Biogenic and biomass burning organic aerosol in a boreal forest at Hyytiälä, Finland, during HUMPPA-COPEC 2010
Author:
Corrigan A. L., Russell L. M.ORCID, Takahama S.ORCID, Äijälä M., Ehn M.ORCID, Junninen H., Rinne J.ORCID, Petäjä T.ORCID, Kulmala M., Vogel A. L.ORCID, Hoffmann T., Ebben C. J., Geiger F. M., Chhabra P., Seinfeld J. H.ORCID, Worsnop D. R., Song W., Auld J., Williams J.
Abstract
Abstract. Submicron aerosol particles were collected during July and August 2010 in Hyytiälä, Finland, to determine the composition and sources of aerosol at that Boreal forest site. Submicron particles were collected on Teflon filters and analyzed by Fourier transform infrared (FTIR) spectroscopy for organic functional groups (OFG). Positive matrix factorization (PMF) was applied to aerosol mass spectrometry (AMS) measurements and FTIR spectra to identify summertime sources of submicron aerosol mass at the sampling site. The two largest sources of organic mass (OM) in particles identified at Hyytiälä were (1) biogenic aerosol from surrounding local forest and (2) biomass burning aerosol, transported 4–5 days from large wildfires burning near Moscow, Russia, and northern Ukraine. The robustness of this apportionment is supported by the agreement of two independent analytical methods for organic measurements with three statistical techniques. FTIR factor analysis was more sensitive to the chemical differences between biogenic and biomass burning organic components, while AMS factor analysis had a higher time resolution that more clearly linked the temporal behavior of separate OM factors to that of different source tracers even though their fragment mass spectrum were similar. The greater chemical sensitivity of the FTIR is attributed to the nondestructive preparation and the functional group specificity of spectroscopy. The FTIR spectra show strong similarities among biogenic and biomass burning factors from different regions as well as with reference OM (namely olive tree burning BBOA and α-pinene chamber secondary organic aerosol (SOA)). The biogenic factor correlated strongly with temperature and oxidation products of biogenic volatile organic compounds (BVOCs), included more than half oxygenated OFGs (carbonyl groups at 29% and carboxylic acid groups at 22%), and represented 35% of the submicron OM. Compared to previous studies at Hyytiälä, the summertime biogenic OM is 1.5 to 3 times larger than springtime biogenic OM (0.64 μg m−3 and 0.4 μg m−3, measured in 2005 and 2007, respectively), even though it contributed only 35% of OM. The biomass burning factor contributed 25% OM on average and up to 62% OM during three periods of transported biomass burning emissions: 26–28 July, 29–30 July, and 8–9 August, with OFG consisting mostly of carbonyl (41%) and alcohol (25%) groups. The high summertime terrestrial biogenic OM (1.7 μg m−3) and the high biomass burning contributions (1.2 μg m−3) were likely due to the abnormally high temperatures that resulted in both stressed boreal forest conditions with high regional BVOC emissions and numerous wildfires in upwind regions.
Funder
European Commission
Publisher
Copernicus GmbH
Reference119 articles.
1. Ahlm, L., Shakya, K. M., Russell, L. M., Schroder, J. C., Wong, J. P. S., Sjostedt, S. J., Hayden, K. L., Liggio, J., Wentzell, J. J. B., Wiebe, H. A., Mihele, C., Leaitch, W. R., and Macdonald, A. M.: Temperature-dependent accumulation mode particle and cloud nuclei concentrations from biogenic sources during WACS 2010, Atmos. Chem. Phys., 13, 3393–3407, https://doi.org/10.5194/acp-13-3393-2013, 2013. 2. Aiken, A. C., DeCarlo, P. F., Kroll, J., Huffman, L. A., Worsnop, D. R., Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Sun, Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratana, M. R., Onasch, T. B., Alfarra, M. R., Prevot, A. S. H., Dommen, J., Duplissy, J., Metzger, A., Baltenperger, U., and Jimenze, J. L.: O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry, Environ. Sci. Technol., 42, 4478–4485, 2008. 3. Alfarra, M. R., Coe, H., Allan, J. D., Bower, K. N., Boudries, H., Canagaratna, M. R., Jimenez, J. L., Jayne, J. T., Garforth, A. A., Li, S. M., and Worsnop, D. R.: Characterization of urban and rural organic particulate in the lower fraser valley using two aerodyne aerosol mass spectrometers, Atmos. Environ., 38, 5745–5758, 2004. 4. Allan, J., Jimenez, J. L., Williams, P., Alfarra, M., Bower, K., jayne, J. T., Coe, H., and Worsnop, D. R.: Quantitative sampling using an aerodyne aerosol mass spectrometer: 1. Techniques of data interpretation and error analysis., J. Geophys. Res.-Atmos., 108, 4090, https://doi.org/10.1029/2002JD002358, 2003. 5. Andreae, M. O.: Soot carbon and excess fine potassium – long-range transport of combustion-derived aerosols, Science, 220, 1148–1151, 1983.
Cited by
2 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|