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Qualitative differences have been observed between two types of "quasi-one-electron" collision systems. We have studied valence-electron excitation at "high" energy (relative collision velocities up to 0.5 a.u.) in the Mg++He and Na++H collision systems, and find that while Mg++He collisions are dominated by "direct" excitation, the Na++H collisions exhibit significant "molecular" excitation, even at the highest velocities. This behavior can be understood in terms of the molecular structure of the respective collision complexes, and the energy separation between the ground and first excited states of the valence electron.