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Wang, Mingyi ; Kong, Weimeng ; Marten, Ruby ; He, Xu-Cheng ; Chen, Dexian ; Pfeifer, Joschka ; Heitto, Arto ; Kontkanen, Jenni ; Dada, Lubna ; Kürten, Christoph Andreas ; Yli-Juuti, Taina ; Manninen, Hanna Elina ; Amanatidis, Stavros ; Amorim, Antonio ; Baalbaki, Rima ; Baccarini, Andrea ; Bell, David M. ; Bertozzi, Barbara ; Bräkling, Steffen ; Brilke, Sophia ; Murillo, Lucía Caudillo ; Chiu, Randall ; Chu, Biwu ; De Menezes, Louis-Philippe ; Duplissy, Jonathan ; Finkenzeller, Henning ; Gonzalez Carracedo, Loic ; Granzin, Manuel ; Guida, Roberto ; Hansel, Armin ; Hofbauer, Victoria ; Krechmer, Jordan ; Lehtipalo, Katrianne ; Lamkaddam, Houssni ; Lampimäki, Marku ; Lee, Chuan Ping ; Makhmutov, Vladimir ; Marie, Guillaume ; Mathot, Serge ; Mauldin, Roy Lee ; Mentler, Bernhard ; Müller, Tatjana ; Onnela, Antti ; Partoll, Eva ; Petäjä, Tuukka ; Philippov, Maxim ; Pospisilova, Veronika ; Ranjithkumar, Ananth ; Rissanen, Matti P. ; Rörup, Birte ; Scholz, Wiebke ; Shen, Jiali ; Simon, Mario ; Sipilä, Mikko ; Steiner, Gerhard ; Stolzenburg, Dominik ; Tham, Yee Jun ; Tomé, António ; Wagner, Andrea Christine ; Wang, Dongyu S. ; Wang, Yonghong ; Weber, Stefan K. ; Winkler, Paul M. ; Wlasits, Peter J. ; Wu, Yusheng ; Xiao, Mao ; Ye, Qing ; Zauner-Wieczorek, Marcel ; Zhou, Xueqin ; Volkamer, Rainer ; Riipinen, Ilona ; Dommen, Josef ; Curtius, Joachim ; Baltensperger, Urs ; Kulmala, Markku ; Worsnop, Douglas R. ; Kirkby, Jasper ; Seinfeld, John H. ; El Haddad, Imad ; Flagan, Richard C. ; Donahue, Neil McPherson
A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog, but how it occurs in cities is often puzzling. If the growth rates of urban particles are similar to those found in cleaner environments (1–10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below −15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid–base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms.
Chan, Arthur Wing Hong ; Kautzman, Kathryn E. ; Chhabra, Puneet Singh ; Surratt, Jason D. ; Chan, Man N. ; Crounse, John D. ; Kürten, Christoph Andreas ; Wennberg, Paul O. ; Flagan, Richard C. ; Seinfeld, John H.
Current atmospheric models do not include secondary organic aerosol (SOA) production from gas-phase reactions of polycyclic aromatic hydrocarbons (PAHs). Recent studies have shown that primary semivolatile emissions, previously assumed to be inert, undergo oxidation in the gas phase, leading to SOA formation. This opens the possibility that low-volatility gas-phase precursors are a potentially large source of SOA. In this work, SOA formation from gas-phase photooxidation of naphthalene, 1-methylnaphthalene (1-MN), 2-methylnaphthalene (2-MN), and 1,2-dimethylnaphthalene (1,2-DMN) is studied in the Caltech dual 28-m3 chambers. Under high-NOx conditions and aerosol mass loadings between 10 and 40 microg m-3, the SOA yields (mass of SOA per mass of hydrocarbon reacted) ranged from 0.19 to 0.30 for naphthalene, 0.19 to 0.39 for 1-MN, 0.26 to 0.45 for 2-MN, and constant at 0.31 for 1,2-DMN. Under low-NOx conditions, the SOA yields were measured to be 0.73, 0.68, and 0.58, for naphthalene, 1-MN, and 2-MN, respectively. The SOA was observed to be semivolatile under high-NOx conditions and essentially nonvolatile under low-NOx conditions, owing to the higher fraction of ring-retaining products formed under low-NOx conditions. When applying these measured yields to estimate SOA formation from primary emissions of diesel engines and wood burning, PAHs are estimated to yield 3–5 times more SOA than light aromatic compounds. PAHs can also account for up to 54% of the total SOA from oxidation of diesel emissions, representing a potentially large source of urban SOA.
