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000022984 1001_ $$0P:(DE-Juel1)144056$$aEhn, M.$$b0$$uFZJ
000022984 245__ $$aGas phase formation of extremely oxidized pinene reaction products in chamber and ambient air
000022984 260__ $$aKatlenburg-Lindau$$bEGU$$c2012
000022984 300__ $$a5113 - 5127
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000022984 440_0 $$09601$$aAtmospheric Chemistry and Physics$$v12$$x1680-7316$$y11
000022984 500__ $$aM. E. gratefully acknowledges financial support by the Emil Aaltonen foundation. This work was supported by the ERC Advanced Grant EU-FP7-ATMNUCLE (project no 227463), and by the Academy of Finland Center of Excellence program (project no 1118615).
000022984 520__ $$aHigh molecular weight (300-650 Da) naturally charged negative ions have previously been observed at a boreal forest site in Hyytiala, Finland. The long-term measurements conducted in this work showed that these ions are observed practically every night between spring and autumn in Hyytiala. The ambient mass spectral patterns could be reproduced in striking detail during additional measurements of alpha-pinene (C10H16) oxidation at low-OH conditions in the Julich Plant Atmosphere Chamber (JPAC). The ions were identified as clusters of the nitrate ion (NO3-) and alpha-pinene oxidation products reaching oxygen to carbon ratios of 0.7-1.3, while retaining most of the initial ten carbon atoms. Attributing the ions to clusters instead of single molecules was based on additional observations of the same extremely oxidized organics in clusters with HSO4- (Hyytiala) and C3F5O2- (JPAC). The most abundant products in the ion spectra were identified as C10H14O7, C10H14O9, C10H16O9, and C10H14O11. The mechanism responsible for forming these molecules is still not clear, but the initial reaction is most likely ozone attack at the double bond, as the ions are mainly observed under dark conditions. beta-pinene also formed highly oxidized products under the same conditions, but less efficiently, and mainly C-9 compounds which were not observed in Hyytiala, where beta-pinene on average is 4-5 times less abundant than alpha-pinene. Further, to explain the high O/C together with the relatively high H/C, we propose that geminal diols and/or hydroperoxide groups may be important. We estimate that the night-time concentration of the sum of the neutral extremely oxidized products is on the order of 0.1-1 ppt (similar to 10(6)-10(7) molec cm(-3)). This is in a similar range as the amount of gaseous H2SO4 in Hyytiala during day-time. As these highly oxidized organics are roughly 3 times heavier, likely with extremely low vapor pressures, their role in the initial steps of new aerosol particle formation and growth may be important and needs to be explored in more detail in the future.
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000022984 7001_ $$0P:(DE-Juel1)129345$$aKleist, E.$$b1$$uFZJ
000022984 7001_ $$0P:(DE-HGF)0$$aJunninen, H.$$b2
000022984 7001_ $$0P:(DE-HGF)0$$aPetäjä, T.$$b3
000022984 7001_ $$0P:(DE-HGF)0$$aLönn, G.$$b4
000022984 7001_ $$0P:(DE-HGF)0$$aSchobesberger, S.$$b5
000022984 7001_ $$0P:(DE-Juel1)VDB46017$$aDal Maso, M.$$b6$$uFZJ
000022984 7001_ $$0P:(DE-Juel1)129266$$aTrimborn, A.$$b7$$uFZJ
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000022984 7001_ $$0P:(DE-Juel1)16324$$aWahner, A.$$b10$$uFZJ
000022984 7001_ $$0P:(DE-Juel1)VDB1780$$aWildt, J.$$b11$$uFZJ
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000022984 773__ $$0PERI:(DE-600)2069847-1$$a10.5194/acp-12-5113-2012$$gVol. 12, p. 5113 - 5127$$p5113 - 5127$$q12<5113 - 5127$$tAtmospheric chemistry and physics$$v12$$x1680-7316$$y2012
000022984 8567_ $$uhttp://dx.doi.org/10.5194/acp-12-5113-2012
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