Articles | Volume 18, issue 3
Atmos. Chem. Phys., 18, 1643–1652, 2018
https://doi.org/10.5194/acp-18-1643-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 18, 1643–1652, 2018
https://doi.org/10.5194/acp-18-1643-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article 06 Feb 2018
Research article | 06 Feb 2018
Effect of relative humidity on the composition of secondary organic aerosol from the oxidation of toluene
Mallory L. Hinks et al.
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Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503, https://doi.org/10.5194/acp-19-1491-2019, https://doi.org/10.5194/acp-19-1491-2019, 2019
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We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Shupeng Zhu, Jeremy R. Horne, Julia Montoya-Aguilera, Mallory L. Hinks, Sergey A. Nizkorodov, and Donald Dabdub
Atmos. Chem. Phys., 18, 3641–3657, https://doi.org/10.5194/acp-18-3641-2018, https://doi.org/10.5194/acp-18-3641-2018, 2018
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For the first time, the interaction between ammonia and secondary organic aerosol (SOA) is integrated in an air quality model and investigated on a national scale. Our original analysis from simulation results indicates that a significant reduction in gas-phase ammonia is possible due to its uptake onto SOA. Significant impact is also observed in the concentration of particulate matter, with a distinct spatial pattern over different seasons.
Julia Montoya-Aguilera, Jeremy R. Horne, Mallory L. Hinks, Lauren T. Fleming, Véronique Perraud, Peng Lin, Alexander Laskin, Julia Laskin, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 17, 11605–11621, https://doi.org/10.5194/acp-17-11605-2017, https://doi.org/10.5194/acp-17-11605-2017, 2017
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Various plant species emit a chemical compound called indole under stressed conditions or during flowering events. Our experiments show that indole can be oxidized in the atmosphere to produce a brownish haze containing well-known indole-derived dyes, such as indigo dye. An airshed model that includes indole chemistry shows that indole aerosol makes a significant contribution to the total aerosol burden and to visibility.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys., 21, 6175–6198, https://doi.org/10.5194/acp-21-6175-2021, https://doi.org/10.5194/acp-21-6175-2021, 2021
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This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show that the equilibration timescale depends on PAH molecular structure, temperature, and particle number concentration. We explore scenarios in which the particulate fraction is perturbed from equilibrium by chemical loss and discuss implications for chemical transport models that assume instantaneous equilibration at each model time step.
Yang Wang, Guangjie Zheng, Michael Jensen, Daniel Knopf, Alexander Laskin, Alyssa Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur Sedlacek, John Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria Zawadowicz, and Jian Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-300, https://doi.org/10.5194/acp-2021-300, 2021
Preprint under review for ACP
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This manuscript reports the vertical profiles of trace gas and aerosol properties over the Eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-17, https://doi.org/10.5194/acp-2021-17, 2021
Revised manuscript under review for ACP
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We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase of viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, https://doi.org/10.5194/acp-21-1565-2021, 2021
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Mass accommodation is a crucial process in secondary organic aerosol partitioning that depends on volatility, diffusivity, reactivity, and particle penetration depth of the chemical species involved. For efficient kinetic modeling, we introduce an effective mass accommodation coefficient that accounts for the above influencing factors, can be applied in the common Fuchs–Sutugin approximation, and helps to resolve inconsistencies and shortcomings of earlier experimental and model investigations.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
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Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
Yue Zhou, Christopher P. West, Anusha P. S. Hettiyadura, Xiaoying Niu, Hui Wen, Jiecan Cui, Tenglong Shi, Wei Pu, Xin Wang, and Alexander Laskin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1260, https://doi.org/10.5194/acp-2020-1260, 2021
Revised manuscript accepted for ACP
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We present a comprehensive characterization of water soluble organic carbon (WSOC) in seasonal snow of northwestern China. We applied complementary multi-modal analytical techniques to investigate bulk and molecular-level composition, optical properties, and sources of WSOC. For the first time, we estimated the extent of radiative forcing due to WSOC in snow using model simulation, and showed profound influences of WSOC on the energy budget of mid-latitude seasonal snowpack.
Ana C. Morales, Thilina Jayarathne, Jonathan H. Slade, Alexander Laskin, and Paul B. Shepson
Atmos. Chem. Phys., 21, 129–145, https://doi.org/10.5194/acp-21-129-2021, https://doi.org/10.5194/acp-21-129-2021, 2021
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Organic nitrates formed from the oxidation of biogenic volatile organic compounds impact both ozone and particulate matter as they remove nitrogen oxides, but they represent important aerosol precursors. We conducted a series of reaction chamber experiments that quantified the total organic nitrate and secondary organic aerosol yield from the OH-radical-initiated oxidation of ocimene, and also measured their hydrolysis lifetimes in the aqueous phase, as a function of pH.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-973, https://doi.org/10.5194/acp-2020-973, 2020
Preprint under review for ACP
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction (RF) of •OH among detected radicals, but negatively correlated with the RF of C-centered radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Matthew Fraund, Daniel J. Bonanno, Swarup China, Don Q. Pham, Daniel Veghte, Johannes Weis, Gourihar Kulkarni, Ken Teske, Mary K. Gilles, Alexander Laskin, and Ryan C. Moffet
Atmos. Chem. Phys., 20, 11593–11606, https://doi.org/10.5194/acp-20-11593-2020, https://doi.org/10.5194/acp-20-11593-2020, 2020
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High viscosity organic particles (HVOPs) in the Southern Great Plains have been analyzed, and two particle types were found. Previously studied tar balls and the recently discovered airborne soil organic particles (ASOPs) are both shown to be brown carbon (BrC). These particle types can be identified in bulk by an absorption Ångström exponent approaching 2.6. HVOP types can be differentiated by comparing carbon absorption spectrum peak ratios between the carboxylic acid, alcohol, and sp2 peaks.
