The CCN radical has been recently detected in the interstellar medium. Accurate modeling of its abundance in such media requires one to model its excitation by both radiation and collisions. Here, we report the first quantum mechanical close-coupling study of CCN—He collisions. Calculations of fine-structure resolved excitation cross sections of CCN(X2Π) induced by collision with He are performed for kinetic energies below 500 cm−1. The calculations are based on new two-dimensional potential energy surfaces obtained from coupled cluster approaches. We found that the inelastic cross sections for spin-orbit conserving transitions are larger than those for spin-orbit changing transitions. The new collisional data should significantly help the interpretation of interstellar CCN emission lines observed with current and future telescopes and we expect that they will allow accurate determination of the CCN abundance in the interstellar medium, which is crucial to understand the chemistry of carbon chain species in the interstellar gas.

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