Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy

Mueller S, Draeger S, Ma X, Hensen M, Kenneweg T, Pfeiffer W, Brixner T (2018)
JOURNAL OF PHYSICAL CHEMISTRY LETTERS 9(8): 1964-1969.

Zeitschriftenaufsatz | Veröffentlicht | Englisch
 
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Abstract / Bemerkung
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 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.
Erscheinungsjahr
2018
Zeitschriftentitel
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Band
9
Ausgabe
8
Seite(n)
1964-1969
ISSN
1948-7185
Page URI
https://pub.uni-bielefeld.de/record/2920333

Zitieren

Mueller S, Draeger S, Ma X, et al. Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy. JOURNAL OF PHYSICAL CHEMISTRY LETTERS. 2018;9(8):1964-1969.
Mueller, S., Draeger, S., Ma, X., Hensen, M., Kenneweg, T., Pfeiffer, W., & Brixner, T. (2018). Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 9(8), 1964-1969. doi:10.1021/acs.jpclett.8b00541
Mueller, S., Draeger, S., Ma, X., Hensen, M., Kenneweg, T., Pfeiffer, W., and Brixner, T. (2018). Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy. JOURNAL OF PHYSICAL CHEMISTRY LETTERS 9, 1964-1969.
Mueller, S., et al., 2018. Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy. JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 9(8), p 1964-1969.
S. Mueller, et al., “Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy”, JOURNAL OF PHYSICAL CHEMISTRY LETTERS, vol. 9, 2018, pp. 1964-1969.
Mueller, S., Draeger, S., Ma, X., Hensen, M., Kenneweg, T., Pfeiffer, W., Brixner, T.: Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy. JOURNAL OF PHYSICAL CHEMISTRY LETTERS. 9, 1964-1969 (2018).
Mueller, Stefan, Draeger, Simon, Ma, Xiaonan, Hensen, Matthias, Kenneweg, Tristan, Pfeiffer, Walter, and Brixner, Tobias. “Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy”. JOURNAL OF PHYSICAL CHEMISTRY LETTERS 9.8 (2018): 1964-1969.

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