Ying Li, Douglas A. Day, Harald Stark, Jose L. Jimenez, and Manabu Shiraiwa
Atmos. Chem. Phys., 20, 8103–8122, https://doi.org/10.5194/acp-20-8103-2020, https://doi.org/10.5194/acp-20-8103-2020, 2020
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Viscosity is an important property of organic aerosols, but viscosity measurements of ambient organic aerosols are scarce. We developed a method to predict glass transition temperatures using volatility and the atomic oxygen-to-carbon ratio. The method was applied to field observations of volatility distributions to predict viscosity of ambient organic aerosols, yielding consistent results with ambient particle phase-state measurements and global simulations.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Lauren T. Fleming, Peng Lin, James M. Roberts, Vanessa Selimovic, Robert Yokelson, Julia Laskin, Alexander Laskin, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, https://doi.org/10.5194/acp-20-1105-2020, 2020
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We have explored the nature and stability of molecules that give biomass burning smoke its faint brown color. Different types of biomass fuels were burned and the resulting smoke was collected for a detailed chemical analysis. We found that brown molecules in smoke become less colored when they are irradiated by sunlight, but this photobleaching process is very slow. This means that biomass burning smoke will remain brown-colored for a long time and efficiently warm up the atmosphere.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Erin Evoy, Adrian M. Maclean, Grazia Rovelli, Ying Li, Alexandra P. Tsimpidi, Vlassis A. Karydis, Saeid Kamal, Jos Lelieveld, Manabu Shiraiwa, Jonathan P. Reid, and Allan K. Bertram
Atmos. Chem. Phys., 19, 10073–10085, https://doi.org/10.5194/acp-19-10073-2019, https://doi.org/10.5194/acp-19-10073-2019, 2019
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We measured the diffusion rates of organic molecules in a number of proxies for secondary organic aerosol (SOA) and compared measured diffusion with predictions from two relations: the Stokes–Einstein relation and a fractional Stokes–Einstein relation. The fractional relation does a better job of predicting diffusion rates in this case. Output from an atmospheric model shows that mixing times predicted using the two relations differ by up to 1 order of magnitude at an altitude of ~ 3 km.
Olli-Pekka Tikkanen, Väinö Hämäläinen, Grazia Rovelli, Antti Lipponen, Manabu Shiraiwa, Jonathan P. Reid, Kari E. J. Lehtinen, and Taina Yli-Juuti
Atmos. Chem. Phys., 19, 9333–9350, https://doi.org/10.5194/acp-19-9333-2019, https://doi.org/10.5194/acp-19-9333-2019, 2019
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We assessed how well the organic aerosol particle composition and viscosity can be captured by optimizing process models to match particle evaporation data. We performed the analysis for both artificial and real evaporation data and tested two optimization algorithms. Our findings show that the optimization method yields a good estimate for the studied properties. The timescale of the evaporation data and particle size was found to be important in identifying the volatility of organic compounds.
Brigitte Rooney, Ran Zhao, Yuan Wang, Kelvin H. Bates, Ajay Pillarisetti, Sumit Sharma, Seema Kundu, Tami C. Bond, Nicholas L. Lam, Bora Ozaltun, Li Xu, Varun Goel, Lauren T. Fleming, Robert Weltman, Simone Meinardi, Donald R. Blake, Sergey A. Nizkorodov, Rufus D. Edwards, Ankit Yadav, Narendra K. Arora, Kirk R. Smith, and John H. Seinfeld
Atmos. Chem. Phys., 19, 7719–7742, https://doi.org/10.5194/acp-19-7719-2019, https://doi.org/10.5194/acp-19-7719-2019, 2019
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Approximately 3 billion people worldwide cook with solid fuels, such as wood, charcoal, and agricultural residues, that are often combusted in inefficient cookstoves. Here, we simulate the distribution of the two major health-damaging outdoor pollution species (PM2.5 and O3) using state-of-the-science emissions databases and atmospheric chemical transport models to estimate the impact of household combustion on ambient air quality in India.
Ying Li and Manabu Shiraiwa
Atmos. Chem. Phys., 19, 5959–5971, https://doi.org/10.5194/acp-19-5959-2019, https://doi.org/10.5194/acp-19-5959-2019, 2019
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Timescales for secondary organic aerosols (SOA) to reach equilibrium were estimated under various temperatures and relative humidities. Equilibration timescales in free troposphere can be longer than hours or days, even at moderate or relatively high relative humidities. These results provide critical insights into thermodynamic or kinetic treatments of SOA partitioning for accurate predictions of gas- and particle-phase concentrations of semi-volatile compounds in chemical transport models.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503, https://doi.org/10.5194/acp-19-1491-2019, https://doi.org/10.5194/acp-19-1491-2019, 2019
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We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Zhijian Li, Sergey A. Nizkorodov, Hong Chen, Xiaohui Lu, Xin Yang, and Jianmin Chen
Atmos. Chem. Phys., 19, 1343–1356, https://doi.org/10.5194/acp-19-1343-2019, https://doi.org/10.5194/acp-19-1343-2019, 2019
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In this work, we found that acrolein, the smallest α,β-unsaturated aldehyde, has the potential to form light-absorbing heterocyclic secondary organic aerosol. In the gaseous phase, acrolein can react with gaseous ammonia, forming 3-picoline. In the liquid phase, the dissolved acrolein can react with ammonium to form higher molecular-weight pyridinium compounds. All the pyridinium compounds can increase the light absorptivity of aerosol particles.
Victoria E. Irish, Sarah J. Hanna, Megan D. Willis, Swarup China, Jennie L. Thomas, Jeremy J. B. Wentzell, Ana Cirisan, Meng Si, W. Richard Leaitch, Jennifer G. Murphy, Jonathan P. D. Abbatt, Alexander Laskin, Eric Girard, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1027–1039, https://doi.org/10.5194/acp-19-1027-2019, https://doi.org/10.5194/acp-19-1027-2019, 2019
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Ice nucleating particles (INPs) are atmospheric particles that catalyse the formation of ice crystals in clouds. INPs influence the Earth's radiative balance and hydrological cycle. In this study we measured the concentrations of INPs in the Canadian Arctic marine boundary layer. Average INP concentrations fell within the range measured in other marine boundary layer locations. We also found that mineral dust is a more important contributor to the INP population than sea spray aerosol.
Chunlin Li, Quanfu He, Julian Schade, Johannes Passig, Ralf Zimmermann, Daphne Meidan, Alexander Laskin, and Yinon Rudich
Atmos. Chem. Phys., 19, 139–163, https://doi.org/10.5194/acp-19-139-2019, https://doi.org/10.5194/acp-19-139-2019, 2019
Lauren T. Fleming, Robert Weltman, Ankit Yadav, Rufus D. Edwards, Narendra K. Arora, Ajay Pillarisetti, Simone Meinardi, Kirk R. Smith, Donald R. Blake, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 15169–15182, https://doi.org/10.5194/acp-18-15169-2018, https://doi.org/10.5194/acp-18-15169-2018, 2018
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Brushwood- and dung-burning cookstoves are used for cooking and heating and influence ambient air quality for millions of people. We report emission factors from the more efficient cookstove, the chulha, compared to the smoldering angithi, for carbon dioxide, carbon monoxide, and 76 volatile organic compounds. This comprehensive gas emission inventory should inform policy makers about the magnitude of the effect of cookstoves on the air quality in India.
