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Search: WFRF:(Lassalle L.) > (2019)

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  • Guillemin, R., et al. (author)
  • Photoelectron-Auger-electron angular-momentum transfer in core-ionized Ar : Beyond the standard post-collision-interaction model
  • 2019
  • In: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : AMER PHYSICAL SOC. - 2469-9926 .- 2469-9934. ; 99:6
  • Journal article (peer-reviewed)abstract
    • Electron-ion coincidence experimental data obtained following argon 1s photoionization are reported. Slow photoelectrons were measured in coincidence with Ar+ and Ar2+ ions, and the beta angular distribution parameter was obtained. The measured beta parameter for the Ar2+-photoelectron coincidence measurements shows a significant deviation from the beta = 2 expected value. With the support of a quantum mechanical theory of post-collision interaction (PCI) which goes beyond the standard model, we attribute this deviation to angular-momentum exchange due to the interaction of the photoelectron with the Auger electron, while the role of the residual ion is negligible. The main mechanism of angular-momentum transfer and its effect on the asymmetry parameter beta near the photoionization threshold are considered.
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3.
  • Lassalle, L., et al. (author)
  • Structure of intermediates of the water oxidation reaction in photosystem II
  • 2019
  • In: Acta Crystallographica Section A. - : International Union of Crystallography. - 2053-2733. ; A75
  • Journal article (other academic/artistic)abstract
    • Photosystem II (PSII) catalyzes the light driven oxidation of water into dioxygen, protons and electrons. This reaction takes place at the oxygen evolving complex (OEC) a Mn4CaO5 cluster, through five intermediate S-states (S0 to S4), S1 being the dark-stable state and S3 the highest oxidized semi-stable state before O-O bond formation and O2 evolution. We have been using fs X-ray pulses from an X-ray free electron laser (XFEL) to study the geometric and electronic structure of the OEC over the reaction cycle and recently reported high-resolution (around 2 Å) structures of PSII at room temperature for the four stable states in the S-state cycle as well as for two time points in the S2-S3 transition. Our results reveal important structural changes including the binding of one additional ‘water’, Ox, during the S2→S3 state transition. The binding of the additional oxygen Ox in the S3 state between Ca and Mn1 suggests O-O bond formation mechanisms involving O5 as one substrate, where Ox is either the other substrate oxygen or is perfectly positioned to refill the O5 position during O2 release. We also explored the extended network of H-bonds between amino acid residues and waters connecting the OEC to the bulk solvent. We observed several significant changes in this network during the S-state cycle. Based on these data we will discuss the dynamics of the catalytic site and its environment over the reaction cycle.
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