With the high-resolution spectroscopy now available in the optical and satellite UV, it is possible to determine the neutral/ionized column density ratios for several different elements in a single cloud. Assuming ionization equilibrium for each element, one can make several independent determinations of the electron density. For the clouds for which such an analysis has been carried out, these different estimates disagree by large factors, suggesting that some process (or processes) besides photoionization and radiative recombination might play an important role in the ionization balance. One candidate process is collisions of ions with dust grains. Making use of recent work quantifying the abundances of polycyclic aromatic hydrocarbon molecules and other grains in the interstellar medium, as well as recent models for grain charging, we estimate the grain-assisted ion recombination rates for several astrophysically important elements. We find that these rates are comparable to the rates for radiative recombination for conditions typical of the cold neutral medium. Including grain-assisted ion recombination in the ionization equilibrium analysis leads to increased consistency in the various electron density estimates for the gas along the line of sight to 23 Orionis. However, not all of the discrepancies can be eliminated in this way; we speculate on some other processes that might play a role. We also note that grain-assisted recombination of H+ and He+ leads to significantly lower electron fractions than usually assumed for the cold neutral medium.
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