The photochemistry and photophysics of papaverine N‐oxide in polar aprotic and protic solvents has been studied in detail. Complex energy and charge‐transfer phenomena between chromophores occur in papaverine. New photochemistry for the papaverine N‐oxide system is reported. Irradiation in protic media results in the formation of an emissive charge‐transfer state with ensuing intramolecular hydroxylation in high isolated yields (75–80%).

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