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O: Fachverband Oberflächenphysik
O 97: Organic Molecules on Inorganic Substrates: Electronic, Optical and Other Properties II
O 97.3: Vortrag
Freitag, 21. März 2025, 11:00–11:15, H6
Disentangling the components of a multireference excited state in an isolated chromophore — Rodrigo Ferreira1,2, Tomáš Neuman1, Amandeep Sagwal1, Jiří Doležal2, Petr Kahan1, and •Martin Švec1,2 — 1Institute of Physics, Czech Academy of Sciences — 2Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences
Excited states of open-shell chromophores are commonly multireference in their nature. Distinguishing the components of these superposition states in a single chromophore by experimental means is a challenging task as it would essentially require capturing their orbital occupancies in the excited state. We demonstrate this can be achieved by atomically precise mapping of photon-induced tunneling current under a varying electric field, on a model case of a PTCDA anionic excited state coupled to a plasmonic nanocavity. To simulate the cascade of energy conversions and charge transfer events occurring within the molecule, a set of rate equations is derived from a many-body state scheme using an input from TD-DFT. The resulting bias-dependent tunneling current maps reach a very good agreement with the experimental data, corroborating the validity of the theoretical understanding.
Keywords: chromophore; multireference; photocurrent; nanocavity; STM