Singlet fission in naturally-organized carotenoid molecules - Archive ouverte HAL
Article Dans Une Revue Physical Chemistry Chemical Physics Année : 2021

Singlet fission in naturally-organized carotenoid molecules

Résumé

We have investigated the photophysics of aggregated lutein/violaxanthin in daffodil chromoplasts. We reveal the presence of three carotenoid aggregate species, the main one composed of a mixture of lutein/violaxanthin absorbing at 481 nm, and two secondary populations of aggregated carotenoids absorbing circa 500 and 402 nm. The major population exhibits an efficient singlet fission process, generating μs-lived triplet states on an ultrafast timescale. The structural organization of aggregated lutein/violaxanthin in daffodil chromoplasts produces well-defined electronic levels that permit the energetic pathways to be disentangled unequivocally, allowing us to propose a consistent mechanism for singlet fission in carotenoid aggregates. Transient absorption measurements on this system reveal for the first time an entangled triplet signature for carotenoid aggregates, and its evolution into dissociated triplet states. A clear picture of the carotenoid singlet fission pathway is obtained, which is usually blurred due to the intrinsic disorder of carotenoid aggregates.
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hal-03282317 , version 1 (13-07-2021)

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Annamaria Quaranta, Anja Krieger-Liszkay, Andrew Pascal, François Perreau, Bruno Robert, et al.. Singlet fission in naturally-organized carotenoid molecules. Physical Chemistry Chemical Physics, 2021, 23 (8), pp.4768-4776. ⟨10.1039/D0CP04493H⟩. ⟨hal-03282317⟩
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