黑碳团簇气溶胶混合生长的红外吸收特性及长波辐射效应

郑利娟; 程天海; 吴俣

doi:10.7498/aps.66.169201

摘要

黑碳气溶胶是当前气溶胶辐射强迫评估中最不确定的因子.本文通过构建黑碳的微物理模型，分别模拟了新鲜状态的黑碳气溶胶和混合生长（老化）后被硫酸盐包裹的黑碳气溶胶，利用叠加T矩阵方法计算获得了具有团簇形态和多成分混合的黑碳气溶胶红外吸收特性，通过大气辐射传输模型模拟了黑碳气溶胶的长波辐射强迫，分析了典型理化参数的敏感性.发现黑碳混合生长可以显著增强其大气层顶的长波辐射强迫，最高可达3倍.而且，包裹黑碳的硫酸盐半径越大，将明显增强大气层顶的黑碳长波辐射强迫.这些发现将有助于降低黑碳气溶胶气候效应评估的不确定性.

关键词:

Abstract

Black carbon aerosols affect the shortwave and longwave radiation in climate in a strong yet uncertain way. In aging process, black carbon particles coated by co-emitted aerosols tend to reduce the shortwave radiative forcing of freshly emitted black carbon at the top of atmosphere (TOA), however, this effect is still unclear in the longwave range. Here in this work, we investigate the effect of black carbon aging on longwave radiative forcing. The freshly emitted black carbon aerosols are simulated to be fractal aggregates consisting of hundreds of small spherical primary particles, and these aggregated black carbon aerosols tend to be fully coated by the large sulfate particles after aging. The optical properties of these freshly emitted and internally mixed black carbon aerosols are simulated using the numerically exact superposition T-matrix method, and their longwave radiative forcings are calculated by the radiative transfer equation solver. The results indicate that the black carbon longwave radiative forcing at TOA is remarkably amplified (up to 3) by coating the large sulfate particles, while the black carbon shortwave radiative forcings decrease during their aging. Moreover, the thicker sulfate coatings tend to increase the longwave radiative forcings of black carbon aerosols at TOA. These findings should improve our understanding of the effect of black carbon aging on their longwave radiative forcings and provide guidance for assessing the climate change.

Keywords:

作者及机构信息

1.
中国科学院遥感与数字地球研究所, 北京 100101;

2.
中国科学院大学, 北京 100049

通信作者: 程天海, chength@radi.ac.cn

基金项目: 国家自然科学基金（批准号：41401386，41371015，41001207）、国家高分辨率对地观测系统重大专项（批准号：30-Y20A21-9003-15/17）和遥感科学国家重点实验室开放基金（批准号：OFSLRSS201619）资助的课题.

Authors and contacts

1.
Institute of Remote Sensing and Digital Earth, Chinese Academy of Sciences, Beijing 100101, China;

2.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Cheng Tian-Hai, chength@radi.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 41401386, 41371015, 41001207), the Major Special Project-the China High-Resolution Earth Observation System (Grant No. 30-Y20A21-9003-15/17) and Open Fund Project of State Key Laboratory of Remote Sensing Science, China (Grant No. OFSLRSS201619).

参考文献

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[50]	Cheng T, Wu Y, Chen H 2014 Opt. Express 22 15904
[51]	Wu Y, Cheng T, Zheng L 2016 J. Quant. Spectrosc. Radiat. Transfer 182 1
[52]	Wu Y, Cheng T, Zheng L, Chen H 2015 Aerosol. Sci. Tech. 49 941
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[55]	Adachi K, Chung S H 2010 J. Geophys. Res.:Atmos. 115 D15206
[56]	Wu Y, Cheng T, Zheng L, Chen H 2016 Sci. Rep. 6 38592

