104 research outputs found
The Spin-SAF transition in NaV2O5 induced by spin-pseudospin coupling
We present microscopic estimates for the spin-spin and spin-speudospin
interactions of the quarter-filled ladder compound NaV2O5, obtained by exactly
diagonalizing appropriate clusters of the underlying generalized Hubbard
Hamiltonian. We present evidence for a substantial interladder spin-pseudospin
interaction term which would allow simultaneously for the
superantiferroelectric (SAF) charge (pseudospin) ordering and spin
dimerization. We discuss the values of the coupling constants appropriate for
NaV2O5 and deduce the absence of a soft antiferroelectric mode
Ab initio evaluation of the charge-ordering in
We report {\it ab initio} calculations of the charge ordering in
using large configurations interaction methods on
embedded fragments. Our major result is that the electrons of the
bridging oxygen of the rungs present a very strong magnetic character and
should thus be explicitly considered in any relevant effective model. The most
striking consequence of this result is that the spin and charge ordering differ
substantially, as differ the experimental results depending on whether they are
sensitive to the spin or charge density.Comment: 4 page
Ferromagnetic Polarons in La0.5Ca0.5MnO3 and La0.33Ca0.67MnO3
Unrestricted Hartree-Fock calculations on La0.5Ca0.5MnO3 and La0.33Ca0.67MnO3
in the full magnetic unit cell show that the magnetic ground states of these
compounds consist of 'ferromagnetic molecules' or polarons ordered in
herring-bone patterns. Each polaron consists of either three or five Mn ions
separated by O- ions with a magnetic moment opposed to those of the Mn ions.
Ferromagnetic coupling within the polarons is strong while coupling between
them is relatively weak. Magnetic moments on the Mn ions range between 3.8 and
3.9 Bohr magnetons in La0.5Ca0.5MnO3 and moments on the O- ions are -0.7 Bohr
magnetons. Each polaron has a net magnetic moment of 7.0 Bohr magnetons, in
good agreement with recently reported magnetisation measurements from electron
microscopy. The polaronic nature of the electronic structure reported here is
obviously related to the Zener polaron model recently proposed for
Pr0.6Ca0.4MnO3 on the basis of neutron scattering data.Comment: 4 pages 5 figure
Electron Correlation Effects in Resonant Inelastic X-ray Scattering of NaV2O5
Element- and site-specific resonant inelastic x-ray scattering spectroscopy
(RIXS) is employed to investigate electron correlation effects in {}. In contrast to single photon techniques, RIXS at the vanadium
edge is able to probe transitions between V d-bands. A sharp energy
loss feature is observed at -1.56 eV, which is well reproduced by a model
calculation including correlation effects. The calculation identifies the loss
feature as excitation between the lower and upper Hubbard bands and permits an
accurate determination of the Hubbard interaction term eV.Comment: 15 pages, four figures, accepted to Phys. Rev. Let
The role of dynamical polarization of the ligand to metal charge transfer excitations in {\em ab initio} determination of effective exchange parameters
The role of the bridging ligand on the effective Heisenberg coupling
parameters is analyzed in detail. This analysis strongly suggests that the
ligand-to-metal charge transfer excitations are responsible for a large part of
the final value of the magnetic coupling constant. This permits to suggest a
new variant of the Difference Dedicated Configuration Interaction (DDCI)
method, presently one of the most accurate and reliable for the evaluation of
magnetic effective interactions. This new method treats the bridging ligand
orbitals mediating the interaction at the same level than the magnetic orbitals
and preserves the high quality of the DDCI results while being much less
computationally demanding. The numerical accuracy of the new approach is
illustrated on various systems with one or two magnetic electrons per magnetic
center. The fact that accurate results can be obtained using a rather reduced
configuration interaction space opens the possibility to study more complex
systems with many magnetic centers and/or many electrons per center.Comment: 7 pages, 4 figure
Salsolinol Facilitates Glutamatergic Transmission to Dopamine Neurons in the Posterior Ventral Tegmental Area of Rats
Although in vivo evidence indicates that salsolinol, the condensation product of acetaldehyde and dopamine, has properties that may contribute to alcohol abuse, the underlying mechanisms have not been fully elucidated. We have reported previously that salsolinol stimulates dopamine neurons in the posterior ventral tegmental area (p-VTA) partly by reducing inhibitory GABAergic transmission, and that ethanol increases glutamatergic transmission to VTA-dopamine neurons via the activation of dopamine D1 receptors (D1Rs). In this study, we tested the hypothesis that salsolinol stimulates dopamine neurons involving activation of D1Rs. By using whole-cell recordings on p-VTA-dopamine neurons in acute brain slices of rats, we found that salsolinol-induced increase in spike frequency of dopamine neurons was substantially attenuated by DL-2-amino-5-phosphono-valeric acid and 6, 7-dinitroquinoxaline-2, 3-dione, the antagonists of glutamatergic N-Methyl-D-aspartic acid and α-amino-3-hydroxy-5-methyl-4-isoxazolepropionic acid receptors. Moreover, salsolinol increased the amplitude of evoked excitatory postsynaptic currents (EPSCs) and the frequency but not the amplitude of spontaneous EPSCs. Additionally, SKF83566, a D1R antagonist attenuated the salsolinol-induced facilitation of EPSCs and of spontaneous firing of dopamine neurons. Our data reveal that salsolinol enhances glutamatergic transmission onto dopamine neurons via activation of D1Rs at the glutamatergic afferents in dopamine neurons, which contributes to salsolinol's stimulating effect on p-VTA dopamine neurons. This appears to be a novel mechanism which contributes toward rewarding properties of salsolinol
Ab initio evaluation of local effective interactions in
We will present the numerical evaluation of the hopping and magnetic exchange
integrals for a nearest-neighbor model of the quarter-filled
compound. The effective integrals are obtained from
valence-spectroscopy {\em ab initio} calculations of embedded crystal fragments
(two pyramids in the different geometries corresponding to the desired
parameters). We are using a large configurations interaction (CI) method, where
the CI space is specifically optimized to obtain accurate energy differences.
