Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy
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- We demonstrate two-quantum (2Q) coherent two-dimensional (2D)electronic spectroscopy using a shot-to-shot-modulated pulse shaper and fluorescence detection. Broadband collinear excitation is realized with the supercontinuum output of an argon-filled hollow-core fiber, enabling us to excite multiple transitions simultaneously in the visible range. The 2Q contribution is extracted via a three-pulse sequence with 16-fold phase cycling and simulated employing cresyl violet as a model system. Furthermore, we report the first experimental realizationWe demonstrate two-quantum (2Q) coherent two-dimensional (2D)electronic spectroscopy using a shot-to-shot-modulated pulse shaper and fluorescence detection. Broadband collinear excitation is realized with the supercontinuum output of an argon-filled hollow-core fiber, enabling us to excite multiple transitions simultaneously in the visible range. The 2Q contribution is extracted via a three-pulse sequence with 16-fold phase cycling and simulated employing cresyl violet as a model system. Furthermore, we report the first experimental realization of one-quantum−two-quantum (1Q-2Q) 2D spectroscopy, offering less congested spectra as compared with the 2Q implementation. We avoid scattering artifacts and nonresonant solvent contributions by using fluorescence as the observable. This allows us to extract quantitative information about doubly excited states that agree with literature expectations. The high sensitivity and background-free nature of fluorescence detection allow for a general applicability of this method to many other systems.…
Autor(en): | Stefan Müller, Simon Draeger, Kiaonan Ma, Matthias Hensen, Tristan Kenneweg, Walter Pfeiffer, Tobias Brixner |
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URN: | urn:nbn:de:bvb:20-opus-173468 |
Dokumentart: | Preprint (Vorabdruck) |
Institute der Universität: | Fakultät für Chemie und Pharmazie / Institut für Physikalische und Theoretische Chemie |
Sprache der Veröffentlichung: | Englisch |
Titel des übergeordneten Werkes / der Zeitschrift (Englisch): | Journal of Physical Chemistry Letters |
Erscheinungsjahr: | 2018 |
Originalveröffentlichung / Quelle: | Journal of Physical Chemistry Letters 2018, 9 (8), pp 1964–1969. doi:10.1021/acs.jpclett.8b00541 |
URL der Erstveröffentlichung: | https://pubs.acs.org/doi/10.1021/acs.jpclett.8b00541 |
DOI: | https://doi.org/10.1021/acs.jpclett.8b00541 |
Sonstige beteiligte Institutionen: | Fakultät für Physik, Universität Bielefeld |
Allgemeine fachliche Zuordnung (DDC-Klassifikation): | 5 Naturwissenschaften und Mathematik / 54 Chemie / 541 Physikalische Chemie |
Normierte Schlagworte (GND): | Fluoreszenz; Optische Spektroskopie; Molekülzustand |
Freie Schlagwort(e): | Doppelquantenkohärenz; Zweidimensionale Spektroskopie; elektronisch angeregte Zustände |
Datum der Freischaltung: | 13.12.2018 |
EU-Projektnummer / Contract (GA) number: | 614623 |
OpenAIRE: | OpenAIRE |
Lizenz (Deutsch): | Deutsches Urheberrecht |