A. Kivimäki

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.

A high-resolution N 1s photoionization study of the molecule in the near-threshold region

The angle-resolved N 1s photoelectron spectrum of has been measured with high resolution in the threshold region. An analysis of the vibrational fine structure yields a vibrational energy of and a lifetime broadening of for the core-ionized molecule. As in the case of C 1s ionization of CO, the vibrational fine structure changes considerably with photon energy in the region of both the shape resonance and the double excitations. Both the vibrationally resolved partial photoionization cross sections and asymmetry parameters have been determined in this photon energy range. The calculated cross sections in the literature are in reasonable agreement with experiment. In addition, we have measured the cross sections and asymmetry parameters of the most intense direct and conjugate shake-up satellites. The behaviour of the satellites is found to differ significantly from that of the corresponding C 1s satellites of CO.

The vibrationally resolved participator Auger spectra of selectively excited C 1s(2σ)−12π1 vibrational states in carbon monoxide

The fully vibrationally resolved participator Auger spectra originating from the decay of the C 1s(2σ)−12π1 resonance in CO are presented. The C 1s(2σ)−12π1 v’=0 resonance has been excited with a 75 meV monochromator bandpass, i.e., in Auger resonant Raman conditions, and the participator Auger spectrum observed. The C 1s(2σ)−12π1 v’=1 resonance is also excited and the corresponding participator Auger spectrum observed with a monochromator bandpass slightly larger than the inherent width. The results are compared to theoretical simulations using coherent lifetime‐vibrational interference theory which accounts for the details of the spectrum. We have observed an interference shift on the transitions to different vibrational sublevels in the final state. A high resolution C 1s photoelectron spectrum of CO is also presented. The lifetime width of the C 1s core–hole state is determined to be 97(10) meV, whereas the C 1s(2σ)−12π1 resonance is measured to have a width of 86(10) meV.

Performance of the modified SX‐700 plane grating monochromator at the Finnish beamline in MAX‐lab

A soft x‐ray beamline designed principally for gas phase measurements has been constructed and tested at the 550‐MeV MAX I electron storage ring in Lund, Sweden. The beamline uses synchrotron radiation from a short 35‐period undulator with a magnetic period of 24 mm. The photon energy range of the undulator is about 60–600 eV covering, e.g., the important C, N and O 1s ionization regions. The beamline is based on a modified SX‐700 plane grating monochromator with a plane elliptical focusing mirror. The beamline has been tested by measuring total ion and electron yield spectra from the rare gases Kr and Ar in the resonance excitation regions just below the Kr M4,5 and Ar L2,3 ionization thresholds. These results show that the monochromator has very high resolution, E/ΔE≊4800 at 244 eV and ≊7600 at 91 eV, comparable with the best spherical and plane grating monochromators. The beamline is equipped with an effective differential pumping system for the gas phase experiments combined with a refocusing mirror i...

A modular end-station for atomic, molecular, and cluster science at the low density matter beamline of FERMI@Elettra

The low density matter end-station at the new seeded free electron laser FERMI@Elettra is a versatile instrument for the study of atoms, molecules and clusters by means of electron and ion spectroscopies. Beams of atoms, molecules and helium droplets as well as clusters of atoms, molecules and metals can be produced by three different pulsed valves. The atomic and molecular beams may be seeded, and the clusters and droplets may be pure, or doped with other atoms and molecules. The electrons and ions produced by the ionization and fragmentation of the samples by the intense light of FERMI can be analysed by the available spectrometers, to give mass spectra and energy as well as angular distributions of charged particles. The design of the detector allows simultaneous detection of electrons and ions using velocity map imaging and time-of-flight techniques respectively. The instruments have a high energy/mass resolution and large solid-angle collection efficiency. We describe the current status of the apparatus and illustrate the potential for future experiments.

