The elusive molecule thioformyl cyanide, S=CH-CN (2), was generated by
flash vacuum pyrolysis of allyl cyanomethyl sulfide (1) and character
ized by argon matrix infrared spectroscopy. The observed infrared abso
rptions (2221, 1320, 1103, 889, and 824 cm-1) are in good agreement wi
th ab initio molecular orbital calculations at the MP2/6-31G level.