Abstract
The D ˜ 2 Σ + state of CaOH was investigated using optical–optical double resonance spectroscopy. A combined least-squares fit of the D ˜ 2 Σ + – A ˜ 2 Π double resonance transition data along with A ˜ 2 Π – X ˜ 2 Σ + optical transition data and the millimeter-wave pure rotational data of the X ˜ 2 Σ + state was performed using an effective Hamiltonian. The spin–rotation constant was determined for the D ˜ 2 Σ + state for the first time. An analysis of these constants showed that the Ca–O bond length and spin–rotation parameter of the D ˜ 2 Σ + state have the smallest values of all the observed 2Σ + states of CaOH. This evidence suggests the assignment of the D ˜ 2 Σ + state as arising from a Ca + atomic orbital of mainly 5 sσ character. This atomic orbital assignment was shown to be consistent with both previous work on CaF and recent theoretical calculations on CaOH.
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