Book Review of David Lester, Making Sense of Suicide: An In-depth Look at Why People Kill Themselves (The Charles Press 1997)

Review of the book David Lester, Making Sense of Suicide: An In-depth Look at Why People Kill Themselves (The Charles Press 1997). Preface, bibliographical references, index. ISBN 0-914783-82-3. [208 pp. Paper $22.95. P.O. Box 15715, Philadelphia, PA 19103.

Computational design of metal-supported molecular switches: Transient ion formation during light- and electron-induced isomerisation of azobenzene

In molecular nanotechnology, a single molecule is envisioned to act as the basic building block of electronic devices. Such devices may be of special interest for organic photovoltaics, data storage, and smart materials. However, more often than not the molecular function is quenched upon contact with a conducting support. Trial-and-error-based decoupling strategies via molecular functionalisation and change of substrate have in many instances proven to yield unpredictable results. The adsorbate-substrate interactions that govern the function can be understood with the help of first-principles simulation. Employing dispersion-corrected Density-Functional Theory (DFT) and linear expansion Delta-Self-Consistent-Field DFT, the electronic structure of a prototypical surface-adsorbed functional molecule, namely azobenzene adsorbed to (111) single crystal facets of copper, silver and gold, is investigated and the main reasons for the loss or survival of the switching function upon adsorption are identified. The light-induced switching ability of a functionalised derivative of azobenzene on Au(111) and azobenzene on Ag(111) and Au(111) is assessed based on the excited-state potential energy landscapes of their transient molecular ions, which are believed to be the main intermediates of the experimentally observed isomerisation reaction. We provide a rationalisation of the experimentally observed function or lack thereof that connects to the underlying chemistry of the metal-surface interaction and provides insights into general design strategies for complex light-driven reactions at metal surfaces.Comment: 14 pages, 5 figures, submitted to J. Phys. Condens. Matte

Bistability loss as key feature in azobenzene (non-)switching on metal surfaces

Coinage metal adsorbed azobenzene is investigated as prototypical molecular switch. It is shown that switching capabilities are not just lost due to excited state quenching, but already due to changes in the ground state energetics. Electron demanding coadsorbates are suggested as strategy to regain the switching function.Comment: 8 pages, 3 figure

Assessing computationally efficient isomerization dynamics: Delta-SCF density-functional theory study of azobenzene molecular switching

We present a detailed comparison of the S0, S1 (n -> \pi*) and S2 (\pi -> \pi*) potential energy surfaces (PESs) of the prototypical molecular switch azobenzene as obtained by Delta-self-consistent-field (Delta-SCF) Density-Functional Theory (DFT), time-dependent DFT (TD-DFT) and approximate Coupled Cluster Singles and Doubles (RI-CC2). All three methods unanimously agree in terms of the PES topologies, which are furthermore fully consistent with existing experimental data concerning the photo-isomerization mechanism. In particular, sum-method corrected Delta-SCF and TD-DFT yield very similar results for S1 and S2, when based on the same ground-state exchange-correlation (xc) functional. While these techniques yield the correct PES topology already on the level of semi-local xc functionals, reliable absolute excitation energies as compared to RI-CC2 or experiment require an xc treatment on the level of long-range corrected hybrids. Nevertheless, particularly the robustness of Delta-SCF with respect to state crossings as well as its numerical efficiency suggest this approach as a promising route to dynamical studies of larger azobenzene-containing systems.Comment: 25 pages, 6 figure

The two-proton shell gap in Sn isotopes

We present an analysis of two-proton shell gaps in Sn isotopes. As the theoretical tool we use self-consistent mean-field models, namely the relativistic mean-field model and the Skyrme-Hartree-Fock approach, both with two different pairing forces, a delta interaction (DI) model and a density-dependent delta interaction (DDDI). We investigate the influence of nuclear deformation as well as collective correlations and find that both effects contribute significantly. Moreover, we find a further significant dependence on the pairing force used. The inclusion of deformation plus correlation effects and the use of DDDI pairing provides agreement with the data.Comment: gzipped tar archiv containing LaTeX source, bibliography file (*.bbl), all figures as *.eps, and the style file

The Skyrme Interaction in finite nuclei and nuclear matter

Self-consistent mean-field models are a powerful tool in the investigation of nuclear structure and low-energy dynamics. They are based on effective energy-density functionals, often formulated in terms of effective density-dependent nucleon-nucleon interactions. The free parameters of the functional are adjusted to empirical data. A proper choice of these parameters requires a comprehensive set of constraints covering experimental data on finite nuclei, concerning static as well as dynamical properties, empirical characteristics of nuclear matter, and observational information on nucleosynthesis, neutron stars and supernovae. This work aims at a comprehensive survey of the performance of one of the most successful non-relativistic self-consistent method, the Skyrme-Hartree-Fock model (SHF), with respect to these constraints. A full description of the Skyrme functional is given and its relation to other effective interactions is discussed. The validity of the application of SHF far from stability and in dense environments beyond the nuclear saturation density is critically assessed. The use of SHF in models extended beyond the mean field approximation by including some correlations is discussed. Finally, future prospects for further development of SHF towards a more consistent application of the existing and promisingly newly developing constraints are outlined.Comment: 71 pages, 22 figures. Accepted for publication in Prog.Part.Nucl.Phy

Misfits in Skyrme-Hartree-Fock

We address very briefly five critical points in the context of the Skyrme-Hartree-Fock (SHF) scheme: 1) the impossibility to consider it as an interaction, 2) a possible inconsistency of correlation corrections as, e.g., the center-of-mass correction, 3) problems to describe the giant dipole resonance (GDR) simultaneously in light and heavy nuclei, 4) deficiencies in the extrapolation of binding energies to super-heavy elements (SHE), and 5) a yet inappropriate trend in fission life-times when going to the heaviest SHE. While the first two points have more a formal bias, the other three points have practical implications and wait for solution.Comment: 9 pages, 4 figure