181 research outputs found
Electronic properties of graphene and graphene nanoribbons with "pseudo-Rashba" spin-orbit coupling
We discuss the electronic properties of graphene and graphene nanoribbons
including "pseudo-Rashba" spin-orbit coupling. After summarizing the bulk
properties, we first analyze the scattering behavior close to an infinite mass
and zigzag boundary. For low energies, we observe strong deviations from the
usual spin-conserving behavior at high energies such as reflection acting as
spin polarizer or switch. This results in a spin polarization along the
direction of the boundary due to the appearance of evanescent modes in the case
of non-equilibrium or when there is no coherence between the two one-particle
branches. We then discuss the spin and density distribution of graphene
nanoribbons.Comment: 18 pages, 9 figures; section on nanoribbons adde
Structure optimization effects on the electronic properties of BiSrCaCuO
We present detailed first-principles calculations for the normal state
electronic properties of the high T superconductor
BiSrCaCuO, by means of the linearized augmented plane wave
(LAPW) method within the framework of density functional theory (DFT). As a
first step, the body centered tetragonal (BCT) cell has been adopted, and
optimized regarding its volume, ratio and internal atomic positions by
total energy and force minimizations. The full optimization of the BCT cell
leads to small but visible changes in the topology of the Fermi surface,
rounding the shape of CuO barrels, and causing both the BiO bands,
responsible for the pockets near the \textit{\=M} 2D symmetry point, to dip
below the Fermi level. We have then studied the influence of the distortions in
the BiO plane observed in nature by means of a
orthorhombic cell (AD-ORTH) with space group. Contrary to what has been
observed for the Bi-2201 compound, we find that for Bi-2212 the distortion does
not sensibly shift the BiO bands which retain their metallic character. As a
severe test for the considered structures we present Raman-active phonon
frequencies () and eigenvectors calculated within the frozen-phonon
approximation. Focussing on the totally symmetric A modes, we observe
that for a reliable attribution of the peaks observed in Raman experiments,
both - and a-axis vibrations must be taken into account, the latter being
activated by the in-plane orthorhombic distortion.Comment: 22 pages, 4 figure
Ab-initio prediction of the electronic and optical excitations in polythiophene: isolated chains versus bulk polymer
We calculate the electronic and optical excitations of polythiophene using
the GW approximation for the electronic self-energy, and include excitonic
effects by solving the electron-hole Bethe-Salpeter equation. Two different
situations are studied: excitations on isolated chains and excitations on
chains in crystalline polythiophene. The dielectric tensor for the crystalline
situation is obtained by modeling the polymer chains as polarizable line
objects, with a long-wavelength polarizability tensor obtained from the
ab-initio polarizability function of the isolated chain. With this model
dielectric tensor we construct a screened interaction for the crystalline case,
including both intra- and interchain screening. In the crystalline situation
both the quasi-particle band gap and the exciton binding energies are
drastically reduced in comparison with the isolated chain. However, the optical
gap is hardly affected. We expect this result to be relevant for conjugated
polymers in general.Comment: 15 pages including 4 figures; to appear in Phys. Rev. B, 6/15/200
First-Principles Calculations of Hyperfine Interactions in La_2CuO_4
We present the results of first-principles cluster calculations of the
electronic structure of La_2CuO_4. Several clusters containing up to nine
copper atoms embedded in a background potential were investigated.
Spin-polarized calculations were performed both at the Hartree-Fock level and
with density functional methods with generalized gradient corrections to the
local density approximation. The distinct results for the electronic structure
obtained with these two methods are discussed. The dependence of the
electric-field gradients at the Cu and the O sites on the cluster size is
studied and the results are compared to experiments. The magnetic hyperfine
coupling parameters are carefully examined. Special attention is given to a
quantitative determination of on-site and transferred hyperfine fields. We
provide a detailed analysis that compares the hyperfine fields obtained for
various cluster sizes with results from additional calculations of spin states
with different multiplicities. From this we conclude that hyperfine couplings
are mainly transferred from nearest neighbor Cu^{2+} ions and that
contributions from further distant neighbors are marginal. The mechanisms
giving rise to transfer of spin density are worked out. Assuming conventional
values for the spin-orbit coupling, the total calculated hyperfine interaction
parameters are compared to informations from experiments.Comment: 23 pages, 9 figure
Spin, charge and orbital ordering in ferrimagnetic insulator YBaMnO
The oxygen-deficient (double) perovskite YBaMnO, containing
corner-linked MnO square pyramids, is found to exhibit ferrimagnetic
ordering in its ground state. In the present work we report
generalized-gradient-corrected, relativistic first-principles full-potential
density-functional calculations performed on YBaMnO in the nonmagnetic,
ferromagnetic and ferrimagnetic states. The charge, orbital and spin orderings
are explained with site-, angular momentum- and orbital-projected density of
states, charge-density plots, electronic structure and total energy studies.
