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• W1603318613 abstract "Understanding the gas-phase chemistry of acetaldehyde can be challenging because the molecule can assume several tautomeric forms, namely keto, enol and carbene. The two last forms are the most stable ionic forms. Here, insight into the gas-phase cluster ion chemistry of homogeneous acetaldehyde and mixed water-acetaldehyde clusters is provided by mass spectrometry/vacuum ultraviolet photoionization combined with density functional theory calculations. (AA)nH(+) clusters (AA = acetaldehyde) and mixed (AA)nH3O(+) clusters were detected using tunable vacuum ultraviolet photoionization. Barrierless proton transfers were observed during the geometry optimization of the most stable dimer structures and helped to explain the cluster ion chemistry induced by photoionization, namely the formation of deprotonated tautomers and protonated keto tautomers. Water was found to catalyze the keto-enol and keto-carbene isomerizations and facilitate the proton transfer from the ionized enol or carbene part of the cluster to the neutral keto part, resulting in protonated keto structures. The production of protonated keto structures was identified to be the main fragmentation channel following ionization of the homogeneous acetaldehyde cluster and a channel for ionized mixed clusters as well. These findings are significant for a broad range of fields, including current atmospheric models, because acetaldehyde is one of the most prominent organic species in the troposphere and ions play a crucial role in aerosol formation." @default.
• W1603318613 created "2016-06-24" @default.
• W1603318613 creator A5034071017 @default.
• W1603318613 creator A5063631838 @default.
• W1603318613 date "2014-07-08" @default.
• W1603318613 modified "2023-10-11" @default.
• W1603318613 title "Tautomerism and proton transfer in photoionized acetaldehyde and acetaldehyde–water clusters" @default.
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• W1603318613 doi "https://doi.org/10.1002/jms.3403" @default.
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