Abstract
We report high-yield triplet generation by singlet fission upon photoexcitation of a new aggregate of the carotenoid all-trans 3R,3′R-zeaxanthin. The yield is determined by picosecond time-resolved resonance Raman spectroscopy, which allows direct characterization and quantification of triplet excited-state signatures and ground-state depletion. The technique and analysis reveals that triplets form within picoseconds. A quantum yield of 90−200% is derived with the assumption of weak exciton-coupling in the zeaxanthin aggregate.

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