Nuclear motion in molecular ions studied with synchrotron radiation and multicoincidence momentum imaging spectrometry

A momentum imaging spectrometer optimized for photoionization experiments with synchrotron radiation was built in 2008. The spectrometer is equipped with an electrostatic lens, that focuses the charged dissociation products on to a position-sensitive multi-hit delay line anode. The possibility of focusing is essential for most applications, where fragment momentum is to be extracted. The apparatus is equipped with a micro-channel-plate detector opposite to the delay line anode, enabling electron-ion coincidence experiments and thereby mass-resolved ion spectroscopy independent of the time structure of the synchrotron radiation. Calibration and characterization of the instrument is explained. Results for the photo-fragmentation of several molecules are presented, including measurements of kinetic and angular distributions as well as momentum correlations between coincident fragments. Various data analysis methods are described. High sensitivity of the instrument enables detection and analysis of weak processes such as isomerization. Full three-dimensional momentum information for each coincidence event is achieved which allows for in depth understanding of geometry, dynamics and energetics. In Ethyne, molecules with a cis-bending motion has been identified. In carbonyl sulfide and carbon dioxide, the Renner-Teller splitting has been analyzed. For the water molecule, transient isomerization has been found to be induced by strong bending vibrations in core-excited states. Also studies have been made on clusters, displaying the capability of the instrument to measure a large range of masses and kinetic energies

The role of charge and proton transfer in fragmentation of hydrogen-bonded nanosystems: the breakup of ammonia clusters upon single photon multi-ionization

The charge and proton dynamics in hydrogen-bonded networks are investigated using ammonia as a model system. The fragmentation dynamics of medium-sized clusters (1-2 nm) upon single photon multi-ionization is studied, by analyzing the momenta of small ionic fragments. The observed fragmentation pattern of the doubly- and triply- charged clusters reveals a spatial anisotropy of emission between fragments (back-to-back). Protonated fragments exhibit a distinct kinematic correlation, indicating a delay between ionization and fragmentation (fission). The different kinematics observed for channels containing protonated and unprotonated species provides possible insights into the prime mechanisms of charge and proton transfer, as well as proton hopping, in such a nanoscale system.Comment: 9 pages, 6 figure

Dynamics of proton migration and dissociation in core-excited ethyne probed by multiple ion momentum imaging

The study focuses on the rapid geometry change in ethyne, excited near the carbon 1s edge. Core excitation and ionization leads to population of dicationic states in ethyne. We study three competing dissociation pathways associated with deprotonation in the linear ethyne molecule, and two cases of rapid proton migration. We investigate the alignment of the molecule in the excited state, and find startling differences in these three cases. We present evidence for a strong anisotropy in the production of H+2 /C+2 fragments through a rapid deformation of the molecule to a dibridged conformation with the transition dipole moment parallel to the polarization of the exciting radiation

Role of the Renner-Teller effect after core hole excitation in the dissociation dynamics of carbon dioxide dication.

The fragmentation of the doubly-charged carbon dioxide molecule is studied after photoexcitation to the C 1s(1)2π(u) and O 1s(1)2π(u) states using a multicoincidence ion-imaging technique. The bent component of the Renner-Teller split states populated in the 1s→ π∗ resonant excitation at both the carbon and oxygen 1s ionization edges opens pathways to potential surfaces in highly bent geometries in the dication. Evidence for a complete deformation of the molecule is found in the coincident detection of C(+) and O(2) (+) ions. The distinct alignment of this fragmentation channel indicates rapid deformation and subsequent fragmentation. Investigation of the complete atomization dynamics in the dication leading to asymmetric charge separation shows that the primary dissociation mechanisms, sequential, concerted, and asynchronous concerted, are correlated to specific fragment kinetic energies. The study shows that the bond angle in fragmentation can extend below 20°

Site-dependent nuclear dynamics in core-excited butadiene

Symmetry breaking and competition between electronic decay and nuclear dynamics are major factors determining whether the memory of the initial core-hole localisation in a molecule is retained long enough to affect fragmentation. We investigate the fate of core holes localised at different sites in the free 1,3 trans butadiene molecule by using synchrotron radiation to selectively excite core electrons from different C 1s sites to π* orbitals. Fragmentation involving bonds localised at the site of the core hole provides clear evidence for preferential bond breaking for a core hole located at the terminal carbon site, while the signature of localisation is weak for a vacancy on the central carbon site. The origin of this difference is attributed to out-of-plane vibrations, and statistical evaporation of protons for vacancies located at the central carbon sites

