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.
引用
收藏
页数:9
相关论文
共 39 条
  • [21] Kroll JH, 2011, NAT CHEM, V3, P133, DOI [10.1038/nchem.948, 10.1038/NCHEM.948]
  • [22] Kulmala M, 2014, BOREAL ENVIRON RES, V19, P122
  • [23] Direct Observations of Atmospheric Aerosol Nucleation
    Kulmala, Markku
    Kontkanen, Jenni
    Junninen, Heikki
    Lehtipalo, Katrianne
    Manninen, Hanna E.
    Nieminen, Tuomo
    Petaja, Tuukka
    Sipila, Mikko
    Schobesberger, Siegfried
    Rantala, Pekka
    Franchin, Alessandro
    Jokinen, Tuija
    Jarvinen, Emma
    Aijala, Mikko
    Kangasluoma, Juha
    Hakala, Jani
    Aalto, Pasi P.
    Paasonen, Pauli
    Mikkila, Jyri
    Vanhanen, Joonas
    Aalto, Juho
    Hakola, Hannele
    Makkonen, Ulla
    Ruuskanen, Taina
    Mauldin, Roy L., III
    Duplissy, Jonathan
    Vehkamaki, Hanna
    Back, Jaana
    Kortelainen, Aki
    Riipinen, Ilona
    Kurten, Theo
    Johnston, Murray V.
    Smith, James N.
    Ehn, Mikael
    Mentel, Thomas F.
    Lehtinen, Kari E. J.
    Laaksonen, Ari
    Kerminen, Veli-Matti
    Worsnop, Douglas R.
    [J]. SCIENCE, 2013, 339 (6122) : 943 - 946
  • [24] High molecular weight SOA formation during limonene ozonolysis: insights from ultrahigh-resolution FT-ICR mass spectrometry characterization
    Kundu, S.
    Fisseha, R.
    Putman, A. L.
    Rahn, T. A.
    Mazzoleni, L. R.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (12) : 5523 - 5536
  • [25] Cloud condensation nuclei (CCN) activity and oxygen-to-carbon elemental ratios following thermodenuder treatment of organic particles grown by α-pinene ozonolysis
    Kuwata, Mikinori
    Chen, Qi
    Martin, Scot T.
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (32) : 14571 - 14583
  • [26] Gas-phase products and secondary aerosol yields from the photooxidation of 16 different terpenes
    Lee, Anita
    Goldstein, Allen H.
    Kroll, Jesse H.
    Ng, Nga L.
    Varutbangkul, Varuntida
    Flagan, Richard C.
    Seinfeld, John H.
    [J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2006, 111 (D17)
  • [27] Aerosol Indirect Effect on Biogeochemical Cycles and Climate
    Mahowald, Natalie
    [J]. SCIENCE, 2011, 334 (6057) : 794 - 796
  • [28] Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks
    Mentel, Th. F.
    Kleist, E.
    Andres, S.
    Dal Maso, M.
    Hohaus, T.
    Kiendler-Scharr, A.
    Rudich, Y.
    Springer, M.
    Tillmann, R.
    Uerlings, R.
    Wahner, A.
    Wildt, J.
    [J]. ATMOSPHERIC CHEMISTRY AND PHYSICS, 2013, 13 (17) : 8755 - 8770
  • [29] The Molecular Identification of Organic Compounds in the Atmosphere: State of the Art and Challenges
    Noziere, Barbara
    Kalberer, Markus
    Claeys, Magda
    Allan, James
    D'Anna, Barbara
    Decesari, Stefano
    Finessi, Emanuela
    Glasius, Marianne
    Grgic, Irena
    Hamilton, Jacqueline F.
    Hoffmann, Thorsten
    Iinuma, Yoshiteru.
    Jaoui, Mohammed
    Kahno, Ariane
    Kampf, Christopher J.
    Kourtchev, Ivan
    Maenhaut, Willy
    Marsden, Nicholas
    Saarikoski, Sanna
    Schnelle-Kreis, Jurgen
    Surratt, Jason D.
    Szidat, Sonke
    Szmigielski, Rafal
    Wisthaler, Armin
    [J]. CHEMICAL REVIEWS, 2015, 115 (10) : 3919 - 3983
  • [30] Paasonen P, 2013, NAT GEOSCI, V6, P438, DOI [10.1038/NGEO1800, 10.1038/ngeo1800]