We note that previous work on pure cholesterol samples prepared without water and without the complicating presence of salts, showed depth profile data of the molecular ion after losing the hydroxyl group [M-OH] + at the outermost surface and the molecular ion [M-H] + below it, consistent with an inward molecular orientation of the hydroxyl group. In this LNP system, we do not see an intense [M-H] + ion, most likely due to adduct formation from sodium present in the PBS. While these two systems are very different and cannot be compared directly, the observation of the different cholesterol fragments suggests molecular orientation in a model pure crystalline system. This is consistent with our observation of molecular orientation of the larger PMG-PEG2k using GCIB etching in this LNP system, suggesting that the orientation of small molecules such as cholesterol may be detectable in some systems.