Submicron particle mass concentrations and sources in the Amazonian wet season (AMAZE-08)

被引:77
作者
Chen, Q. [1 ,2 ]
Farmer, D. K. [3 ,4 ]
Rizzo, L. V. [5 ]
Pauliquevis, T. [5 ]
Kuwata, M. [1 ,2 ]
Karl, T. G. [6 ,13 ]
Guenther, A. [6 ]
Allan, J. D. [7 ,8 ]
Coe, H. [7 ,8 ]
Andreae, M. O. [9 ,10 ]
Poeschl, U. [9 ,10 ]
Jimenez, J. L. [3 ,4 ]
Artaxo, P. [11 ,12 ]
Martin, S. T. [1 ,2 ]
机构
[1] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 USA
[2] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA
[3] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA
[4] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[5] Univ Fed Sao Paulo, Dept Nat & Earth Sci, Diadema, Brazil
[6] Natl Ctr Atmospher Res, Boulder, CO 80307 USA
[7] Univ Manchester, Natl Ctr Atmospher Sci, Manchester, Lancs, England
[8] Univ Manchester, Sch Earth Atmospher & Environm Sci, Manchester, Lancs, England
[9] Max Planck Inst Chem, Biogeochem Dept, D-55128 Mainz, Germany
[10] Max Planck Inst Chem, Multiphase Chem Dept, D-55128 Mainz, Germany
[11] Univ Sao Paulo, Appl Phys Dept, Sao Paulo, Brazil
[12] Univ Sao Paulo, Dept Atmospher Sci, Sao Paulo, Brazil
[13] Univ Innsbruck, Inst Meteorol & Geophys, Innsbruck, Austria
基金
巴西圣保罗研究基金会; 美国国家科学基金会;
关键词
SECONDARY ORGANIC AEROSOL; POSITIVE MATRIX FACTORIZATION; CLOUD CONDENSATION NUCLEI; ISOPRENE EPOXYDIOLS; RAIN-FOREST; REACTIVE UPTAKE; CHEMISTRY; PHASE; BASIN; SOA;
D O I
10.5194/acp-15-3687-2015
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Real-time mass spectra of the non-refractory species in submicron aerosol particles were recorded in a tropical rainforest in the central Amazon Basin during the wet season from February to March 2008, as a part of the Amazonian Aerosol Characterization Experiment (AMAZE-08). Organic material accounted on average for more than 80% of the non-refractory submicron particle mass concentrations during the period of measurements. There was insufficient ammonium to neutralize sulfate. In this acidic, isoprene-rich, HO2-dominant environment, positive-matrix factorization of the time series of particle mass spectra identified four statistical factors to account for the 99% of the variance in the signal intensities of the organic constituents. The first factor was identified as associated with regional and local pollution and labeled "HOA" for its hydrocarbon-like characteristics. A second factor was associated with long-range transport and labeled "OOA-1" for its oxygenated characteristics. A third factor, labeled "OOA-2," was implicated as associated with the reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets. A fourth factor, labeled "OOA-3," was consistent with an association with the fresh production of secondary organic material (SOM) by the mechanism of gasphase oxidation of biogenic volatile organic precursors followed by gas-to-particle conversion of the oxidation products. The suffixes 1, 2, and 3 on the OOA labels signify ordinal ranking with respect to the extent of oxidation represented by the factor. The process of aqueous-phase oxidation of water-soluble products of gas-phase photochemistry might also have been associated to some extent with the OOA-2 factor. The campaign-average factor loadings had a ratio of 1.4 : 1 for OOA-2 : OOA-3, suggesting the comparable importance of particle-phase compared to gas-phase pathways for the production of SOM during the study period.
引用
收藏
页码:3687 / 3701
页数:15
相关论文
共 61 条
[1]   Aerosol number fluxes over the Amazon rain forest during the wet season [J].
Ahlm, L. ;
Nilsson, E. D. ;
Krejci, R. ;
Martensson, E. M. ;
Vogt, M. ;
Artaxo, P. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (24) :9381-9400
[2]   O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry [J].
Aiken, Allison C. ;
Decarlo, Peter F. ;
Kroll, Jesse H. ;
Worsnop, Douglas R. ;
Huffman, J. Alex ;
Docherty, Kenneth S. ;
Ulbrich, Ingrid M. ;
Mohr, Claudia ;
Kimmel, Joel R. ;
Sueper, Donna ;
Sun, Yele ;
Zhang, Qi ;
Trimborn, Achim ;
Northway, Megan ;
Ziemann, Paul J. ;
Canagaratna, Manjula R. ;
Onasch, Timothy B. ;
Alfarra, M. Rami ;
Prevot, Andre S. H. ;
Dommen, Josef ;
Duplissy, Jonathan ;
Metzger, Axel ;
Baltensperger, Urs ;
Jimenez, Jose L. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (12) :4478-4485
[3]   Aerosols before pollution [J].
Andreae, Meinrat O. .
SCIENCE, 2007, 315 (5808) :50-51
[4]   THE ATMOSPHERIC SULFUR CYCLE OVER THE AMAZON BASIN .2. WET SEASON [J].
ANDREAE, MO ;
BERRESHEIM, H ;
BINGEMER, H ;
JACOB, DJ ;
LEWIS, BL ;
LI, SM ;
TALBOT, RW .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1990, 95 (D10) :16813-16824
[5]  
[Anonymous], 2013, CONTRIBUTION WORKING
[6]   Further evidence for significant smoke transport from Africa to Amazonia [J].
Baars, H. ;
Ansmann, A. ;
Althausen, D. ;
Engelmann, R. ;
Artaxo, P. ;
Pauliquevis, T. ;
Souza, R. .
GEOPHYSICAL RESEARCH LETTERS, 2011, 38
[7]   Transport of North African dust from the Bod,l, depression to the Amazon Basin: a case study [J].
Ben-Ami, Y. ;
Koren, I. ;
Rudich, Y. ;
Artaxo, P. ;
Martin, S. T. ;
Andreae, M. O. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (16) :7533-7544
[8]   Real-Time Continuous Characterization of Secondary Organic Aerosol Derived from Isoprene Epoxydiols in Downtown Atlanta, Georgia, Using the Aerodyne Aerosol Chemical Speciation Monitor [J].
Budisulistiorini, Sri Hapsari ;
Canagaratna, Manjula R. ;
Croteau, Philip L. ;
Marth, Wendy J. ;
Baumann, Karsten ;
Edgerton, Eric S. ;
Shaw, Stephanie L. ;
Knipping, Eladio M. ;
Worsnop, Douglas R. ;
Jayne, John T. ;
Gold, Avram ;
Surratt, Jason D. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (11) :5686-5694
[9]   Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications [J].
Canagaratna, M. R. ;
Jimenez, J. L. ;
Kroll, J. H. ;
Chen, Q. ;
Kessler, S. H. ;
Massoli, P. ;
Hildebrandt Ruiz, L. ;
Fortner, E. ;
Williams, L. R. ;
Wilson, K. R. ;
Surratt, J. D. ;
Donahue, N. M. ;
Jayne, J. T. ;
Worsnop, D. R. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2015, 15 (01) :253-272
[10]   Chase studies of particulate emissions from in-use New York City vehicles [J].
Canagaratna, MR ;
Jayne, JT ;
Ghertner, DA ;
Herndon, S ;
Shi, Q ;
Jimenez, JL ;
Silva, PJ ;
Williams, P ;
Lanni, T ;
Drewnick, F ;
Demerjian, KL ;
Kolb, CE ;
Worsnop, DR .
AEROSOL SCIENCE AND TECHNOLOGY, 2004, 38 (06) :555-573