Lawler, Michael Joseph ; Winkler, Paul M. ; Kim, Jaeseok ; Ahlm, Lars ; Tröstl, Jasmin ; Praplan, Arnaud Patrick ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Kirkby, Jasper ; Bianchi, Federico ; Duplissy, Jonathan ; Hansel, Armin ; Jokinen, Tuija ; Keskinen, Helmi ; Lehtipalo, Katrianne ; Leiminger, Markus ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Simon, Mario ; Sipilä, Mikko ; Williamson, Christina ; Wimmer, Daniela ; Riipinen, Ilona ; Virtanen, Annele ; Smith, James N.
New particle formation driven by acid–base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10–30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid–base pairs in particles as small as 10 nm.
Lawler, Michael Joseph ; Winkler, Paul M. ; Kim, Jaeseok ; Ahlm, Lars ; Tröstl, Jasmin ; Praplan, Arnaud Patrick ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Kirkby, Jasper ; Bianchi, Federico ; Duplissy, Jonathan ; Hansel, Armin ; Jokinen, Tuija ; Keskinen, Helmi ; Lehtipalo, Katrianne ; Lehtipalo, Katrianne ; Leiminger, Markus ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Simon, Mario ; Sipilä, Mikko ; Williamson, Christina ; Wimmer, Daniela ; Riipinen, Ilona ; Virtanen, Annele ; Smith, James N.
New particle formation driven by acid-base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10-30 nm VMD particles. This behavior is not consistent with present nanoparticle physico-chemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base:acid ratios lower than 1:1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient that suggests a change to a mixed-phase state as the particles grew beyond this size. The reasons for the very acidic composition remain uncertain, but a possible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid-base pairs in particles as small as 10 nm.
Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments
(2015)
Kim, Jaeseok ; Ahlm, Lars ; Yli-Juuti, Taina ; Lawler, Michael Joseph ; Keskinen, Helmi ; Tröstl, Jasmin ; Schobesberger, Siegfried ; Duplissy, Jonathan ; Amorim, Antonio ; Bianchi, Federico ; Donahue, Neil McPherson ; Flagan, Richard C. ; Hakala, Jani ; Heinritzi, Martin ; Jokinen, Tuija ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Miettinen, Pasi ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Sengupta, Kamalika ; Simon, Mario ; Tomé, Antonio ; Williamson, Christina ; Wimmer, Daniela ; Winkler, Paul M. ; Ehrhart, Sebastian ; Ye, Penglin ; Kirkby, Jasper ; Curtius, Joachim ; Kulmala, Markku ; Lehtinen, Kari E. J. ; Smith, James N. ; Riipinen, Ilona ; Virtanen, Annele
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e. particles that have grown to diameters of 10 and 15nm following nucleation, and measure their water uptake. Water uptake constrains their chemical composition. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90% relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) experiments performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter Κ decreased with increasing particle size indicating decreasing acidity of particles. No clear effect of the sulfuric acid monomer concentrations on the hygroscopicities of 10nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15nm particles sharply decreased with decreasing sulfuric acid monomer concentrations. In 20 particular, when the concentrations of sulfuric acid was 5.1 x 106 molecules cm exp -3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured Κ of 15nm particles was 0.3 ± 0.01 close to the value reported for dimethylamine sulfate (DMAS) (Κ DMAS ~ 0.28). Furthermore, the difference in Κ between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The Κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth already at 10nm sizes.
Hygroscopicity of nanoparticles produced from homogeneous
nucleation in the CLOUD experiments
(2016)
Kim, Jaeseok ; Ahlm, Lars ; Yli-Juuti, Taina ; Lawler, Michael Joseph ; Keskinen, Helmi ; Tröstl, Jasmin ; Schobesberger, Siegfried ; Duplissy, Jonathan ; Amorim, Antonio ; Bianchi, Federico ; Donahue, Neil McPherson ; Flagan, Richard C. ; Hakala, Jani ; Heinritzi, Martin ; Jokinen, Tuija ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Miettinen, Pasi ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Sengupta, Kamalika ; Simon, Mario ; Tomé, Antonio ; Williamson, Christina ; Wimmer, Daniela ; Winkler, Paul M. ; Ehrhart, Sebastian ; Ye, Penglin ; Kirkby, Jasper ; Curtius, Joachim ; Baltensperger, Urs ; Kulmala, Markku ; Lehtinen, Kari E. J. ; Smith, James N. ; Riipinen, Ilona ; Virtanen, Annele
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid–dimethylamine, and sulfuric acid–organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106 molecules cm−3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (κDMAS ∼ 0.28). Furthermore, the difference in κ between sulfuric acid and sulfuric acid–imethylamine experiments increased with increasing particle size. The κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10 nm sizes.