YBaMnO is found to stabilize in a G-type ferrimagnetic state in
accordance with experimental results. The experimentally observed insulating
behavior appears only when we include ferrimagnetic ordering in our
calculation. We observed significant optical anisotropy in this material
originating from the combined effect of ferrimagnetic ordering and crystal
field splitting. In order to gain knowledge about the presence of different
valence states for Mn in YBaMnO we have calculated -edge x-ray
absorption near-edge spectra for the Mn and O atoms. The presence of the
different valence states for Mn is clearly established from the x-ray
absorption near-edge spectra, hyperfine field parameters and the magnetic
properties study. Among the experimentally proposed structures, the recently
reported description based on 4/ is found to represent the stable
structure
Response theory for time-resolved second-harmonic generation and two-photon photoemission
A unified response theory for the time-resolved nonlinear light generation
and two-photon photoemission (2PPE) from metal surfaces is presented. The
theory allows to describe the dependence of the nonlinear optical response and
the photoelectron yield, respectively, on the time dependence of the exciting
light field. Quantum-mechanical interference effects affect the results
significantly. Contributions to 2PPE due to the optical nonlinearity of the
surface region are derived and shown to be relevant close to a plasmon
resonance. The interplay between pulse shape, relaxation times of excited
electrons, and band structure is analyzed directly in the time domain. While
our theory works for arbitrary pulse shapes, we mainly focus on the case of two
pulses of the same mean frequency. Difficulties in extracting relaxation rates
from pump-probe experiments are discussed, for example due to the effect of
detuning of intermediate states on the interference. The theory also allows to
determine the range of validity of the optical Bloch equations and of
semiclassical rate equations, respectively. Finally, we discuss how collective
plasma excitations affect the nonlinear optical response and 2PPE.Comment: 27 pages, including 11 figures, version as publishe
Linear and Second-order Optical Response of the III-V Mono-layer Superlattices
We report the first fully self-consistent calculations of the nonlinear
optical properties of superlattices. The materials investigated are mono-layer
superlattices with GaP grown on the the top of InP, AlP and GaAs (110)
substrates. We use the full-potential linearized augmented plane wave method
within the generalized gradient approximation to obtain the frequency dependent
dielectric tensor and the second-harmonic-generation susceptibility. The effect
of lattice relaxations on the linear optical properties are studied. Our
calculations show that the major anisotropy in the optical properties is the
result of strain in GaP. This anisotropy is maximum for the superlattice with
maximum lattice mismatch between the constituent materials. In order to
differentiate the superlattice features from the bulk-like transitions an
improvement over the existing effective medium model is proposed. The
superlattice features are found to be more pronounced for the second-order than
the linear optical response indicating the need for full supercell calculations
in determining the correct second-order response.Comment: 9 pages, 4 figures, submitted to Phy. Rev.