Amy L. Bondy, Daniel Bonanno, Ryan C. Moffet, Bingbing Wang, Alexander Laskin, and Andrew P. Ault
Atmos. Chem. Phys., 18, 12595–12612, https://doi.org/10.5194/acp-18-12595-2018, https://doi.org/10.5194/acp-18-12595-2018, 2018
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To determine important sources of aerosols during the Southern Oxidant and Aerosol Study (SOAS), as well as their mixing with secondary species, individual particles were analyzed with electron and X-ray microscopy to determine size and chemical composition. Secondary organic aerosol, sea spray aerosol, and mineral dust each dominated during different periods. Particles were less similar chemically to each other than is commonly assumed, which is important for air quality and climate models.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
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The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Rachel M. Kirpes, Amy L. Bondy, Daniel Bonanno, Ryan C. Moffet, Bingbing Wang, Alexander Laskin, Andrew P. Ault, and Kerri A. Pratt
Atmos. Chem. Phys., 18, 3937–3949, https://doi.org/10.5194/acp-18-3937-2018, https://doi.org/10.5194/acp-18-3937-2018, 2018
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Arctic atmospheric particles have important climate impacts via cloud formation and precipitation, particularly in the wintertime. We show that sulfate, formed during atmospheric transport, is within individual sea spray particles and organic particles measured in the Alaskan Arctic. Greater contributions of combustion emissions were observed when the wind direction came from the Prudhoe Bay oil fields, showing its regional influence.
Shupeng Zhu, Jeremy R. Horne, Julia Montoya-Aguilera, Mallory L. Hinks, Sergey A. Nizkorodov, and Donald Dabdub
Atmos. Chem. Phys., 18, 3641–3657, https://doi.org/10.5194/acp-18-3641-2018, https://doi.org/10.5194/acp-18-3641-2018, 2018
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For the first time, the interaction between ammonia and secondary organic aerosol (SOA) is integrated in an air quality model and investigated on a national scale. Our original analysis from simulation results indicates that a significant reduction in gas-phase ammonia is possible due to its uptake onto SOA. Significant impact is also observed in the concentration of particulate matter, with a distinct spatial pattern over different seasons.
Lauren T. Fleming, Peng Lin, Alexander Laskin, Julia Laskin, Robert Weltman, Rufus D. Edwards, Narendra K. Arora, Ankit Yadav, Simone Meinardi, Donald R. Blake, Ajay Pillarisetti, Kirk R. Smith, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 2461–2480, https://doi.org/10.5194/acp-18-2461-2018, https://doi.org/10.5194/acp-18-2461-2018, 2018
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Household cooking emissions in India, which rely on traditional meal preparation with dung- and brushwood-fueled cookstoves, produce copious amounts of particulate matter. Detailed chemical analysis of the compounds found in this particulate matter detected a large number of previously unidentified nitrogen-containing organic compounds, originating from dung-fueled cookstoves.
Ryan D. Cook, Ying-Hsuan Lin, Zhuoyu Peng, Eric Boone, Rosalie K. Chu, James E. Dukett, Matthew J. Gunsch, Wuliang Zhang, Nikola Tolic, Alexander Laskin, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 15167–15180, https://doi.org/10.5194/acp-17-15167-2017, https://doi.org/10.5194/acp-17-15167-2017, 2017
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Reactions occur within water in both atmospheric particles and cloud droplets, yet little is known about the organic compounds in cloud water. In this work, cloud water samples were collected at Whiteface Mountain, New York, and analyzed using ultra-high-resolution mass spectrometry to investigate the molecular composition of the dissolved organic compounds. The results focus on changes in cloud water composition with air mass origin – influences of forest, urban, and wildfire emissions.
Man Mei Chim, Chiu Tung Cheng, James F. Davies, Thomas Berkemeier, Manabu Shiraiwa, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 17, 14415–14431, https://doi.org/10.5194/acp-17-14415-2017, https://doi.org/10.5194/acp-17-14415-2017, 2017
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In this work, we report that methyl-substituted succinic acid present at or near the surface of aqueous organic droplets can be efficiently oxidized by gas-phase OH radicals. The alkoxy radical chemistry appears to be an important reaction pathway. In addition, our model simulations reveal the relative importance of functionalization and fragmentation processes, alongside volatilization, in the evolution of the particle-phase reaction, which is largely dependent on the extent of oxidation.
Qing Mu, Gerhard Lammel, Christian N. Gencarelli, Ian M. Hedgecock, Ying Chen, Petra Přibylová, Monique Teich, Yuxuan Zhang, Guangjie Zheng, Dominik van Pinxteren, Qiang Zhang, Hartmut Herrmann, Manabu Shiraiwa, Peter Spichtinger, Hang Su, Ulrich Pöschl, and Yafang Cheng
Atmos. Chem. Phys., 17, 12253–12267, https://doi.org/10.5194/acp-17-12253-2017, https://doi.org/10.5194/acp-17-12253-2017, 2017
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Polycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants with the largest emissions in East Asia. The regional WRF-Chem-PAH model has been developed to reflect the state-of-the-art understanding of current PAHs studies with several new or updated features. It is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions.
Julia Montoya-Aguilera, Jeremy R. Horne, Mallory L. Hinks, Lauren T. Fleming, Véronique Perraud, Peng Lin, Alexander Laskin, Julia Laskin, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 17, 11605–11621, https://doi.org/10.5194/acp-17-11605-2017, https://doi.org/10.5194/acp-17-11605-2017, 2017
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Various plant species emit a chemical compound called indole under stressed conditions or during flowering events. Our experiments show that indole can be oxidized in the atmosphere to produce a brownish haze containing well-known indole-derived dyes, such as indigo dye. An airshed model that includes indole chemistry shows that indole aerosol makes a significant contribution to the total aerosol burden and to visibility.
Yevgeny Derimian, Marie Choël, Yinon Rudich, Karine Deboudt, Oleg Dubovik, Alexander Laskin, Michel Legrand, Bahaiddin Damiri, Ilan Koren, Florin Unga, Myriam Moreau, Meinrat O. Andreae, and Arnon Karnieli
Atmos. Chem. Phys., 17, 11331–11353, https://doi.org/10.5194/acp-17-11331-2017, https://doi.org/10.5194/acp-17-11331-2017, 2017
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We present influence of daily occurrence of the sea breeze flow from the Mediterranean Sea on physicochemical and optical properties of atmospheric aerosol deep inland in the Negev Desert of Israel. Sampled airborne dust was found be internally mixed with sea-salt particles and reacted with anthropogenic pollution, which makes the dust highly hygroscopic and a liquid coating of particles appears. These physicochemical transformations are associated with a change in aerosol radiative properties.
