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

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

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

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

Fusion process studied with preequilibrium giant dipole resonance in time dependent Hartree-Fock theory

15 pages, 19 figures, revised versionInternational audienceThe equilibration of macroscopic degrees of freedom during the fusion of heavy nuclei, like the charge and the shape, are studied in the Time-Dependent Hartree-Fock theory. The pre-equilibrium Giant Dipole Resonance (GDR) is used to probe the fusion path. It is shown that such isovector collective state is excited in N/Z asymmetric fusion and to a less extent in mass asymmetric systems. The characteristics of this GDR are governed by the structure of the fused system in its preequilibrium phase, like its deformation, rotation and vibration. In particular, we show that a lowering of the pre-equilibrium GDR energy is expected as compared to the statistical one. Revisiting experimental data, we extract an evidence of this lowering for the first time. We also quantify the fusion-evaporation enhancement due to gamma-ray emission from the pre-equilibrium GDR. This cooling mechanism along the fusion path may be suitable to synthesize in the future super heavy elements using radioactive beams with strong N/Z asymmetries in the entrance channel

C60_{60} in intense femtosecond laser pulses: nonlinear dipole response and ionization

We study the interaction of strong femtosecond laser pulses with the C$_{60}$ molecule employing time-dependent density functional theory with the ionic background treated in a jellium approximation. The laser intensities considered are below the threshold of strong fragmentation but too high for perturbative treatments such as linear response. The nonlinear response of the model to excitations by short pulses of frequencies up to 45eV is presented and analyzed with the help of Kohn-Sham orbital resolved dipole spectra. In femtosecond laser pulses of 800nm wavelength ionization is found to occur multiphoton-like rather than via excitation of a ``giant'' resonance.Comment: 14 pages, including 1 table, 5 figure

Matrix metalloproteinase-10 is upregulated by thrombin in endothelial cells and increased in patients with enhanced thrombin generation

OBJECTIVE: Thrombin is a multifunctional serine protease that promotes vascular proinflammatory responses whose effect on endothelial MMP-10 expression has not previously been evaluated. METHODS AND RESULTS: Thrombin induced endothelial MMP-10 mRNA and protein levels, through a protease-activated receptor-1 (PAR-1)-dependent mechanism, in a dose- and time-dependent manner. This effect was mimicked by a PAR-1 agonist peptide (TRAP-1) and antagonized by an anti-PAR-1 blocking antibody. MMP-10 induction was dependent on extracellular regulated kinase1/2 (ERK1/2) and c-jun N-terminal kinase (JNK) pathways. By serial deletion analysis, site-directed mutagenesis and electrophoretic mobility shift assay an AP-1 site in the proximal region of MMP-10 promoter was found to be critical for thrombin-induced MMP-10 transcriptional activity. Thrombin and TRAP-1 upregulated MMP-10 in murine endothelial cells in culture and in vivo in mouse aorta. This effect of thrombin was not observed in PAR-1-deficient mice. Interestingly, circulating MMP-10 levels (P<0.01) were augmented in patients with endothelial activation associated with high (disseminated intravascular coagulation) and moderate (previous acute myocardial infarction) systemic thrombin generation. CONCLUSIONS: Thrombin induces MMP-10 through a PAR-1-dependent mechanism mediated by ERK1/2, JNK, and AP-1 activation. Endothelial MMP-10 upregulation could be regarded as a new proinflammatory effect of thrombin whose pathological consequences in thrombin-related disorders and plaque stability deserve further investigation

An exact stochastic mean-field approach to the fermionic many-body problem

We investigate a reformulation of the dynamics of interacting fermion systems in terms of a stochastic extension of Time Dependent Hartree-Fock equations. The noise is found from a path-integral representation of the evolution operator and allows to interpret the exact N-body state as a coherent average over Slater determinants evolving under the random mean-fied. The full density operator and the expectation value of any observable are then reconstructed using pairs of stochastic uncorrelated wave functions. The imaginary time propagation is also presented and gives a similar stochastic one-body scheme which converges to the exact ground state without developing a sign problem. In addition, the growth of statistical errors is examined to show that the stochastic formulation never explode in a finite dimensional one-body space. Finally, we consider initially correlated systems and present some numerical implementations in exactly soluble models to analyse the precision and the stability of the approach in practical cases

Ionic and electronic structure of sodium clusters up to N=59

We determined the ionic and electronic structure of sodium clusters with even electron numbers and 2 to 59 atoms in axially averaged and three-dimensional density functional calculations. A local, phenomenological pseudopotential that reproduces important bulk and atomic properties and facilitates structure calculations has been developed. Photoabsorption spectra have been calculated for $\mathrm{Na}_2$, $\mathrm{Na}_8$, and $\mathrm{Na}_9^+$ to $\mathrm{Na}_{59}^+$. The consistent inclusion of ionic structure considerably improves agreement with experiment. An icosahedral growth pattern is observed for $\mathrm{Na}_{19}^+$ to $\mathrm{Na}_{59}^+$. This finding is supported by photoabsorption data.Comment: To appear in Phys. Rev. B 62. Version with figures in better quality can be requested from the author