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Helium nanodroplets ("HNDs") are widely used for forming tailor-made clustersand molecular complexes in a cold, transparent, and weakly-interacting matrix.Characterization of embedded species by mass spectrometry is often complicatedby fragmentation and trapping of ions in the HNDs. Here, we systematicallystudy fragment ion mass spectra of HND-aggregated water and oxygen clustersfollowing their ionization by charge transfer ionization ("CTI") and Penningionization ("PEI"). While the efficiency of PEI of embedded clusters is lowerthan for CTI by about factor 10, both the mean sizes of detected water clustersand the relative yields of unprotonated cluster ions are significantly larger,making PEI a ``soft ionization'' scheme. However, the tendency of ions toremain bound to HNDs leads to a reduced detection efficiency for large HNDscontaining $>10^4$ helium atoms. These results are instrumental for determiningoptimal conditions for mass spectrometry and photoionization spectroscopy ofmolecular complexes and clusters aggregated in HNDs.

Fragmentation of Water Clusters Formed in Helium Nanodroplets by Charge Transfer and Penning Ionization