Abstract
We report the first coherent Raman detection of small van der Waals aggregates formed in dilute CO 2/He free-jet expansions. CARS spectra show distinct features attributable to dimers and higher-order polymers of CO 2. Comparison of these Raman data with infrared spectra in the ν 1 region of CO 2 indicates that the rule of mutual exclusion is operative for the dimer vibrations. This result favors an offset parallel C 2h structure for the most stable dimer configuration rather than a polar T-shaped arrangement proposed from recent electric deflection experiments.
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