Physics

Azophenine has previously been identified as a controllable molecular switch when deposited on a Cu(110) surface, where it can be in two symmetry-equivalent states. Each of the two states can be set as well as read by means of a scanning tunneling microscope (STM). We propose a family of molecules based on the same quinone core, which show similar switching behavior without a supporting metal surface. Such a molecule could be an element in a molecular circuit or computer. Using the example of a simple hypothetical molecule, we show that it is possible to create molecules that show the necessary properties: two conformations with similar energy but different electric conductivity, and the possibility to switch between those by applying an external electric field.

High harmonic generation is a convenient way to obtain extreme ultraviolet light from table-top laser systems and the experimental tools to exploit this simple and powerful light source for time-resolved spectroscopy are being developed by several groups. For these applications, brightness and stability of the high harmonic generation is a key feature. This article focuses on practical aspects in the generation of extreme ultraviolet pulses with ultrafast commercial lasers, namely generation parameters and online monitoring as well as analysis of generation yield and stability.

Photoionization from atom-C60 hybrid levels in halogen endufullerene molecules, Cl@C60, Br@C60 and I@C60, are calculated using a linear response density functional method. Both the ordinary electron-configuration where the open shell halogen is at the center of C60 and the stable configuration after the atom receives an electron from C60 to form a closed shell anion are considered. Similar ground state hybridization is found for all three systems while, in general, a slight weakening of the effect is noticed after the electron transfer. At lower photon energies, cross sections of the outer hybrid levels attain identical shapes from enhancements driven by the C60 plasmon resonances, while the higher energy emissions remain distinguishable from the differences in atomic responses. These results further show near insensitivity to the choice of a configuration. The inner hybrid cross sections in general exhibit similar overall structures, although differ in details between molecules. However, for these states the results significantly differ before and after the electron transfer -- a feature that can be useful to experimentally determine the real configuration of the molecules via photoelectron spectroscopy.

When matter is exposed to a high-intensity x-ray free-electron-laser pulse, the x rays excite inner-shell electrons leading to the ionization of the electrons through various atomic processes and creating high-energy-density plasma, i.e., warm or hot dense matter. The resulting system consists of atoms in various electronic configurations, thermalizing on sub-picosecond to picosecond timescales after photoexcitation. We present a simulation study of x-ray-heated solid-density matter. For this we use XMDYN, a Monte-Carlo molecular-dynamics-based code with periodic boundary conditions, which allows one to investigate non-equilibrium dynamics. XMDYN is capable of treating systems containing light and heavy atomic species with full electronic configuration space and 3D spatial inhomogeneity. For the validation of our approach we compare for a model system the electron temperatures and the ion charge-state distribution from XMDYN to results for the thermalized system based on the average-atom model implemented in XATOM, an ab-initio x-ray atomic physics toolkit extended to include a plasma environment. Further, we also compare the average charge evolution of diamond with the predictions of a Boltzmann continuum approach. We demonstrate that XMDYN results are in good quantitative agreement with the above mentioned approaches, suggesting that the current implementation of XMDYN is a viable approach to simulate the dynamics of x-ray-driven non-equilibrium dynamics in solids. In order to illustrate the potential of XMDYN for treating complex systems we present calculations on the triiodo benzene derivative 5-amino-2,4,6-triiodoisophthalic acid (I3C), a compound of relevance of biomolecular imaging, consisting of heavy and light atomic species.

We propose and demonstrate a momentum filter for atomic gas based on a designed Talbot-Lau interferometer. It consists in two identical optical standing wave pulses separated by a delay equal to odd multiples of the half Talbot time. The one dimensional momentum width along the long direction of a cigar shape condensate is rapidly and greatly purified to a minimum, which corresponds to the ground state energy of the confining trap in our experiment. We find good agreement between theoretical analysis and experimental results. The filter is also effective for non-condensed cold atoms and could be applied widely.