A comprehensive photoabsorption, photoionization, and shake-up excitation study of the C 1s cross section of benzene

The absolute photoabsorption cross section of benzene (C6H6), encompassing the C 1s−1 π*e2u resonance, the C 1s threshold, the satellite thresholds, and extending up to 800 eV, has been measured using synchrotron radiation. Measurements of the discrete absorption structure from below the C 1s ionization threshold have been performed at high resolution. In order to unambiguously assign all structure present in the photoabsorption cross section, C 1s photoelectron spectra were measured from the C 1s threshold region up to 350 eV along with satellite spectra. The C 1s−1 single-hole and the satellite cross sections have been derived in absolute units, and their angular distributions have been determined. Resonant and normal Auger spectra were taken on the main features of the photoabsorption and single-hole cross sections. From the best resolved photoelectron spectra the underlying structure in the asymmetric benzene photoelectron peak can be partly disentangled. The experimental data show that at least two v...

Auger decay of the dissociating core‐excited states in the HCl and DCl molecules

High‐resolution Auger electron spectra from the decay of the Cl 2p→σ* excitation in HCl and DCl have been measured. The spectra are analyzed, separating molecular and atomic features, which are assigned to transitions to the HCl (5σ2π)4σ* and Cl (3s3p)6 states, respectively. Auger line shapes, as affected by the molecular dissociation, are studied by comparing the experiment with the results of Monte‐Carlo computer simulations based on a semiclassical model.

The C 1s and N 1s near edge x-ray absorption fine structure spectra of five azabenzenes in the gas phase

Near edge x-ray absorption fine structure spectra have been measured and interpreted by means of density functional theory for five different azabenzenes (pyridine, pyridazine, pyrimidine, pyrazine, and s-triazine) in the gas phase. The experimental and theoretical spectra at the N 1s and C 1s edges show a strong resonance assigned to the transition of the 1s electron in the respective N or C atoms to the lowest unoccupied molecular orbital with pi(*) symmetry. As opposed to the N 1s edge, at the C 1s edge this resonance is split due to the different environments of the core hole atom in the molecule. The shift in atomic core-level energy due to a specific chemical environment is explained with the higher electronegativity of the N atom compared to the C atom. The remaining resonances below the ionization potential (IP) are assigned to sigma or pi [corrected] orbitals with mixed valence/Rydberg [corrected] character. Upon N addition, a reduction of intensity is observed in the Rydberg region at both edges as compared to the intensity in the continuum. Above the IP one or more resonances are seen and ascribed here to transitions to sigma(*) orbitals. Calculating the experimental and theoretical Delta(pi) term values at both edges, we observe that they are almost the same within +/-1 eV as expected for isoelectronic bonded pairs. The term values of the pi(*) and sigma(*) resonances are discussed in terms of the total Z number of the atoms participating in the bond.

FINNISH BEAMLINE AT MAX-LABORATORY - PROGRESS IN THE PHOTON ENERGY RESOLUTION

The photon energy resolution of the modified SX‐700 plane grating monochromator at the Finnish beamline (BL51) at MAX‐laboratory in Lund, Sweden, has improved considerably after proper alignment of the monochromator. Resolving powers of about 10 000 at hν≊90 eV and 5000 at hν≊400 eV have been achieved at the first diffraction order, as inferred from total ion yield measurements at the Kr 3d5/2→5p and N2 N1s→π* resonances. The total linewidth of ≤121 meV recorded for the Ar 2p3/2→4s excitation suggests that the lifetime broadening could be smaller than 116 meV obtained from electron energy‐loss spectroscopy.

Vibrational excitation in C 1s and O 1s photoionization of CO

The C 1s and O 1s photoelectron spectra of the CO molecule have been measured with high resolution. The vibrational spacing of the state is significantly lower than in the state and in the molecular ground state. Compared to the ground-state equilibrium C - O distance of 1.128 A, we extract from the analysis of the Franck - Condon factors bond lengths of 1.079(2) A and 1.167(4) A for the C 1s and O 1s core-ionized states, respectively.