Journal Article FZJ-2019-03534

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Identifying surface reaction intermediates with photoemission tomography

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2019
Nature Publishing Group UK [London]

Nature Communications 10(1), 3189 () [10.1038/s41467-019-11133-9]

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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.

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Contributing Institute(s):
  1. Funktionale Nanostrukturen an Oberflächen (PGI-3)
Research Program(s):
  1. 141 - Controlling Electron Charge-Based Phenomena (POF3-141) (POF3-141)
  2. DFG project 396769409 - Grundlagen der Photoemissionstomographie (396769409)

Appears in the scientific report 2019
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 Record created 2019-06-27, last modified 2023-08-15