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J Phys Chem Lett. 2018 Apr 19;9(8):1964-1969. doi: 10.1021/acs.jpclett.8b00541. Epub 2018 Apr 5.

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

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Institut für Physikalische und Theoretische Chemie , Universität Würzburg , Am Hubland , 97074 Würzburg , Germany.
Fakultät für Physik , Universität Bielefeld , Universitätsstr. 25 , 33615 Bielefeld , Germany.
Center for Nanosystems Chemistry (CNC) , Universität Würzburg , Theodor-Boveri-Weg , 97074 Würzburg , Germany.


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.

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