Identifying surface reaction intermediates with photoemission tomography

Xiaosheng Yang, Larissa Egger, Philipp Hurdax, Hendrik Kaser, Daniel Lüftner, François C. Bocquet, Georg Koller, Alexander Gottwald, Petra Tegeder, Mathias Richter, Michael G. Ramsey, Peter Puschnig, Serguei Soubatch () and F. Stefan Tautz
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Xiaosheng Yang: Forschungszentrum Jülich
Larissa Egger: University of Graz
Philipp Hurdax: University of Graz
Hendrik Kaser: Physikalisch-Technische Bundesanstalt (PTB)
Daniel Lüftner: University of Graz
François C. Bocquet: Forschungszentrum Jülich
Georg Koller: University of Graz
Alexander Gottwald: Physikalisch-Technische Bundesanstalt (PTB)
Petra Tegeder: Ruprecht-Karls-Universität Heidelberg
Mathias Richter: Physikalisch-Technische Bundesanstalt (PTB)
Michael G. Ramsey: University of Graz
Peter Puschnig: University of Graz
Serguei Soubatch: Forschungszentrum Jülich
F. Stefan Tautz: Forschungszentrum Jülich

Nature Communications, 2019, vol. 10, issue 1, 1-6

Abstract: Abstract The determination of reaction pathways and the identification of reaction intermediates are key issues in chemistry. Surface reactions are particularly challenging, since many methods of analytical chemistry are inapplicable at surfaces. Recently, atomic force microscopy has been employed to identify surface reaction intermediates. While providing an excellent insight into the molecular backbone structure, atomic force microscopy is less conclusive about the molecular periphery, where adsorbates tend to react with the substrate. Here we show that photoemission tomography is extremely sensitive to the character of the frontier orbitals. Specifically, hydrogen abstraction at the molecular periphery is easily detected, and the precise nature of the reaction intermediates can be determined. This is illustrated with the thermally induced reaction of dibromo-bianthracene to graphene which is shown to proceed via a fully hydrogenated bisanthene intermediate. We anticipate that photoemission tomography will become a powerful companion to other techniques in the study of surface reaction pathways.

Date: 2019
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DOI: 10.1038/s41467-019-11133-9

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