XAS studies of pressure-induced structural and electronic transformations in α-FeOOH.

Structural and electronic transformation taking place in α-FeOOH goethite have been studied by Fe K-edge x-ray absorption spectroscopy at pressures up to 50 GPa. These studies have shown the symmetrization of FeO6 octahedra coinciding with the Fe3+ high to low spin transition at pressure above ~45 GPa. Our data are in excellent agreement with the results of recent single crystal XRD and Mössbauer spectroscopy studies (Xu et al 2013 Phys. Rev. Lett. 111 175501), supporting the H-bonds symmetrization in iron oxyhydroxide, resulting from the Fe3+ high-to-low spin crossover at above 45 GPa. Our study shows an applicability of the x-ray absorption spectroscopy in a further study of the H-bonds symmetrization phenomenon.

The LUCIA beamline at SOLEIL.

Commissioned in May 2004 on the SLS machine, the LUCIA beamline was moved to the synchrotron SOLEIL during the summer of 2008. To take advantage of this new setting several changes to its design were introduced. Here, a review of the various improvements of the mechanics and, mostly, of the optics is given. Described in detail are the results of a new multilayer grating monochromator implemented on the Kohzu vessel already holding the two-crystal set-up. It consists of a grating grooved onto a multilayer (replacing the first crystal) associated to a multilayer (as a second crystal). It allows a shift of the low-energy limit of the beamline to around 500 eV with an energy resolution and a photon flux comparable with those of the previous couples of crystals (KTP and beryl).

Study by EXAFS of the local structure around Si on silicene deposited on Ag(1 1 0) and Ag(1 1 1) surfaces.

The local structure around the silicon atoms of silicene deposited onto Ag(1 1 0) and Ag(1 1 1) has been determined by extended x-ray absorption fine structure spectroscopy at the silicon K-edge. This study shows that silicon atoms are not in a flat honeycomb network locally buckled, but that this structure mimics the double Si(1 1 1)-plane of crystalline silicon with almost the same first and second interatomic distances (2.35 and 3.83 Å) on a regularly buckled geometry. Moreover the results evidence silver atoms at a well-defined distance from the silicon ones, a signature for an interaction between the silicene sheet and silver atoms released from the substrate.

Selecting core-hole localization or delocalization in CS2 by photofragmentation dynamics.

Electronic core levels in molecules are highly localized around one atomic site. However, in single-photon ionization of symmetric molecules, the question of core-hole localization versus delocalization over two equivalent atoms has long been debated as the answer lies at the heart of quantum mechanics. Here, using a joint experimental and theoretical study of core-ionized carbon disulfide (CS2), we demonstrate that it is possible to experimentally select distinct molecular-fragmentation pathways in which the core hole can be considered as either localized on one sulfur atom or delocalized between two indistinguishable sulfur atoms. This feat is accomplished by measuring photoelectron angular distributions within the frame of the molecule, directly probing entanglement or disentanglement of quantum pathways as a function of how the molecule dissociates.

Double momentum spectrometer for ion-electron vector correlations in dissociative photoionization.

We have developed a new momentum spectrometer dedicated to momentum vector correlations in the context of deep core photoionization of atomic and molecular species in the gas phase. In this article, we describe the design and operation of the experimental setup. The capabilities of the apparatus are illustrated with a set of measurements done on the sulphur core 1s photoionization of gas-phase CS2.

Ultrafast dynamics in postcollision interaction after multiple auger decays in argon 1s photoionization.

Argon 1s photoionization followed by multiple Auger decays is investigated both experimentally, by means of photoelectron-ion coincidences, and theoretically. A strong influence of the different Auger decays on the photoelectron spectra is observed through postcollision interaction which shifts the maximum of the energy distribution and distorts the spectral shape. A good agreement between the calculated and measured spectra for selected Ar(n+) ions (n=1-5) allows one to estimate the widths (lifetimes) of the intermediate states for each specific decay pathway.

Many-Pole Model of Inelastic Losses Applied to Calculations of XANES.

Conventional Kohn-Sham band-structure methods for calculating deep-core x-ray spectra typically neglect photoelectron self-energy effects, which give rise to an energy-dependent shift and broadening of the spectra. Here an a posteriori procedure is introduced to correct for these effects. The method is based on ab initio calculations of the GW self-energy using a many-pole model and a calculation of the dielectric function in the long wavelength limit using either the FEFF8 real-space Green's function code, or the AI2NBSE interface between the National Institute of Standards and Technology (NIST) Bethe-Salpeter equation solver (NBSE) and the ABINIT pseudopotential code. As an example the method is applied to core level x-ray spectra of LiF and MgAl2O4 calculated using (respectively) OCEAN, an extension of the AI2NBSE code for core level excitations, and the PARATEC pseudopotential code with the core-hole treated using a super-cell. The method satisfactorily explains the discrepancy between experiment and calculations.