Combined orbital tomography study of multi-configurational molecular adsorbate systems.

Autor:	Kliuiev P; Department of Physics, University of Zurich, 8057, Zurich, Switzerland.; Department of Applied Physics, Aalto University School of Science, FI-00076, Aalto, Finland., Zamborlini G; Peter Grünberg Institute (PGI-6), Forschungszentrum Jülich, 52425, Jülich, Germany.; Technische Universität Dortmund, Experimentelle Physik VI, 44227, Dortmund, Germany., Jugovac M; Peter Grünberg Institute (PGI-6), Forschungszentrum Jülich, 52425, Jülich, Germany., Gurdal Y; Department of Chemistry, University of Zurich, 8057, Zurich, Switzerland.; Department of Bioengineering, Adana Alparslan Turkes Science and Technology University, 01250, Adana, Turkey., Arx KV; Department of Physics, University of Zurich, 8057, Zurich, Switzerland., Waltar K; Department of Physics, University of Zurich, 8057, Zurich, Switzerland., Schnidrig S; Department of Chemistry, University of Zurich, 8057, Zurich, Switzerland., Alberto R; Department of Chemistry, University of Zurich, 8057, Zurich, Switzerland., Iannuzzi M; Department of Chemistry, University of Zurich, 8057, Zurich, Switzerland., Feyer V; Peter Grünberg Institute (PGI-6), Forschungszentrum Jülich, 52425, Jülich, Germany., Hengsberger M; Department of Physics, University of Zurich, 8057, Zurich, Switzerland., Osterwalder J; Department of Physics, University of Zurich, 8057, Zurich, Switzerland., Castiglioni L; Department of Physics, University of Zurich, 8057, Zurich, Switzerland. castiglioni@physik.uzh.ch.
Jazyk:	angličtina
Zdroj:	Nature communications [Nat Commun] 2019 Nov 20; Vol. 10 (1), pp. 5255. Date of Electronic Publication: 2019 Nov 20.
DOI:	10.1038/s41467-019-13254-7
Abstrakt:	Molecular reactivity is determined by the energy levels and spatial extent of the frontier orbitals. Orbital tomography based on angle-resolved photoelectron spectroscopy is an elegant method to study the electronic structure of organic adsorbates, however, it is conventionally restricted to systems with one single rotational domain. In this work, we extend orbital tomography to systems with multiple rotational domains. We characterise the hydrogen evolution catalyst Co-pyrphyrin on an Ag(110) substrate and compare it with the empty pyrphyrin ligand. In combination with low-energy electron diffraction and DFT simulations, we fully determine adsorption geometry and both energetics and spatial distributions of the valence electronic states. We find two states close to the Fermi level in Co-pyrphyrin with Co [Formula: see text] character that are not present in the empty ligand. In addition, we identify several energetically nearly equivalent adsorption geometries that are important for the understanding of the electronic structure. The ability to disentangle and fully elucidate multi-configurational systems renders orbital tomography much more useful to study realistic catalytic systems.
Databáze:	MEDLINE
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