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The parent thioketene S‐oxide H2CCSO has been generated in the gas phase through flash vacuum pyrolysis (ca. 1000 K) of vinyl sulfoxide H2CC(Br)−S(O)CF3 via the intermediacy of a novel vinyl sulfinyl radical H2C=C(Br)−SO (syn and anti conformers). Upon irradiation at 266 nm, H2CCSO decomposes into HCCH/SO and H2CS/CO in cryogenic Ar matrix. Whereas, visible‐light irradiations result in syn↔anti conformational...
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