Bonn 2025 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 22: Ultrafast Dynamics III
MO 22.5: Vortrag
Donnerstag, 13. März 2025, 12:00–12:15, HS XVI
Resolving higher-order signals through intensity cycling in two-dimensional electronic spectroscopy on the example of a squaraine dimer — •Katja Mayershofer1, Jacob J. Krich2,3, Luisa Brenneis1, Simon Büttner1, Peter A. Rose2, Julian Lüttig4, Pavel Malý5, and Tobias Brixner1 — 1Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg, Germany — 2Department of Physics, University of Ottawa, Ottawa, Ontario, Canada — 3Nexus for Quantum Technologies, University of Ottawa, Ottawa, Ontario, Canada — 4Department of Physics, University of Michigan, Ann Arbor, MI, USA — 5Faculty of Mathematics and Physics, Charles University, Prague, Czech Republic
Recently, we developed a variant of transient absorption spectroscopy that separates different perturbative orders of nonlinear response through “intensity cycling” [1]. We now extend this method, enabling separation of third- and higher-order contributions in two-dimensional (2D) spectra, by multiplication of a Vandermonde matrix with fluence-dependent 2D data. We apply this new method on a squaraine dimer to resolve nonlinear orders, allowing us to analyze uncontaminated signals and compare the lineshapes of different orders of nonlinear response. We perform simulations using the Ultrafast Spectroscopy Suite toolbox [2,3] to gain insight into the differences in lineshapes.
[1] P. Malý et al., Nature 2023, 616, 280.
[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