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R. Claessen

Publications and source records attributed to R. Claessen.

At least 37 records · Page 2Linked to original sources

Direct k-space mapping of the electronic structure in an oxide-oxide interface

The interface between LaAlO3 and SrTiO3 hosts a two-dimensional electron system of itinerant carriers, although both oxides are band insulators. Interface ferromagnetism coexisting with superconductivity has been found and attributed to local moments. Experimentally, it has been established that Ti 3d electrons are confined to the interface. Using soft x-ray angle-resolved resonant photoelectron spectroscopy we have directly mapped the interface states in k-space. Our data demonstrate a charge dichotomy. A mobile fraction contributes to Fermi surface sheets, whereas a localized portion at higher binding energies is tentatively attributed to electrons trapped by O-vacancies in the SrTiO3. While photovoltage effects in the polar LaAlO3 layers cannot be excluded, the apparent absence of surface-related Fermi surface sheets could also be fully reconciled in a recently proposed electronic reconstruction picture where the built-in potential in the LaAlO3 is compensated by surface O-vacancies serving also as charge reservoir.

cond-mat.str-el↗

Pressure dependence of the Verwey transition in magnetite: an infrared spectroscopic point of view

We investigated the electronic and vibrational properties of magnetite at temperatures from 300 K down to 10 K and for pressures up to 10 GPa by far-infrared reflectivity measurements. The Verwey transition is manifested by a drastic decrease of the overall reflectance and the splitting of the phonon modes as well as the activation of additional phonon modes. In the whole studied pressure range the down-shift of the overall reflectance spectrum saturates and the maximum number of phonon modes is reached at a critical temperature, which sets a lower bound for the Verwey transition temperature T$_{\mathrm{v}}$. Based on these optical results a pressure-temperature phase diagram for magnetite is proposed.

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Polaron physics and crossover transition in magnetite probed by pressure-dependent infrared spectroscopy

The optical properties of magnetite at room temperature were studied by infrared reflectivity measurements as a function of pressure up to 8 GPa. The optical conductivity spectrum consists of a Drude term, two sharp phonon modes, a far-infrared band at around 600 cm$^{-1}$, and a pronounced mid-infrared absorption band. With increasing pressure both absorption bands shift to lower frequencies and the phonon modes harden in a linear fashion. Based on the shape of the MIR band, the temperature dependence of the dc transport data, and the occurrence of the far-infrared band in the optical conductivity spectrum the polaronic coupling strength in magnetite at room temperature should be classified as intermediate. For the lower-energy phonon mode an abrupt increase of the linear pressure coefficient occurs at around 6 GPa, which could be attributed to minor alterations of the charge distribution among the different Fe sites.

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Structural Examination of Au/Ge(001) by Surface X-Ray Diffraction and Scanning Tunneling Microscopy

The one-dimensional reconstruction of Au/Ge(001) was investigated by means of autocorrelation functions from surface x-ray diffraction (SXRD) and scanning tunneling microscopy (STM). Interatomic distances found in the SXRD-Patterson map are substantiated by results from STM. The Au coverage, recently determined to be 3/4 of a monolayer of gold, together with SXRD leads to three non-equivalent positions for Au within the c(8x2) unit cell. Combined with structural information from STM topography and line profiling, two building blocks are identified: Au-Ge hetero-dimers within the top wire architecture and Au homo-dimers within the trenches. The incorporation of both components is discussed using density functional theory and model based Patterson maps by substituting Germanium atoms of the reconstructed Ge(001) surface.

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Symmetry-Breaking Phase Transition without Peierls Mechanism in Conducting Monoatomic Chains

The one-dimensional (1D) model system Au/Ge(001), consisting of linear chains of single atoms on a surface, is scrutinized for lattice instabilities predicted in the Peierls paradigm. By scanning tunneling microscopy and electron diffraction we reveal a second-order phase transition at 585 K. It leads to charge ordering with transversal and vertical displacements and complex interchain correlations. However, the structural phase transition is not accompanied by the electronic signatures of a charge density wave, thus precluding a Peierls instability as origin. Instead, this symmetry-breaking transition exhibits three-dimensional critical behavior. This reflects a dichotomy between the decoupled 1D electron system and the structural elements that interact via the substrate. Such substrate-mediated coupling between the wires thus appears to have been underestimated also in related chain systems.

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Photoemission of a doped Mott insulator: spectral weight transfer and qualitative Mott-Hubbard description

The spectral weight evolution of the low-dimensional Mott insulator TiOCl upon alkali-metal dosing has been studied by photoelectron spectroscopy. We observe a spectral weight transfer between the lower Hubbard band and an additional peak upon electron-doping, in line with quantitative expectations in the atomic limit for changing the number of singly and doubly occupied sites. This observation is an unconditional hallmark of correlated bands and has not been reported before. In contrast, the absence of a metallic quasiparticle peak can be traced back to a simple one-particle effect.

