Resonant Inelastic X-Ray Scattering Reveals Hidden Local Transitions of the Aqueous OH Radical.

Autor: Kjellsson L; Department of Physics and Astronomy, Uppsala University, Box 516, S-751 20 Uppsala, Sweden., Nanda KD; Department of Chemistry, University of Southern California, Los Angeles, California 90007, USA., Rubensson JE; Department of Physics and Astronomy, Uppsala University, Box 516, S-751 20 Uppsala, Sweden., Doumy G; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Southworth SH; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Ho PJ; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., March AM; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Al Haddad A; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Kumagai Y; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Tu MF; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA., Schaller RD; Center for Nanoscale Materials, Argonne National Laboratory, Lemont, Illinois 60439, USA.; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA., Debnath T; Division of Chemistry and Biological Chemistry, Nanyang Technological University, Singapore 639798., Bin Mohd Yusof MS; Division of Chemistry and Biological Chemistry, Nanyang Technological University, Singapore 639798., Arnold C; Center for Free-Electron Laser Science, DESY, 22607 Hamburg, Germany.; Department of Physics, Universität Hamburg, 20146 Hamburg, Germany.; Hamburg Centre for Ultrafast Imaging, 22607 Hamburg, Germany., Schlotter WF; LCLS, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA., Moeller S; LCLS, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA., Coslovich G; LCLS, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA., Koralek JD; LCLS, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA., Minitti MP; LCLS, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA., Vidal ML; DTU Chemistry-Department of Chemistry, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark., Simon M; Sorbonne Université and CNRS, Laboratoire de Chimie Physique-Matière et Rayonnement, 75252 Paris Cedex 05, France., Santra R; Center for Free-Electron Laser Science, DESY, 22607 Hamburg, Germany.; Department of Physics, Universität Hamburg, 20146 Hamburg, Germany.; Hamburg Centre for Ultrafast Imaging, 22607 Hamburg, Germany., Loh ZH; Division of Chemistry and Biological Chemistry, Nanyang Technological University, Singapore 639798., Coriani S; DTU Chemistry-Department of Chemistry, Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark., Krylov AI; Department of Chemistry, University of Southern California, Los Angeles, California 90007, USA., Young L; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, USA.; Department of Physics and James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA.
Jazyk: angličtina
Zdroj: Physical review letters [Phys Rev Lett] 2020 Jun 12; Vol. 124 (23), pp. 236001.
DOI: 10.1103/PhysRevLett.124.236001
Abstrakt: Resonant inelastic x-ray scattering (RIXS) provides remarkable opportunities to interrogate ultrafast dynamics in liquids. Here we use RIXS to study the fundamentally and practically important hydroxyl radical in liquid water, OH(aq). Impulsive ionization of pure liquid water produced a short-lived population of OH(aq), which was probed using femtosecond x-rays from an x-ray free-electron laser. We find that RIXS reveals localized electronic transitions that are masked in the ultraviolet absorption spectrum by strong charge-transfer transitions-thus providing a means to investigate the evolving electronic structure and reactivity of the hydroxyl radical in aqueous and heterogeneous environments. First-principles calculations provide interpretation of the main spectral features.
Databáze: MEDLINE