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Infrared combination bands of the polar isomer of the N2O dimer are observedfor the first time, using a tunable infrared laser source to probe a pulsedslit-jet supersonic expansion in the N2O nu1 region (~2240 cm-1). One bandinvolves the torsional (out-of-plane) intermolecular mode and yields atorsional frequency of 19.83 cm-1 if associated with the out-of-phasefundamental (N2O nu1) vibration of the N2O monomers in the dimer. The otherband, which is highly perturbed, yields an intermolecular in-plane geared bendfrequency of 22.74 cm-1. The results are compared with high level ab initiocalculations. The less likely alternate assignment to the in-phase fundamentalwould give torsional and geared bend frequencies of 17.25 and 20.16 cm-1,respectively.

Intermolecular vibrational states far above the van der Waals minimum: combination bands of the polar N2O dimer