Matthew J. Gunsch, Rachel M. Kirpes, Katheryn R. Kolesar, Tate E. Barrett, Swarup China, Rebecca J. Sheesley, Alexander Laskin, Alfred Wiedensohler, Thomas Tuch, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 10879–10892, https://doi.org/10.5194/acp-17-10879-2017, https://doi.org/10.5194/acp-17-10879-2017, 2017
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Arctic sea ice loss is leading to increasing petroleum extraction and shipping. It is necessary to identify emissions from these activities for improved Arctic air quality and climate assessment. Atmospheric particles were measured from August to September 2015 in Utqiaġvik, AK. For periods influenced by Prudhoe Bay, significant influence associated with combustion emissions was observed, compared to fresh sea spray influence during Arctic Ocean periods.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Wei Nie, Juan Hong, Silja A. K. Häme, Aijun Ding, Yugen Li, Chao Yan, Liqing Hao, Jyri Mikkilä, Longfei Zheng, Yuning Xie, Caijun Zhu, Zheng Xu, Xuguang Chi, Xin Huang, Yang Zhou, Peng Lin, Annele Virtanen, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, Jianzhen Yu, Veli-Matti Kerminen, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 3659–3672, https://doi.org/10.5194/acp-17-3659-2017, https://doi.org/10.5194/acp-17-3659-2017, 2017
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HULIS are demonstrated to be important low-volatility, or even extremely low volatility, compounds in the organic aerosol phase. This sheds new light on the connection between atmospheric HULIS and ELVOCs. The interaction between HULIS and ammonium sulfate was found to decrease the volatility of the HULIS part in HULIS-AS mixed samples, indicating multiphase processes have the potential to lower the volatility of organic compounds in the aerosol phase.
Alba Badia, Oriol Jorba, Apostolos Voulgarakis, Donald Dabdub, Carlos Pérez García-Pando, Andreas Hilboll, María Gonçalves, and Zavisa Janjic
Geosci. Model Dev., 10, 609–638, https://doi.org/10.5194/gmd-10-609-2017, https://doi.org/10.5194/gmd-10-609-2017, 2017
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This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMB-MONARCH), an online chemical weather prediction system conceived for both the regional and global scales. We provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations, ozonesondes, aircraft data and satellite observations.
Adam P. Bateman, Zhaoheng Gong, Tristan H. Harder, Suzane S. de Sá, Bingbing Wang, Paulo Castillo, Swarup China, Yingjun Liu, Rachel E. O'Brien, Brett B. Palm, Hung-Wei Shiu, Glauber G. Cirino, Ryan Thalman, Kouji Adachi, M. Lizabeth Alexander, Paulo Artaxo, Allan K. Bertram, Peter R. Buseck, Mary K. Gilles, Jose L. Jimenez, Alexander Laskin, Antonio O. Manzi, Arthur Sedlacek, Rodrigo A. F. Souza, Jian Wang, Rahul Zaveri, and Scot T. Martin
Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, https://doi.org/10.5194/acp-17-1759-2017, 2017
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The occurrence of nonliquid and liquid physical states of submicron atmospheric particulate matter (PM) downwind of an urban region in central Amazonia was investigated. Air masses representing background conditions, urban pollution, and regional- and continental-scale biomass were measured. Anthropogenic influences contributed to the presence of nonliquid PM in the atmospheric particle population, while liquid PM dominated during periods of biogenic influence.
Ryan C. Moffet, Rachel E. O'Brien, Peter A. Alpert, Stephen T. Kelly, Don Q. Pham, Mary K. Gilles, Daniel A. Knopf, and Alexander Laskin
Atmos. Chem. Phys., 16, 14515–14525, https://doi.org/10.5194/acp-16-14515-2016, https://doi.org/10.5194/acp-16-14515-2016, 2016
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Atmospheric black carbon (BC), commonly known as soot, is an important constituent of the earth that imparts a warming similar to that of carbon dioxide. However, BC is much shorter lived and has uncertain warming due to its mixture with other solid and liquid components. Here, advanced microscopic methods have provided a detailed look at thousands of BC particles sampled from central California; these measurements will lead towards a better understanding of the effects that BC has on climate.
Andrea M. Arangio, Haijie Tong, Joanna Socorro, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, https://doi.org/10.5194/acp-16-13105-2016, 2016
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We have quantified environmentally persistent free radicals and reactive oxygen species (ROS) in size-segregated atmospheric aerosol particles. We suggest that ROS were formed by decomposition of secondary organic aerosols interacting with transition metal ions and quinones contained in humic-like substances. The results have significant implications for aqueous-phase and cloud processing of organic aerosols as well as adverse health effects upon respiratory deposition of aerosol particles.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Jiumeng Liu, Peng Lin, Alexander Laskin, Julia Laskin, Shawn M. Kathmann, Matthew Wise, Ryan Caylor, Felisha Imholt, Vanessa Selimovic, and John E. Shilling
Atmos. Chem. Phys., 16, 12815–12827, https://doi.org/10.5194/acp-16-12815-2016, https://doi.org/10.5194/acp-16-12815-2016, 2016
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Light absorbing organic aerosols (BrC) absorb sunlight thereby influencing climate; however, understanding of the link between their optical properties and environmental variables remains limited. Our chamber experiment results suggest that variables including NOx concentration, RH level, and photolysis time have considerable influence on secondary BrC optical properties. The results contribute to a more accurate characterization of the impacts of aerosols on climate, especially in urban areas.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
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Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
Matthew L. Dawson, Jialu Xu, Robert J. Griffin, and Donald Dabdub
Geosci. Model Dev., 9, 2143–2151, https://doi.org/10.5194/gmd-9-2143-2016, https://doi.org/10.5194/gmd-9-2143-2016, 2016
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The atmospheric oxidation of aromatic compounds is an important source of aerosol-forming species, and thus contributes to pollution in urban areas. However, details of the mechanisms by which oxidation occurs are only recently being elucidated. Here we report the incorporation of a newly developed mechanism for aromatic oxidation into the UCI-CIT regional air quality model. Results suggest an unexpected role for chemical pathways typically associated with cleaner environments.
Xianda Gong, Ci Zhang, Hong Chen, Sergey A. Nizkorodov, Jianmin Chen, and Xin Yang
Atmos. Chem. Phys., 16, 5399–5411, https://doi.org/10.5194/acp-16-5399-2016, https://doi.org/10.5194/acp-16-5399-2016, 2016
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In this study, we used a Single Particle Aerosol Mass Spectrometer and a Single Particle Soot Photometer to investigate the chemical and physical properties of black carbon (BC) aerosols during a regional air pollution episode in urban Shanghai. BC containing particles were mainly attributed to biomass burning and traffic emissions. We observed a group of highly aged traffic emitted particles with a relatively small BC core (~ 60–80 nm) and a very thick absolute coating thickness (~ 130–300 nm).