Down regulation of E-Cadherin (ECAD) - a predictor for occult metastatic disease in sentinel node biopsy of early squamous cell carcinomas of the oral cavity and oropharynx
<p>Abstract</p> <p>Background</p> <p>Prognostic factors in predicting occult lymph node metastasis in patients with head and neck squamous-cell carcinoma (HNSCC) are necessary to improve the results of the sentinel lymph node procedure in this tumour type. The E-Cadherin glycoprotein is an intercellular adhesion molecule in epithelial cells, which plays an important role in establishing and maintaining intercellular connections.</p> <p>Objectives</p> <p>To determine the value of the molecular marker E-Cadherin in predicting regional metastatic disease.</p> <p>Methods</p> <p>E-Cadherin expression in tumour tissue of 120 patients with HNSCC of the oral cavity and oropharynx were evaluated using the tissue microarray technique. 110 tumours were located in the oral cavity (91.7%; mostly tongue), 10 tumours in the oropharynx (8.3%). Intensity of E-Cadherin expression was quantified by the Intensity Reactivity Score (IRS). These results were correlated with the lymph node status of biopsied sentinel lymph nodes. Univariate and multivariate analysis was used to determine statistical significance.</p> <p>Results</p> <p>pT-stage, gender, tumour side and location did not correlate with lymph node metastasis. Differentiation grade (<it>p </it>= 0.018) and down regulation of E-Cadherin expression significantly correlate with positive lymph node status (<it>p </it>= 0.005) in univariate and multivariate analysis.</p> <p>Conclusion</p> <p>These data suggest that loss of E-cadherin expression is associated with increased lymhogeneous metastasis of HNSCC. E-cadherin immunohistochemistry may be used as a predictor for lymph node metastasis in squamous cell carcinoma of the oral cavity and oropharynx.</p> <p><b>Level of evidence: 2b</b></p
Resolution-of-identity approach to Hartree-Fock, hybrid density functionals, RPA, MP2, and \textit{GW} with numeric atom-centered orbital basis functions
Efficient implementations of electronic structure methods are essential for
first-principles modeling of molecules and solids. We here present a
particularly efficient common framework for methods beyond semilocal
density-functional theory, including Hartree-Fock (HF), hybrid density
functionals, random-phase approximation (RPA), second-order M{\o}ller-Plesset
perturbation theory (MP2), and the method. This computational framework
allows us to use compact and accurate numeric atom-centered orbitals (popular
in many implementations of semilocal density-functional theory) as basis
functions. The essence of our framework is to employ the "resolution of
identity (RI)" technique to facilitate the treatment of both the two-electron
Coulomb repulsion integrals (required in all these approaches) as well as the
linear density-response function (required for RPA and ). This is possible
because these quantities can be expressed in terms of products of
single-particle basis functions, which can in turn be expanded in a set of
auxiliary basis functions (ABFs). The construction of ABFs lies at the heart of
the RI technique, and here we propose a simple prescription for constructing
the ABFs which can be applied regardless of whether the underlying radial
functions have a specific analytical shape (e.g., Gaussian) or are numerically
tabulated. We demonstrate the accuracy of our RI implementation for Gaussian
and NAO basis functions, as well as the convergence behavior of our NAO basis
sets for the above-mentioned methods. Benchmark results are presented for the
ionization energies of 50 selected atoms and molecules from the G2 ion test set
as obtained with and MP2 self-energy methods, and the G2-I atomization
energies as well as the S22 molecular interaction energies as obtained with the
RPA method.Comment: 58 pages, 15 figures, and 7 table
Tuning intermolecular interactions in di-octyl substituted polyfluorene via hydrostatic pressure
Polyfluorenes (PFs) represent a unique class of poly para-phenylene based
blue-emitting polymers with intriguing structure-property relationships. Slight
variations in the choice of functionalizing side chains result in dramatic
differences in the inter- and intra-chain structures in PFs. We present
photoluminescence (PL) and Raman scattering studies of bulk samples and thin
films of dioctyl-substituted PF (PF8) under hydrostatic pressure. The bulk
sample was further thermally annealed at 1.9 GPa. The PL vibronics of the as-is
sample red-shift at an average rate of 26 meV/GPa. The thermally annealed
sample is characterized by at least two phase transitions at 1.1 GPa and 4.2
GPa, each of which has a different pressure coefficient for PL vibronics. The
Huang-Rhys factor, a measure of the electron-phonon interaction, is found to
increase with increasing pressures signaling a higher geometric relaxation of
the electronic states. The Raman peaks harden with increasing pressures; the
intra-ring C-C stretch frequency at 1600 cm has a pressure coefficient
of 7.2 cm/GPa and exhibits asymmetric line shapes at higher pressures,
characteristic of a strong electron-phonon interaction. The optical properties
of PF8 under high pressure are further contrasted with those of a branched side
chain substituted PF.Comment: 22 pages, 10 figure
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