Target Analysis Resolves the Ground and Excited State Properties from Femtosecond Stimulated Raman Spectra

Overview

Journal J Phys Chem Lett

Publisher American Chemical Society

Specialty Chemistry

Date 2024 Sep 6

PMID 39241188

Authors

Ivo H M van Stokkum

Joris J Snellenburg

Petra Chrupkova

Jakub Dostal

Sebastian Weigand

Jorn Weissenborn

John T M Kennis

Miroslav Kloz

Affiliations

Soon will be listed here.

Abstract

Target analysis is employed to resolve the ground and excited state properties from simultaneously measured Femtosecond Stimulated Raman Spectra (FSRS) and Transient Absorption Spectra (TAS). FSRS is a three-pulse technique, involving picosecond Raman pump pulses and femtosecond visible pump and probe pulses. The TAS are needed to precisely estimate the properties of the Instrument Response Function. The prezero "coherent artifact" present during the overlap of the three pulses is described by a damped oscillation with a frequency (ω - ) where is a ground state resonance Raman frequency. Simultaneous target analysis of the FSRS and TAS allows the complete excited state dynamics to be resolved with a time resolution better than 100 fs. The model system studied is the carotenoid lycopene in tetrahydrofuran. The lycopene dynamics show a spectral evolution with seven states, including a biphasic cooling process during the S2-S1 internal conversion, multiple S1 lifetimes, and an S* state decaying with a lifetime of 7 ps.

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