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MO: Fachverband Molekülphysik
MO 22: Ultrafast Dynamics III
MO 22.4: Talk
Thursday, March 13, 2025, 11:45–12:00, HS XVI
Higher-order signal separation in nonlinear spectroscopy: An intensity-based general approach — •Luisa Brenneis1, Jacob J. Krich2,3, Peter A. Rose2, Katja Mayershofer1, Simon Büttner1, 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, ON, Canada — 3Nexus for Quantum Technologies, University of Ottawa, Ottawa, ON, Canada — 4Department of Physics, University of Michigan, Ann Arbor, MI, USA — 5Faculty of Mathematics and Physics, Charles University, 121 16 Prague, Czech Republic
Nonlinear spectroscopic techniques, like two-dimensional electronic spectroscopy (2DES), are powerful tools for investigating multiparticle correlations and complex dynamics. However, depending on the pulse intensities, the detected signal consists of multiple perturbative orders exhibiting different lineshapes and dynamics. Separating these orders remains a universal challenge, especially while maintaining a high signal-to-noise ratio. Recently, we published an intensity-cycling scheme to extract nonlinear orders in transient absorption spectroscopy[1]. Now we present a generalized version to separate the perturbative orders in a wide range of spectroscopy techniques. In an experimental demonstration, we perform order separation in 2DES of squaraine polymers. We also derive the optimal intesities to minimize the combined effect of random and systematic errors.
[1] P. Malý et al., Nature 616, 280 (2023).
Keywords: 2D spectroscopy; Intensity dependency; Higher-order signals; Multiquantum 2D spectra; Ultrafast spectroscopy