Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

被引:76
作者
Kourtchev, Ivan [1 ,2 ,3 ]
Giorio, Chiara [1 ]
Manninen, Antti [4 ]
Wilson, Eoin [2 ,3 ]
Mahon, Brendan [1 ]
Aalto, Juho [4 ,5 ,6 ]
Kajos, Maija [4 ]
Venables, Dean [2 ,3 ,7 ]
Ruuskanen, Taina
Levula, Janne [4 ,6 ]
Loponen, Matti [4 ,6 ]
Connors, Sarah [1 ]
Harris, Neil [1 ,8 ]
Zhao, Defeng [9 ]
Kiendler-Scharr, Astrid [9 ]
Mentel, Thomas [9 ]
Rudich, Yinon [10 ]
Hallquist, Mattias [11 ]
Doussin, Jean-Francois [12 ]
Maenhaut, Willy [13 ,14 ]
Back, Jaana [5 ]
Petaja, Tuukka [4 ]
Wenger, John [2 ,3 ]
Kulmala, Markku [4 ]
Kalberer, Markus [1 ]
机构
[1] Univ Cambridge, Dept Chem, Cambridge CB2 1EW, England
[2] Univ Coll Cork, Dept Chem, Cork, Ireland
[3] Univ Coll Cork, Environm Res Inst, Cork, Ireland
[4] Univ Helsinki, Dept Phys, POB 64, FIN-00014 Helsinki, Finland
[5] Univ Helsinki, Dept Forest Sci, POB 27, FI-00014 Helsinki, Finland
[6] Hyytiala Forestry Field Stn, Hyytialantie 124, Korkeakoski 35500, Finland
[7] Leibniz Inst Tropospher Res TROPOS, Permoserstr 15, D-04318 Leipzig, Germany
[8] Cranfield Univ, Ctr Atmospher Informat & Emiss Technol, Cranfield MK43 0AL, Beds, England
[9] Forschungszentrum Julich, Inst Energie & Klimaforsch IEK 8, D-52425 Julich, Germany
[10] Weizmann Inst Sci, Dept Earth & Planetary Sci & Energy Res, IL-76100 Rehovot, Israel
[11] Univ Gothenburg, Dept Chem, Atmospher Sci, S-41296 Gothenburg, Sweden
[12] Univ Paris Est Creteil & Paris Diderot, CNRS UMR 7583, Inst Pierre Simon Laplace, LISA, 61 Ave Gen Gaulle, F-94010 Creteil, France
[13] Univ Ghent, Dept Analyt Chem, Krijgslaan 281, B-9000 Ghent, Belgium
[14] Univ Antwerp, Dept Pharmaceut Sci, Univ Pl 1, B-2610 Antwerp, Belgium
来源
SCIENTIFIC REPORTS | 2016年 / 6卷
基金
芬兰科学院; 英国工程与自然科学研究理事会;
关键词
MOLECULAR COMPOSITION; VOC CONCENTRATIONS; SCOTS PINE; OZONOLYSIS; PARTICLES; EVOLUTION; IDENTIFICATION; PRODUCTS; PHASE; STATE;
D O I
10.1038/srep35038
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.
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收藏
页数:9
相关论文
共 39 条
  • [1] Physical characterization of aerosol particles during nucleation events
    Aalto, P
    Hämeri, K
    Becker, E
    Weber, R
    Salm, J
    Mäkelä, JM
    Hoell, C
    O'Dowd, CD
    Karlsson, H
    Hansson, HC
    Väkevä, M
    Koponen, IK
    Buzorius, G
    Kulmala, M
    [J]. TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 2001, 53 (04): : 344 - 358
  • [2] Chemodiversity of a Scots pine stand and implications for terpene air concentrations
    Back, J.
    Aalto, J.
    Henriksson, M.
    Hakola, H.
    He, Q.
    Boy, M.
    [J]. BIOGEOSCIENCES, 2012, 9 (02) : 689 - 702
  • [3] Distribution of gaseous and particulate organic composition during dark α-pinene ozonolysis
    Camredon, M.
    Hamilton, J. F.
    Alam, M. S.
    Wyche, K. P.
    Carr, T.
    White, I. R.
    Monks, P. S.
    Rickard, A. R.
    Bloss, W. J.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (06) : 2893 - 2917
  • [4] A review of natural aerosol interactions and feedbacks within the Earth system
    Carslaw, K. S.
    Boucher, O.
    Spracklen, D. V.
    Mann, G. W.
    Rae, J. G. L.
    Woodward, S.
    Kulmala, M.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (04) : 1701 - 1737
  • [5] Thermodynamics of oligomer formation: implications for secondary organic aerosol formation and reactivity
    DePalma, Joseph W.
    Horan, Andrew J.
    Hall, Wiley A.
    Johnston, Murray V.
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (18) : 6935 - 6944
  • [6] Molecular characterization of free tropospheric aerosol collected at the Pico Mountain Observatory: a case study with a long-range transported biomass burning plume
    Dzepina, K.
    Mazzoleni, C.
    Fialho, P.
    China, S.
    Zhang, B.
    Owen, R. C.
    Helmig, D.
    Hueber, J.
    Kumar, S.
    Perlinger, J. A.
    Kramer, L. J.
    Dziobak, M. P.
    Ampadu, M. T.
    Olsen, S.
    Wuebbles, D. J.
    Mazzoleni, L. R.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2015, 15 (09) : 5047 - 5068
  • [7] Evolution of the complex refractive index in the UV spectral region in ageing secondary organic aerosol
    Flores, J. M.
    Zhao, D. F.
    Segev, L.
    Schlag, P.
    Kiendler-Scharr, A.
    Fuchs, H.
    Watne, A. K.
    Bluvshtein, N.
    Mentel, Th F.
    Hallquist, M.
    Rudich, Y.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2014, 14 (11) : 5793 - 5806
  • [8] Hakola H, 2009, BOREAL ENVIRON RES, V14, P722
  • [9] The formation, properties and impact of secondary organic aerosol: current and emerging issues
    Hallquist, M.
    Wenger, J. C.
    Baltensperger, U.
    Rudich, Y.
    Simpson, D.
    Claeys, M.
    Dommen, J.
    Donahue, N. M.
    George, C.
    Goldstein, A. H.
    Hamilton, J. F.
    Herrmann, H.
    Hoffmann, T.
    Iinuma, Y.
    Jang, M.
    Jenkin, M. E.
    Jimenez, J. L.
    Kiendler-Scharr, A.
    Maenhaut, W.
    McFiggans, G.
    Mentel, Th. F.
    Monod, A.
    Prevot, A. S. H.
    Seinfeld, J. H.
    Surratt, J. D.
    Szmigielski, R.
    Wildt, J.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (14) : 5155 - 5236
  • [10] Investigating the use of secondary organic aerosol as seed particles in simulation chamber experiments
    Hamilton, J. F.
    Alfarra, M. Rami
    Wyche, K. P.
    Ward, M. W.
    Lewis, A. C.
    McFiggans, G. B.
    Good, N.
    Monks, P. S.
    Carr, T.
    White, I. R.
    Purvis, R. M.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (12) : 5917 - 5929