89 research outputs found
Transport, optical and electronic properties of the half metal CrO2
The electronic structure of CrO_2 is critically discussed in terms of the
relation of existing experimental data and well converged LSDA and GGA
calculations of the electronic structure and transport properties of this half
metal magnet, with a particular emphasis on optical properties. We find only
moderate manifestations of many body effects. Renormalization of the density of
states is not large and is in the typical for transition metals range. We find
substantial deviations from Drude behavior in the far-infrared optical
conductivity. These appear because of the unusually low energy of interband
optical transitions. The calculated mass renormalization is found to be rather
sensitive to the exchange-correlation functional used and varies from 10%
(LSDA) to 90% (GGA), using the latest specific heat data. We also find that
dressing of the electrons by spin fluctuations, because of their high energy,
renormalizes the interband optical transition at as high as 4 eV by about 20%.
Although we find no clear indications of strong correlations of the Hubbard
type, strong electron-magnon scattering related to the half metallic band
structure is present and this leads to a nontrivial temperature dependence of
the resistivity and some renormalization of the electron spectra.Comment: 9 Revtex 2 column pages, including 8 postscript figures. Two more
figures are included in the submission that are not embedded in the paper,
representing DOS and bandstructure of the paramagnetic CrO
Ground-state properties of rutile: electron-correlation effects
Electron-correlation effects on cohesive energy, lattice constant and bulk
compressibility of rutile are calculated using an ab-initio scheme. A
competition between the two groups of partially covalent Ti-O bonds is the
reason that the correlation energy does not change linearly with deviations
from the equilibrium geometry, but is dominated by quadratic terms instead. As
a consequence, the Hartree-Fock lattice constants are close to the experimental
ones, while the compressibility is strongly renormalized by electronic
correlations.Comment: 1 figure to appear in Phys. Rev.
Metastable precursors during the oxidation of the Ru(0001) surface
Using density-functional theory, we predict that the oxidation of the
Ru(0001) surface proceeds via the accumulation of sub-surface oxygen in
two-dimensional islands between the first and second substrate layer. This
leads locally to a decoupling of an O-Ru-O trilayer from the underlying metal.
Continued oxidation results in the formation and stacking of more of these
trilayers, which unfold into the RuO_2(110) rutile structure once a critical
film thickness is exceeded. Along this oxidation pathway, we identify various
metastable configurations. These are found to be rather close in energy,
indicating a likely lively dynamics between them at elevated temperatures,
which will affect the surface chemical and mechanical properties of the
material.Comment: 11 pages including 9 figures. Submitted to Phys. Rev. B. Related
publications can be found at http://www.fhi-berlin.mpg.de/th/paper.htm
Composition, structure and stability of RuO_2(110) as a function of oxygen pressure
Using density-functional theory (DFT) we calculate the Gibbs free energy to
determine the lowest-energy structure of a RuO_2(110) surface in thermodynamic
equilibrium with an oxygen-rich environment. The traditionally assumed
stoichiometric termination is only found to be favorable at low oxygen chemical
potentials, i.e. low pressures and/or high temperatures. At realistic O
pressure, the surface is predicted to contain additional terminal O atoms.
Although this O excess defines a so-called polar surface, we show that the
prevalent ionic model, that dismisses such terminations on electrostatic
grounds, is of little validity for RuO_2(110). Together with analogous results
obtained previously at the (0001) surface of corundum-structured oxides, these
findings on (110) rutile indicate that the stability of non-stoichiometric
terminations is a more general phenomenon on transition metal oxide surfaces.Comment: 12 pages including 5 figures. Submitted to Phys. Rev. B. Related
publications can be found at http://www.fhi-berlin.mpg.de/th/paper.htm
First-principles study of the ferroelastic phase transition in CaCl_2
First-principles density-functional calculations within the local-density
approximation and the pseudopotential approach are used to study and
characterize the ferroelastic phase transition in calcium chloride (CaCl_2). In
accord with experiment, the energy map of CaCl_2 has the typical features of a
pseudoproper ferroelastic with an optical instability as ultimate origin of the
phase transition. This unstable optic mode is close to a pure rigid unit mode
of the framework of chlorine atoms and has a negative Gruneisen parameter. The
ab-initio ground state agrees fairly well with the experimental low temperature
structure extrapolated at 0K. The calculated energy map around the ground state
is interpreted as an extrapolated Landau free-energy and is successfully used
to explain some of the observed thermal properties. Higher-order anharmonic
couplings between the strain and the unstable optic mode, proposed in previous
literature as important terms to explain the soft-phonon temperature behavior,
are shown to be irrelevant for this purpose. The LAPW method is shown to
reproduce the plane-wave results in CaCl_2 within the precision of the
calculations, and is used to analyze the relative stability of different phases
in CaCl_2 and the chemically similar compound SrCl_2.Comment: 9 pages, 6 figures, uses RevTeX
Composition and structure of the RuO2(110) surface in an O2 and CO environment: implications for the catalytic formation of CO2
The phase diagram of surface structures for the model catalyst RuO2(110) in
contact with a gas environment of O2 and CO is calculated by density-functional
theory and atomistic thermodynamics. Adsorption of the reactants is found to
depend crucially on temperature and partial pressures in the gas phase.