Ionization-site effects on the photofragmentation of chloro- and bromoacetic acid molecules

Fragmentation of gas-phase chloro- and bromoacetic acid samples, particularly its dependency on the atomic site of the initial core ionization, was studied in photoelectron-photoion-photoion coincidence (PEPIPICO) measurements. The fragmentation was investigated after ionizing carbon 1s and bromine 3d or chlorine 2p core orbitals. It was observed that the samples had many similar fragmentation pathways and that their relative weights depended strongly on the initial ionization site. Additional Auger PEPIPICO measurements revealed a clear dependence of fragment pair intensities on the kinetic energy of the emitted Auger electrons. The modeled and measured Auger electron spectra indicated that the average internal energy of the molecule was larger following the carbon 1s core-hole decay than after the decay of the halogen core hole. This difference in the internal energies was found to be the source of the site-dependent photofragmentation behavior.</p

Multiple-core-hole resonance spectroscopy with ultraintense X-ray pulses

Understanding the interaction of intense, femtosecond X-ray pulses with heavy atoms is crucial for gaining insights into the structure and dynamics of matter. One key aspect of nonlinear light-matter interaction was, so far, not studied systematically at free-electron lasers -- its dependence on the photon energy. Using resonant ion spectroscopy, we map out the transient electronic structures occurring during the complex charge-up pathways. Massively hollow atoms featuring up to six simultaneous core holes determine the spectra at specific photon energies and charge states. We also illustrate how the influence of different X-ray pulse parameters that are usually intertwined can be partially disentangled. The extraction of resonance spectra is facilitated by the fact that the ion yields become independent of the peak fluence beyond a saturation point. Our study lays the groundwork for novel spectroscopies of transient atomic species in exotic, multiple-core-hole states that have not been explored previously.Comment: Supplementary information is include

Opportunities for Two-Color Experiments in the Soft X-ray Regime at the European XFEL

X-ray pump/X-ray probe applications are made possible at X-ray Free Electron Laser (XFEL) facilities by generating two X-ray pulses with different wavelengths and controllable temporal delay. In order to enable this capability at the European XFEL, an upgrade project to equip the soft X-ray SASE3 beamline with a magnetic chicane is underway. In the present paper we describe the status of the project, its scientific focus and expected performance, including start-to-end simulations of the photon beam transport up to the sample, as well as recent experimental results demonstrating two-color lasing at photon energies of 805 eV + 835 eV and 910 eV + 950 eV. Additionally, we discuss methods to analyze the spectral properties and the intensity of the generated radiation to provide on-line diagnostics for future user experiments

Dissociative double-photoionization of butadiene in the 25-45 eV energy range using 3-D multi-coincidence ion momentum imaging spectrometry

Dissociative double-photoionization of butadiene in the 25-45 eV energy range has been studied with tunable synchrotron radiation using full three-dimensional ion momentum imaging. Using ab initio calculations, the electronic states of the molecular dication below 33 eV are identified. The results of the measurement and calculation show that double ionization from π orbitals selectively triggers twisting about the terminal or central C–C bonds. We show that this conformational rearrangement depends upon the dication electronic state, which effectively acts as a gateway for the dissociation reaction pathway. For photon energies above 33 eV, three-body dissociation channels where neutral H-atom evaporation precedes C–C charge-separation in the dication species appear in the correlation map. The fragment angular distributions support a model where the dication species is initially aligned with the molecular backbone parallel to the polarization vector of the light, indicating a high probability for double-ionization to the “gateway states” for molecules with this orientation

Brandteknisk riskvärdering av Göteborgs stadsbibliotek

This report is a fire safety evaluation of Gothenburg’s public library. It includes a visit of the library where the writers of the report control and evaluate the existing fire safety procedures and equipment. Focus lies on the human safety in the means of evacuation and critical conditions during that time. The goal is that no critical conditions occur during the time it takes to evacuate the library or a specified compartment in the library. Computer modeled simulations and hand calculations are used in the process when controlling and evaluating if the fire safety is sufficient. If not, a list of improvements and recommendations are suggested to the library. The report includes three specified scenarios in which the writers control existing conditions, calculate and at the end suggest improvements for the library. The overall suggestion for increasing and insuring human safety during evacuation includes an installation of sprinklers in the building. This requirement is to be met if a satisfied evacuation is to be made