Exploring three-dimensional orbital imaging with energy-dependent photoemission tomography

S. Weiß, D. Lüftner, T. Ules, E. M. Reinisch, H. Kaser, A. Gottwald, M. Richter, S. Soubatch, G. Koller, M. G. Ramsey, F. S. Tautz and P. Puschnig ()
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S. Weiß: Peter Grünberg Institut (PGI-3), Forschungszentrum Jülich
D. Lüftner: Institute of Physics, University of Graz, NAWI Graz
T. Ules: Institute of Physics, University of Graz, NAWI Graz
E. M. Reinisch: Institute of Physics, University of Graz, NAWI Graz
H. Kaser: Physikalisch-Technische Bundesanstalt (PTB)
A. Gottwald: Physikalisch-Technische Bundesanstalt (PTB)
M. Richter: Physikalisch-Technische Bundesanstalt (PTB)
S. Soubatch: Peter Grünberg Institut (PGI-3), Forschungszentrum Jülich
G. Koller: Institute of Physics, University of Graz, NAWI Graz
M. G. Ramsey: Institute of Physics, University of Graz, NAWI Graz
F. S. Tautz: Peter Grünberg Institut (PGI-3), Forschungszentrum Jülich
P. Puschnig: Institute of Physics, University of Graz, NAWI Graz

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: Abstract Recently, it has been shown that experimental data from angle-resolved photoemission spectroscopy on oriented molecular films can be utilized to retrieve real-space images of molecular orbitals in two dimensions. Here, we extend this orbital tomography technique by performing photoemission initial state scans as a function of photon energy on the example of the brickwall monolayer of 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA) on Ag(110). The overall dependence of the photocurrent on the photon energy can be well accounted for by assuming a plane wave for the final state. However, the experimental data, both for the highest occupied and the lowest unoccupied molecular orbital of PTCDA, exhibits an additional modulation attributed to final state scattering effects. Nevertheless, as these effects beyond a plane wave final state are comparably small, we are able, with extrapolations beyond the attainable photon energy range, to reconstruct three-dimensional images for both orbitals in agreement with calculations for the adsorbed molecule.

Date: 2015
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DOI: 10.1038/ncomms9287

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