Catalysis in real time using X-ray lasers

Research output: Contribution to journalJournal article – Annual report year: 2017Researchpeer-review

Without internal affiliation

  • Author: Nilsson, A.

    Royal Institute of Technology

  • Author: LaRue, J.

    Chapman University

  • Author: Öberg, H.

    Royal Institute of Technology

  • Author: Ogasawara, H.

    Stanford University

  • Author: Dell'Angela, M.

    Consiglio Nazionale delle Ricerche - Istituto Officina dei Materiali

  • Author: Beye, M.

    German Electron Synchrotron

  • Author: Öström, H.

    Royal Institute of Technology

  • Author: Gladh, J.

    Royal Institute of Technology

  • Author: Nørskov, J. K.

    Stanford University

  • Author: Wurth, W.

    University of Hamburg

  • Author: Abild-Pedersen, F.

    Stanford University

  • Author: Pettersson, L. G. M.

    Royal Institute of Technology

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We describe how the unique temporal and spectral characteristics of X-ray free-electron lasers (XFEL) can be utilized to follow chemical transformations in heterogeneous catalysis in real time. We highlight the systematic study of CO oxidation on Ru(0 0 0 1), which we initiate either using a femtosecond pulse from an optical laser or by activating only the oxygen atoms using a THz pulse. We find that CO is promoted into an entropy-controlled precursor state prior to desorbing when the surface is heated in the absence of oxygen, whereas in the presence of oxygen, CO desorbs directly into the gas phase. We monitor the activation of atomic oxygen explicitly by the reduced split between bonding and antibonding orbitals as the oxygen comes out of the strongly bound hollow position. Applying these novel XFEL techniques to the full oxidation reaction resulted in the surprising observation of a significant fraction of the reactants at the transition state through the electronic signature of the new bond formation.

Original languageEnglish
JournalChemical Physics Letters
Pages (from-to)145-173
Number of pages29
Publication statusPublished - 2017
Externally publishedYes
CitationsWeb of Science® Times Cited: No match on DOI

ID: 160466027