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

Submicron particle mass concentrations and sources in the Amazonian wet season (AMAZE-08)
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DOI:
10.5194/acp-15-3687-2015
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发表时间:
2015-04
影响因子:
6.3
通讯作者:
Qi Chen;D. Farmer;L. Rizzo;T. Pauliquevis;M. Kuwata;T. Karl;A. Guenther;J. Allan;H. Coe;M. Andreae;U. Pöschl;J. Jimenez;P. Artaxo;S. Martin
Qi Chen;D. Farmer;L. Rizzo;T. Pauliquevis;M. Kuwata;T. Karl;A. Guenther;J. Allan;H. Coe;M. Andreae;U. Pöschl;J. Jimenez;P. Artaxo;S. Martin
中科院分区:
地球科学1区
文献类型:
--
作者:
Qi Chen;D. Farmer;L. Rizzo;T. Pauliquevis;M. Kuwata;T. Karl;A. Guenther;J. Allan;H. Coe;M. Andreae;U. Pöschl;J. Jimenez;P. Artaxo;S. Martin

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抽象的。作为亚马逊气溶胶表征实验 (AMAZE-08) 的一部分,2008 年 2 月至 3 月雨季期间,在亚马逊盆地中部的热带雨林中记录了亚微米气溶胶颗粒中非难熔物质的实时质谱。在测量期间,有机材料平均占非难熔亚微米颗粒质量浓度的 80% 以上。没有足够的铵来中和硫酸盐。在这种酸性、富含异戊二烯、HO2 占主导地位的环境中,颗粒质谱时间序列的正矩阵分解确定了四个统计因素,以解释有机成分信号强度中 99% 的方差。第一个因素被确定为与区域和当地污染有关,并因其类似碳氢化合物的特征而被标记为“HOA”。第二个因素与长程运输有关,因其含氧特性而被标记为“OOA-1”。第三个因素,标记为“OOA-2”,与异戊二烯氧化产物的反应性吸收有关,尤其是环氧二醇对酸性薄雾、雾或云滴的反应性吸收。第四个因素,标记为“OOA-3”,与通过生物挥发性有机前体的气相氧化机制以及氧化产物的气体到颗粒转化的机制与二次有机材料(SOM)的新鲜生产相关。 OOA 标签上的后缀 1、2 和 3 表示相对于该因子所代表的氧化程度的顺序排列。气相光化学水溶性产物的水相氧化过程也可能在某种程度上与 OOA-2 因子有关。 OOA-2 : OOA-3 的活动平均因子负荷比率为 1.4:1,表明在研究期间颗粒相与气相途径对于 SOM 的生产具有相当的重要性。
Abstract. 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 gas-phase 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.