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CPP: Fachverband Chemische Physik und Polymerphysik

CPP 15: Poster Session I

CPP 15.12: Poster

Montag, 17. März 2025, 19:00–21:00, P4

Impact of Classical and Quantum Light on Donor-Acceptor-Donor Molecules — •Haraprasad Mandal1,2, Sajal Kumar Giri3, Sara Jovanovski1, Oleg Varnavski1, Malgorzata Zagorska4, Roman Ganczarczyk4, Tse-Min Chiang3, George C. Schatz3, and Theodore Goodson III11Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, United States — 2Department of Chemistry, University of Graz, Heinrichstrasse 28, 8010 Graz, Austria — 3Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States — 4Faculty of Chemistry, Warsaw University of Technology, Noakowskiego 3, 00-664 Warsaw, Poland

Investigations of entangled and classical two-photon absorption have been carried out for six donor (D)-acceptor (A)-donor (D) compounds containing the dithieno pyrrole (DTP) unit as donor and acceptors with systematically varied electronic properties. Comparing ETPA (quantum) and TPA (classical) results reveals that the ETPA cross section decreases with increasing TPA cross section for molecules with highly off-resonant excited states for single-photon excitation. Theory (TDDFT) results are in semiquantitative agreement with this anticorrelated behavior due to the dependence of the ETPA cross section but not TPA on the two-photon excited state lifetime. The largest cross section is found for a DTP derivative that has a single photon excitation energy closest to resonance with half the two-photon excitation energy. These results are important for the possible use of quantum light for low-intensity energy-conversion applications

Keywords: Entangled two-photon absorption; ETPA cross-section; Entangled light; non-linear optics; Spontaneous parametric down-conversion

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