Combined orbital tomography study of multi-configurational molecular adsorbate systems

Pavel Kliuiev, Giovanni Zamborlini, Matteo Jugovac, Yeliz Gurdal, Karin von Arx, Kay Waltar, Stephan Schnidrig, Roger Alberto, Marcella Iannuzzi, Vitaliy Feyer, Matthias Hengsberger, Jürg Osterwalder and Luca Castiglioni ()
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Pavel Kliuiev: University of Zurich
Giovanni Zamborlini: Forschungszentrum Jülich
Matteo Jugovac: Forschungszentrum Jülich
Yeliz Gurdal: University of Zurich
Karin von Arx: University of Zurich
Kay Waltar: University of Zurich
Stephan Schnidrig: University of Zurich
Roger Alberto: University of Zurich
Marcella Iannuzzi: University of Zurich
Vitaliy Feyer: Forschungszentrum Jülich
Matthias Hengsberger: University of Zurich
Jürg Osterwalder: University of Zurich
Luca Castiglioni: University of Zurich

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

Abstract: Abstract 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 $$3d$$3d 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.

Date: 2019
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DOI: 10.1038/s41467-019-13254-7

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