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MO: Fachverband Molekülphysik

MO 7: Poster: Spectroscopy

MO 7.18: Poster

Tuesday, March 12, 2024, 17:00–19:00, Tent C

Cross-peak analysis of multiquantum signals with polarization-controlled higher-order transient absorption spectroscopy — •Katja Mayershofer1, Simon Büttner1, Julian Lüttig2, Peter A. Rose3, Jacob J. Krich3,4, and Tobias Brixner11Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg — 2Department of Physics, University of Michigan, Ann Arbor, MI, USA — 3Department of Physics, University of Ottawa, Ottawa, Ontario, Canada — 4Nexus for Quantum Technologies, University of Ottawa, Ottawa, Ontario, Canada

A well-established application of two-dimensional (2D) spectroscopy is the characterization of energy transfer processes via analyzing of 2D cross-peaks. In transient absorption (TA) measurements, by contrast, signals from 2D off-diagonal and on-diagonal contributions overlap on the detection axis. In a recent paper, Zanni’s group [1] presented a new polarization scheme that suppresses diagonal peaks and makes it possible to investigate cross-peak features with TA spectroscopy. We adapted and applied this polarization scheme to the new method of higher-order TA spectroscopy [2] that separates signals of different orders and thus isolates signals stemming from exciton–exciton interactions (EEI). Through the combination of higher-order TA spectroscopy and polarization control we aim to analyze cross-peak features in fifth-order signals originating from EEI in a squaraine heterodimer.

[1] K. M. Farrell et al., PNAS 2022, 119, e2117398118.

[2] P. Malý et al., Nature 2023, 616, 280.

Keywords: 2D Spectroscopy; Transient absorption spectroscopy; Polarization control; Multiquantum processes; Higher-order spectroscopy

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