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Electron-induced chemistry in microhydrated sulfuric acid clusters
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SYSNO ASEP 0482678 Druh ASEP J - Článek v odborném periodiku Zařazení RIV J - Článek v odborném periodiku Poddruh J Článek ve WOS Název Electron-induced chemistry in microhydrated sulfuric acid clusters Tvůrce(i) Lengyel, Jozef (UFCH-W) RID, ORCID
Pysanenko, Andriy (UFCH-W) RID, ORCID
Fárník, Michal (UFCH-W) RID, ORCIDZdroj.dok. Atmospheric Chemistry and Physics. - : Copernicus - ISSN 1680-7316
Roč. 17, č. 22 (2017), s. 14171-14180Poč.str. 10 s. Jazyk dok. eng - angličtina Země vyd. DE - Německo Klíč. slova induced aerosol formation ; particle formation ; atmospheric implication Vědní obor RIV CF - Fyzikální chemie a teoretická chemie Obor OECD Physical chemistry CEP GA17-04068S GA ČR - Grantová agentura ČR Způsob publikování Open access Institucionální podpora UFCH-W - RVO:61388955 UT WOS 000416439400001 EID SCOPUS 85035801941 DOI 10.5194/acp-17-14171-2017 Anotace We investigate the mixed sulfuric acid-water clusters in a molecular beam experiment with electron attachment and negative ion mass spectrometry and complement the experiment by density functional theory (DFT) calculations. The microhydration of (H2SO4)(m)(H2O)(n) clusters is controlled by the expansion conditions, and the electron attachment yields the main cluster ion series (H2SO4)(m)(H2O)(n)HSO4- and (H2O)(n)H2SO4-. The mass spectra provide an experimental evidence for the onset of the ionic dissociation of sulfuric acid and ion-pair (HSO4-center dot center dot center dot H3O+) formation in the neutral H2SO4(H2O)(n) clusters with n >= 5 water molecules, in excellent agreement with the theoretical predictions. In the clusters with two sulfuric acid molecules (H2SO4)(2)(H2O)(n) this process starts as early as n >= 2 water molecules. The (H2SO4)(m) (H2O)(n)HSO4 clusters are formed after the dissociative electron attachment to the clusters containing the (HSO4-center dot center dot center dot H3O+) ion-pair structure, which leads to the electron recombination with the H3O+ moiety generating H2O molecule and the H-atom dissociation from the cluster. The (H2O)(n) H2SO4- cluster ions point to an efficient caging of the H-atom by the surrounding water molecules. The electron-energy dependencies exhibit an efficient electron attachment at low electron energies below 3 eV, and no resonances above this energy, for all the measured mass peaks. This shows that in the atmospheric chemistry only the low-energy electrons can be efficiently captured by the sulfuric acid-water clusters and converted into the negative ions. Possible atmospheric consequences of the acidic dissociation in the clusters and the electron attachment to the sulfuric acid-water aerosols are discussed. Pracoviště Ústav fyzikální chemie J.Heyrovského Kontakt Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Rok sběru 2018
Počet záznamů: 1