Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

被引:104
作者
Gordon, Hamish [1 ]
Sengupta, Kamalika [2 ]
Rap, Alexandru [2 ]
Duplissy, Jonathan [3 ]
Frege, Carla [4 ]
Williamson, Christina [5 ,6 ,7 ]
Heinritzi, Martin [5 ]
Simon, Mario [5 ]
Yan, Chao [8 ]
Almeida, Joao [1 ,5 ]
Trostl, Jasmin
Nieminen, Tuomo [3 ,9 ]
Ortega, Ismael K. [10 ,25 ]
Wagner, Robert [8 ]
Dunne, Eimear M. [2 ,11 ]
Adamov, Alexey [8 ]
Amorim, Antonio [12 ,13 ]
Bernhammer, Anne-Kathrin [14 ,15 ]
Bianchi, Federico [4 ,8 ]
Breitenlechner, Martin [14 ]
Brilke, Sophia [5 ]
Chen, Xuemeng [8 ]
Craven, Jill S. [16 ]
Dias, Antonio [1 ]
Ehrhart, Sebastian [1 ,5 ]
Fischer, Lukas [14 ]
Flagan, Richard C. [16 ]
Franchin, Alessandro [8 ]
Fuchs, Claudia [4 ]
Guida, Roberto [1 ]
Hakala, Jani [8 ]
Hoyle, Christopher R. [4 ,17 ]
Jokinen, Tuija [8 ]
Junninen, Heikki [8 ]
Kangasluoma, Juha [8 ]
Kim, Jaeseok [9 ,18 ]
Kirkby, Jasper [1 ,5 ]
Krapf, Manuel [4 ]
Kuerten, Andreas [5 ]
Laaksonen, Ari [9 ,19 ]
Lehtipalo, Katrianne [4 ,8 ]
Makhmutov, Vladimir [20 ]
Mathot, Serge [1 ]
Molteni, Ugo [4 ]
Monks, Sarah A. [6 ,7 ]
Onnela, Antti [1 ]
Perakyla, Otso [8 ]
Piel, Felix [5 ]
Petaja, Tuukka [8 ]
Praplan, Arnaud P. [8 ]
机构
[1] CERN, European Org Nucl Res, Dept Expt Phys, CH-1211 Geneva, Switzerland
[2] Univ Leeds, Sch Earth & Environm, Leeds LS2 9JT, W Yorkshire, England
[3] Univ Helsinki, Helsinki Inst Phys, FI-00014 Helsinki, Finland
[4] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland
[5] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, D-60438 Frankfurt, Germany
[6] Univ Colorado, CIRES, Boulder, CO 80309 USA
[7] NOAA, Earth Syst Res Lab, Div Chem Sci, Boulder, CO 80305 USA
[8] Univ Helsinki, Dept Phys, FI-00014 Helsinki, Finland
[9] Univ Eastern Finland, Dept Appl Phys, FI-70211 Kuopio, Finland
[10] Univ Lille 1, UMR CNRS 8523, Lab Phys Lasers Atomes & Mol, F-59655 Villeneuve Dascq, France
[11] Finnish Meteorol Inst, Atmospher Res Ctr Eastern Finland, Kuopio 70211, Finland
[12] Univ Lisbon, Lab Syst Instrumentat & Modeling Sci & Technol Sp, P-1849016 Lisbon, Portugal
[13] Univ Beira Interior, P-1849016 Lisbon, Portugal
[14] Univ Innsbruck, Inst Ion & Appl Phys, A-6020 Innsbruck, Austria
[15] Ionicon Analyt GmbH, A-6020 Innsbruck, Austria
[16] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
[17] Eidgenoss Forschungsanstalt Wald Schnee & Landsch, Inst Snow & Avalanche Res, Schnee & Lawinenforsch SLF, CH-7260 Davos, Switzerland
[18] Korea Polar Res Inst, 26 Songdomirae Ro, Inchon 21990, South Korea
[19] Finnish Meteorol Inst, Climate Change Res Unit, FI-00101 Helsinki, Finland
[20] Lebedev Phys Inst, Solar & Cosm Ray Res Lab, Moscow 119991, Russia
[21] Univ Leeds, Natl Ctr Earth Observat, Leeds LS2 9JT, W Yorkshire, England
[22] Univ Vienna, Fac Phys, A-1090 Vienna, Austria
[23] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA
[24] Aerodyne Res Inc, Billerica, MA 01821 USA
[25] French Aerosp Lab, ONERA, F-91123 Palaiseau, France
基金
美国国家科学基金会; 瑞典研究理事会; 英国自然环境研究理事会; 欧洲研究理事会; 芬兰科学院; 俄罗斯基础研究基金会; 奥地利科学基金会; 瑞士国家科学基金会;
关键词
aerosol; biogenic; forcing; climate; SULFURIC-ACID; ORGANIC-COMPOUNDS; FORMATION EVENTS; NUCLEATION; EMISSIONS; MODEL; SECONDARY; IMPACT; MICROPHYSICS; UNCERTAINTY;
D O I
10.1073/pnas.1602360113
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
The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by 0.22 W m(-2) (27%) to -0.60 W m(-2). Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.
引用
收藏
页码:12053 / 12058
页数:6
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