Photoionization dynamics of excited molecular states. Photoelectron angular distributions and rotational and vibrational branching ratios for H2 C 1Πu, v=0–4

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Abstract
Photoelectron angular distributions following three photon resonant, four photon (3+1) ionization of H2 via the C 1Πu, v′=0–4 ← X 1Σ+g, v″=0 Q(1) transitions are reported. The observed angular distributions are generally more isotropic for v+≠v′ than for v+=v′. Photoelectron spectra obtained along the polarization axis of the laser following (3+1) ionization via the C 1Πu, v′=4 ← X 1Σ+g, v″=0 R(0) and R(1) transitions are also reported. These spectra are rotationally resolved and exhibit strongly v+‐dependent rotational branching ratios. The comparison of the angular distribution data with available theoretical calculations indicates good agreement for some transitions and poor agreement for others, suggesting the need for substantial progress in understanding the photoionization dynamics of even the simplest excited molecular states.