Photogeneration of Long-Lived Triplet States through Singlet Fission in Lycopene H-Aggregates

Molecular triplet excitons produced through singlet fission (SF) usually have shorter triplet lifetimes due to exciton–exciton recombination and relaxation pathways, thereby resulting in complex device architectures for SF-boosted solar cells. Using broadband transient absorption spectroscopy, we here show that the photoexcitation of nanostructured lycopene H-aggregates at room temperature produces free triplets with an unprecedented 35-fold enhancement in the lifetime compared to those localized on the monomer backbone. The observed rise of a spectrally blue-shifted correlated T–T pair state in ∼19 ps with distinct vibronic features provides the basis for SF-induced triplet generation.