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We have carried out a combined theoretical (at the TDDFT BLYP/6-311++G** level of theory) and experimental study of the mechanism of phototautmerization of the N(3)H oxo tautomer of isocytosine dissolved in a water medium. The study reveals that this photoreaction occurs along the 1πσ* excited-state reaction paths of the oxo and hydroxy tautomers of the compound through conical intersections S0/S1...