The infrared spectrum of the cross-shaped van der Waals complex N2O-CS2 is observed in the region of the N2O nu1 fundamental band (~2220 cm-1) using a tuneable diode laser to probe a pulsed supersonic slit jet expansion. Both 14N- and 15N-substituted species are studied. Analysis of their spectra establishes that this dimer has a cross-shaped structure, similar to its isoelectronic cousin CO2-CS2. This is the first spectroscopic observation of N2O-CS2, and the molecular parameters determined here should be useful for detection of its pure rotational microwave spectrum.
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