Novel π-extended coumarin-based chromophores were designed with two-photon absorption (TPA) character in the near-IR region. Caged benzoates with a TP-responsive chromophore were synthesized, and their TP-uncaging reactions were conducted under near-IR light. The 6,7-dimethoxy-substituted derivative had a high TPA cross-section of 69 GM at 740 nm. The 7-methoxy-substituted derivative showed a high TPA uncaging efficiency with a TPA efficiency of 3.4 GM at 710 nm.
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