Lu Yu, Jeremy Smith, Alexander Laskin, Katheryn M. George, Cort Anastasio, Julia Laskin, Ann M. Dillner, and Qi Zhang
Atmos. Chem. Phys., 16, 4511–4527, https://doi.org/10.5194/acp-16-4511-2016, https://doi.org/10.5194/acp-16-4511-2016, 2016
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The chemical evolution of SOA formed during aqueous reactions of phenolic compounds is studied via combined bulk and molecular analysis. Phenolic SOA evolve dynamically during photochemical aging, with different reaction mechanisms (oligomerization, fragmentation, and functionalization) leading to different generations of products that span an enormous range in volatilities and a large range in oxidation state and composition. Aqueous reactions of phenols are likely an important source of ELVOC.
Ying Li, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 3327–3344, https://doi.org/10.5194/acp-16-3327-2016, https://doi.org/10.5194/acp-16-3327-2016, 2016
Haijie Tong, Andrea M. Arangio, Pascale S. J. Lakey, Thomas Berkemeier, Fobang Liu, Christopher J. Kampf, William H. Brune, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, https://doi.org/10.5194/acp-16-1761-2016, 2016
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We provide experimental evidence that terpene and isoprene SOA form substantial amounts of OH radicals upon interaction with liquid water and iron. Our measurements and model results imply that the chemical reactivity of SOA in the atmosphere, particularly in clouds, can be faster than previously thought. Inhalation and deposition of SOA particles in the human respiratory tract may lead to a substantial release of OH radicals in vivo, causing oxidative stress and adverse aerosol health effects.
H. M. Allen, D. C. Draper, B. R. Ayres, A. Ault, A. Bondy, S. Takahama, R. L. Modini, K. Baumann, E. Edgerton, C. Knote, A. Laskin, B. Wang, and J. L. Fry
Atmos. Chem. Phys., 15, 10669–10685, https://doi.org/10.5194/acp-15-10669-2015, https://doi.org/10.5194/acp-15-10669-2015, 2015
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We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the SOAS 2013 field study. Our particular focus is on inorganic nitrate aerosol formation via HNO3 uptake onto coarse-mode dust and sea salt particles, which we find to be the dominant source of episodic inorganic nitrate at this site, due to the high acidity of the particles preventing formation of NH4NO3. We calculate a production rate of inorganic nitrate aerosol.
E. F. Mikhailov, G. N. Mironov, C. Pöhlker, X. Chi, M. L. Krüger, M. Shiraiwa, J.-D. Förster, U. Pöschl, S. S. Vlasenko, T. I. Ryshkevich, M. Weigand, A. L. D. Kilcoyne, and M. O. Andreae
Atmos. Chem. Phys., 15, 8847–8869, https://doi.org/10.5194/acp-15-8847-2015, https://doi.org/10.5194/acp-15-8847-2015, 2015
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Our manuscript describes the hygroscopic properties of accumulation- and coarse-mode aerosol particles sampled at the ZOTTO in central Siberia (61º N, 89º E). The hygroscopic growth measurements were supplemented with chemical analyses of the samples. In addition, the microstructure and chemical composition of aerosol particles were analyzed by x-ray micro-spectroscopy (STXM-NEXAFS) and transmission electron microscopy (TEM).
M. J. Tang, M. Shiraiwa, U. Pöschl, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 15, 5585–5598, https://doi.org/10.5194/acp-15-5585-2015, https://doi.org/10.5194/acp-15-5585-2015, 2015
B. Y. Kuang, P. Lin, X. H. H. Huang, and J. Z. Yu
Atmos. Chem. Phys., 15, 1995–2008, https://doi.org/10.5194/acp-15-1995-2015, https://doi.org/10.5194/acp-15-1995-2015, 2015
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Humic-like substances (HULIS), the hydrophobic part of water soluble organic material, account for ~10% of PM2.5 mass in the Pearl River Delta, China. Source analysis using PM2.5 chemical composition data revealed that secondary formation process, biomass burning, and residual oil combustion from shipping as significant sources of HULIS. Vehicle emissions contributed little to HULIS. Primary sources of HULIS appeared to be linked to inefficient combustion.
L. Yu, J. Smith, A. Laskin, C. Anastasio, J. Laskin, and Q. Zhang
Atmos. Chem. Phys., 14, 13801–13816, https://doi.org/10.5194/acp-14-13801-2014, https://doi.org/10.5194/acp-14-13801-2014, 2014
T. Berkemeier, M. Shiraiwa, U. Pöschl, and T. Koop
Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, https://doi.org/10.5194/acp-14-12513-2014, 2014
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Glassy organic particles can serve as ice nuclei at low temperatures. We provide a rationale for these findings using a numerical aerosol diffusion model that describes particle phase state and its kinetics during simulated atmospheric updrafts dependent upon composition, size, updraft velocity, temperature and humidity. Our simulations suggest that aerosols from anthropogenic aromatic organics can be particularly relevant for ice cloud formation.
