Why do organic aerosols exist? Understanding aerosol lifetimes using the two-dimensional volatility basis set

Donahue, Neil M.; Chuang, Wayne K.; Epstein, Scott A.; Kroll, J. H.; Worsnop, Douglas R.; Robinson, Allen L.; Adams, P. J.; Pandis, Spyros Ν.

doi:10.1071/en13022

Cited by 112 publications

(119 citation statements)

References 52 publications

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“…Figure 5b shows the OOM mass spectrum, which contained less CO C and more CO C 2 than the POM spectrum. While the OOM mass spectrum may have reflected a mixture of SOM and oxidized POM (Hennigan et al 2011), the MSC residence time of seconds, the much slower rate of heterogeneous versus gas-phase oxidation of organics (Lambe et al 2009;Donahue et al 2013), and the elevated temperatures within the MSC (Section 2.3) suggest that SOM condensed from gas-phase reaction products may have dominated the OOM mass spectrum in this study. This is consistent with the qualitative similarity between the OOM and SOM mass spectra (Figure 3b and c), which differ mainly in a slightly lower CO C :CO C 2 ratio of SOM (Section 2.6).…”

Section: Om Mass Spectrummentioning

confidence: 98%

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Corbin

Keller

Lohmann

et al. 2015

Aerosol Science and Technology

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Logwood and pellet stoves are popular heating sources around the world. The particulate matter emitted from such stoves contains organic particulate matter (OM), soot, and ash, each of which may have significant effects on climate and health. In this study, the primary OM (POM) emitted from a wood stove and a pellet stove operated according to standard Swiss testing protocols were characterized using aerosol mass spectrometry. The POM mass spectra were found to be highly reproducible, and contained CO C as the dominant ion. Because the POM emitted by such stoves is typically enhanced by the condensation of gaseous organics following atmospheric aging, the secondary OM (SOM) formation potential of these stoves was simulated using the Micro Smog Chamber (MSC) designed by Keller and Burtscher in 2012. In general, OM emission factors from MSCaged aerosols were comparable to lower-time-resolution results from the literature, although the MSC exposed aerosols to much higher concentrations of oxidants and therefore produced OM that was more oxidized than expected for atmospheric samples. In addition, the logwood-stove particles remained highly aspherical even after oxidation, indicating that mixing with an external aerosol is required for these particles to become spherical. The one exception to this observation occurred when the wood failed to ignite and appeared to generate tar-ball OM particles.

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Section: Om Mass Spectrummentioning

confidence: 98%

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Corbin

Keller

Lohmann

et al. 2015

Aerosol Science and Technology

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“…In this way, the particulate phase appears to provide a "safe" environment for organic compounds, prolonging their atmospheric life. Donahue et al (2013) proposed that OAs exist throughout the troposphere in part because their heterogeneous oxidation by OH radicals is 1 order of magnitude slower than the corresponding reaction in the gas phase.…”

Section: Condensed Phase Of Organic and Inorganic Chemistrymentioning

confidence: 99%

Particulate matter, air quality and climate: lessons learned and future needs

et al. 2015

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Abstract. The literature on atmospheric particulate matter (PM), or atmospheric aerosol, has increased enormously over the last 2 decades and amounts now to some 1500-2000 papers per year in the refereed literature. This is in part due to the enormous advances in measurement technologies, which have allowed for an increasingly accurate understanding of the chemical composition and of the physical properties of atmospheric particles and of their processes in the atmosphere. The growing scientific interest in atmospheric aerosol particles is due to their high importance for environmental policy. In fact, particulate matter constitutes one of the most challenging problems both for air quality and for climate change policies. In this context, this paper reviews the most recent results within the atmospheric aerosol sciences and the policy needs, which have driven much of the increase in monitoring and mechanistic research over the last 2 decades.The synthesis reveals many new processes and developments in the science underpinning climate-aerosol interactions and effects of PM on human health and the environment. However, while airborne particulate matter is responsible for globally important influences on premature human mortality, we still do not know the relative importance of the different chemical components of PM for these effects. Likewise, the magnitude of the overall effects of PM on climate remains highly uncertain. Despite the uncertainty there are many things that could be done to mitigate local and global problems of atmospheric PM. Recent analyses have shown that reducing black carbon (BC) emissions, using known control measures, would reduce global warming and delay the time when anthropogenic effects on global temperature would exceed 2 • C. Likewise, cost-effective control measures on ammonia, an important agricultural precursor gas for secondary inorganic aerosols (SIA), would reduce regional eutrophication and PM concentrations in large areas of Europe, China and the USA. Thus, there is much that could be done to reduce the effects of atmospheric PM on the climate and the health of the environment and the human population.A prioritized list of actions to mitigate the full range of effects of PM is currently undeliverable due to shortcomings in the knowledge of aerosol science; among the shortcomings, the roles of PM in global climate and the relative roles of Published by Copernicus Publications on behalf of the European Geosciences Union. 8218S. Fuzzi et al.: Particulate matter, air quality and climate different PM precursor sources and their response to climate and land use change over the remaining decades of this century are prominent. In any case, the evidence from this paper strongly advocates for an integrated approach to air quality and climate policies.

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“…Hydrogen numbers were calculated from the van Krevelen relation (Heald et al, 2010 Ciarelli et al (2017). b Molecular structure as in Koo et al (2014) and Ciarelli et al (2016). pogenic sources as already proposed by more recent studies for the range of saturation concentrations used here (Donahue et al, 2013). No heterogeneous oxidation of organic particles or oligomerization processes are included in the model.…”

Section: Organic Aerosol Schemementioning

confidence: 99%

“…The third set allocates oxidation products from the traditional VOCs and biogenic precursors (xylene, toluene, isoprene, monoterpenes and sesquiterpenes) and from non-traditional SOA precursors retrieved from chamber data (∼ 4.75 times the amount of organic material in the semivolatile range; Ciarelli et al, 2017). Primary and secondary semivolatile compounds react with OH in the gas phase with a rate constant of 4 × 10 −11 cm 3 molec −1 s −1 (Donahue et al, 2013), which decreases their saturation concentration by 1 order of magnitude. This implies that aging of biogenic products is also implicitly taken into account.…”

Section: Organic Aerosol Schemementioning

confidence: 99%

Modelling winter organic aerosol at the European scale with CAMx: evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments

et al. 2017

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Abstract. We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from −61 to −29 %.We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88 % (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64 % of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain.Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40 % to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges werePublished by Copernicus Publications on behalf of the European Geosciences Union. 7654 G. Ciarelli et al.: Modelling winter organic aerosol at the European scale with CAMx also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38 % with no specific gradient among the stations.Although the new parameterization leads to a better agreement between model results and observations, it still underpredicts the SOA fraction, suggesting that uncertainties in the new scheme ...

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Why do organic aerosols exist? Understanding aerosol lifetimes using the two-dimensional volatility basis set

Cited by 112 publications

References 52 publications

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Organic Emissions from a Wood Stove and a Pellet Stove Before and After Simulated Atmospheric Aging

Particulate matter, air quality and climate: lessons learned and future needs

Modelling winter organic aerosol at the European scale with CAMx: evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments

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