The 266 nm pulsed laser photodissociation of cyanogen isothiocyanate (NCNCS) in a static cell was investigated leading to the detection of the gas phase Raman spectra of NCNCS and its photolysis product, isocyanogen (CNCN). The strongest Raman-active vibrational bands for both molecules were recorded using Coherent Anti-Stokes Raman Scattering (CARS) Spectroscopy around 5 mum. Direct C-S bond cleavage as a result of the photodissociation of NCNCS appears to be the most likely route for the generation of CNCN from NCNCS. (C) 2003 Elsevier B.V. All rights reserved.