Rostock 2019 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 14: Ultrafast Multidimensional and Control Approaches
MO 14.2: Vortrag
Mittwoch, 13. März 2019, 14:15–14:30, S HS 001 Biologie
Rapid coherent three-dimensional fluorescence spectroscopy disentangles quantum pathways of a molecular dianion — •Stefan Müller1, Julian Lüttig1, Lei Ji2, Jie Han3, Michael Moos5, Todd B. Marder2, Uwe H. F. Bunz4, Andreas Dreuw3, Christoph Lambert5, and Tobias Brixner1 — 1Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg — 2Institut für Anorganische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg — 3Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 205, 69120 Heidelberg — 4Organisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 270, 69120 Heidelberg — 5Institut für Organische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg
We developed a rapid shot-to-shot operating single-beam setup for electronic three-dimensional (3D) spectroscopy that uses fluorescence as an observable [1]. With this, we systematically acquire various types of 3D spectra, including multiple-quantum coherences, simultaneously, background free, inherently phased and within a few minutes. This allows us to study systems of limited chemical stability, such as the dianion of TIPS-tetraazapentacene [2]. Using a 125-fold phase cycling scheme, we isolate multiple 3D spectra that provide rich information up to sixth order in perturbation theory, revealing electronic coupling, nuclear wavepacket dynamics, highly-excited states, and more.
[1] S. Draeger et al., Opt. Express 25, 3259 (2017).
[2] L. Ji et al., J. Am. Chem. Soc. 139, 15968-15976 (2017).