TY  - INPR
A1  - Müller, Stefan
A1  - Draeger, Simon
A1  - Ma, Kiaonan
A1  - Hensen, Matthias
A1  - Kenneweg, Tristan
A1  - Pfeiffer, Walter
A1  - Brixner, Tobias
T1  - Fluorescence-Detected Two-Quantum and One-Quantum-Two-Quantum 2D Electronic Spectroscopy
T2  - Journal of Physical Chemistry Letters
N2  - 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.
KW  - Zweidimensionale Spektroskopie
KW  - elektronisch angeregte Zustände
KW  - Doppelquantenkohärenz
KW  - Fluoreszenz
KW  - Optische Spektroskopie
KW  - Molekülzustand
Y1  - 2018
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-173468
UR  - https://pubs.acs.org/doi/10.1021/acs.jpclett.8b00541
ER  -