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CPP: Fachverband Chemische Physik und Polymerphysik
CPP 27: Molecular Electronics and Excited State Properties II
CPP 27.5: Vortrag
Mittwoch, 19. März 2025, 12:30–12:45, H38
Computational insights into open-shell molecules for applications in molecular electronics — •Susanne Leitherer1 and Gemma C. Solomon1,2 — 1Department of Chemistry and Center of Nanoscience, University of Copenhagen, Denmark — 2Niels Bohr Institute, University of Copenhagen, Denmark
Recent studies have explored a range of molecules with unpaired electrons, represented by their spin. These investigations focused on the charge transport characteristics of the molecules when interfaced with electrodes, as well as their structural rearrangements in electric fields and interactions with surfaces. The theoretical analysis of these systems frequently employs spin-polarized or symmetry-broken unrestricted density functional theory (DFT). This method has proven effective in modeling oxidized molecules exhibiting highly conductive low-energy states, characterized as 1D topological insulators[1]. However, it is well known that DFT can pose challenges for open-shell structures due to their multiconfigurational nature. We demonstrate how for a selection of polycyclic aromatic hydrocarbons - previously investigated in recent scanning probe experiments[2] - the ground state can be accurately determined using a multi-configurational short-range DFT approach[3]. [1] High Molecular Conductance and Inverted Conductance Decay over 3nm in Aminium-Terminated Carbon-Bridged Oligophenylene-Vinylenes, Krieger et al, JACS (2024); [2] Atomically resolved single-molecule triplet quenching, Peng et al., Science 373 (2021); [3] Multiconfigurational sr-DFT for open-shell systems, Hedegard et al, J. Chem. Phys. 148, 214103 (2018)
Keywords: Molecular electronics; Electron transport; Multiconfigurational electronic structure; Density functional theory; Spin