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl
Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, https://doi.org/10.5194/acp-14-8323-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
S. A. Epstein, E. Tapavicza, F. Furche, and S. A. Nizkorodov
Atmos. Chem. Phys., 13, 9461–9477, https://doi.org/10.5194/acp-13-9461-2013, https://doi.org/10.5194/acp-13-9461-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Heterogeneous interactions between SO2 and organic peroxides in submicron aerosol
Temperature and acidity dependence of secondary organic aerosol formation from α-pinene ozonolysis with a compact chamber system
Production of HONO from NO2 uptake on illuminated TiO2 aerosol particles and following the illumination of mixed TiO2∕ammonium nitrate particles
Characterization of secondary organic aerosol from heated-cooking-oil emissions: evolution in composition and volatility
Measurement report: Diurnal and temporal variations of sugar compounds in suburban aerosols from the northern vicinity of Beijing, China – an influence of biogenic and anthropogenic sources
Pre-deliquescent water uptake in deposited nanoparticles observed with in situ ambient pressure X-ray photoelectron spectroscopy
Technical note: Emission factors, chemical composition, and morphology of particles emitted from Euro 5 diesel and gasoline light-duty vehicles during transient cycles
Measurement report: Distinct emissions and volatility distribution of intermediate-volatility organic compounds from on-road Chinese gasoline vehicles: implication of high secondary organic aerosol formation potential
Emissions of intermediate-volatility and semi-volatile organic compounds from domestic fuels used in Delhi, India
Effects of liquid–liquid phase separation and relative humidity on the heterogeneous OH oxidation of inorganic–organic aerosols: insights from methylglutaric acid and ammonium sulfate particles
Measurement report: Sulfuric acid nucleation and experimental conditions in a photolytic flow reactor
Ozonolysis of fatty acid monolayers at the air–water interface: organic films may persist at the surface of atmospheric aerosols
Formation kinetics and mechanism of ozone and secondary organic aerosols from photochemical oxidation of different aromatic hydrocarbons: dependence of NOx and organic substituent
SO2 and NH3 emissions enhance organosulfur compounds and fine particles formation from the photooxidation of a typical aromatic hydrocarbon
Quantification of the role of stabilized Criegee intermediates in the formation of aerosols in limonene ozonolysis
Photochemical degradation of iron(III) citrate/citric acid aerosol quantified with the combination of three complementary experimental techniques and a kinetic process model
The production and hydrolysis of organic nitrates from OH radical oxidation of β-ocimene
Emission factors for PM10 and polycyclic aromatic hydrocarbons (PAHs) from illegal burning of different types of municipal waste in households
Kinetic modeling of formation and evaporation of secondary organic aerosol from NO3 oxidation of pure and mixed monoterpenes
On the similarities and differences between the products of oxidation of hydrocarbons under simulated atmospheric conditions and cool-flames
Water uptake of subpollen aerosol particles: hygroscopic growth, CCN activation, and liquid-liquid phase separation
Direct contribution of ammonia to α-pinene secondary organic aerosol formation
Enhanced secondary organic aerosol formation from the photo-oxidation of mixed anthropogenic volatile organic compounds
Hygroscopic behavior of aerosols generated from solutions of 3-methyl-1,2,3-butanetricarboxylic acid, its sodium salts, and its mixtures with NaCl
Chemical composition, structures, and light absorption of N-containing aromatic compounds emitted from burning wood and charcoal in household cookstoves
Source Apportionment of Carbonaceous Aerosols in Beijing with Radiocarbon and Organic Tracers: Insight into the Differences between Urban and Rural Sites
Chemical composition and light absorption of carbonaceous aerosols emitted from crop residue burning: influence of combustion efficiency
On mineral dust aerosol hygroscopicity
Distinct chemical and mineralogical composition of Icelandic dust compared to northern African and Asian dust
Secondary organic aerosol yields from the oxidation of benzyl alcohol
The Aarhus Chamber Campaign on Highly Oxygenated Organic Molecules and Aerosols (ACCHA): particle formation, organic acids, and dimer esters from α-pinene ozonolysis at different temperatures
Molecular understanding of the suppression of new-particle formation by isoprene
Complex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?
Liquid–liquid phase separation and morphologies in organic particles consisting of α-pinene and β-caryophyllene ozonolysis products and mixtures with commercially available organic compounds
Characterization of primary and aged wood burning and coal combustion organic aerosols in environmental chamber and its implications for atmospheric aerosols
Oligomer and highly oxygenated organic molecule formation from oxidation of oxygenated monoterpenes emitted by California sage plants
Increased Primary and Secondary H2SO4 Showing the Opposing Roles in SOA Formation from Ethyl Methacrylate Ozonolysis
Laboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 2: Chemical properties and characterization
Impact of NOx on secondary organic aerosol (SOA) formation from α-pinene and β-pinene photooxidation: the role of highly oxygenated organic nitrates
Laboratory study of the collection efficiency of submicron aerosol particles by cloud droplets. Part II – Influence of electric charges
Evaluation of the chemical composition of gas- and particle-phase products of aromatic oxidation
Glyoxal's impact on dry ammonium salts: fast and reversible surface aerosol browning
Oxygenated products formed from OH-initiated reactions of trimethylbenzene: autoxidation and accretion
Biomass-burning-derived particles from a wide variety of fuels – Part 2: Effects of photochemical aging on particle optical and chemical properties
Measured solid state and subcooled liquid vapour pressures of nitroaromatics using Knudsen effusion mass spectrometry
Polar semivolatile organic compounds in biomass-burning emissions and their chemical transformations during aging in an oxidation flow reactor
Temperature effects on optical properties and chemical composition of secondary organic aerosol derived from n-dodecane
An investigation on hygroscopic properties of 15 black carbon (BC)-containing particles from different carbon sources: roles of organic and inorganic components
Deconvolution of FIGAERO–CIMS thermal desorption profiles using positive matrix factorisation to identify chemical and physical processes during particle evaporation
Mineralogy and geochemistry of Asian dust: dependence on migration path, fractionation, and reactions with polluted air
Shunyao Wang, Tengyu Liu, Jinmyung Jang, Jonathan P. D. Abbatt, and Arthur W. H. Chan
Atmos. Chem. Phys., 21, 6647–6661, https://doi.org/10.5194/acp-21-6647-2021, https://doi.org/10.5194/acp-21-6647-2021, 2021
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Discrepancies between atmospheric modeling and field observations, especially in highly polluted cities, have highlighted the lack of understanding of sulfate formation mechanisms and kinetics. Here, we directly quantify the reactive uptake coefficient of SO2 onto organic peroxides and study the important governing factors. The SO2 uptake rate was observed to depend on RH, peroxide amount and reactivity, pH, and ionic strength, which provides a framework to better predict sulfate formation.
Yange Deng, Satoshi Inomata, Kei Sato, Sathiyamurthi Ramasamy, Yu Morino, Shinichi Enami, and Hiroshi Tanimoto
Atmos. Chem. Phys., 21, 5983–6003, https://doi.org/10.5194/acp-21-5983-2021, https://doi.org/10.5194/acp-21-5983-2021, 2021
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The temperature and acidity dependence of yields and chemical compositions of the α-pinene ozonolysis SOA were systematically investigated using a newly developed compact chamber system. Increases in SOA yields were observed with the decrease in temperature and under acidic seed conditions. The differences in chemical compositions between acidic and neutral seed conditions were characterized and explained from the viewpoints of acid-catalyzed reactions. Some organosulfates were newly detected.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 5755–5775, https://doi.org/10.5194/acp-21-5755-2021, https://doi.org/10.5194/acp-21-5755-2021, 2021
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight on aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, a model consistent with the data is developed and aerosol production of HONO in the atmosphere is shown to be significant.
Manpreet Takhar, Yunchun Li, and Arthur W. H. Chan
Atmos. Chem. Phys., 21, 5137–5149, https://doi.org/10.5194/acp-21-5137-2021, https://doi.org/10.5194/acp-21-5137-2021, 2021
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Our study highlights the importance of molecular composition in constraining the chemical properties of cooking SOA as well as understanding the contribution of aldehydes in formation of SOA from cooking emissions. We show that fragmentation reactions are key in atmospheric processing of cooking SOA, and aldehydes emitted from cooking emissions contribute substantially to SOA formation. Our study provides a framework to better predict SOA formation in and downwind of urban atmospheres.