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Strictly One-Dimensional Electron System in Au Chains on Ge(001) Revealed By Photoelectron K-Space Mapping

Atomic nanowires formed by Au on Ge(001) are scrutinized for the band topology of the conduction electron system by k-resolved photoemission. Two metallic electron pockets are observed. Their Fermi surface sheets form straight lines without undulations perpendicular to the chains within experimental uncertainty. The electrons hence emerge as strictly confined to one dimension. Moreover, the system is stable against a Peierls distortion down to 10 K, lending itself for studies of the spectral function. Indications for unusually low spectral weight at the chemical potential are discussed.

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Two pressure-induced structural phase transitions in TiOCl

We studied the crystal structure of TiOCl up to pressures of $p$=25~GPa at room temperature by x-ray powder diffraction measurements. Two pressure-induced structural phase transitions are observed: At $p_{c1}$$\approx$15~GPa emerges an 2$a$$\times$2$b$$\times$$c$ superstructure with $b$-axis unique monoclinic symmetry (space group P2$_1$/$m$). At $p_{c2}$$\approx$22~GPa all lattice parameters of the monoclinic phase show a pronounced anomaly. A fraction of the sample persists in the ambient orthorhombic phase (space group $Pmmn$) over the whole pressure range.

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Heat conductivity of the spin-Peierls compounds TiOCl and TiOBr

We report experimental results on the heat conductivity κof the S=1/2 spin chain compounds TiOBr and TiOCl for temperatures 5K<T<300K and magnetic fields up to 14. Surprisingly, we find no evidence of a significant magnetic contribution to κ, which is in stark contrast to recent results on S=1/2 spin chain cuprates. Despite this unexpected result, the thus predominantly phononic heat conductivity of these spin-Peierls compounds exhibits a very unusual behavior. In particular, we observe strong anomalies at the phase transitions Tc1 and Tc2. Moreover, we find an overall but anisotropic suppression of κin the intermediate phase which extends even to temperatures higher than Tc2. An external magnetic field causes a slight downshift of the transition at Tc1 and enhances the suppression of κup to Tc2. We interprete our findings in terms of strong spin-phonon coupling and phonon scattering arising from spin-driven lattice distortions.

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Epitaxial growth of Fe3O4 thin films on ZnO and MgO substrates

Magnetite thin fims have been grown epitaxially on ZnO and MgO substrates using molecular beam epitaxy. The film quality was found to be strongly dependent on the oxygen partial pressure during growth. Structural, electronic, and magnetic properties were analyzed utilizing Low Energy Electron Diffraction (LEED), HArd X-ray PhotoElectron Spectroscopy (HAXPES), Magneto Optical Kerr Effect (MOKE), and X-ray Magnetic Circular Dichroism (XMCD). Diffraction patterns show clear indication for growth in the (111) direction on ZnO. Vertical structure analysis by HAXPES depth profiling revealed uniform magnetite thin films on both type of substrates. Both, MOKE and XMCD measurements show in-plane easy magnetization with a reduced magnetic moment in case of the films on ZnO.

cond-mat.mtrl-sci↗

Electronic structure of the two-dimensional Heisenberg antiferromagnet VOCl: a multi-orbital Mott insulator

We have studied the electronic structure of the two-dimensional Heisenberg antiferromagnet VOCl using photoemission spectroscopy and density functional theory including local Coulomb repulsion. From calculated exchange integrals and the observed energy dispersions we argue that the degree of one-dimensionality regarding both the magnetic and electronic properties is noticeably reduced compared to the isostructural compounds TiOCl and TiOBr. Also, our analysis provides conclusive justification to classify VOCl as a multi-orbital Mott insulator. In contrast to the titanium based compounds density functional theory here gives a better description of the electronic structure. However, a quantitative account of the low-energy features and detailed line shapes calls for further investigations including dynamical and spatial correlations.

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Momentum-resolved single-particle spectral function for TiOCl from a combination of density functional and variational cluster calculations

We present results for the momentum-resolved single-particle spectral function of the low-dimensional system TiOCl in the insulating state, obtained by a combination of ab initio Density Functional Theory (DFT) and Variational Cluster (VCA) calculations. This approach allows to combine a realistic band structure and a thorough treatment of the strong correlations. We show that it is important to include a realistic two-dimensional band structure of TiOCl into the effective strongly-correlated models in order to explain the spectral weight behavior seen in angle-resolved photoemission (ARPES) experiments. In particular, we observe that the effect of the interchain couplings is a considerable redistribution of the spectral weight around the Gamma point from higher to lower binding energies as compared to a purely one-dimensional model treatment. Hence, our results support a description of TiOCl as a two-dimensional compound with strong anisotropy and also set a benchmark on the spectral features of correlated coupled-chain systems.

