Effects of aging on organic aerosol from open biomass burning smoke in aircraft and lab studies

Cubison, M. J.; Ortega, A. M.; Hayes, Patrick L.; Farmer, Delphine K.; Day, Douglas A.; Lechner, M.; Brune, W. H.; Apel, E. C.; Diskin, G. S.; Fisher, Jenny A.; Fuelberg, Henry E.; Hecobian, A.; Knapp, D. J.; Mikoviny, Tomáš; Riemer, D. D.; Sachse, G. W.; Sessions, W. R.; Weber, R. J.; Weinheimer, A. J.; Wisthaler, Armin; Jimenez, J. L.

doi:10.5194/acpd-11-12103-2011

Cited by 27 publications

(37 citation statements)

References 73 publications

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“…Our estimated SOA source from ageing of POA (23 Tg (SOA) a −1 ) is within the range (10-66 Tg (SOA) a −1 ) from Hallquist et al (2009) and is greater than that directly from biomass burning which is consistent with recent field observations (Cubison et al, 2011). Our estimated biogenic SOA source (13 Tg (SOA) a −1 ) is at the lower end of previous estimates, being 1-2 orders-of-magnitude lower than the range of estimates from Goldstein and Galbally (2007) although within the very broad range (0-360 Tg (SOA) a −1 ) from Hallquist et al (2009).…”

Section: Discussion Of Our Estimated Soa Sourcessupporting

confidence: 78%

Aerosol mass spectrometer constraint on the global secondary organic aerosol budget

et al. 2011

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Abstract.The budget of atmospheric secondary organic aerosol (SOA) is very uncertain, with recent estimates suggesting a global source of between 12 and 1820 Tg (SOA) a −1 . We used a dataset of aerosol mass spectrometer (AMS) observations from 34 different surface locations to evaluate the GLOMAP global chemical transport model. The standard model simulation (which included SOA from monoterpenes only) underpredicted organic aerosol (OA) observed by the AMS and had little skill reproducing the variability in the dataset. We simulated SOA formation from biogenic (monoterpenes and isoprene), lumped anthropogenic and lumped biomass burning volatile organic compounds (VOCs) and varied the SOA yield from each precursor source to produce the best overall match between model and observations. We assumed that SOA is essentially non-volatile and condenses irreversibly onto existing aerosol. Our best estimate of the SOA source is 140 Tg (SOA) a −1 but with a large uncertainty range which we estimate to be 50-380 Tg (SOA) a −1 . We found the minimum in normalised mean error (NME) between model and the AMS dataset when we assumed a large SOA source (100 Tg (SOA) a −1 ) from sources that spatially matched anthropogenic pollution (which we term antropogenically controlled SOA). We used organic carbon observations compiled by Bahadur et al. (2009) to evaluate our estimated SOA sources. We found that the model with a large anthropogenic SOA source was the most consistent with these observaCorrespondence to: D. V. Spracklen (dominick@env.leeds.ac.uk) tions, however improvement over the model with a large biogenic SOA source (250 Tg (SOA) a −1 ) was small. We used a dataset of 14 C observations from rural locations to evaluate our estimated SOA sources. We estimated a maximum of 10 Tg (SOA) a −1 (10 %) of the anthropogenically controlled SOA source could be from fossil (urban/industrial) sources. We suggest that an additional anthropogenic source is most likely due to an anthropogenic pollution enhancement of SOA formation from biogenic VOCs. Such an anthropogenically controlled SOA source would result in substantial climate forcing. We estimated a global mean aerosol direct effect of −0.26 ± 0.15 Wm −2 and indirect (cloud albedo) effect of −0.6 +0.24 −0.14 Wm −2 from anthropogenically controlled SOA. The biogenic and biomass SOA sources are not well constrained with this analysis due to the limited number of OA observations in regions and periods strongly impacted by these sources. To further improve the constraints by this method, additional OA observations are needed in the tropics and the Southern Hemisphere.

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Section: Discussion Of Our Estimated Soa Sourcessupporting

confidence: 78%

Aerosol mass spectrometer constraint on the global secondary organic aerosol budget

et al. 2011

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“…During the different seasons, m/z 60 had a small contribution to total OA (around 0.3 %). Such low contribution of m/z 60 to total OA was considered as representative for a background level value of SOA dominated ambient organic aerosol (Cubison et al, 2011). Based on the m/z 60 contribution, it is concluded that there is only a minor influence of biomass burning aerosol on total OA, even during winter.…”

