425 research outputs found
Renormalization of the quasiparticle hopping integrals by spin interactions in layered copper oxides
Holes doped within the square CuO2 network specific to the cuprate
superconducting materials have oxygen 2p character. We investigate the basic
properties of such oxygen holes by wavefunction-based quantum chemical
calculations on large embedded clusters. We find that a 2p hole induces
ferromagnetic correlations among the nearest-neighbor Cu 3d spins. When moving
through the antiferromagnetic background the hole must bring along this spin
polarization cloud at nearby Cu sites, which gives rise to a substantial
reduction of the effective hopping parameters. Such interactions can explain
the relatively low values inferred for the effective hoppings by fitting the
angle-resolved photoemission data. The effect of the background
antiferromagnetic couplings of renormalizing the effective nearest-neighbor
hopping is also confirmed by density-matrix renormalization-group model
Hamiltonian calculations for chains and ladders of CuO4 plaquettes
Orbital Localization and Delocalization Effects in the U 5f^2 Configuration: Impurity Problem
Anderson models, based on quantum chemical studies of the molecule of
U(C_8H_8)_2, are applied to investigate the problem of an U impurity in a
metal. The special point here is that the U 5f-orbitals are divided into two
subsets: an almost completely localized set and a considerably delocalized one.
Due to the crystal field, both localized and delocalized U 5f-orbitals affect
the low-energy physics. A numerical renormalization group study shows that
every fixed point is characterized by a residual local spin and a phase shift.
The latter changes between 0 and \pi/2, which indicates the competition between
two different fixed points. Such a competition between the different local
spins at the fixed points reflects itself in the impurity magnetic
susceptibility at high temperatures. These different features cannot be
obtained if the special characters of U 5f-orbitals are neglected.Comment: 4 pages, REVTeX, email to [email protected]
A multideterminant assessment of mean field methods for the description of electron transfer in the weak coupling regime
Multideterminant calculations have been performed on model systems to
emphasize the role of many-body effects in the general description of charge
quantization experiments. We show numerically and derive analytically that a
closed-shell ansatz, the usual ingredient of mean-field methods, does not
properly describe the step-like electron transfer characteristic in weakly
coupled systems. With the multideterminant results as a benchmark, we have
evaluated the performance of common ab initio mean field techniques, such as
Hartree Fock (HF) and Density Functional Theory (DFT) with local and hybrid
exchange correlation functionals, with a special focus on spin-polarization
effects. For HF and hybrid DFT, a qualitatively correct open-shell solution
with distinct steps in the electron transfer behaviour can be obtained with a
spin-unrestricted (i.e., spin-polarized) ansatz though this solution differs
quantitatively from the multideterminant reference. We also discuss the
relationship between the electronic eigenvalue gap and the onset of charge
transfer for both HF and DFT and relate our findings to recently proposed
practical schemes for calculating the addition energies in the Coulomb blockade
regime for single molecule junctions from closed-shell DFT within the local
density approximation
Wave-function-based approach to quasiparticle bands: new insight into the electronic structure of c-ZnS
Ab initio wave-function-based methods are employed for the study of
quasiparticle energy bands of zinc-blende ZnS, with focus on the Zn 3d
"semicore" states. The relative energies of these states with respect to the
top of the S 3p valence bands appear to be poorly described as compared to
experimental values not only within the local density approximation (LDA), but
also when many-body corrections within the GW approximation are applied to the
LDA or LDA+U mean-field solutions [T. Miyake, P. Zhang, M. L. Cohen, and S. G.
Louie, Phys. Rev. B 74, 245213 (2006)]. In the present study, we show that for
the accurate description of the Zn 3d states a correlation treatment based on
wave function methods is needed. Our study rests on a local Hamiltonian
approach which rigorously describes the short-range polarization and charge
redistribution effects around an extra hole or electron placed into the valence
respective conduction bands of semiconductors and insulators. The method also
facilitates the computation of electron correlation effects beyond relaxation
and polarization. The electron correlation treatment is performed on finite
clusters cut off the infinite system. The formalism makes use of localized
Wannier functions and embedding potentials derived explicitly from prior
periodic Hartree-Fock calculations. The on-site and nearest-neighbor charge
relaxation lead to corrections of several eV to the Hartree-Fock band energies
and gap. Corrections due to long-range polarization are of the order of 1.0 eV.
The dispersion of the Hartree-Fock bands is only little affected by electron
correlations. We find the Zn 3d "semicore" states to lie about 9.0 eV below the
top of the S 3p valence bands, in very good agreement with values from
valence-band x-ray photoemission.Comment: 44 pages, 8 figures, submitted to Phys. Rev.
