0.7Ce0.3MnO3 is an electron doped colossal magnetoresistive manganite, a finding that may open up new opportunities both for device applications as well as for further basic research towards a better modelling of the colossal magnetoresistance phenomenon in these materials.

cond-mat.str-el↗