Large Distortion of Fused Aromatics on Dielectric Interlayers Quantified by Photoemission Orbital Tomography.

Autor:	Hurdax P; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Kern CS; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Boné TG; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Haags A; Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425Jülich, Germany.; Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, 52425Jülich, Germany.; Experimentalphysik IV A, RWTH Aachen University, 52074Aachen, Germany., Hollerer M; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Egger L; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Yang X; Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425Jülich, Germany.; Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, 52425Jülich, Germany.; Experimentalphysik IV A, RWTH Aachen University, 52074Aachen, Germany., Kirschner H; Physikalisch-Technische Bundesanstalt (PTB), 10587Berlin, Germany., Gottwald A; Physikalisch-Technische Bundesanstalt (PTB), 10587Berlin, Germany., Richter M; Physikalisch-Technische Bundesanstalt (PTB), 10587Berlin, Germany., Bocquet FC; Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425Jülich, Germany.; Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, 52425Jülich, Germany., Soubatch S; Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425Jülich, Germany.; Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, 52425Jülich, Germany., Koller G; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Tautz FS; Peter Grünberg Institute (PGI-3), Forschungszentrum Jülich, 52425Jülich, Germany.; Jülich Aachen Research Alliance (JARA), Fundamentals of Future Information Technology, 52425Jülich, Germany.; Experimentalphysik IV A, RWTH Aachen University, 52074Aachen, Germany., Sterrer M; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Puschnig P; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria., Ramsey MG; Institute of Physics, University of Graz, NAWI Graz, Universitätsplatz 5, 8010Graz, Austria.
Jazyk:	angličtina
Zdroj:	ACS nano [ACS Nano] 2022 Oct 25; Vol. 16 (10), pp. 17435-17443. Date of Electronic Publication: 2022 Oct 14.
DOI:	10.1021/acsnano.2c08631
Abstrakt:	Polycyclic aromatic compounds with fused benzene rings offer an extraordinary versatility as next-generation organic semiconducting materials for nanoelectronics and optoelectronics due to their tunable characteristics, including charge-carrier mobility and optical absorption. Nonplanarity can be an additional parameter to customize their electronic and optical properties without changing the aromatic core. In this work, we report a combined experimental and theoretical study in which we directly observe large, geometry-induced modifications in the frontier orbitals of a prototypical dye molecule when adsorbed on an atomically thin dielectric interlayer on a metallic substrate. Experimentally, we employ angle-resolved photoemission experiments, interpreted in the framework of the photoemission orbital tomography technique. We demonstrate its sensitivity to detect geometrical bends in adsorbed molecules and highlight the role of the photon energy used in experiment for detecting such geometrical distortions. Theoretically, we conduct density functional calculations to determine the geometric and electronic structure of the adsorbed molecule and simulate the photoemission angular distribution patterns. While we found an overall good agreement between experimental and theoretical data, our results also unveil limitations in current van der Waals corrected density functional approaches for such organic/dielectric interfaces. Hence, photoemission orbital tomography provides a vital experimental benchmark for such systems. By comparison with the state of the same molecule on a metallic substrate, we also offer an explanation why the adsorption on the dielectric induces such large bends in the molecule.
Databáze:	MEDLINE
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