Low-energy electrons (LEEs) are known to be effective in causing strand breaks in DNA. Recent experiments show that an important direct source of LEEs is the intermolecular Coulombic decay (ICD) process. Here we propose a new cascade mechanism initiated by core excitation and terminated by ICD and demonstrate its properties. Explicit calculations show that the energies of the emitted ICD-electrons can be controlled by selecting the initial atomic excitation. The properties of the cascade may have interesting applications in the fields of electron spectroscopy and radiation damage. Initiating such a cascade by resonant X-ray absorption from a high-Z element embedded in a cancerous cell nucleus, ICD will deliver genotoxic particles \textit{locally} at the absorption site, increasing in that way the controllability of the induced damage.

We propose a relaxation time approximation for the description of the dynamics of strongly excited fermion systems. Our approach is based on time-dependent density functional theory at the level of the local density approximation. This mean-field picture is augmented by collisional correlations handled in relaxation time approximation which is inspired from the corresponding semi-classical picture. The method involves the estimate of microscopic relaxation rates/times which is presently taken from the well established semi-classical experience. The relaxation time approximation implies evaluation of the instantaneous equilibrium state towards which the dynamical state is progressively driven at the pace of the microscopic relaxation time. As test case, we consider Na clusters of various sizes excited either by a swift ion projectile or by a short and intense laser pulse, driven in various dynamical regimes ranging from linear to strongly non-linear reactions. We observe a strong effect of dissipation on sensitive observables such as net ionization and angular distributions of emitted electrons. The effect is especially large for moderate excitations where typical relaxation/dissipation time scales efficiently compete with ionization for dissipating the available excitation energy. Technical details on the actual procedure to implement a working recipe of such a quantum relaxation approximation are given in appendices for completeness.

We apply a recently introduced model for an independent-atom-like calculation of ion-impact electron transfer and ionization cross sections to proton collisions from water, neon, and carbon clusters. The model is based on a geometrical interpretation of the cluster cross section as an effective area composed of overlapping circular disks that are representative of the atomic contributions. The latter are calculated using a time-dependent density-functional-theory-based single-particle description with accurate exchange-only ground-state potentials. We find that the net capture and ionization cross sections in p-X n collisions are proportional to n α with 2/3≤α≤1 . For capture from water clusters at 100 keV impact energy α is close to one, which is substantially different from the value α=2/3 predicted by a previous theoretical work based on the simplest-level electron nuclear dynamics method. For ionization at 100 keV and for capture at lower energies we find smaller α values than for capture at 100 keV. This can be understood by considering the magnitude of the atomic cross sections and the resulting overlaps of the circular disks that make up the cluster cross section in our model. Results for neon and carbon clusters confirm these trends. Simple parametrizations are found which fit the cross sections remarkably well and suggest that they depend on the relevant bond lengths.

To solve the time-dependent Schrödinger equation in spatially inhomogeneous pulses of electromagnetic radiation, we propose an iterative semi-classical complex trajectory approach. In numerical applications, we validate this method against ab initio numerical solutions by scrutinizing (a) electronic states in combined Coulomb and spatially homogeneous laser fields and (b) streaked photoemission from hydrogen atoms and plasmonic gold nanospheres. In comparison with streaked photoemission calculations performed in strong-field approximation, we demonstrate the improved reconstruction of the spatially inhomogeneous induced plasmonic infrared field near a nanoparticle surface from streaked photoemission spectra.

We present a proof-of-principle study of superconducting single photon detectors (SSPD) for the detection of individual neutral molecules/nanoparticles at low energies. The new detector is applied to characterize a laser desorption source for biomolecules and it allows to retrieve the arrival time distribution of a pulsed molecular beam containing the amino acid tryptophan, the polypeptide gramicidin as well as insulin, myoglobin and hemoglobin. We discuss the experimental evidence that the detector is actually sensitive to isolated neutral particles.