Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.168
Publication date: 18th July 2019
The S1 (21Ag-) state is an optically dark state of natural and synthetic pi-conjugated materials that can play a critical role in optoelectronic processes such as, energy harvesting, photoprotection and singlet fission [1,2]. Despite this widespread importance, direct experimental characterisations of the electronic structure of the S1 (21Ag-) wave function have remained scarce and uncertain, although advanced theory predicts it to have a rich multi-excitonic character [3]. Here, studying an archetypal polymer, polydiacetylene, and carotenoids, we experimentally demonstrate that S1 (21Ag-) is a superposition state with strong contributions from spin-entangled pairs of triplet excitons (1(TT)). We further show that optical manipulation of the S1 (21Ag-) wave function using triplet absorption transitions allows selective projection of the 1(TT) component into a manifold of spatially separated triplet-pairs with lifetimes enhanced by up to one order of magnitude and whose yield is strongly dependent on the level of inter-chromophore coupling. Our results provide a unified picture of 21Ag- states in pi-conjugated materials and open new routes to exploit their dynamics in singlet fission, photobiology and for the generation of entangled (spin-1) particles for molecular quantum technologies [4].
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