Dresden 2014 – scientific programme
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O: Fachverband Oberflächenphysik
O 69: Focussed Session: Towards a Quantitative Understanding of Complex Adsorption Structures: Surface Science goes Organic II
O 69.9: Talk
Thursday, April 3, 2014, 13:00–13:15, HSZ 01
3D Tomographic Imaging of Molecular Orbitals in Real Space — •Pascal Nigge1,2, Martin Graus1,2, Vitaliy Feyer3,4, Michael Wiessner1,2, Achim Schöll1,2, and Friedrich Reinert1,2 — 1Universität Würzburg, 97074 Würzburg, Germany — 2Karlsruher Institut für Technologie KIT, 76021 Karlsruhe, Germany — 3Research Center Jülich, 52425 Jülich, Germany — 4Sincrotrone Trieste, 34012 Basovizza, Trieste, Italy
The imaging of molecular orbitals by angle resolved photoelectron spectroscopy (ARPES) or photoemission electron microscopy (PEEM) has shown to be a very powerful tool for the investigation of molecular materials. By mapping the angle dependent intensity patterns of photoelectrons this technique provides tomographic images of the density distribution of the orbitals in k-space. The full potential of the tomographic mapping of molecular orbitals becomes obvious by providing three-dimensional images of orbitals in real space. While this has already been proposed theoretically, the practical realization requires access to variable photon energies at a synchrotron. We present first experimental data that demonstrates how 3D-imaging of molecular orbitals is feasible with a PEEM, which allows reconstruction of the molecular orbital in momentum space from the hemispherical k-space tomograms. Utilizing the additional phase information derived from experiments with circular light polarization, the full molecular orbital can be uncovered in 3D in real space by a Fourier transformation, thus providing unprecedented insight into the electronic structure of molecules.