GSTDTAP  > 气候变化
DOI10.1002/2017GL073056
Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate
Rastak, N.1,2; Pajunoja, A.3; Navarro, J. C. Acosta1,2; Ma, J.4; Song, M.5,6; Partridge, D. G.1,2; Kirkevag, A.7; Leong, Y.3,8; Hu, W. W.9,10; Taylor, N. F.11; Lambe, A.12,13; Cerully, K.14; Bougiatioti, A.15,16; Liu, P.17; Krejci, R.1,2; Petaja, T.18; Percival, C.19; Davidovits, P.13; Worsnop, D. R.12; Ekman, A. M. L.20; Nenes, A.14,15,16,21; Martin, S.13; Jimenez, J. L.9,10; Collins, D. R.11; Topping, D. O.19,22; Bertram, A. K.6; Zuend, A.4; Virtanen, A.3; Riipinen, I.1,2
2017-05-28
发表期刊GEOPHYSICAL RESEARCH LETTERS
ISSN0094-8276
EISSN1944-8007
出版年2017
卷号44期号:10
文章类型Article
语种英语
国家Sweden; Finland; Canada; South Korea; Norway; USA; Greece; England
英文摘要

A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH-dependent SOA water-uptake with solubility and phase separation; (2) show that laboratory data on IP- and MT-SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single-parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.


Plain Language Summary The interaction of airborne particulate matter ("aerosols") with water is of critical importance for processes governing climate, precipitation, and public health. It also modulates the delivery and bioavailability of nutrients to terrestrial and oceanic ecosystems. We present a microphysical explanation to the humidity-dependent water uptake behavior of organic aerosol, which challenges the highly simplified theoretical descriptions used in, e.g., present climate models. With the comprehensive analysis of laboratory data using molecular models, we explain the microphysical behavior of the aerosol over the range of humidity observed in the atmosphere, in a way that has never been done before. We also demonstrate the presence of these phenomena in the ambient atmosphere from data collected in the field. We further show, using two state-of-the-art climate models, that misrepresenting the water affinity of atmospheric organic aerosol can lead to significant biases in the estimates of the anthropogenic influence on climate.


领域气候变化
收录类别SCI-E
WOS记录号WOS:000404131900093
WOS关键词CONDENSATION NUCLEI ACTIVITY ; LIQUID PHASE-SEPARATION ; DROPLET ACTIVATION KINETICS ; REGIONAL DUST SAMPLES ; EARTH SYSTEM MODEL ; HYGROSCOPIC GROWTH ; BOREAL FOREST ; RELATIVE HUMIDITIES ; CLOUD ACTIVATION ; ELEMENTAL RATIO
WOS类目Geosciences, Multidisciplinary
WOS研究方向Geology
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/28086
专题气候变化
作者单位1.Stockholm Univ, Dept Environm Sci & Analyt Chem ACES, Stockholm, Sweden;
2.Stockholm Univ, Bolin Ctr Climate Res, Stockholm, Sweden;
3.Univ Eastern Finland, Dept Appl Phys, Kuopio, Finland;
4.McGill Univ, Dept Atmospher & Ocean Sci, Montreal, PQ, Canada;
5.Chonbuk Natl Univ, Dept Earth & Environm Sci, Jeonju, South Korea;
6.Univ British Columbia, Dept Chem, Vancouver, BC, Canada;
7.Norwegian Meteorol Inst, Oslo, Norway;
8.Rice Univ, Dept Civil & Environm Engn, Houston, TX USA;
9.Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA;
10.Univ Colorado, Dept Chem & Biochem, Boulder, CO USA;
11.Texas A&M Univ, Dept Atmospher Sci, College Stn, TX USA;
12.Aerodyne Res Inc, Billerica, MA USA;
13.Boston Coll, Dept Chem, Chestnut Hill, MA 02167 USA;
14.Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA;
15.Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA;
16.Natl Observ Athens, Inst Environm Res & Sustainable Dev, Palea Penteli, Greece;
17.Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA;
18.Univ Helsinki, Dept Phys, Helsinki, Finland;
19.Univ Manchester, Sch Earth & Environm Sci, Manchester, Lancs, England;
20.Stockholm Univ, Dept Meteorol, Stockholm, Sweden;
21.Fdn Res & Technol Hellas, Inst Chem Engn Sci, Patras, Greece;
22.Univ Manchester, NCAS, Manchester, Lancs, England
推荐引用方式
GB/T 7714
Rastak, N.,Pajunoja, A.,Navarro, J. C. Acosta,et al. Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate[J]. GEOPHYSICAL RESEARCH LETTERS,2017,44(10).
APA Rastak, N..,Pajunoja, A..,Navarro, J. C. Acosta.,Ma, J..,Song, M..,...&Riipinen, I..(2017).Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate.GEOPHYSICAL RESEARCH LETTERS,44(10).
MLA Rastak, N.,et al."Microphysical explanation of the RH-dependent water affinity of biogenic organic aerosol and its importance for climate".GEOPHYSICAL RESEARCH LETTERS 44.10(2017).
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