Santosh Kumar Verma, Kimitaka Kawamura, Fei Yang, Pingqing Fu, Yugo Kanaya, and Zifa Wang
Atmos. Chem. Phys., 21, 4959–4978, https://doi.org/10.5194/acp-21-4959-2021, https://doi.org/10.5194/acp-21-4959-2021, 2021
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We studied aerosol samples collected in autumn 2007 with day and night intervals in a rural site of Mangshan, north of Beijing, for sugar compounds (SCs) that are abundant organic aerosol components and can influence the air quality and climate. We found higher concentrations of biomass burning (BB) products at nighttime than daytime, whereas pollen tracers and other SCs showed an opposite diurnal trend, because this site is meteorologically characterized by a mountain/valley breeze.
Jack J. Lin, Kamal Raj R, Stella Wang, Esko Kokkonen, Mikko-Heikki Mikkelä, Samuli Urpelainen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 4709–4727, https://doi.org/10.5194/acp-21-4709-2021, https://doi.org/10.5194/acp-21-4709-2021, 2021
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We used surface-sensitive X-ray photoelectron spectroscopy (XPS) to study laboratory-generated nanoparticles of atmospheric interest at 0–16 % relative humidity. XPS gives direct information about changes in the chemical state from the binding energies of probed elements. Our results indicate water adsorption and associated chemical changes at the particle surfaces well below deliquescence, with distinct features for different particle components and implications for atmospheric chemistry.
Evangelia Kostenidou, Alvaro Martinez-Valiente, Badr R'Mili, Baptiste Marques, Brice Temime-Roussel, Amandine Durand, Michel André, Yao Liu, Cédric Louis, Boris Vansevenant, Daniel Ferry, Carine Laffon, Philippe Parent, and Barbara D'Anna
Atmos. Chem. Phys., 21, 4779–4796, https://doi.org/10.5194/acp-21-4779-2021, https://doi.org/10.5194/acp-21-4779-2021, 2021
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Passenger vehicle emissions can be a significant source of particulate matter in urban areas. In this study the particle-phase emissions of seven Euro 5 passenger vehicles were characterized. Changes in engine technologies and after-treatment devices can alter the chemical composition and the size of the emitted particulate matter. The condition of the diesel particle filter (DPF) plays an important role in the emitted pollutants.
Rongzhi Tang, Quanyang Lu, Song Guo, Hui Wang, Kai Song, Ying Yu, Rui Tan, Kefan Liu, Ruizhe Shen, Shiyi Chen, Limin Zeng, Spiro D. Jorga, Zhou Zhang, Wenbin Zhang, Shijin Shuai, and Allen L. Robinson
Atmos. Chem. Phys., 21, 2569–2583, https://doi.org/10.5194/acp-21-2569-2021, https://doi.org/10.5194/acp-21-2569-2021, 2021
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We performed chassis dynamometer experiments to investigate the emissions and secondary organic aerosol (SOA) formation potential of intermediate volatility organic compounds (IVOCs) from an on-road Chinese gasoline vehicle. High IVOC emission factors (EFs) and distinct volatility distribution were recognized. Our results indicate that vehicular IVOCs contribute significantly to SOA, implying the importance of reducing IVOCs when making air pollution control policies in urban areas of China.
Gareth J. Stewart, Beth S. Nelson, W. Joe F. Acton, Adam R. Vaughan, Naomi J. Farren, James R. Hopkins, Martyn W. Ward, Stefan J. Swift, Rahul Arya, Arnab Mondal, Ritu Jangirh, Sakshi Ahlawat, Lokesh Yadav, Sudhir K. Sharma, Siti S. M. Yunus, C. Nicholas Hewitt, Eiko Nemitz, Neil Mullinger, Ranu Gadi, Lokesh K. Sahu, Nidhi Tripathi, Andrew R. Rickard, James D. Lee, Tuhin K. Mandal, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 2407–2426, https://doi.org/10.5194/acp-21-2407-2021, https://doi.org/10.5194/acp-21-2407-2021, 2021
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Biomass burning releases many lower-molecular-weight organic species which are difficult to analyse but important for the formation of organic aerosol. This study examined a new high-resolution technique to better characterise these difficult-to-analyse organic components. Some burning sources analysed in this study, such as cow dung cake and municipal solid waste, released extremely complex mixtures containing many thousands of different lower-volatility organic compounds.
Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys., 21, 2053–2066, https://doi.org/10.5194/acp-21-2053-2021, https://doi.org/10.5194/acp-21-2053-2021, 2021
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This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The heterogeneous reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
David R. Hanson, Seakh Menheer, Michael Wentzel, and Joan Kunz
Atmos. Chem. Phys., 21, 1987–2001, https://doi.org/10.5194/acp-21-1987-2021, https://doi.org/10.5194/acp-21-1987-2021, 2021
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We report experimental measurements of particle formation in a flow reactor that extend the results from this experiment to a total of more than 270 runs over a time period of ~3 years. This has allowed us to detect a general increase in the cleanliness of the system and improve our knowledge of its chemistry. In-house simulations allowed us to construct phenomenological free energies of molecular clusters of sulfuric acid and ammonia that are appropriate for application to the atmosphere.
Benjamin Woden, Maximilian W. A. Skoda, Adam Milsom, Curtis Gubb, Armando Maestro, James Tellam, and Christian Pfrang
Atmos. Chem. Phys., 21, 1325–1340, https://doi.org/10.5194/acp-21-1325-2021, https://doi.org/10.5194/acp-21-1325-2021, 2021
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Atmospheric aerosols contain a large amount of organic compounds, whose oxidation affects their physical properties through a process known as ageing. We have simulated atmospheric ageing experimentally to elucidate the nature and behaviour of residual surface films. Our results show an increasing amount of residue at near-zero temperatures, demonstrating that an inert product film may build up during droplet ageing, even if only ordinarily short-lived reactive species are initially emitted.
Hao Luo, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-29, https://doi.org/10.5194/acp-2021-29, 2021
Revised manuscript accepted for ACP
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Formation kinetics & mechanism of O3 and SOA from different AHs are still unclear. Thus photochemical oxidation mechanism of 9 AHs with NO2 is comparably studied. Increased formation rate and yield of O3 and SOA is observed via promoting AH content. Raising number of AH's substituent enhances O3 formation, but decreases SOA yield, which is promoted by increasing methyl group number of AHs. Results are helpful to clear conversion of AHs to secondary pollutants in real atmospheric environment.
Zhaomin Yang, Li Xu, Narcisse T. Tsona, Jianlong Li, Xin Luo, and Lin Du
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-61, https://doi.org/10.5194/acp-2021-61, 2021
Revised manuscript accepted for ACP
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The promotion effects of SO2 and NH3 on aerosol particles and organosulfur compounds formation from 1,2,4-trimethylbenzene (TMB) photooxidation were observed for the first time. The enhanced organosulfur compounds included hitherto unidentified aromatic sulfonates and organosulfates, which were produced via acid-driven heterogeneous chemistry of hydroperoxides. The production of organosulfur compounds might provide a new pathway for the fate of TMB in regions with considerable SO2 emissions.
