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Fluorescent photosensitizers (PSs) often encounter low singlet oxygen (O) quantum yields and fluorescence quenching in the aggregated state, mainly involving the intersystem crossing process. Herein, we successfully realize maximizing O quantum yields of fluorescent PSs through promoting radical-pair intersystem crossing (RP-ISC), which serves as a molecular symmetry-controlling strategy of donor-acceptor (D-A) motifs. The symmetric quadrupolar A-D-A molecule PTP exhibits an excellent O quantum yield of 97.

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