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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 Brixner11Institut 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).

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DPG-Physik > DPG-Verhandlungen > 2019 > Rostock