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.

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