Stacey Ristinmaa Sörensen

Beam line I411 at MAX II - Performance and first results

We report on the characteristics and first results from the soft X-ray beam line I411, based on an undulator at the third generation synchrotron facility MAX II, Sweden. The beam line is designed for high-resolution, angle-resolved electron spectroscopy on gases, liquids and solids. Main components are the modified SX700 monochromator and the end station, both of which were previously used at beam line 51 at MAX I. The end station is equipped with a rotatable SES-200 hemispherical electron-analyser. Before the end station, a one-metre section is reserved for exchangeable experimental set-ups. The usable photon energy range is 50-1500 eV and the photon flux is two orders of magnitudes higher compared to beam line 51. At 400 eV a resolving power of about 5700 in the first order of the monochromator grating could be obtained. In gas phase, a total electron energy resolution of 16 meV has been achieved. Detailed results on the undulator performance, flux, photon and electron energy resolution as well as some technical details are presented here. As an example of the capabilities of the beam line I411, we present the fully vibrationally resolved Auger resonant Raman electron spectrum of gas-phase N 2.

Vibrational fine structure in the C 1s core level photoemission of chemisorbed molecules : Ethylene and ethylidyne on Rh(111)

The origin of fine structure in the core-level photoemission spectra of the C2H4, C2D4, C2H3 and C2D3 molecules chemisorbed on Rh(111) is probed in a careful high-resolution study showing that this structure arises from internal molecular vibrations rather than from other chemically-shifted carbon atoms. It is shown by comparison of the adsorbate and gas-phase spectra that the underlying features are the same despite differences arising from adsorption. This new approach to the investigation of adsorbed molecules may prove to be useful in further studies of other systems and the possibility that such effects may exist could lead to the reinterpretation of other adsorbate systems.

Vibrational fine structure in the C 1s photoemission spectrum of the methoxy species chemisorbed on Cu(100)

The C 1s photoemission spectrum of methoxy (CH3O) chemisorbed on Cu(100) is demonstrated to contain a resolvable fine structure due to excitation of the molecular C-H normal vibrational mode. The origin of the fine structure is ascertained by substituting hydrogen with deuterium in the methoxy overlayers and by comparison to gas-phase C 1s spectra for methanol (CH3OH). The vibrational fine structure is demonstrated to provide a fingerprint of the hydrocarbon group present on the surface.

The surface core-level shift of the Pd(100) single-crystal surface

The surface core-level shift of the Pd(100) single-crystal surface has been measured from high-resolution Pd 3d core-level spectra. The surface atoms are found to have 0.44+or-0.03 eV lower binding energy than the bulk atoms. The result is compared with theoretical estimates.

The O 1s photoelectron spectrum of molecular oxygen revisited

High-resolution photoelectron spectra of the inner-shell levels of molecular oxygen have been measured using synchrotron radiation. The vibrational structure of the two magnetically-split core-shell components is analyzed based upon ab initio calculations. The ratio between the intensities of the two components was analyzed at several different ionization energies up to about 600 eV, and the same is discussed and compared to high-energy ionization intensities. A theoretical calculation shows very good agreement with the measured spectra. The calculation implements a model where two parity components make up the 4Σ peak profile. The gerade–ungerade energy split for this state is found to be 50 meV.

Specific production of very long-lived core-excited sulfur atoms by 2p−1σ* excitation of the OCS molecule followed by ultrafast dissociation

A core-excited sulfur state with a lifetime almost one order of magnitude longer than in molecular 2p core-hole states is selectively produced by ultrafast dissociation of S 2p -> sigma* excited OCS. Clear evidence for this is provided by strong atomic peaks (20% of the total intensity) in x-ray fluorescence but very weak ones (2%) in the corresponding resonant Auger spectrum. Corroborating the assignment of the spectra, ab initio calculations explain the enhanced lifetime: the Auger decay of the produced D-3(3) (2p(5)3p(5)) sulfur state is strongly decreased as it contradicts a newly derived propensity rule of the L2,3MM Auger decay.

Development and characterization of a multiple-coincidence ion-momentum imaging spectrometer.

The design and performance of a high-resolution momentum-imaging spectrometer for ions which is optimized for experiments using synchrotron radiation is presented. High collection efficiency is achieved by a focusing electrostatic lens; a long drift tube improves mass resolution and a position-sensitive detector enables measurement of the transverse momentum of ions. The optimisation of the lens for particle momentum measurement at the highest resolution is described. We discuss the overall performance of the spectrometer and present examples demonstrating the momentum resolution for both kinetics and for angular measurements in molecular fragmentation for carbon monoxide and fullerenes. Examples are presented that confirm that complete space-time focussing is possible for a two-field three-dimensional imaging spectrometer.

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 lead 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.

Magnetron-based source of neutral metal vapors for photoelectron spectroscopy

The construction of a magnetron-based source for neutral metal vapors is presented. The first photoelectron spectroscopy experiments with the source using synchrotron radiation at MAX-lab, Sweden are described. Photoelectron spectra of atomic copper, silver, and nickel are reported with an 80 meV resolution for Cu and Ag, previously not achieved in experiments using synchrotron light. (c) 2006 American Institute of Physics.

Nuclear motion and symmetry breaking of the B 1s-excited BF3 molecule

Out-of-plane nuclear motion stimulated in the core-excited state and symmetry breaking due to this nuclear motion have been investigated for B Is excitation in the BF3 molecule by a combination of three different experimental methods: angle-resolved ion-yield spectroscopy, vibrationally resolved resonant Auger electron spectroscopy and quadruple-ion coincidence momentum-imaging technique