We show that the system can be seen as a
two-dimensional asymmetric triangular Heisenberg lattice where the effective
sites represent delocalized rung entities supporting the magnetic
electrons.Comment: 24 pages, 5 figure
A microscopic model for the structural transition and spin gap formation in alpha'-NaV2O5
We present a microscopic model for alpha'-NaV2O5. Using an extended Hubbard
model for the vanadium layers we derive an effective low-energy model
consisting of pseudospin Ising chains and Heisenberg chains coupled to each
other. We find a ``spin-Peierls-Ising'' phase transition which causes charge
ordering on every second ladder and superexchange alternation on the other
ladders. This transition can be identified with the first transition of the two
closeby transitions observed in experiment. Due to charge ordering the
effective coupling between the lattice and the superexchange is enhanced. This
is demonstrated within a Slater-Koster approximation. It leads to a second
instability with superexchange alternation on the charge-ordered ladders due to
an alternating shift of the O sites on the rungs of that ladder. We can explain
within our model the observed spin gap, the anomalous BCS ratio, and the
anomalous shift of the critical temperature of the first transition in a
magnetic field. To test the calculated superstructure we determine the
low-energy magnon dispersion and find agreement with experiment.Comment: 32 pages, 12 figures include
Theoretical investigation of the electronic structure of Fe(II) complexes at spin-state transitions
The electronic structure relevant to low spin (LS)high spin (HS) transitions in Fe(II) coordination compounds with a FeN6 core are studied. The selected [Fe(tz)6]2+(1) (tz=1H-tetrazole), [Fe(bipy)3]2+(2) (bipy=2,2’-bipyridine) and [Fe(terpy)2]2+ (3) (terpy=2,2’:6’,2’’-terpyridine) complexes have been actively studied experimentally, and with their respective mono-, bi-, and tridentate ligands, they constitute a comprehensive set for theoretical case studies. The methods in this work include density functional theory (DFT), time-dependent DFT (TD-DFT) and multiconfigurational second order perturbation theory (CASPT2). We determine the structural parameters as well as the energy splitting of the LS-HS states (ΔEHL) applying the above methods, and comparing their performance. We also determine the potential energy curves representing the ground and low-energy excited singlet, triplet, and quintet d6 states along the mode(s) that connect the LS and HS states. The results indicate that while DFT is well suited for the prediction of structural parameters, an accurate multiconfigurational approach is essential for the quantitative determination of ΔEHL. In addition, a good qualitative agreement is found between the TD-DFT and CASPT2 potential energy curves. Although the TD-DFT results might differ in some respect (in our case, we found a discrepancy at the triplet states), our results suggest that this approach, with due care, is very promising as an alternative for the very expensive CASPT2 method. Finally, the two dimensional (2D) potential energy surfaces above the plane spanned by the two relevant configuration coordinates in [Fe(terpy)2]2+ were computed both at the DFT and CASPT2 levels. These 2D surfaces indicate that the singlet-triplet and triplet-quintet states are separated along different coordinates, i.e. different vibration modes. Our results confirm that in contrast to the case of complexes with mono- and bidentate ligands, the singlet-quintet transitions in [Fe(terpy)2]2+ cannot be described using a single configuration coordinate
Uma Igreja distante de Roma: circulação internacional e gerações de missionários no Maranhão
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