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Rapid multiple-quantum three-dimensional fluorescence spectroscopy disentangles quantum pathways

Please always quote using this URN: urn:nbn:de:bvb:20-opus-202529
  • 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.show moreshow less

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Metadaten
Author: 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
URN:urn:nbn:de:bvb:20-opus-202529
Document Type:Journal article
Faculties: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
Language:English
Parent Title (English):Nature Communications
Year of Completion:2019
Volume:10
Pagenumber:4735
Source:Nature Communications (2019) 10:4735. https://doi.org/10.1038/s41467-019-12602-x
DOI:https://doi.org/10.1038/s41467-019-12602-x
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Tag:Atomic and molecular interactions with photons; Optical spectroscopy
Release Date:2020/05/14
Collections:Open-Access-Publikationsfonds / Förderzeitraum 2019
Licence (German):License LogoCC BY: Creative-Commons-Lizenz: Namensnennung 4.0 International