Abstract

Coherent anti-Stokes Raman spectra are reported for solid, nanometer-sized C2H2 and CO2 aggregates formed in free jet expansions. From comparisons with spectra of equilibrium samples, the clusters are seen to be face centered cubic with a crystalline character indicated by the appearance of vibrational factor group splittings and, for CO2, by the observation of two external lattice librations.

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