Ab initio investigation of intermolecular interactions in solid benzene

A computational strategy for the evaluation of the crystal lattice constants and cohesive energy of the weakly bound molecular solids is proposed. The strategy is based on the high level ab initio coupled-cluster determination of the pairwise additive contribution to the interaction energy. The zero-point-energy correction and non-additive contributions to the interaction energy are treated using density functional methods. The experimental crystal lattice constants of the solid benzene are reproduced, and the value of 480 meV/molecule is calculated for its cohesive energy

Low-Energy Scale Excitations in the Spectral Function of Organic Monolayer Systems

Using high-resolution photoemission spectroscopy we demonstrate that the electronic structure of several organic monolayer systems, in particular 1,4,5,8-naphthalene tetracarboxylic dianhydride and Copper-phtalocyanine on Ag(111), is characterized by a peculiar excitation feature right at the Fermi level. This feature displays a strong temperature dependence and is immediatly connected to the binding energy of the molecular states, determined by the coupling between the molecule and the substrate. At low temperatures, the line-width of this feature, appearing on top of the partly occupied lowest unoccupied molecular orbital of the free molecule, amounts to only $\approx 25$ meV, representing an unusually small energy scale for electronic excitations in these systems. We discuss possible origins, related e.g. to many-body excitations in the organic-metal adsorbate system, in particular a generalized Kondo scenario based on the single impurity Anderson model.Comment: 6 pages, 3 figures, accepted as PRB Rapid Communication

The reflectivity of relativistic ultra-thin electron layers

The coherent reflectivity of a dense, relativistic, ultra-thin electron layer is derived analytically for an obliquely incident probe beam. Results are obtained by two-fold Lorentz transformation. For the analytical treatment, a plane uniform electron layer is considered. All electrons move with uniform velocity under an angle to the normal direction of the plane; such electron motion corresponds to laser acceleration by direct action of the laser fields, as it is described in a companion paper. Electron density is chosen high enough to ensure that many electrons reside in a volume \lambda_R^3, where \lambda_R is the wavelength of the reflected light in the rest frame of the layer. Under these conditions, the probe light is back-scattered coherently and is directed close to the layer normal rather than the direction of electron velocity. An important consequence is that the Doppler shift is governed by \gamma_x=(1-(V_x/c)^2)^{-1/2} derived from the electron velocity component V_x in normal direction rather than the full \gamma-factor of the layer electrons.Comment: 7 pages, 4 figures, submitted to the special issue "Fundamental Physics with Ultra-High Fields" in The European Physical Journal

All-optical measurement of the hot electron sheath driving laser ion acceleration from thin foils

We present experimental results from an all-optical diagnostic method to directly measure the evolution of the hot-electron distribution driving the acceleration of ions from thin foils using high-intensity lasers. Central parameters of laser ion acceleration such as the hot-electron density, the temperature distribution and the conversion efficiency from laser pulse energy into hot electrons become comprehensively accessible with this technique.Deutsche Forschungsgemeinschaft (DFG) (contract number TR18)Germany. Bundesministerium für Bildung und Forschung (contract number 03ZIK445)Germany. Bundesministerium für Bildung und Forschung (contract number 03ZIK052

Intense high-quality medical proton beams via laser fields

During the past decade, the interaction of high-intensity lasers with solid targets has attracted much interest, regarding its potential in accelerating charged particles. In spite of tremendous progress in laser-plasma based acceleration, it is still not clear which particle beam quality will be accessible within the upcoming multi petawatt (1 PW = 10$^{15}$ W) laser generation. Here, we show with simulations based on the coupled relativistic equations of motion that protons stemming from laser-plasma processes can be efficiently post-accelerated using crossed laser beams focused to spot radii of a few laser wavelengths. We demonstrate that the crossed beams produce monoenergetic accelerated protons with kinetic energies $> 200$ MeV, small energy spreads ($\approx$ 1$$) and high densities as required for hadron cancer therapy. To our knowledge, this is the first scheme allowing for this important application based on an all-optical set-up.Comment: 14 pages, 3 figures, 1 tabl

Nuclear dynamics of singlet exciton fission: a direct observation in pentacene single crystals

Singlet exciton fission (SEF) is a key process in the development of efficient opto-electronic devices. An aspect that is rarely probed directly, and yet has a tremendous impact on SEF properties, is the nuclear structure and dynamics involved in this process. Here we directly observe the nuclear dynamics accompanying the SEF process in single crystal pentacene using femtosecond electron diffraction. The data reveal coherent atomic motions at 1 THz, incoherent motions, and an anisotropic lattice distortion representing the polaronic character of the triplet excitons. Combining molecular dynamics simulations, time-dependent density functional theory and experimental structure factor analysis, the coherent motions are identified as collective sliding motions of the pentacene molecules along their long axis. Such motions modify the excitonic coupling between adjacent molecules. Our findings reveal that long-range motions play a decisive part in the disintegration of the electronically correlated triplet pairs, and shed light on why SEF occurs on ultrafast timescales

Lattice dynamics and correlated atomic motion from the atomic pair distribution function

The mean-square relative displacements (MSRD) of atomic pair motions in crystals are studied as a function of pair distance and temperature using the atomic pair distribution function (PDF). The effects of the lattice vibrations on the PDF peak widths are modelled using both a multi-parameter Born von-Karman (BvK) force model and a single-parameter Debye model. These results are compared to experimentally determined PDFs. We find that the near-neighbor atomic motions are strongly correlated, and that the extent of this correlation depends both on the interatomic interactions and crystal structure. These results suggest that proper account of the lattice vibrational effects on the PDF peak width is important in extracting information on static disorder in a disordered system such as an alloy. Good agreement is obtained between the BvK model calculations of PDF peak widths and the experimentally determined peak widths. The Debye model successfully explains the average, though not detailed, natures of the MSRD of atomic pair motion with just one parameter. Also the temperature dependence of the Debye model largely agrees with the BvK model predictions. Therefore, the Debye model provides a simple description of the effects of lattice vibrations on the PDF peak widths.Comment: 9 pages, 11 figure

Spectral shaping of laser generated proton beams

The rapid progress in the field of laser particle acceleration has stimulated a debate about the promising perspectives of laser based ion beam sources. For a long time, the beams produced exhibited quasi-thermal spectra. Recent proof-of-principle experiments demonstrated that ion beams with narrow energy distribution can be generated from special target geometries. However, the achieved spectra were strongly limited in terms of monochromacity and reproducibility. We show that microstructured targets can be used to reliably produce protons with monoenergetic spectra above 2 MeV with less than 10% energy spread. Detailed investigations of the effects of laser ablation on the target resulted in a significant improvement of the reproducibility. Based on statistical analysis, we derive a scaling law between proton peak position and laser energy, underlining the suitability of this method for future applications. Both the quality of the spectra and the scaling law are well reproduced by numerical simulations

Nuclear Inelastic X-Ray Scattering of FeO to 48 GPa

The partial density of vibrational states has been measured for Fe in compressed FeO (w\"ustite) using nuclear resonant inelastic x-ray scattering. Substantial changes have been observed in the overall shape of the density of states close to the magnetic transiton around 20 GPa from the paramagnetic (low pressure) to the antiferromagnetic (high pressure) state. Our data indicate a substantial softening of the aggregate sound velocities far below the transition, starting between 5 and 10 GPa. This is consistent with recent radial x-ray diffraction measurements of the elastic constants in FeO. The results indicate that strong magnetoelastic coupling in FeO is the driving force behind the changes in the phonon spectrum of FeO.Comment: 4 pages, 4 figure