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The thermal decomposition of cyanogen azide (NCN3) and the subsequent collision‐induced intersystem crossing (CIISC) process of cyanonitrene (NCN) have been investigated by monitoring excited electronic state 1NCN and ground state 3NCN radicals. NCN was generated by the pyrolysis of NCN3 behind shock waves and by the photolysis of NCN3 at room temperature. Falloff rate constants of the thermal unimolecular...
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