TY  - JOUR
A1  - Malý, Pavel
A1  - Brixner, Tobias
T1  - Fluorescence‐Detected Pump–Probe Spectroscopy
JF  - Angewandte Chemie International Edition
N2  - We introduce a new approach to transient spectroscopy, fluorescence‐detected pump–probe (F‐PP) spectroscopy, that overcomes several limitations of traditional PP. F‐PP suppresses excited‐state absorption, provides background‐free detection, removes artifacts resulting from pump–pulse scattering, from non‐resonant solvent response, or from coherent pulse overlap, and allows unique extraction of excited‐state dynamics under certain conditions. Despite incoherent detection, time resolution of F‐PP is given by the duration of the laser pulses, independent of the fluorescence lifetime. We describe the working principle of F‐PP and provide its theoretical description. Then we illustrate specific features of F‐PP by direct comparison with PP, theoretically and experimentally. For this purpose, we investigate, with both techniques, a molecular squaraine heterodimer, core–shell CdSe/ZnS quantum dots, and fluorescent protein mCherry. F‐PP is broadly applicable to chemical systems in various environments and in different spectral regimes.
KW  - femtochemistry
KW  - FL spectroscopy
KW  - time-resolved spectroscopy
KW  - transient absorption
Y1  - 2021
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-244811
VL  - 60
IS  - 34
SP  - 18867
EP  - 18875
ER  -