We have experimentally determined total carbon yields per incident H atom in the energy range 36–300eV/H for H + , H2+, and H3+ projectiles incident normally on ∼60nm thick a-C:H films, using 2-D ellipsometry determination of erosion crater volumes ex vacuo, the separately characterized thin film carbon density, and the incident beam current integration accumulated on target during the crater evolution. During each beam exposure, methane production was monitored using in situ quadrupole mass spectrometry (QMS). The present total carbon yields/H for incident H3+ ions obtained via ellipsometry are in agreement with total mass loss measurements for H3+ by Balden and Roth [1] over the investigated energy range. The observed methane production per incident H for the molecular ions exhibits molecular size effects over the entire energy range investigated, confirming the trend observed in the ellipsometry-based total C yields/H.