Hecobian, Arsineh ; Liu, Zhen ; Hennigan, Christopher J. ; Huey, L. Gregory ; Jimenez, Jose Luis ; Cubison, Michael J. ; Vay, Stephanie ; Diskin, Glenn S. ; Sachse, Glen W. ; Wisthaler, Armin ; Mikoviny, Tomas ; Weinheimer, Andrew J. ; Liao, Jin ; Knapp, David J. ; Wennberg, Paul O. ; Kürten, Christoph Andreas ; Crounse, John D. ; St. Clair, Jason M. ; Wang, Yuxuan ; Weber, Rodney J.
This paper compares measurements of gaseous and particulate emissions from a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS-2008 experiment: ARCTAS-A, based out of Fairbanks, Alaska USA (3 April to 19 April 2008); ARCTAS-B based out of Cold Lake, Alberta, Canada (29 June to 13 July 2008); and ARCTAS-CARB, based out of Palmdale, California, USA (18 June to 24 June 2008). Extensive investigations of boreal fire plume evolution were undertaken during ARCTAS-B, where four distinct fire plumes that were intercepted by the aircraft over a range of down-wind distances (0.1 to 16 hr transport times) were studied in detail. Based on these analyses, there was no evidence for ozone production and a box model simulation of the data confirmed that net ozone production was slow (on average 1 ppbv h−1 in the first 3 h and much lower afterwards) due to limited NOx. Peroxyacetyl nitrate concentrations (PAN) increased with plume age and the box model estimated an average production rate of ~80 pptv h−1 in the first 3 h. Like ozone, there was also no evidence for net secondary inorganic or organic aerosol formation. There was no apparent increase in aerosol mass concentrations in the boreal fire plumes due to secondary organic aerosol (SOA) formation; however, there were indications of chemical processing of the organic aerosols. In addition to the detailed studies of boreal fire plume evolution, about 500 smoke plumes intercepted by the NASA DC-8 aircraft were segregated by fire source region. The normalized excess mixing ratios (i.e. ΔX/ΔCO) of gaseous (carbon dioxide, acetonitrile, hydrogen cyanide, toluene, benzene, methane, oxides of nitrogen (NOx), ozone, PAN) and fine aerosol particulate components (nitrate, sulfate, ammonium, chloride, organic aerosols and water soluble organic carbon) of these plumes were compared.
Hecobian, Arsineh ; Liu, Zhen ; Hennigan, Christopher J. ; Huey, L. Gregory ; Jimenez, Jose Luis ; Cubison, Michael J. ; Vay, Stephanie ; Diskin, Glenn S. ; Sachse, Glen W. ; Wisthaler, Armin ; Mikoviny, Tomas ; Weinheimer, Andrew J. ; Liao, Jin ; Knapp, David J. ; Wennberg, Paul O. ; Kürten, Christoph Andreas ; Crounse, John D. ; St. Clair, Jason M. ; Wang, Yuxuan ; Weber, Rodney J.
This paper compares measurements of gaseous and particulate emissions from a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS-2008 experiment: ARCTAS-A, based out of Fairbanks, Alaska, USA (3 April to 19 April 2008); ARCTAS-B based out of Cold Lake, Alberta, Canada (29 June to 13 July 2008); and ARCTAS-CARB, based out of Palmdale, California, USA (18 June to 24 June 2008). Approximately 500 smoke plumes from biomass burning emissions that varied in age from minutes to days were segregated by fire source region and urban emission influences. The normalized excess mixing ratios (NEMR) of gaseous (carbon dioxide, acetonitrile, hydrogen cyanide, toluene, benzene, methane, oxides of nitrogen and ozone) and fine aerosol particulate components (nitrate, sulfate, ammonium, chloride, organic aerosols and water soluble organic carbon) of these plumes were compared. A detailed statistical analysis of the different plume categories for different gaseous and aerosol species is presented in this paper.
The comparison of NEMR values showed that CH4 concentrations were higher in air-masses that were influenced by urban emissions. Fresh biomass burning plumes mixed with urban emissions showed a higher degree of oxidative processing in comparison with fresh biomass burning only plumes. This was evident in higher concentrations of inorganic aerosol components such as sulfate, nitrate and ammonium, but not reflected in the organic components. Lower NOx NEMRs combined with high sulfate, nitrate and ammonium NEMRs in aerosols of plumes subject to long-range transport, when comparing all plume categories, provided evidence of advanced processing of these plumes.
