This study presents a source for studying thin‐film deposition utilizing vacuum UV (VUV) radiation from a remote argon or helium atmospheric plasma to initiate photochemistry in the precursor gas. We aim to assess how this radiation affects the deposition process and film structure while avoiding deposition inside the plasma source or particle formation. Deposition occurs where radiation interacts with the precursor and the growing film, as well as further downstream. The measured film properties clearly show that photon interaction with the film has a significant effect. Using hexamethyldisiloxane (HMDSO) as a precursor, we achieved nearly carbon‐free silicon dioxide () film growth due to photodesorption of hydrocarbons from the growing film, as confirmed by infrared spectra and positive ion mass spectrometry.