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An optical–optical double resonance study of the perturbed O2 d3sσg(1Πg) Rydberg state excited via single rotational levels of the b(1Σg+) valence state

The perturbed v=3 level of the d3sσg(1Πg) Rydberg state of O2 has been excited in an optical–optical double resonance (OODR) experiment via J=0–16 of v=0 of the b(1Σg+) state. The d(1Πg) state resonances were detected by ionization with one further probe photon near 340 nm. The range of J levels of the d(1Πg) state now accessed reveals a lack of variation in line widths that is not predicted by previous models of state-dependent predissociation. Instead, intensities of rotational lines in the ionization spectrum appear to be controlled by a J-dependent mixing of the d(1Πg) state with a nearby valence state that has a much lower ionization cross section at the probe wavelengths used.