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Our article was placed on the cover of the prestigious ChemPhotoChem journal. In this work we have studied the ability of a series of azoarylfuroxans to photoisomerization. Upon visible light irradiation, (E)‐arylazo‐1,2,5‐oxadiazoles underwent photoisomerization to the corresponding (Z)‐isomers which are stable under ambient conditions. Structural factors affecting the photoswitching ability were also revealed. NO donor properties of the synthesized arylazofuroxans were also evaluated in vitro and it was found that (Z)‐arylazofuroxans released significantly larger amounts of NO than the corresponding (E)‐isomers, which suggests strong potential of these molecular photoswitches in photopharmacology and other biomedical applications.

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