Heteroatom oxidation controls singlet-triplet energy splitting in singlet fission building blocks.

Singlet fission (SF) is a promising multiexciton-generating process. Its demanding energy splitting criterion - that the S 1 energy must be at least twice that of T 1 - has limited the range of materials capable of SF. We propose heteroatom oxidation as a robust strategy to achieve sufficient S 1 /T 1 splitting, and demonstrate the potential of this approach for intramolecular SF.