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Understanding the quantum nature of low-energy C(3Pj) + He inelastic collisions

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Authors : Astrid Bergeat, Simon Chefdeville, Michel Costes, Sébastien B. Morales, Christian Naulin, Uzi Even, Jacek Kłos and François Lique
Inelastic collisions that occur between open-shell atoms and other atoms or molecules, and that promote a spin–orbit transition, involve multiple interaction potentials. They are non-adiabatic by nature and cannot be described within the Born–Oppenheimer approximation ; in particular, their theoretical modelling becomes very challenging when the collision energies have values comparable to the spin–orbit splitting. Here we study inelastic collisions between carbon in its ground state C(3Pj=0) and helium atoms—at collision energies in the vicinity of spin–orbit excitation thresholds ( 0.2 and 0.5 kJmol−1)—that result in spin–orbit excitation to C(3Pj=1) and C(3Pj=2). State-to-state integral cross-sections are obtained from crossed-beam experiments with a beam source that provides an almost pure beam of C(3Pj=0) . We observe very good agreement between experimental and theoretical results (acquired using newly calculated potential energy curves), which validates our characterization of the quantum dynamical resonances that are observed. Rate coefficients at very low temperatures suitable for chemical modelling of the interstellar medium are also calculated.
Journal : Nature Chemistry NatChem