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The chemistry in the diffuse interstellar medium initiates the gradual increase of molecular complexity during the life cycle of matter. A key molecule that enables build-up of new molecular bonds and new molecules via proton-donation is H3+. Its evolution is tightly related to molecular hydrogen and thought to be well understood. However, recent observations of ortho and para lines of H2 and H3+ in the diffuse ISM showed a puzzling discrepancy in nuclear spin excitation temperatures and populations between these two key species. H3+, unlike H2, seems to be out of thermal equilibrium, contrary to the predictions of modern astrochemical models. We conduct the first time-dependent modeling of the para-fractions of H2 and H3+ in the diffuse ISM and compare our results to a set of line-of-sight observations, including new measurements presented in this study. We isolate a set of key reactions for H3+ and find that the destruction of the lowest rotational states of H3+ by dissociative recombination largely control its ortho/para ratio. A plausible agreement with observations cannot be achieved unless a ratio larger than 1:5 for the destruction of (1,1)- and (1,0)-states of H3+ is assumed. Additionally, an increased CR ionization rate to 10(-15) 1/s further improves the fit whereas variations of other individual physical parameters, such as density and chemical age, have only a minor effect on the predicted ortho/para ratios. Thus our study calls for new laboratory measurements of the dissociative recombination rate and branching ratio of the key ion H3+ under interstellar conditions.
Interstellar dark clouds are the sites of star formation. Their main component, dihydrogen, exists under two states, ortho and para. H2 is supposed to form in the ortho:para ratio (OPR) of 3:1 and to subsequently decay to almost pure para-H2 (OPR <=
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