Carotenoids are an integral part of natural photosynthetic complexes, with tasks ranging from light harvesting to photoprotection. Their underlying energy deactivation network of optically dark and bright excited states is extremely efficient: after excitation of light with up to 2.5 eV of photon energy, the system relaxes back to ground state on a time scale of a few picoseconds. In this article, we summarize how a model based on the vibrational energy relaxation approach (VERA) explains the main characteristics of relaxation dynamics after one-photon excitation with special emphasis on the so-called S* state. Lineshapes after two-photon excitation are beyond the current model of VERA. We outline this future line of research in our article. In terms of experimental method development, we discuss which techniques are needed to better describe energy dissipation effects in carotenoids and within the first solvation shell.

Biology Centre Institute of Plant Molecular Biology Czech Academy of Sciences Branišovská 1160 31 370 05 České Budějovice Czech Republic

Department of Physics Faculty of Science University of South Bohemia Branišovská 1760 370 05 České Budějovice Czech Republic

Digital Environment Research Institute Queen Mary University of London London E1 4NS U K

Dynamical Spectroscopy Department of Chemistry Technical University of Munich Lichtenbergstraße 4 85748 Garching bei Munich Germany

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