149 research outputs found
Efficient implementation of the Gutzwiller variational method
We present a self-consistent numerical approach to solve the Gutzwiller
variational problem for general multi-band models with arbitrary on-site
interaction. The proposed method generalizes and improves the procedure derived
by Deng et al., Phys. Rev. B. 79 075114 (2009), overcoming the restriction to
density-density interaction without increasing the complexity of the
computational algorithm. Our approach drastically reduces the problem of the
high-dimensional Gutzwiller minimization by mapping it to a minimization only
in the variational density matrix, in the spirit of the Levy and Lieb
formulation of DFT. For fixed density the Gutzwiller renormalization matrix is
determined as a fixpoint of a proper functional, whose evaluation only requires
ground-state calculations of matrices defined in the Gutzwiller variational
space. Furthermore, the proposed method is able to account for the symmetries
of the variational function in a controlled way, reducing the number of
variational parameters. After a detailed description of the method we present
calculations for multi-band Hubbard models with full (rotationally invariant)
Hund's rule on-site interaction. Our analysis shows that the numerical
algorithm is very efficient, stable and easy to implement. For these reasons
this method is particularly suitable for first principle studies -- e.g., in
combination with DFT -- of many complex real materials, where the full
intra-atomic interaction is important to obtain correct results.Comment: 19 pages, 7 figure
The Dynamical Mean Field Theory phase space extension and critical properties of the finite temperature Mott transition
We consider the finite temperature metal-insulator transition in the half
filled paramagnetic Hubbard model on the infinite dimensional Bethe lattice. A
new method for calculating the Dynamical Mean Field Theory fixpoint surface in
the phase diagram is presented and shown to be free from the convergence
problems of standard forward recursion. The fixpoint equation is then analyzed
using dynamical systems methods. On the fixpoint surface the eigenspectra of
its Jacobian is used to characterize the hysteresis boundaries of the first
order transition line and its second order critical end point. The critical
point is shown to be a cusp catastrophe in the parameter space, opening a
pitchfork bifurcation along the first order transition line, while the
hysteresis boundaries are shown to be saddle-node bifurcations of two merging
fixpoints. Using Landau theory the properties of the critical end point is
determined and related to the critical eigenmode of the Jacobian. Our findings
provide new insights into basic properties of this intensively studied
transition.Comment: 11 pages, 12 figures, 1 tabl
Electron-hole pairs during the adsorption dynamics of O2 on Pd(100) - Exciting or not?
During the exothermic adsorption of molecules at solid surfaces dissipation
of the released energy occurs via the excitation of electronic and phononic
degrees of freedom. For metallic substrates the role of the nonadiabatic
electronic excitation channel has been controversially discussed, as the
absence of a band gap could favour an easy coupling to a manifold of
electronhole pairs of arbitrarily low energies. We analyse this situation for
the highly exothermic showcase system of molecular oxygen dissociating at
Pd(100), using time-dependent perturbation theory applied to first-principles
electronic-structure calculations. For a range of different trajectories of
impinging O2 molecules we compute largely varying electron-hole pair spectra,
which underlines the necessity to consider the high-dimensionality of the
surface dynamical process when assessing the total energy loss into this
dissipation channel. Despite the high Pd density of states at the Fermi level,
the concomitant non-adiabatic energy losses nevertheless never exceed about 5%
of the available chemisorption energy. While this supports an electronically
adiabatic description of the predominant heat dissipation into the phononic
system, we critically discuss the non-adiabatic excitations in the context of
the O2 spin transition during the dissociation process.Comment: 20 pages including 7 figures; related publications can be found at
http://www.fhi-berlin.mpg.de/th/th.html [added two references, changed
V_{fsa} to V_{6D}, modified a few formulations in interpretation of spin
asymmetry of eh-spectra, added missing equals sign in Eg.(2.10)
Forces on Dust Grains Exposed to Anisotropic Interstellar Radiation Fields
Grains exposed to anisotropic radiation fields are subjected to forces due to
the asymmetric photon-stimulated ejection of particles. These forces act in
addition to the ``radiation pressure'' due to absorption and scattering. Here
we model the forces due to photoelectron emission and the photodesorption of
adatoms. The ``photoelectric'' force depends on the ambient conditions relevant
to grain charging. We find that it is comparable to the radiation pressure when
the grain potential is relatively low and the radiation spectrum is relatively
hard. The calculation of the ``photodesorption'' force is highly uncertain,
since the surface physics and chemsitry of grain materials are poorly
understood at present. For our simple yet plausible model, the photodesorption
force dominates the radiation pressure for grains with size >~0.1 micron
exposed to starlight from OB stars. We find that the anisotropy of the
interstellar radiation field is ~10% in the visible and ultraviolet. We
estimate size-dependent drift speeds for grains in the cold and warm neutral
media and find that micron-sized grains could potentially be moved across a
diffuse cloud during its lifetime.Comment: LaTeX(41 pages, 19 figures), submitted to Ap
Role of bulk and surface phonons in the decay of metal surface states
We present a comprehensive theoretical investigation of the electron-phonon
contribution to the lifetime broadening of the surface states on Cu(111) and
Ag(111), in comparison with high-resolution photoemission results. The
calculations, including electron and phonon states of the bulk and the surface,
resolve the relative importance of the Rayleigh mode, being dominant for the
lifetime at small hole binding energies. Including the electron-electron
interaction, the theoretical results are in excellent agreement with the
measured binding energy and temperature dependent lifetime broadening.Comment: 4 pages, 3 figure
Model study of adsorbed metallic quantum dots: Na on Cu(111)
We model electronic properties of the second monolayer Na adatom islands
(quantum dots) on the Cu(111) surface covered homogeneously by the first Na
monolayer. An axially-symmetric three-dimensional jellium model, taking into
account the effects due to the first Na monolayer and the Cu substrate, has
been developed. The electronic structure is solved within the local-density
approximation of the density-functional theory using a real-space multigrid
method. The model enables the study of systems consisting of thousands of
Na-atoms. The results for the local density of states are compared with
differential conductance () spectra and constant current topographs from
Scanning Tunneling Microscopy.Comment: 10 pages, 8 figures. For better quality figures, download
http://www.fyslab.hut.fi/~tto/cylart1.pd
Theory of inelastic lifetimes of surface-state electrons and holes at metal surfaces
After the early suggestion by John Pendry to probe unoccupied bands at
surfaces through the time reversal of the photoemission process, the
inverse-photoemission technique yielded the first conclusive experimental
evidence for the existence of image-potential bound states at metal surfaces
and has led over the last two decades to an active area of research in
condensed-matter and surface physics. Here we describe the current status of
the many-body theory of inelastic lifetimes of these image-potential states and
also the Shockley surface states that exist near the Fermi level in the
projected bulk band gap of simple and noble metals. New calculations of the
self-energy and lifetime of surface states on Au surfaces are presented as
well, by using the approximation of many-body theory.Comment: 17 pages, 7 figures, to appear in J Phys-Condens Ma
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