Mainz 2026 – scientific programme
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MO: Fachverband Molekülphysik
MO 5: Ultrafast Electronic Dynamics
MO 5.6: Talk
Monday, March 2, 2026, 18:30–18:45, P 204
Efficient Two-Dimensional Spectroscopy Simulations including Realistic Pulse Shapes, Overlapping, and Time-Ordering Effects — •Rémi Gilliot1,2, Matteo Russo1, Alexander Blech1, Manuel Joffre2, Christiane Koch1, and Hélène Seiler1 — 1Freie Universität Berlin, Berlin, Germany — 2Institut Polytechnique de Paris, Palaiseau, France
Two-dimensional (2D) spectroscopy is a powerful pump-pump-probe method to reveal coupling between quantum states and disentangle optical response contributions. We present an efficient approach for simulating 2D spectra with arbitrary pulse shapes including overlapping and time-ordering. Under the assumption of simple dephasing, we show that the emitted signal expression reduces to three independent nested integrals, that can be computed in linear time. We utilize this approach to study the impact of spectral phase distortions and strongly non-Gaussian pulse shapes - such as those produced experimentally by hollow-core fibers.
Keywords: 2D Spectroscopy; Efficient Simulations; Realistic Pulse Shapes; Overlapping Effects; Time-Ordering Effects