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Structural calculations and high-resolution infrared spectra are reported fortrimers and tetramers containing CO$_2$ together with CO and/or N$_2$. Amongthe 9 clusters studied here, only (CO$_2$)$_2$-CO was previously observed byhigh-resolution spectroscopy. The spectra, which occur in the region of the$\nu_3$ fundamental of CO$_2$ (~2350 cm$^{-1}$), were recorded using a tunableoptical parametric oscillator source to probe a pulsed supersonic slit jetexpansion. The trimers (CO$_2$)$_2$-CO and (CO$_2$)$_2$-N$_2$ have structuresin which the CO or N$_2$ is aligned along the symmetry axis of a staggeredside-by-side CO$_2$ dimer unit. The observation of two fundamental bands for(CO$_2$)$_2$-CO and (CO$_2$)$_2$-N$_2$ shows that this CO$_2$ dimer unit isnon-planar, unlike (CO$_2$)$_2$ itself. For the trimers CO$_2$-(CO)$_2$ andCO$_2$-(N$_2$)$_2$, the CO or N$_2$ monomers occupy equivalent positions in the'equatorial plane' of the CO$_2$, pointing toward its C atom. To form thetetramers CO$_2$-(CO)$_3$ and CO$_2$-(N$_2$)$_3$, a third CO or N$_2$ monomeris then added off to the 'side' of the first two. In the mixed tetramersCO$_2$-(CO)$_2$-N$_2$ and CO$_2$-CO-(N$_2$)$_2$, this 'side' position is takenby N2 and not CO. In addition to the fundamental bands, combination bands arealso observed for (CO$_2$)$_2$-CO, CO$_2$-(CO)$_2$, and CO$_2$-(N$_2$)$_2$,yielding some information about their low-frequency intermolecular vibrations.

physical chemistry chemical physics/pccp. physical chemistry chemical physics

Weakly-bound clusters of atmospheric molecules: infrared spectra and  structural calculations of (CO$_2$)$_n$-(CO)$_m$-(N$_2$)$_p$, $(n, m, p)$ =  (2, 1, 0), (2, 0, 1), (1, 2, 0), (1, 0, 2), (1, 1, 1), (1, 3, 0), (1, 0, 3),  (1, 2, 1), (1, 1, 2)