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Analysis of functional groups in atmospheric aerosols by infrared spectroscopy: method development for probabilistic modeling of organic carbon and organic matter concentrations
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Analysis of functional groups in atmospheric aerosols by infrared spectroscopy: method development for probabilistic modeling of organic carbon and organic matter concentrations
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Analysis of functional groups in atmospheric aerosols by infrared spectroscopy: method development for probabilistic modeling of organic carbon and organic matter concentrations
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Journal Article
Analysis of functional groups in atmospheric aerosols by infrared spectroscopy: method development for probabilistic modeling of organic carbon and organic matter concentrations
2020
Overview
The Fourier transform infrared (FTIR) spectra of fine particulate matter (PM2.5) contain many important absorption bands relevant for characterizing organic matter (OM) and obtaining organic matter to organic carbon (OM∕OC) ratios. However, extracting this information quantitatively – accounting for overlapping absorption bands and relating absorption to molar abundance – and furthermore relating abundances of functional groups to that of carbon atoms poses several challenges. In this work, we define a set of parameters that model these relationships and apply a probabilistic framework to identify values consistent with collocated field measurements of thermal–optical reflectance organic carbon (TOR OC). Parameter values are characterized for various sample types identified by cluster analysis of sample FTIR spectra, which are available for 17 sites in the Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring network (7 sites in 2011 and 10 additional sites in 2013). The cluster analysis appears to separate samples according to predominant influence by dust, residential wood burning, wildfire, urban sources, and biogenic aerosols. Functional groups calibrations of aliphatic CH, alcohol COH, carboxylic acid COOH, carboxylate COO, and amine NH2 combined together reproduce TOR OC concentrations with reasonable agreement (r=0.96 for 2474 samples) and provide OM∕OC values generally consistent with our current best estimate of ambient OC. The mean OM∕OC ratios corresponding to sample types determined from cluster analysis range between 1.4 and 2.0, though ratios for individual samples exhibit a larger range. Trends in OM∕OC for sites aggregated by region or year are compared with another regression approach for estimating OM∕OC ratios from a mass closure equation of the major chemical species contributing to PM fine mass. Differences in OM∕OC estimates are observed according to estimation method and are explained through the sample types determined from spectral profiles of the PM.