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Self-organized atomic nanowires of noble metals on Ge(001): atomic structure and electronic properties

Atomic structures of quasi-one-dimensional (1D) character can be grown on semiconductor substrates by metal adsorption. Significant progress concerning study of their 1D character has been achieved recently by condensing noble metal atoms on the Ge(001) surface. In particular, Pt and Au yield high quality reconstructions with low defect densities. We reported on the self-organized growth and the long-range order achieved, and present data from scanning tunneling microscopy (STM) on the structural components. For Pt/Ge(001), we find hot substrate growth is the preferred method for self-organization. Despite various dimerized bonds, these atomic wires exhibit metallic conduction at room temperature, as documented by low-bias STM. For the recently discovered Au/Ge(001) nanowires, we have developed a deposition technique that allows complete substrate coverage. The Au nanowires are extremely well separated spatially, exhibit a continuous 1D charge density, and are of solid metallic conductance. In this review we present structural details for both types of nanowires, and discuss similarities and differences. A perspective is given for their potential to host a one-dimensional electron system. The ability to condense different noble metal nanowires demonstrates how atomic control of the structure affects the electronic properties.

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Profiling the interface electron gas of LaAlO3/SrTiO3 heterostructures by hard X-ray photoelectron spectroscopy

The conducting interface of LaAlO$_3$/SrTiO$_3$ heterostructures has been studied by hard X-ray photoelectron spectroscopy. From the Ti~2$p$ signal and its angle-dependence we derive that the thickness of the electron gas is much smaller than the probing depth of 4 nm and that the carrier densities vary with increasing number of LaAlO$_3$ overlayers. Our results point to an electronic reconstruction in the LaAlO$_3$ overlayer as the driving mechanism for the conducting interface and corroborate the recent interpretation of the superconducting ground state as being of the Berezinskii-Kosterlitz-Thouless type.

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Renormalization of Bulk Magnetic Electron States at High Binding Energies

The quasiparticle dynamics of electrons in a magnetically ordered state is investigated by high-resolution angle-resolved photoemission of Ni(110) at 10 K. The self-energy is extracted for high binding energies reaching up to 500 meV, using a Gutzwiller calculation as a reference frame for correlated quasiparticles. Significant deviations exist in the 300 meV range, as identified on magnetic bulk bands for the first time. The discrepancy is strikingly well described by a self-energy model assuming interactions with spin excitations. Implications relating to different electron-electron correlation regimes are discussed.

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Probing the interface of Fe3O4/GaAs thin films by hard x-ray photoelectron spectroscopy

Magnetite (Fe3O4) thin films on GaAs have been studied with HArd X-ray PhotoElectron Spectroscopy (HAXPES) and low-energy electron diffraction. Films prepared under different growth conditions are compared with respect to stoichiometry, oxidation, and chemical nature. Employing the considerably enhanced probing depth of HAXPES as compared to conventional x-ray photoelectron spectroscopy (XPS) allows us to investigate the chemical state of the film-substrate interfaces. The degree of oxidation and intermixing at the interface are dependent on the applied growth conditions; in particular, we found that metallic Fe, As2O3, and Ga2O3 exist at the interface. These interface phases might be detrimental for spin injection from magnetite into GaAs.

cond-mat.mtrl-sci↗

New Model System for a One-Dimensional Electron Liquid: Self-Organized Atomic Gold Chains on Ge(001)

Unique electronic properties of self-organized Au atom chains on Ge(001) in novel c(8x2) long-range order are revealed by scanning tunneling microscopy. Along the nanowires an exceptionally narrow conduction path exists which is virtually decoupled from the substrate. It is laterally confined to the ultimate limit of single atom dimension, and is strictly separated from its neighbors, as not previously reported. The resulting tunneling conductivity shows a dramatic inhomogeneity of two orders of magnitude. The atom chains thus represent an outstandingly close approach to a one-dimensional electron liquid.

cond-mat.str-el↗

Mott-Hubbard gap closure and structural phase transition in the oxyhalides TiOBr and TiOCl under pressure

Pressure-dependent transmittance and reflectance spectra of TiOBr and TiOCl single crystals at room temperature suggest the closure of the Mott-Hubbard gap, i.e., the gap is filled with additional electronic states extending down to the far-infrared range. According to pressure-dependent x-ray powder diffraction data the gap closure coincides with a structural phase transition. The transition in TiOBr occurs at slightly lower pressure ($p$=14 GPa) compared to TiOCl ($p$=16 GPa) under hydrostatic conditions, which is discussed in terms of the chemical pressure effect. The results of pressure-dependent transmittance measurements on TiOBr at low temperatures reveal similar effects at 23 K, where the compound is in the spin-Peierls phase at ambient pressure.

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