Optical Cycling Functionalization of Arenes

Closed, laser-induced optical transitions (“optical cycling transitions”) of molecules can be used for state preparation and measurement in quantum information science sensing. Increasingly complex molecular species supporting provide new capabilities science, it is not clear if there a limit on their size or complexity. We explore Ca–O–L constructs to support the center, Ca, with ligands, L, being arenes. find that L as large coronene (i.e., CaOC24H11) without losing diagonality Franck–Condon factor (FCF). Furthermore, substituted electron-withdrawing groups improve FCF. Larger beyond ∼7 rings, disrupt FCF by closing HOMO–LUMO ligand electronic gap reordering local states center. Overall, we retained arenes, offer principle design.