Rapid multiple-quantum three-dimensional fluorescence spectroscopy disentangles quantum pathways
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- Coherent two-dimensional spectroscopy is a powerful tool for probing ultrafast quantum dynamics in complex systems. Several variants offer different types of information but typically require distinct beam geometries. Here we introduce population-based three-dimensional (3D) electronic spectroscopy and demonstrate the extraction of all fourth- and multiple sixth-order nonlinear signal contributions by employing 125-fold (1⨯5⨯5⨯5) phase cycling of a four-pulse sequence. Utilizing fluorescence detection and shot-to-shot pulse shaping inCoherent two-dimensional spectroscopy is a powerful tool for probing ultrafast quantum dynamics in complex systems. Several variants offer different types of information but typically require distinct beam geometries. Here we introduce population-based three-dimensional (3D) electronic spectroscopy and demonstrate the extraction of all fourth- and multiple sixth-order nonlinear signal contributions by employing 125-fold (1⨯5⨯5⨯5) phase cycling of a four-pulse sequence. Utilizing fluorescence detection and shot-to-shot pulse shaping in single-beam geometry, we obtain various 3D spectra of the dianion of TIPS-tetraazapentacene, a fluorophore with limited stability at ambient conditions. From this, we recover previously unknown characteristics of its electronic two-photon state. Rephasing and nonrephasing sixth-order contributions are measured without additional phasing that hampered previous attempts using noncollinear geometries. We systematically resolve all nonlinear signals from the same dataset that can be acquired in 8 min. The approach is generalizable to other incoherent observables such as external photoelectrons, photocurrents, or photoions.…
Autor(en): | Stefan Mueller, Julian Lüttig, Pavel Malý, Lei Ji, Jie Han, Michael Moos, Todd B. Marder, Uwe H. F. Bunz, Andreas Dreuw, Christoph Lambert, Tobias Brixner |
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URN: | urn:nbn:de:bvb:20-opus-202529 |
Dokumentart: | Artikel / Aufsatz in einer Zeitschrift |
Institute der Universität: | Fakultät für Chemie und Pharmazie / Institut für Anorganische Chemie |
Fakultät für Chemie und Pharmazie / Institut für Organische Chemie | |
Fakultät für Chemie und Pharmazie / Institut für Physikalische und Theoretische Chemie | |
Sprache der Veröffentlichung: | Englisch |
Titel des übergeordneten Werkes / der Zeitschrift (Englisch): | Nature Communications |
Erscheinungsjahr: | 2019 |
Band / Jahrgang: | 10 |
Seitenangabe: | 4735 |
Originalveröffentlichung / Quelle: | Nature Communications (2019) 10:4735. https://doi.org/10.1038/s41467-019-12602-x |
DOI: | https://doi.org/10.1038/s41467-019-12602-x |
Allgemeine fachliche Zuordnung (DDC-Klassifikation): | 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
Freie Schlagwort(e): | Atomic and molecular interactions with photons; Optical spectroscopy |
Datum der Freischaltung: | 14.05.2020 |
Sammlungen: | Open-Access-Publikationsfonds / Förderzeitraum 2019 |
Lizenz (Deutsch): | CC BY: Creative-Commons-Lizenz: Namensnennung 4.0 International |