132 research outputs found
Two-Photon Excitation of Low-Lying Electronic Quadrupole States in Atomic Clusters
A simple scheme of population and detection of low-lying electronic
quadrupole modes in free small deformed metal clusters is proposed. The scheme
is analyzed in terms of the TDLDA (time-dependent local density approximation)
calculations. As test case, the deformed cluster is considered.
Long-living quadrupole oscillations are generated via resonant two-photon
(two-dipole) excitation and then detected through the appearance of satellites
in the photoelectron spectra generated by a probe pulse. Femtosecond pump and
probe pulses with intensities and
pulse duration fs are found to be optimal. The modes of
interest are dominated by a single electron-hole pair and so their energies,
being combined with the photoelectron data for hole states, allow to gather new
information about mean-field spectra of valence electrons in the HOMO-LUMO
region. Besides, the scheme allows to estimate the lifetime of electron-hole
pairs and hence the relaxation time of electronic energy into ionic heat.Comment: 4 pages, 4 figure
Hindered Coulomb explosion of embedded Na clusters -- stopping, shape dynamics and energy transport
We investigate the dynamical evolution of a Na cluster embedded in Ar
matrices of various sizes from N=30 to 1048. The system is excited by an
intense short laser pulse leading to high ionization stages. We analyze the
subsequent highly non-linear motion of cluster and Ar environment in terms of
trajectories, shapes, and energy flow. The most prominent effects are:
temporary stabilization of high charge states for several ps, sudden stopping
of the Coulomb explosion of the embedded Na clusters associated with an
extremely fast energy transfer to the Ar matrix, fast distribution of energy
throughout the Ar layers by a sound wave. Other ionic-atomic transfer and
relaxation processes proceed at slower scale of few ps. The electron cloud is
almost thermally decoupled from ions and thermalizes far beyond the ps scale.Comment: 12 pages, 10 figures, accepted in Euro. Phys. J.
Hartree-Fock dynamics in highly excited quantum dots
Time-dependent Hartree-Fock theory is used to describe density oscillations
of symmetry-unrestricted two-dimensional nanostructures. In the small amplitude
limit the results reproduce those obtained within a perturbative approach such
as the linearized time-dependent Hartree-Fock one. The nonlinear regime is
explored by studying large amplitude oscillations in a non-parabolic potential,
which are shown to introduce a strong coupling with internal degrees of
freedom. This excitation of internal modes, mainly of monopole and quadrupole
character, results in sizeable modifications of the dipole absorption.Comment: 4 pages, 4 embedded figure
Enhanced ionization in small rare gas clusters
A detailed theoretical investigation of rare gas atom clusters under intense
short laser pulses reveals that the mechanism of energy absorption is akin to
{\it enhanced ionization} first discovered for diatomic molecules. The
phenomenon is robust under changes of the atomic element (neon, argon, krypton,
xenon), the number of atoms in the cluster (16 to 30 atoms have been studied)
and the fluency of the laser pulse. In contrast to molecules it does not
dissappear for circular polarization. We develop an analytical model relating
the pulse length for maximum ionization to characteristic parameters of the
cluster
Time-Dependent Density Functional Theory with Ultrasoft Pseudopotential: Real-Time Electron Propagation across Molecular Junction
A practical computational scheme based on time-dependent density functional
theory (TDDFT) and ultrasoft pseudopotential (USPP) is developed to study
electron dynamics in real time. A modified Crank-Nicolson time-stepping
algorithm is adopted, under planewave basis. The scheme is validated by
calculating the optical absorption spectra for sodium dimer and benzene
molecule. As an application of this USPP-TDDFT formalism, we compute the time
evolution of a test electron packet at the Fermi energy of the left metallic
lead crossing a benzene-(1,4)-dithiolate junction. A transmission probability
of 5-7%, corresponding to a conductance of 4.0-5.6muS, is obtained. These
results are consistent with complex band structure estimates, and Green's
function calculation results at small bias voltages
Charge-Induced Fragmentation of Sodium Clusters
The fission of highly charged sodium clusters with fissilities X>1 is studied
by {\em ab initio} molecular dynamics. Na_{24}^{4+} is found to undergo
predominantly sequential Na_{3}^{+} emission on a time scale of 1 ps, while
Na_{24}^{Q+} (5 \leq Q \leq 8) undergoes multifragmentation on a time scale
\geq 0.1 ps, with Na^{+} increasingly the dominant fragment as Q increases. All
singly-charged fragments Na_{n}^{+} up to size n=6 are observed. The observed
fragment spectrum is, within statistical error, independent of the temperature
T of the parent cluster for T \leq 1500 K. These findings are consistent with
and explain recent trends observed experimentally.Comment: To appear in Physical Review Letter
Scissors modes in triaxial metal clusters
We study the scissors mode (orbital M1 excitations) in small Na clusters,
triaxial metal clusters and and the
close-to-spherical , all described in DFT with detailed ionic
background. The scissors modes built on spin-saturated ground and
spin-polarized isomeric states are analyzed in virtue of both macroscopic
collective and microscopic shell-model treatments. It is shown that the mutual
destruction of Coulomb and the exchange-correlation parts of the residual
interaction makes the collective shift small and the net effect can depend on
details of the actual excited state. The crosstalk with dipole and spin-dipole
modes is studied in detail. In particular, a strong crosstalk with spin-dipole
negative-parity mode is found in the case of spin-polarized states. Triaxiality
and ionic structure considerably complicate the scissors response, mainly at
expense of stronger fragmentation of the strength. Nevertheless, even in these
complicated cases the scissors mode is mainly determined by the global
deformation. The detailed ionic structure destroys the spherical symmetry and
can cause finite M1 response (transverse optical mode) even in clusters with
zero global deformation. But its strength turns out to be much smaller than for
the genuine scissors modes in deformed systems.Comment: 17 pages, 5 figure
Cluster ionization via two-plasmon excitation
We calculate the two-photon ionization of clusters for photon energies near
the surface plasmon resonance. The results are expressed in terms of the
ionization rate of a double plasmon excitation, which is calculated
perturbatively. For the conditions of the experiment by Schlipper et al., we
find an ionization rate of the order of 0.05-0.10 fs^(-1). This rate is used to
determine the ionization probability in an external field in terms of the
number of photons absorbed and the duration of the field. The probability also
depends on the damping rate of the surface plasmon. Agreement with experiment
can only be achieved if the plasmon damping is considerably smaller than its
observed width in the room-temperature single-photon absorption spectrum.Comment: 17 pages and 6 PostScript figure
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