Assuming that a catalyst surface under steady-state operation conditions is
close to a constrained thermodynamic equilibrium, we are able to rationalize a
number of experimental findings on the CO oxidation over RuO2(110). We also
calculated reaction pathways and energy barriers. Based on the various results
the importance of phase coexistence conditions is emphasized as these will lead
to an enhanced dynamics at the catalyst surface. Such conditions may actuate an
additional, kinetically controlled reaction mechanism on RuO2(110).Comment: 12 pages including 8 figure files. Submitted to Phys. Rev. B. Related
publications can be found at http://www.fhi-berlin.mpg.de/th/paper.htm
Orbital character of O 2p unoccupied states near the Fermi level in CrO2
The orbital character, orientation, and magnetic polarization of the O 2
unoccupied states near the Fermi level () in CrO was determined using
polarization-dependent X-ray absorption spectroscopy (XAS) and X-ray magnetic
circular dichroism (XMCD) from high-quality, single-crystal films. A sharp peak
observed just above is excited only by the electric field vector () normal to the tetragonal -axis, characteristic of a narrow band
( 0.7 eV bandwidth) constituted from O 2 orbitals perpendicular to
(O 2) hybridized with Cr 3 states. By comparison
with band-structure and configuration-interaction (CI) cluster calculations our
results support a model of CrO as a half-metallic ferromagnet with large
exchange-splitting energy ( 3.0 eV) and
substantial correlation effects.Comment: 4 pages, 3 figures, accepted for publication in Phys. Rev. B Rapid
Com
First principles electronic structure of spinel LiCr2O4: A possible half-metal?
We have employed first-principles electronic structure calculations to
examine the hypothetical (but plausible) oxide spinel, LiCr2O4 with the d^{2.5}
electronic configuration. The cell (cubic) and internal (oxygen position)
structural parameters have been obtained for this compound through structural
relaxation in the first-principles framework. Within the one-electron band
picture, we find that LiCr2O4 is magnetic, and a candidate half-metal. The
electronic structure is substantially different from the closely related and
well known rutile half-metal CrO2. In particular, we find a smaller conduction
band width in the spinel compound, perhaps as a result of the distinct topology
of the spinel crystal structure, and the reduced oxidation state. The magnetism
and half-metallicity of LiCr2O4 has been mapped in the parameter space of its
cubic crystal structure. Comparisons with superconducting LiTi2O4 (d^{0.5}),
heavy-fermion LiV2O4 (d^{1.5}) and charge-ordering LiMn2O4 (d^{3.5}) suggest
the effectiveness of a nearly-rigid band picture involving simple shifts of the
position of E_F in these very different materials. Comparisons are also made
with the electronic structure of ZnV2O4 (d^{2}), a correlated insulator that
undergoes a structural and antiferromagnetic phase transition.Comment: 9 pages, 7 Figures, version as published in PR
Model selection based algorithm in neonatal Chest EIT
This paper presents a new method for selecting a patient specific forward model to compensate for anatomical variations in electrical impedance tomography (EIT) monitoring of neonates. The method uses a combination of shape sensors and absolute reconstruction. It takes advantage of a probabilistic approach which automatically selects the best estimated forward model fit from pre-stored library models. Absolute/static image reconstruction is performed as the core of the posterior probability calculations. The validity and reliability of the algorithm in detecting a suitable model in the presence of measurement noise is studied with simulated and measured data from 11 patients.
The paper also demonstrates the potential improvements on the clinical parameters extracted from EIT images by
considering a unique case study with a neonate patient undergoing computed tomography imaging as clinical indication prior to EIT monitoring. Two well-known image reconstruction techniques, namely GREIT and tSVD, are implemented to create the final tidal images. The impacts of appropriate model selection on the clinical extracted parameters such as center of ventilation and silent spaces are investigated.
The results show significant improvements to the final reconstructed images and more importantly to the clinical EIT parameters extracted from the images that are crucial for decision-making and further interventions
- âŠ