660 research outputs found
Microscopic theory of multipole ordering in NpO2
In order to examine the mysterious ordered phase of NpO2 from a microscopic
viewpoint, we investigate an f-electron model on an fcc lattice constructed
based on a j-j coupling scheme. First, an effective model with multipole
interactions is derived in the strong-coupling limit. Numerical analysis of the
model clearly indicates that the interactions for \Gamma_{4u} and \Gamma_{5u}
moments are relevant to the ground state. Then, by applying mean-field theory
to the simplified model including only such interactions, we conclude that
longitudinal triple-q \Gamma_{5u} octupole order is realized in NpO2 through
the combined effects of multipole interactions and anisotropy of the
\Gamma_{5u} moment.Comment: 5 pages, 2 figure
DFT/TD-DFT molecular design of porphyrin analogues for use in dye-sensitized solar cells
Density functional theory (DFT) and time-dependent DFT calculations have been employed to model Zn meso-tetraphenylporphyrin (ZnTPP) complexes having different b-substituents, in order to design an efficient sensitizer for dye-sensitized solar cells. To calculate the excited states of the porphyrin analogues, at least the TD-B3LYP/6-31G* level of theory is needed to replicate the experimental absorption spectra. Solvation results were found to be invariant with respect to the type of model used (PCM vs. C-PCM). Most of the electronic transitions based on Gouterman’s four-orbital model of ZnTPP-A and ZnTPP-B are p - p* transitions, so that cell efficiency can be enhanced by increasing the p-conjugation and electron-withdrawing capability of the bsubstituent.
This proposition was tested by inserting thiophene into the b-substituent of ZnTPP-A
to form a new analogue, ZnTPP-C. Compared with ZnTPP-A and ZnTPP-B, ZnTPP-C has a smaller band gap, which brings LUMO closer to the conduction band of TiO2, and a red-shifted absorption spectrum with higher extinction coefficients, especially in the Q-band positio
Experimental and theoretical analysis of organic dyes having a double D-π-A configurations for dye-sensitized solar cells
Two spiro-like organic dyes linked at the thiophene bridge (KS-11 and KS-12) together with the original rod-shaped D-π-A configuration (C1) were designed, synthesized, and characterized based on their electronic structure, and determine the photophysical and photovoltaic properties for its application in dye-sensitized solar cells. Compared to C1, the double D-π-A spiro-like configuration, which consists of two separated light-harvesting moieties, was found to be beneficial to photocurrent generation provided that they are separated properly to prevent intramolecular exciton annihilation. This was observed when KS-11, which is linked at the β-position of the thiophene moiety of D-π-A, was compared with KS-12, where the two D-π-A are linked with an additional thiophene using a α-β linkage. The results show that KS-12 produced a 20% and 17% increase in photovoltaic efficiency under simulated AM 1.5G solar irradiation compared to KS-11 and C1, respectively. This increase in photovoltaic performance is credited mostly to the reduction of recombination effects and the increase in the density of states at the semiconductor surface due to high dye loading and better charge-transfer properties
Resonant X-Ray Scattering on the M-Edge Spectra from Triple-k Structure Phase in U_{0.75}Np_{0.25}O_{2} and UO_{2}
We derive an expression for the scattering amplitude of resonant x-ray
scattering under the assumption that the Hamiltonian describing the
intermediate state preserves spherical symmetry. On the basis of this
expression, we demonstrate that the energy profile of the RXS spectra expected
near U and Np M_4 edges from the triple-k antiferromagnetic ordering phase in
UO_{2} and U_{0.75}Np_{0.25}O_{2} agree well with those from the experiments.
We demonstrate that the spectra in the \sigma-\sigma' and \sigma-\pi' channels
exhibit quadrupole and dipole natures, respectively.Comment: 3 pages, 3 figures, to be published in J. Phys. Soc. Jpn. Supp
Evidence for Octupole Order in CeLaB from Resonant X-ray Scattering
The azimuthal angle dependence observed in the resonant X-ray scattering in
phase IV of CeLaB is analyzed theoretically. It is shown
that the peculiar angle dependence observed in the E2 channel is consistent
with the Gamma_{5u}-type octupole order with principal axis along (111) and
equivalent directions. Under the assumption that the four equivalent octupole
domains are nearly equally populated in the sample, the observed angle
dependences are reproduced by calculation for both sigma-sigma' and sigma-pi'
polarizations. The calculation for various symmetries of order parameters
excludes unambiguously other order parameters than the Gamma_{5u}-type
octupole.Comment: 4 pages, 2 figures, 3 tables, in JPSJ forma
Multipole correlations in low-dimensional f-electron systems
By using a density matrix renormalization group method, we investigate the
ground-state properties of a one-dimensional three-orbital Hubbard model on the
basis of a j-j coupling scheme. For , where is a parameter
to control cubic crystalline electric field effect, one orbital is itinerant,
while other two are localized. Due to the competition between itinerant and
localized natures, we obtain orbital ordering pattern which is sensitive to
, leading to a characteristic change of quadrupole state
into an incommensurate structure. At , all the three orbitals are
degenerate, but we observe a peak at in quadrupole
correlation, indicating a ferro-orbital state, and the peak at in
dipole correlation, suggesting an antiferromagnetic state. We
also discuss the effect of octupole on magnetic anisotropy.Comment: 4 pages, 3 figures, Proceedings of ASR-WYP-2005 (September 27-29,
2005, Tokai
Satellite holmium M-edge spectra from the magnetic phase via resonant x-ray scattering
Developing an expression of resonant x-ray scattering (RXS) amplitude which
is convenient for investigating the contributions from the higher rank tensor
on the basis of a localized electron picture, we analyze the RXS spectra from
the magnetic phases of Ho near the absorption edges. At the
edge in the uniform helical phase, the calculated spectra of the absorption
coefficient, the RXS intensities at the first and second satellite spots
capture the properties the experimental data possess, such as the spectral
shapes and the peak positions. This demonstrates the plausibility of the
adoption of the localized picture in this material and the effectiveness of the
spectral shape analysis. The latter point is markedly valuable since the
azimuthal angle dependence, which is one of the most useful informations RXS
can provides, is lacking in the experimental conditions. Then, by focusing on
the temperature dependence of the spectral shape at the second satellite spot,
we expect that the spectrum is the contribution of the pure rank two profile in
the uniform helical and the conical phases while that is dominated by the rank
one profile in the intermediate temperature phase, so-called spin slip phase.
The change of the spectral shape as a function of temperature indicates a
direct evidence of the change of magnetic structures undergoing. Furthermore,
we predict that the intensity, which is the same order observed at the second
satellite spot, is expected at the fourth satellite spot from the conical phase
in the electric dipolar transition.Comment: 24 pages, 5 figure
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