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In this paper, we report the results of ab initio calculations of photoelectron angular distributions and vibrational branching ratios for the (2+1) REMPI of H_2 via the E, F^(1)Σ^+_g state, and compare these with the experimental data of Anderson et al. [Chem. Phys. Lett. 105, 22 (1984)]. These results show that the observed non‐Franck–Condon behavior is predominantly due to the R dependence of the transition matrix elements, and to a lesser degree to the energy dependence. This work presents the first molecular REMPI study employing a correlated wave function to describe the Rydberg–valence mixing in the resonant intermediate state.

(2+1) resonant enhanced multiphoton ionization of H2 via the E,F 1Σ+g state