Mainz 2026 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 5: Ultrafast Electronic Dynamics
MO 5.5: Vortrag
Montag, 2. März 2026, 18:15–18:30, P 204
Investigating higher-excited-state properties through nonlinear order separation in two-dimensional electronic spectroscopy — •Katja Mayershofer1, Peter A. Rose2, Julian Lüttig2, Luisa Brenneis1, Simon Büttner1, Jacob J. Krich2,3, and Tobias Brixner1 — 1Institut für Physikalische und Theoretische Chemie, Universität Würzburg, 97074 Würzburg, Germany — 2Department of Physics, University of Ottawa, Ottawa, Ontario, Canada — 3Nexus for Quantum Technologies, University of Ottawa, Ottawa, Ontario, Canada
Recently, we developed an implementation of coherent two-dimensional (2D) electronic spectroscopy that enables us to separate signals of different pertubative orders through intensity variation and inversion with a Vandermonde matrix [1]. We applied this new technique to investigate a squaraine dimer. This procedure allowed us to obtain signals of different nonlinear orders that are uncontaminated from overlapping higher orders. We observe changes in the lineshapes from third to higher orders. To gain further insight into the higher-excited states of our sample, we performed simulations using the Ultrafast Spectroscopy Suite toolbox [2,3]. Through the combination of uncontaminated higher-order 2D signals and simulations, we retrieve transition dipole moments and energy levels of higher-excited states, giving us a new way to verify and improve theoretical models.
[1] J. J. Krich et al., J. Phys. Chem. Lett. 2025, 16, 5897.
[2] P. A. Rose & J. J. Krich, J. Chem. Phys 2021, 154, 034108.
[3] P. A. Rose & J. J. Krich, J. Chem. Phys 2021, 154, 034109.
Keywords: 2D spectroscopy; Intensity dependency; Higher-order signals; Multiquantum 2D spectra; Ultrafast spectroscopy