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Catalysis in real time using X-ray lasers
Stockholm University, Faculty of Science, Department of Physics.
Stockholm University, Faculty of Science, Department of Physics.
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Number of Authors: 12
2017 (English)In: Chemical Physics Letters, ISSN 0009-2614, E-ISSN 1873-4448, Vol. 675, 145-173 p.Article in journal (Refereed) Published
Abstract [en]

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(0001), 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.

Place, publisher, year, edition, pages
2017. Vol. 675, 145-173 p.
National Category
Chemical Sciences Physical Sciences
Identifiers
URN: urn:nbn:se:su:diva-143458DOI: 10.1016/j.cplett.2017.02.018ISI: 000400200800025OAI: oai:DiVA.org:su-143458DiVA: diva2:1106264
Available from: 2017-06-07 Created: 2017-06-07 Last updated: 2017-06-07Bibliographically approved

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Nilsson, AndersÖberg, HenrikÖström, HenrikGladh, JörgenPettersson, Lars G. M.
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