2024/06/21 by Sebastian V. Pios, Maxim F. Gelin, Pios, Sebastian V. +6 · 1 citation
Biochemistry, Genetics and Molecular Biology · Environmental Science · Medicine · #Advanced Fluorescence Microscopy Techniques #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Optical Imaging and Spectroscopy Techniques #Water Quality Monitoring and Analysis
paper · pdf · doi:10.48550/arxiv.2406.15262
openalex publication_date 2024/06/21 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
Two-dimensional (2D) fluorescence-excitation (2D-FLEX) spectroscopy is a recently proposed nonlinear femtosecond technique for the detection of photoinduced dynamics. The method records a time-resolved fluorescence signal in its excitation- and detection-frequency dependence, and hence combines the exclusive detection of excited state dynamics (fluorescence) with signals resolved in both excitation and emission frequencies (2D electronic spectroscopy). In this work, we develop an on-the-fly protocol for the simulation of 2D-FLEX spectra of molecular systems, which is based on interfacing the classical doorway-window representation of spectroscopic responses with trajectory surface hopping simulations. Applying this methodology to the gas-phase pyrazine, we show that femtosecond 2D-FLEX spectra can deliver detailed information otherwise obtainable via attosecond spectroscopy.