Cluster analysis of the organic peaks in bulk mass spectra obtained during the 2002 New England Air Quality Study with an Aerodyne aerosol mass spectrometer
Cluster analysis of the organic peaks in bulk mass spectra obtained during the 2002 New England Air Quality Study with an Aerodyne aerosol mass spectrometer
复制标题
使用 Aerodyne 气溶胶质谱仪对 2002 年新英格兰空气质量研究期间获得的整体质谱中的有机峰进行聚类分析
DOI：
10.5194/acp-6-5649-2006
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发表时间：
2006
影响因子：
6.3
通讯作者：
A. Middlebrook
中科院分区：
文献类型：
--
作者：
C. Marcolli;M. Canagaratna;D. Worsnop;R. Bahreini;J. Gouw;C. Warneke;P. Goldan;W. Kuster;Eric J. Williams;B. Lerner;J. Roberts;J. F. Meagher;F. Fehsenfeld;M. Marchewka;S. Bertman;A. Middlebrook
我们将层次聚类分析应用于2002年美国东海岸新英格兰空气质量研究期间NOAA科考船罗纳德·H·布朗号上收集的Aerodyne气溶胶质谱仪(AMS)大量质谱仪数据集。通过强调有机峰，聚类分析产生了一系列类别，这些类别可以根据它们的质谱图和它们作为时间函数出现的情况来区分。类别之间的差异主要源于相对强度的变化，而不是特定峰的存在或不存在。最常见的类别在m/z 44处表现出强烈的信号，代表氧化有机质，很可能来自人为和生物来源。根据光谱和痕量气体关联，在m/z 29、43和44处有强信号的第二种最常见的类别包含异戊二烯氧化产物的贡献。第三种到第五种最常见的种类具有单萜类氧化产物的特征峰型，最常在单萜类富集区的气团中观察到。总而言之，第二到第五种最常见的类别代表了高达5微克/立方米的有机气溶胶质量？占总有机质量的17%？这可以归因于生物来源。这些数字必须被视为下限，因为在这一计算中，最常见的类别归因于人为来源。在识别一些在前处理过程中未被去除的受污染的质谱图方面，聚类分析也非常有效。这项研究表明，系统聚类法是一种有用的工具，可以用来分析大量气溶胶质量谱中有机峰的复杂模式。
We applied hierarchical cluster analysis to an Aerodyne aerosol mass spectrometer (AMS) bulk mass spectral dataset collected aboard the NOAA research vessel Ronald H. Brown during the 2002 New England Air Quality Study off the east coast of the United States. Emphasizing the organic peaks, the cluster analysis yielded a series of categories that are distinguishable with respect to their mass spectra and their occurrence as a function of time. The differences between the categories mainly arise from relative intensity changes rather than from the presence or absence of specific peaks. The most frequent category exhibits a strong signal at m/z 44 and represents oxidized organic matter most probably originating from both, anthropogenic as well as biogenic sources. On the basis of spectral and trace gas correlations, the second most common category with strong signals at m/z 29, 43, and 44 contains contributions from isoprene oxidation products. The third through the fifth most common categories have peak patterns characteristic of monoterpene oxidation products and were most frequently observed when air masses from monoterpene rich regions were sampled. Taken together, the second through the fifth most common categories represent as much as 5 µg/m3 organic aerosol mass ? 17% of the total organic mass ? that can be attributed to biogenic sources. These numbers have to be viewed as lower limits since the most common category was attributed to anthropogenic sources for this calculation. The cluster analysis was also very effective in identifying a few contaminated mass spectra that were not removed during pre-processing. This study demonstrates that hierarchical clustering is a useful tool to analyze the complex patterns of the organic peaks in bulk aerosol mass spectra from a field study.