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Due to their reactivity with electrophiles, enols can play a crucial role in our understanding of the molecular complexity in the interstellar medium and in comets and meteorites. To study the enolization of aldehydes in interstellar ices by interaction with galactic cosmic rays (GCRs), we irradiated acetaldehyde ices with energetic electrons as proxies of secondary electrons generated in the track of GCRs while penetrating interstellar ices. The results indicate that GCRs can induce enolization of acetaldehyde and that intra\u2010 as well as intermolecular processes are relevant. Therefore, enols should be ubiquitous in the interstellar medium and could be searched for using radio telescopes such as ALMA. Once enols are detected and abundances are established, they can serve as tracers for the non\u2010equilibrium chemistry in interstellar ices thus eventually constraining fundamental reaction mechanisms deep inside interstellar ices.<\/jats:p>","DOI":"10.1002\/cphc.202100111","type":"journal-article","created":{"date-parts":[[2021,4,28]],"date-time":"2021-04-28T21:58:23Z","timestamp":1619647103000},"page":"1229-1236","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":29,"title":["Interstellar Enolization\u2010Acetaldehyde (CH<sub>3<\/sub>CHO) and Vinyl Alcohol (H<sub>2<\/sub>CCH(OH)) as a Case Study"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1767-897X","authenticated-orcid":false,"given":"N. Fabian","family":"Kleimeier","sequence":"first","affiliation":[{"name":"Department of Chemistry and W. M. 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