施引文献

[1]	Jacobson M Z 2001 Nature 409 695
[2]	Bellouin N, Boucher O, Haywood J, Reddy M S 2005 Nature 438 1138
[3]	Shindell D, Faluvegi G 2009 Nature Geosci. 2 294
[4]	Ramanathan V, Carmichael G 2008 Nature Geosci. 1 221
[5]	Bond T C, Doherty S J, Fahey D W, Forster P M, Berntsen T, Boucher O, DeAngelo B J, Flanner M G, Ghan S, Krcher B, Koch D, Kinne S, Kondo Y, Quinn P K, Sarofim M C, Schultz M G, Schulz M, Venkataraman C, Zhang H, Zhang S, Bellouin N, Guttikunda S K, Hopke P K, Jacobson M Z, Kaiser J W, Klimont Z, Lohmann U, Schwarz J P, Shindell D, Storelvmo T, Warren S G, Zender C S 2013 J. Geophys. Res.:Atmos. 118 5380
[6]	Adachi K, Buseck P R 2008 Atmos. Chem. Phys. 8 6469
[7]	China S, Mazzoleni C, Gorkowski K, Aiken A C, Dubey M K 2013 Nat. Commun. 4 2122
[8]	McFiggans G, Artaxo P, Baltensperger U, Coe H, Facchini M C, Feingold G, Fuzzi S, Gysel M, Laaksonen A, Lohmann U, Mentel T F, Murphy D M, O'Dowd C D, Snider J R, Weingartner E 2006 Atmos. Chem. Phys. 6 2593
[9]	Zhou Y, Savijrvi H 2014 Atmos. Res. 135 102
[10]	Ramana, M V, Ramanathan V, Feng Y, Yoon S C, Kim S W, Carmichael G R, Schauer J J 2010 Nature Geosci. 3 542
[11]	Kahnert M, Nousiainen T, Lindqvist H, Ebert M 2012 Opt. Express 20 10042
[12]	Cappa C D, Onasch T B, Massoli P, Worsnop D R, Bates T S, Cross E S, Davidovits P, Hakala J, Hayden K L, Jobson B T, Kolesar K R, Lack D A, Lerner B M, Li S M, Mellon D, Nuaaman I, Olfert J S, Petj T, Quinn P K, Song C, Subramanian R, Williams E J, Zaveri R A 2012 Science 337 1078
[13]	Jacobson M Z 2013 Science 339 393
[14]	Cappa C D, Onasch T B, Massoli P, Worsnop D R, Bates T S, Cross E S, Davidovits P, Hakala J, Hayden K L, Jobson B T, Kolesar K R, Lack D A, Lerner B M, Li S M, Mellon D, Nuaaman I, Olfert J S, Petj T, Quinn P K, Song C, Subramanian R, Williams E J, Zaveri R A 2013 Science 339 393
[15]	Stocker T F, Qin D, Plattner G K, Tignor M, Allen S K, Boschung J, Nauels A, Xia Y, Bex V, Midgley P M 2013 Climate Change 2013:The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change (Cambridge:Cambridge University Press) p573
[16]	Widmann J F, Yang J C, Smith T J, Manzello S L, Mulholland G W 2003 Combust. Flame 134 119
[17]	Kahnert M 2010 Atmos. Chem. Phys. 10 8319
[18]	Prasanna S, Rivire P H, Soufiani A 2014 J. Quant. Spectrosc. Radiat. Transfer 148 141
[19]	Smith A J A, Peters D M, McPheat R, Lukanihins S, Grainger R G 2015 J. Geophys. Res.:Atmos. 120 9670
[20]	Heinson W R, Chakrabarty R K 2016 Opt. Lett. 41 808
[21]	Mikhailov E F, Vlasenko S S, Podgorny I A, Ramanathan V, Corrigan C E 2006 J. Geophy. Res.:Atmos. 111 D7
[22]	Zhang R, Khalizov A F, Pagels J, Zhang D, Xue H, McMurry P H 2008 Proc. Natl. Acad. Sci. 105 10291
[23]	Khalizov A F, Xue H, Wang L, Zheng J, Zhang R 2009 J. Phys. Chem. A 113 1066
