The vibrational infrared absorption spectra of the molecules CSe2, SCSe, and SCTe have been recorded and analyzed. Some Raman data are also reported. The fundamental frequencies (in em-I) of these molecules, UI (symmetric stretching), U2 (bending), and U3 (asymmetric stretching) are, respectively: CSe2 (gas) 368,308, and 1303; CSe2 (liquid) 368, 310, and 1267; SCSe (g) 506,355, and 1435; SCSe (I) 502,350, and 1408; SCTe (CS 2 solution) 423, 337, and 1347. Observed isotopic shifts due to CI3 in all three compounds are reported and discussed. The expected linearity of CSe2 is confirmed. The synthesis and purification of the more unstable members of the CX2-XCZ family (X, Z=O, S, Se, or Te) are discussed. Some predictions, of possible use in identification, for the intense fundamental U3 of the so far unreported and probably very unstable OCTe, SeCTe, and CTe. are made. These are based on a treatment using a uniform potential energy function for all these molecules, to be presented in a subsequent paper.