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We show that rapid evolution of a Rydberg orbital with internuclear distance in a resonance enhanced multiphoton ionization (REMPI) process can have a profound influence on the production of molecular ions in alternative rotational states. This is illustrated by calculations of ionic rotational branching ratios for (2+1′) REMPI via the O11 (20.5) branch of the E′ ^2Σ^+(3pσ) Rydberg state of CH. The rotational propensity rule for ionization changes from ΔN=odd (ΔN=N_+−N_i) at lower vibrational excitation, as expected from the ΔN+l=odd selection rule, to ΔN=even at higher vibrational levels. This effect is expected to be quite general and should be most readily observable in diatomic hydrides.

Vibrational state dependence of ionic rotational branching ratios in resonance enhanced multiphoton ionization of CH