[24]	Bueno P A, Havey D K, Mulholland G W, Hodges J T, Gillis K A, Dickerson R R, Zachariah M R 2011 Aerosol. Sci. Tech. 45 1217
[25]	Mishchenko M I, Dlugach J M 2012 Opt. Lett. 37 704
[26]	Cheng T, Gu X, Wu Y, Chen H 2014 J. Quant. Spectrosc. Radiat. Transfer 147 196
[27]	Wu Y, Cheng T, Zheng L, Chen H, Xu H 2015 J. Quant. Spectrosc. Radiat. Transfer 157 1
[28]	Fierce L, Bond T C, Bauer S E, Mena F, Riemer N 2016 Nat. Commun. 7 1
[29]	You R, Radney J G, Zachariah M R, Zangmeister C D 2016 Environ. Sci. Technol. 50 7982
[30]	Schwarz J P, Gao R S, Spackman J R, Watts L A, Thomson D S, Fahey D W, Ryerson T B, Peischl J, Holloway J S, Trainer M, Frost G J, Baynard T, Lack D A, Gouw J A de, Warneke C, Del Negro L A 2008 Geophys. Res. Lett. 35 L13810
[31]	Lack D A, Moosmller H, McMeeking G R, Chakrabarty R K, Baumgardner D 2014 Anal. Bioanal. Chem. 406 99
[32]	Chakrabarty R K, Beres N D, Moosmller H, China S, Mazzoleni C, Dubey M K, Liu L, Mishchenko M I 2014 Sci. Rep. 4 1
[33]	Li W, Shao L, Zhang D, Ro C, Hu M, Bi X, Geng H, Matsuki A, Niu H, Chen J 2016 J. Clean. Prod. 112 1330
[34]	Liu L, Mishchenko M I, Arnott W P 2008 J. Quant. Spectrosc. Radiat. Transfer 109 2656
[35]	Wu Y, Cheng T, Gu X, Zheng L, Chen H, Xu H 2014 J. Quant. Spectrosc. Radiat. Transfer 135 9
[36]	Hentschel H G E 1984 Phys. Rev. Lett. 52 212
[37]	Cheng T, Wu Y, Gu X, Chen H 2015 Opt. Express 23 10808
[38]	Bond T C, Bergstrom R W 2006 Aerosol. Sci. Tech. 40 27
[39]	John W, Wall S M, Ondo J L, Winklmayr W 1990 Atmos. Environ. Part A. General Topics 24 2349
[40]	Chang H, Charalampopoulos T T 1990 Procee. Roy. Soc. Lon. Ser. A:Math. Phys. Sci. 430 577
[41]	Toon O B, Pollack J B, Khare B N 1976 J. Geophys. Res. 81 5733
[42]	Mackowski D W, Mishchenko M I 2011 J. Quant. Spectrosc. Radiat. Transfer 112 2182
[43]	Mishchenko M I, Liu L, Mackowski D W 2013 J. Quant. Spectrosc. Radiat. Transfer 123 135
[44]	Mackowski D W 2014 J. Quant. Spectrosc. Radiat. Transfer 133 264
[45]	Buras R, Dowling T, Emde C 2011 J. Quant. Spectrosc. Radiat. Transfer 112 2028
[46]	Mayer B, Kylling A 2005 Atmos. Chem. Phys. 5 1855
[47]	Gasteiger J, Emde C, Mayer B, Buras R, Buehler S A, Lemke O 2014 J. Quant. Spectrosc. Radiat. Transfer 148 99
[48]	Kahnert M, Nousiainen T, Lindqvist H 2013 Opt. Express 21 7974
[49]	Wu Y, Cheng T, Zheng L, Chen H 2016 J. Quant. Spectrosc. Radiat. Transfer 179 139
[50]	Cheng T, Wu Y, Chen H 2014 Opt. Express 22 15904
[51]	Wu Y, Cheng T, Zheng L 2016 J. Quant. Spectrosc. Radiat. Transfer 182 1
[52]	Wu Y, Cheng T, Zheng L, Chen H 2015 Aerosol. Sci. Tech. 49 941
[53]	Lubin D, Satheesh S K, McFarquar G, Heymsfield A J 2007 J. Geophys. Res.:Atmos. 107 1
[54]	Kahnert M, Devasthale A 2011 Atmos. Chem. Phys. 11 11745
[55]	Adachi K, Chung S H 2010 J. Geophys. Res.:Atmos. 115 D15206
[56]	Wu Y, Cheng T, Zheng L, Chen H 2016 Sci. Rep. 6 38592

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