Erlangen 2018 – scientific programme

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MO: Fachverband Molekülphysik

MO 21: Advanced Time-Resolved Spectroscopy

MO 21.1: Talk

Thursday, March 8, 2018, 14:00–14:15, PA 2.150

Broadband fluorescence-detected one- and two-quantum 2D electronic spectroscopy — •Stefan Müller, Simon Draeger, Xiaonan Ma, Matthias Hensen, and Tobias Brixner — Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg, Germany

We developed a single-beam setup for 2D electronic spectroscopy in the liquid phase using fluorescence as an observable [1]. Collinear femtosecond phase-modulated pulse trains are generated by an acousto-optic dispersive filter on a 1 kHz shot-to-shot basis. Broadband excitation in the visible spectral range is provided by the supercontinuum output of an argon-filled hollow-core fiber. By utilizing phase cycling we demonstrate the simultaneous acquisition of different nonlinear signal contributions such as photon-echo, two-quantum coherence and one-quantum-two-quantum signals without nonresonant solvent response or scattering artifacts that pose a substantial challenge in noncollinear coherence-detected 2D spectroscopy. We show that information about nuclear wave-packet dynamics, doubly excited states as well as coupling between excited states can be received from these nonlinear signals.
[1] S. Draeger, S. Roeding, and T. Brixner, Opt. Express 25, 3259 (2017).