Singlet fission (SF) in two or more electronically coupled organic chromophores converts a high-energy singlet excitoninto two low-energy triplet excitons, which can be used to increase solar cell efficiency. Many known SF chromophoresare unsuitable for device applications due to chemical instability and low triplet state energies. This work summarizesstructurally dependent SF dynamics for 9,10-bis(phenylethynyl)anthracene (BPEA) and its derivatives in the solid-stateusing time-resolved optical spectroscopies, and electronic structure calculations. By modulating the packing structure inthin films, we can effectively tune electronic energy and coupling. The systematic study in BPEA organicsemiconductors shows that maximizing the thermodynamic driving force can achieve the highest SF rate and efficiency.
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