Abstract
Abstract A colour-centre laser has been used in conjunction with a molecular-beam apparatus to study the infrared vibrational predissociation spectra of nitrous oxide clusters near the ν1 + ν3 vibrational combination band of the momomer. These spectra were recorded as a function of source pressure in order to measure their dependence on cluster size. A frequency shift, corresponding to a gradual transition from the vapour to the solid state, is observed as the cluster size increases. The cluster-size distributions were estimated using both quadrupole and ion time-of-flight mass spectrometry. The latter technique shows cluster sizes well in excess of (N2O)100. Semiclassical studies based on Monte Carlo simulations and local mode analysis of representative cluster configurations are used to account for line profiles and shifts.
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