Journal
CHEMICAL PHYSICS
Volume 357, Issue 1-3, Pages 181-187Publisher
ELSEVIER
DOI: 10.1016/j.chemphys.2009.01.002
Keywords
Artificial light harvesting; Carotenoid deactivation; Ultrafast spectroscopy; Energy transfer; Excitation energy dependence
Funding
- Nederlandse organisatie voor Wetenschappelijk Onderzoek (NWO)
- Spanish Ministry of Education and Science [FIS2008-06368-C02-02]
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Ultrafast relaxation of a carotenoid in an artificial light harvesting complex has been studied by transient absorption spectroscopy. The transient signal amplitudes at several wavelengths as well as the amplitudes of the underlying species associated spectra (SAS) are analysed for several excitation energies ranging over more than two orders of magnitude (10 nJ/pulse LIP to 3000 nJ/pulse). Our analysis shows that the contribution from the so-called S* signal on the long-wavelength side of the first allowed S-0 -> S-2 transition has a markedly different excitation energy dependence and saturation behaviour than the electronic excited state S-1. These observations are modelled and explained in terms of a two-photon excitation of a vibrationally hot ground state via an impulsive stimulated Raman scattering (ISRS). The experimental observations of the varying pulse energy dependencies of different excited state species are supported by an analysis based on a density-matrix formalism. (C) 2009 Elsevier B.V. All rights reserved.
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