Changes in organic aerosol composition with aging inferred from aerosol mass spectra

Ng, N. L.; Canagaratna, Manjula R.; Jimenez, José L.; Chhabra, P. S.; Seinfeld, John H.; Worsnop, Douglas R.

doi:10.5194/acp-11-6465-2011

Cited by 550 publications

(720 citation statements)

References 28 publications

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“…The solid black line represents observations of ambient aerosol at moderate levels of oxidation 19 . The dashed black line represents measurements of ambient OOA at higher oxidation levels 20 . Red contours represent lines of constant volatility-the approximate number of carbon atoms a molecule must have at a given elemental composition in order to retain a saturation concentration of 500 g m -3 .…”

Section: Resultsmentioning

confidence: 99%

“…In order to compare the results with similar studies of ambient organic aerosol 19,20 , we apply the method of Aiken et al 15,16 with no additional correction factor. The measured H/C and O/C values of the pure compounds tend to be lower than their exact values; however, the overall trends observed in the trajectories remain unchanged, regardless of the correction factor used.…”

Section: Elemental Analysismentioning

confidence: 99%

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OH-Initiated Heterogeneous Aging of Highly Oxidized Organic Aerosol

et al. 2012

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The oxidative evolution ("aging") of organic species in the atmosphere is thought to have a major influence on the composition and properties of organic particulate matter, but remains poorly understood, particularly for the most oxidized fraction of the aerosol. Here we measure the kinetics and products of the heterogeneous oxidation of highly oxidized organic aerosol, with an aim of better constraining such atmospheric aging processes. Submicron particles composed of model oxidized organics-1,2,3,4-butanetetracarboxylic acid (C 8 H 10 O 8 ), citric acid (C 6 H 8 O 7 ), tartaric acid (C 4 H 6 O 6 ), and Suwannee River fulvic acid-were oxidized by gas-phase OH in a flow reactor, and the masses and elemental composition of the particles were monitored as a function of OH exposure. In contrast to our previous studies of less-oxidized model systems (squalane, erythritol, and levoglucosan), particle mass did not decrease significantly with heterogeneous oxidation. Carbon content of the aerosol always decreased somewhat, but this mass loss was approximately balanced by an increase in oxygen content. The estimated reactive 2 uptake coefficients of the reactions range from 0.37 to 0.51 and indicate that such transformations occur at rates corresponding to 1-2 weeks in the atmosphere, suggesting their importance in the atmospheric lifecycle of organic particulate matter.

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Section: Resultsmentioning

confidence: 99%

Section: Elemental Analysismentioning

confidence: 99%

OH-Initiated Heterogeneous Aging of Highly Oxidized Organic Aerosol

et al. 2012

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“…Fig. 3A shows the O:C and the hydrogento-carbon (H:C) values of the aqSOA and BBOA factors in the Van Krevelen (VK) diagram, which is typically used to investigate the OA evolution during field and laboratory experiments (34,35). We plot the elemental ratios of the PMF factors to remove the effect of physical mixing between secondary and primary aerosols, allowing for a clearer and stronger interpretation of the results in the VK space.…”

Section: Discussionmentioning

confidence: 99%

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

Gilardoni

Massoli

Paglione

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

306

275

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The mechanisms leading to the formation of secondary organic aerosol (SOA) are an important subject of ongoing research for both air quality and climate. Recent laboratory experiments suggest that reactions taking place in the atmospheric liquid phase represent a potentially significant source of SOA mass. Here, we report direct ambient observations of SOA mass formation from processing of biomass-burning emissions in the aqueous phase. Aqueous SOA (aqSOA) formation is observed both in fog water and in wet aerosol. The aqSOA from biomass burning contributes to the "brown" carbon (BrC) budget and exhibits light absorption wavelength dependence close to the upper bound of the values observed in laboratory experiments for fresh and processed biomass-burning emissions. We estimate that the aqSOA from residential wood combustion can account for up to 0.1-0.5 Tg of organic aerosol (OA) per y in Europe, equivalent to 4-20% of the total OA emissions. Our findings highlight the importance of aqSOA from anthropogenic emissions on air quality and climate.particulate matter | air quality | secondary organic aerosol | biomass burning | aqueous processing

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“…In contrast, SOAs are formed by the atmospheric oxidation of gas phase species and represent up to 80% of the total organic aerosols in urban locations . The rapidly evolving and transforming nature of organics in polluted urban and semiurban regions around the globe demand temporally resolved and size-resolved chemical composition measurements to account for the role of organic aerosols in CCN activity Ng et al, 2011]. This need has been fulfilled by the advent of Aerodyne high-resolution-time-of-flight-aerosol mass spectrometer (HR-ToF-AMS).…”

Section: Introductionmentioning

confidence: 99%

CCN closure study: Effects of aerosol chemical composition and mixing state

Bhattu

Tripathi

2015

JGR Atmospheres

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This study presents a detailed cloud condensation nuclei (CCN) closure study that investigates the effects of chemical composition (bulk and size resolved) and mixing state (internal and external) on CCN activity of aerosols. Measurements of the chemical composition, aerosol size distribution, total number concentration, and CCN concentration at supersaturation (SS = 0.2–1.0%) were performed during the winter season in Kanpur, India. Among the two cases considered here, better closure results are obtained for case 1 (low total aerosol loading, 49.54 ± 26.42 μg m−3, and high O:C ratio, 0.61 ±0.07) compared to case 2 (high total aerosol loading, 101.05 ± 18.73 μg m−3, and low O:C ratio, 0.42 ±0.06), with a maximum reduction of 3–81% in CCN overprediction for all depleted SS values (0.18–0.60%). Including the assumption that less volatile oxidized organic aerosols represent the soluble organic fraction reduced the overprediction to at most 40% and 129% in the internal and external mixing scenarios, respectively. At higher depleted SS values (0.34–0.60%), size‐resolved chemical composition with an internal mixing state performed well in CCN closure among all organic solubility scenarios. However, at a lower depleted SS value (0.18%), closure is found to be more sensitive to both the chemical composition and mixing state of aerosols. At higher SS values, information on the solubility of organics and size‐resolved chemical composition is required for accurate CCN predictions, whereas at lower SS values, information on the mixing state in addition to the solubility of organics and size‐resolved chemical composition is required. Overall, κtotal values are observed to be independent of the O:C ratio [κtotal= (0.36 ±0.01) × O:C − (0.03 ± 0.01)] in the range of 0.2

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Changes in organic aerosol composition with aging inferred from aerosol mass spectra

Cited by 550 publications

References 28 publications

OH-Initiated Heterogeneous Aging of Highly Oxidized Organic Aerosol

OH-Initiated Heterogeneous Aging of Highly Oxidized Organic Aerosol

Direct observation of aqueous secondary organic aerosol from biomass-burning emissions

CCN closure study: Effects of aerosol chemical composition and mixing state

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