Section: Comparison Of the Organic Aerosol Mass Spectramentioning

confidence: 99%

Seasonal and diurnal variations of particulate nitrate and organic matter at the IfT research station Melpitz

et al. 2011

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Ammonium nitrate and several organic compounds such as dicarboxylic acids (e.g. succinic acid, glutaric acid), some Polycyclic Aromatic Hydrocarbon (PAHs) or some n-alkanes are semi-volatile. The transition of these compounds between the gas and particulate phase may significantly change the aerosol particles radiative properties, the heterogeneous chemical properties, and, naturally, the total particulate mass concentration. To better assess these time-dependent effects, three intensive field experiments were conducted in 2008–2009 at the Central European EMEP research station Melpitz (Germany) using an Aerodyne Aerosol Mass Spectrometer (AMS). Data from all seasons highlight organic matter as being the most important particulate fraction of PM1 in summer (59%) while in winter, the nitrate fraction was more prevalent (34.4%). The diurnal variation of nitrate always showed the lowest concentration during the day while its concentration increased during the night. This night increase of nitrate concentration was higher in winter (ΔNO3− = 3.6 μg m−3) than in summer (ΔNO3− = 0.7 μg m−3). The variation in particulate nitrate was inherently linked to the gas-to-particle-phase equilibrium of ammonium nitrate and the dynamics of the atmosphere during day. The results of this study suggest that during summer nights, the condensation of HNO3 and NH3 on pre-existing particles represents the most prevalent source of nitrate, whereas during winter, nighttime chemistry is the predominant source of nitrate. During the summer 2008's campaign, a clear diurnal evolution in the oxidation state of the organic matter became evident (Organic Mass to Organic Carbon ratio (OM/OC) ranging from 1.65 during night to 1.80 during day and carbon oxidation state (OSc) from −0.66 to −0.4), which could be correlated to hydroxyl radical (OH) and ozone concentrations, indicating a photochemical transformation process. In summer, the organic particulate matter seemed to be heavily influenced by regional secondary formation and transformation processes, facilitated by photochemical production processes as well as a diurnal cycling of the substances between the gas and particulate phase. In winter, these processes were obviously less pronounced (OM/OC ranging from 1.60 to 1.67 and OSc from −0.8 to −0.7), so that organic matter apparently originated mainly from aged particles and long range transport

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“…However, levoglucosan or its markers have been reported to degrade in aged BB plumes (Hennigan et al, 2010;Cubison et al, 2011). As much as 80 % degradation of levogucosan has been observed in the laboratory under typical atmospheric oxidation conditions (Hennigan et al, 2011).…”

Section: Spectra Categories and Source Contributions From Regression mentioning

confidence: 99%

“…The oxygenated fraction of BB aerosol is also reported to change with age. Levoglucosan (and presumably other anhydrous sugars) are reported to degrade in BB plumes (Hennigan et al, 2010(Hennigan et al, , 2011Cubison et al, 2011), while mass ratios of organic acid to carbonyl are reported to increase with age of airmass in BB plumes Hawkins and Russell (2010).…”

Section: Introductionmentioning

confidence: 99%

Organic functional groups in aerosol particles from burning and non-burning forest emissions at a high-elevation mountain site

et al. 2011

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Abstract. Ambient particles collected on teflon filters at the Peak of Whistler Mountain, British Columbia (2182 m a.s.l.) during spring and summer 2009 were measured by Fourier transform infrared (FTIR) spectroscopy for organic functional groups (OFG). The project mean and standard deviation of organic aerosol mass concentrations (OM) for all samples was 3.2±3.3 (µg m −3 ). Measurements of aerosol mass fragments, size, and number concentrations were used to separate fossil-fuel combustion and burning and non-burning forest sources of the measured organic aerosol. The OM was composed of the same anthropogenic and non-burning forest components observed at Whistler mid-valley in the spring of 2008; during the 2009 campaign, biomass burning aerosol was additionally observed from fire episodes occurring between June and September. On average, organic hydroxyl, alkane, carboxylic acid, ketone, and primary amine groups represented 31 %±11 %, 34 %±9 %, 23 %±6 %, 6 %±7 %, and 6 %±3 % of OM, respectively. Ketones in aerosols were associated with burning and non-burning forest origins, and represented up to 27 % of the OM. The organic aerosol fraction resided almost entirely in the submicron fraction without significant diurnal variations. OM/OC mass ratios ranged mostly between 2.0 and 2.2 and O/C atomic ratios between 0.57 and 0.76, indicating that the organic aerosol reaching the site was highly aged and possibly formed through secondary formation processes.

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Effects of aging on organic aerosol from open biomass burning smoke in aircraft and lab studies

Cited by 27 publications

References 73 publications

Aerosol mass spectrometer constraint on the global secondary organic aerosol budget

Aerosol mass spectrometer constraint on the global secondary organic aerosol budget

Seasonal and diurnal variations of particulate nitrate and organic matter at the IfT research station Melpitz

Organic functional groups in aerosol particles from burning and non-burning forest emissions at a high-elevation mountain site

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