129 research outputs found
An Empirical Charge Transfer Potential with Correct Dissociation Limits
The empirical valence bond (EVB) method [J. Chem. Phys. 52, 1262 (1970)] has
always embodied charge transfer processes. The mechanism of that behavior is
examined here and recast for use as a new empirical potential energy surface
for large-scale simulations. A two-state model is explored. The main features
of the model are: (1) Explicit decomposition of the total system electron
density is invoked; (2) The charge is defined through the density decomposition
into constituent contributions; (3) The charge transfer behavior is controlled
through the resonance energy matrix elements which cannot be ignored; and (4) A
reference-state approach, similar in spirit to the EVB method, is used to
define the resonance state energy contributions in terms of "knowable"
quantities. With equal validity, the new potential energy can be expressed as a
nonthermal ensemble average with a nonlinear but analytical charge dependence
in the occupation number. Dissociation to neutral species for a gas-phase
process is preserved. A variant of constrained search density functional theory
is advocated as the preferred way to define an energy for a given charge.Comment: Submitted to J. Chem. Phys. 11/12/03. 14 pages, 8 figure
Relativistic Klein-Gordon charge effects by information-theoretic measures
The charge spreading of ground and excited states of Klein-Gordon particles
moving in a Coulomb potential is quantitatively analyzed by means of the
ordinary moments and the Heisenberg measure as well as by use of the most
relevant information-theoretic measures of global (Shannon entropic power) and
local (Fisher's information) types. The dependence of these complementary
quantities on the nuclear charge Z and the quantum numbers characterizing the
physical states is carefully discussed. The comparison of the relativistic
Klein-Gordon and non-relativistic Schrodinger values is made. The
non-relativistic limits at large principal quantum number n and for small
values of Z are also reached.Comment: Accepted in New Journal of Physic
Current-density functional for disordered systems
The effective action for the current and density is shown to satisfy an
evolution equation, the functional generalization of Callan-Symanzik equation.
The solution describes the dependence of the one-particle irreducible vertex
functions on the strength of the quenched disorder and the annealed Coulomb
interaction. The result is non-perturbative, no small parameter is assumed. The
a.c. conductivity is obtained by the numerical solution of the evolution
equation on finite lattices in the absence of the Coulomb interaction. The
static limit is performed and the conductivity is found to be vanishing beyond
a certain threshold of the impurity strength.Comment: final version, 28 pages, 17 figures, to appear in Phys. Rev.
Nature of the 5f states in actinide metals
Actinide elements produce a plethora of interesting physical behaviors due to
the 5f states. This review compiles and analyzes progress in understanding of
the electronic and magnetic structure of the 5f states in actinide metals.
Particular interest is given to electron energy-loss spectroscopy and
many-electron atomic spectral calculations, since there is now an appreciable
library of core d -> valence f transitions for Th, U, Np, Pu, Am, and Cm. These
results are interwoven and discussed against published experimental data, such
as x-ray photoemission and absorption spectroscopy, transport measurements, and
electron, x-ray, and neutron diffraction, as well as theoretical results, such
as density-functional theory and dynamical mean-field theory.Comment: 136 pages in Word format, 29 Figures; Accepted to Reviews of Modern
Physic
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