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Molecular electronic or vibrational states can be superimposed temporarily in an extremely short laser pulse, and the superposition-state transients formed therein receive much attention, owing to the extensive interest in molecular fundamentals and the potential applications in quantum information processing. Using the crossed-beam ion velocity map imaging technique, we disentangle two distinctly different pathways leading to the forward-scattered N2+ yields in the large impact-parameter charge transfer from low-energy Ar+ to N2. Besides the ground-state (X2Σg+) N2+ produced in the energy-resonant charge transfer, a few slower N2+ ions are proposed to be in the superpositions of the X2Σg+-A2Πu and A2Πu-B2Σu+ states on the basis of the accidental degeneracy or energetic closeness of the vibrational states around the X2Σg+-A2Πu and A2Πu-B2Σu+ crossings in the non-Franck–Condon region. This finding potentially shows a brand-new way to prepare the superposition-state molecular ion.

Here we report a pulsed low-energy ion beam source for ion-molecule reaction study, in which the ions produced by the pulsed electron impact are confined well in the spatial size of each bunch. In contrast to the ion focusing method to reduce the transverse section of the beam, the longitudinal section in the translational direction is compressed by introducing a second pulse in the ion time-of-flight system. The test experiments for the low-energy argon ions are performed. The present beam source is ready for applications in the ion-molecule reaction dynamics experiments, in particular, in combination with the ion velocity map imaging technique.