Almeida, Joao ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Ortega, Ismael K. ; Kupiainen-Määttä, Oona ; Praplan, Arnaud Patrick ; Adamov, Alexey ; Amorim, Antonio ; Bianchi, Federico ; Breitenlechner, Martin ; David, André ; Dommen, Josef ; Donahue, Neil McPherson ; Downard, Andrew ; Dunne, Eimear M. ; Duplissy, Jonathan ; Ehrhart, Sebastian ; Flagan, Richard C. ; Franchin, Alessandro ; Guida, Roberto ; Hakala, Jani ; Hansel, Armin ; Heinritzi, Martin ; Henschel, Henning ; Jokinen, Tuija ; Junninen, Heikki ; Kajos, Maija ; Kangasluoma, Juha ; Keskinen, Helmi ; Kupc, Agnieszka ; Kurtén, Theo ; Kvashin, Alexander N. ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Leiminger, Markus ; Leppä, Johannes ; Loukonen, Ville ; Makhmutov, Vladimir ; Mathot, Serge ; McGrath, Matthew J. ; Nieminen, Tuomo ; Olenius, Tinja ; Onnela, Antti ; Petäjä, Tuukka ; Riccobono, Francesco ; Riipinen, Ilona ; Rissanen, Matti P. ; Rondo, Linda ; Ruuskanen, Taina ; Santos, Filipe Duarte ; Sarnela, Nina ; Schallhart, Simon ; Schnitzhofer, Ralf ; Seinfeld, John H. ; Simon, Mario ; Sipilä, Mikko ; Stozhkov, Yuri ; Stratmann, Frank ; Tomé, Antonio ; Tröstl, Jasmin ; Tsagkogeorgas, Georgios ; Vaattovaara, Petri ; Viisanen, Yrjo ; Virtanen, Annele ; Vrtala, Aron ; Wagner, Paul E. ; Weingartner, Ernest ; Wex, Heike ; Williamson, Christina ; Wimmer, Daniela ; Ye, Penglin ; Yli-Juuti, Taina ; Carslaw, Kenneth S. ; Kulmala, Markku ; Curtius, Joachim ; Baltensperger, Urs ; Worsnop, Douglas R. ; Vehkamäki, Hanna ; Kirkby, Jasper
Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei. Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes. Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases. However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere. It is thought that amines may enhance nucleation, but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid–amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid–dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
Chan, Arthur Wing Hong ; Kautzman, Kathryn E. ; Chhabra, Puneet Singh ; Surratt, Jason D. ; Chan, Man N. ; Crounse, John D. ; Kürten, Christoph Andreas ; Wennberg, Paul O. ; Flagan, Richard C. ; Seinfeld, John H.
Current atmospheric models do not include secondary organic aerosol (SOA) production from gas-phase reactions of polycyclic aromatic hydrocarbons (PAHs). Recent studies have shown that primary semivolatile emissions, previously assumed to be inert, undergo oxidation in the gas phase, leading to SOA formation. This opens the possibility that low-volatility gas-phase precursors are a potentially large source of SOA. In this work, SOA formation from gas-phase photooxidation of naphthalene, 1-methylnaphthalene (1-MN), 2-methylnaphthalene (2-MN), and 1,2-dimethylnaphthalene (1,2-DMN) is studied in the Caltech dual 28-m3 chambers. Under high-NOx conditions and aerosol mass loadings between 10 and 40 μg m, the SOA yields (mass of SOA per mass of hydrocarbon reacted) ranged from 0.19 to 0.30 for naphthalene, 0.19 to 0.39 for 1-MN, 0.26 to 0.45 for 2-MN, and constant at 0.31 for 1,2-DMN. Under low-NOx conditions, the SOA yields were measured to be 0.73, 0.68, and 0.58, for naphthalene, 1-MN, and 2-MN, respectively. The SOA was observed to be semivolatile under high-NOx conditions and essentially nonvolatile under low-NOx conditions, owing to the higher fraction of ring-retaining products formed under low-NOx conditions. When applying these measured yields to estimate SOA formation from primary emissions of diesel engines and wood burning, PAHs are estimated to yield 3–5 times more SOA than light aromatic compounds. PAHs can also account for up to 54% of the total SOA from oxidation of diesel emissions, representing a potentially large source of urban SOA.