Superconductivity, magnetic order, and quadrupolar order in the filled skutterudite system PrNdOsSb
Superconductivity, magnetic order, and quadrupolar order have been
investigated in the filled skutterudite system
PrNdOsSb as a function of composition in magnetic
fields up to 9 tesla and at temperatures between 50 mK and 10 K. Electrical
resistivity measurements indicate that the high field ordered phase (HFOP),
which has been identified with antiferroquadruoplar order, persists to
0.5. The superconducting critical temperature of PrOsSb
is depressed linearly with Nd concentration to 0.55, whereas the
Curie temperature of NdOsSb is depressed linearly with Pr
composition to () 0.45. In the superconducting region, the upper
critical field is depressed quadratically with in the range 0
0.3, exhibits a kink at 0.3, and then
decreases linearly with in the range 0.3 0.6. The
behavior of appears to be due to pair breaking caused by the
applied magnetic field and the exhange field associated with the polarization
of the Nd magnetic moments, in the superconducting state. From magnetic
susceptibility measurements, the correlations between the Nd moments in the
superconducting state appear to change from ferromagnetic in the range 0.3
0.6 to antiferromagnetic in the range 0
0.3. Specific heat measurements on a sample with 0.45
indicate that magnetic order occurs in the superconducting state, as is also
inferred from the depression of with .Comment: 7 pages, 7 figures, currently submitted to Phys. Rev.
Temperature dependent band structure of the Kondo insulator
We present a Qantum Monte Carlo (QMC) study of the temperature dependent
dynamics of the Kondo insulator. Working at the so-called symmetrical point
allows to perform minus-sign free QMC simulations and thus reach temperatures
of less than 1% of the conduction electron bandwidth. Study of the temperature
dependence of the single particle Green's function and dynamical spin
correlation function shows a surprisingly intricate low temperature band
structure and gives evidence for two characteristic temperatures, which we
identify with the Kondo and coherence temperature, respectively. In particular,
the data show a temperature induced metal-insulator transition at the coherence
temperature.Comment: RevTex-file, 4 PRB pages with 4 eps figures. Hardcopies of figures
(or the entire manuscript) can be obtained by e-mail request to:
[email protected]
Cohesive energies of cubic III-V semiconductors
Cohesive energies for twelve cubic III-V semiconductors with zincblende
structure have been determined using an ab-initio scheme. Correlation
contributions, in particular, have been evaluated using the coupled-cluster
approach with single and double excitations (CCSD). This was done by means of
increments obtained for localized bond orbitals and for pairs and triples of
such bonds. Combining these results with corresponding Hartree-Fock data, we
recover about 92 \% of the experimental cohesive energies.Comment: 16 pages, 1 figure, late
Reentrant charge order transition in the extended Hubbard model
We study the extended Hubbard model with both on-site and nearest neighbor
Coulomb repulsion ( and , respectively) in the Dynamical Mean Field
theory. At quarter filling, the model shows a transition to a charge ordered
phase with different sublattice occupancies n_A \nen_B. The effective mass
increases drastically at the critical and a pseudo-gap opens in the
single-particle spectral function for higher values of . The -curve
has a negative slope for small temperatures, i.e. the charge ordering
transition can be driven by increasing the temperature. This is due to the
higher spin-entropy of the charge ordered phase.Comment: 4 pages, 4 EPS figures included, REVTe
Correlation in the transition metal based Heusler compounds CoMnSi and CoFeSi
Half-metallic ferromagnets like the full Heusler compounds with formula
XYZ are supposed to show an integer value of the spin magnetic moment.
Calculations reveal in certain cases of X = Co based compounds non-integer
values, in contrast to experiments. In order to explain deviations of the
magnetic moment calculated for such compounds, the dependency of the electronic
structure on the lattice parameter was studied theoretically. In local density
approximation (LDA), the minimum total energy of CoFeSi is found for the
experimental lattice parameter, but the calculated magnetic moment is about 12%
too low. Half-metallic ferromagnetism and a magnetic moment equal to the
experimental value of are found, however, only after increasing the
lattice parameter by more than 6%.
To overcome this discrepancy, the LDA scheme was used to respect on-site
electron correlation in the calculations. Those calculations revealed for
CoFeSi that an effective Coulomb-exchange interaction in the
range of about 2eV to 5eV leads to half-metallic ferromagnetism and the
measured, integer magnetic moment at the measured lattice parameter. Finally,
it is shown in the case of CoMnSi that correlation may also serve to
destroy the half-metallic behavior if it becomes too strong (for CoMnSi
above 2eV and for CoFeSi above 5eV). These findings indicate that on-site
correlation may play an important role in the description of Heusler compounds
with localized moments.Comment: submitted to Phys. Rev.
Optical spectra of the heavy fermion uniaxial ferromagnet UGe
We report a detailed study of UGe single crystals using infrared
reflectivity and spectroscopic ellipsometry. The optical conductivity suggests
the presence of a low frequency interband transition and a narrow free-carrier
response with strong frequency dependence of the scattering rate and effective
mass. We observe sharp changes in the low frequency mass and scattering rate
below the upper ferromagnetic transition . The characteristic
changes are exhibited most strongly at an energy scale of around 12 meV (100
cm). They recover their unrenormalized value above and for 40 meV. In contrast no sign of an anomaly is seen at the lower transition
temperature of unknown nature 30 K, observed in transport and
thermodynamic experiments. In the ferromagnetic state we find signatures of a
strong coupling to the longitudinal magnetic excitations that have been
proposed to mediate unconventional superconductivity in this compound
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