Yiwei Gong and Zhongming Chen
Atmos. Chem. Phys., 21, 813–829, https://doi.org/10.5194/acp-21-813-2021, https://doi.org/10.5194/acp-21-813-2021, 2021
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Stabilized Criegee intermediates (SCIs) are important factors in estimating aerosol formation in the atmosphere. Here the results show that SCIs account for more than 60 % of aerosol formation in limonene ozonolysis and water is an uncertainty in SCI performances. The aerosol formation potential of SCIs under high-humidity conditions is double that under dry and low-humidity conditions, suggesting SCI reactions are still important in contributing to aerosols at high relative humidity.
Jing Dou, Peter A. Alpert, Pablo Corral Arroyo, Beiping Luo, Frederic Schneider, Jacinta Xto, Thomas Huthwelker, Camelia N. Borca, Katja D. Henzler, Jörg Raabe, Benjamin Watts, Hartmut Herrmann, Thomas Peter, Markus Ammann, and Ulrich K. Krieger
Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, https://doi.org/10.5194/acp-21-315-2021, 2021
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Photochemistry of iron(III) complexes plays an important role in aerosol aging, especially in the lower troposphere. Ensuing radical chemistry leads to decarboxylation, and the production of peroxides, and oxygenated volatile compounds, resulting in particle mass loss due to release of the volatile products to the gas phase. We investigated kinetic transport limitations due to high particle viscosity under low relative humidity conditions. For quantification a numerical model was developed.
Ana C. Morales, Thilina Jayarathne, Jonathan H. Slade, Alexander Laskin, and Paul B. Shepson
Atmos. Chem. Phys., 21, 129–145, https://doi.org/10.5194/acp-21-129-2021, https://doi.org/10.5194/acp-21-129-2021, 2021
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Organic nitrates formed from the oxidation of biogenic volatile organic compounds impact both ozone and particulate matter as they remove nitrogen oxides, but they represent important aerosol precursors. We conducted a series of reaction chamber experiments that quantified the total organic nitrate and secondary organic aerosol yield from the OH-radical-initiated oxidation of ocimene, and also measured their hydrolysis lifetimes in the aqueous phase, as a function of pH.
András Hoffer, Beatrix Jancsek-Turóczi, Ádám Tóth, Gyula Kiss, Anca Naghiu, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 20, 16135–16144, https://doi.org/10.5194/acp-20-16135-2020, https://doi.org/10.5194/acp-20-16135-2020, 2020
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Emission factors for PM10 and polycyclic aromatic hydrocarbons (PAHs) are reported for the first time ever for the indoor combustion of 12 common types of municipal solid waste that are frequently burned in households worldwide. We have found that waste burning emits up to 40 times more PM10 and 800 times more PAHs than the combustion of dry firewood. Our finding highlights the need for coordinated actions against illegal waste combustion and the extreme health hazard associated with it.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys., 20, 15513–15535, https://doi.org/10.5194/acp-20-15513-2020, https://doi.org/10.5194/acp-20-15513-2020, 2020
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This paper presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modeling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas–particle partitioning, and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Roland Benoit, Nesrine Belhadj, Maxence Lailliau, and Philippe Dagaut
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1070, https://doi.org/10.5194/acp-2020-1070, 2020
Revised manuscript accepted for ACP
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This study compares different modes of limonene oxidation (ozonolysis, photooxidation and cool flame) on the basis of review articles and experimental results. Although the oxidation conditions are totally different, the results obtained present great similarities on the nature of the products, but also specificities related to autooxidation such as the presence of ketohydroperoxides.
Eugene F. Mikhailov, Mira L. Pöhlker, Kathrin Reinmuth-Selzle, Sergey S. Vlasenko, Ovid O. Krüger, Janine Fröhlich-Nowoisky, Christopher Pöhlker, Olga A. Ivanova, Alexey A. Kiselev, Leslie A. Kremper, and Ulrich Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1224, https://doi.org/10.5194/acp-2020-1224, 2020
Revised manuscript accepted for ACP
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Subpollen particles are a relatively new subset of atmospheric aerosol particles. When pollen grains rupture, they release cytoplasmic fragments known as subpollen particles (SPP) ranged from several nanometers to about 1 μm. It has been shown that SPP exhibit abnormally high hygroscopicity due to forming a water-rich phase that, in particular, may influence the life cycle of SPP and the related direct and indirect effects on radiation budget as well as reinforce their allergic potential.
Liqing Hao, Eetu Kari, Ari Leskinen, Douglas R. Worsnop, and Annele Virtanen
Atmos. Chem. Phys., 20, 14393–14405, https://doi.org/10.5194/acp-20-14393-2020, https://doi.org/10.5194/acp-20-14393-2020, 2020
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Our work presents the observational results of secondary organic aerosol (SOA) formation in the presence of ammonia. The particle-phase ammonium was continuously produced even after SOA formation had ceased. The gas-phase organic acids were observed to contribute to the formed particle-phase ammonium salts. This study suggests that the presence of ammonia may change the mass and chemical composition of large-size SOA particles and can potentially alter the aerosol impact on climate change.
Junling Li, Hong Li, Kun Li, Yan Chen, Hao Zhang, Xin Zhang, Zhenhai Wu, Yongchun Liu, Xuezhong Wang, Weigang Wang, and Maofa Ge
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1189, https://doi.org/10.5194/acp-2020-1189, 2020
Revised manuscript accepted for ACP
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SOA formation from the mixed anthropogenic volatile organic compounds was enhanced compared to the predicted SOA mass concentration based on the SOA yield of single species; interaction occurred between intermediate products from the two precursors. Interactions between the intermediate products from the mixtures and the effect on SOA formation give us a further understanding of the SOA formed in the atmosphere.
Li Wu, Clara Becote, Sophie Sobanska, Pierre-Marie Flaud, Emilie Perraudin, Eric Villenave, Young-Chul Song, and Chul-Un Ro
Atmos. Chem. Phys., 20, 14103–14122, https://doi.org/10.5194/acp-20-14103-2020, https://doi.org/10.5194/acp-20-14103-2020, 2020
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MBTCA (3-methyl-1,2,3-butanetricarboxylic acid), a second-generation product of monoterpenes, is one of the most relevant tracer compounds for biogenic secondary organic aerosols (SOAs). Laboratory-generated, micrometer-sized, pure-MBTCA, mono-/di-/trisodium MBTCA salts and MBTCA–NaCl mixture aerosol particles were examined systematically to observe their hygroscopic behavior, and it was also observed that the monosodium MBTCA salt aerosols were formed through a reaction between MBTCA and NaCl.
Mingjie Xie, Zhenzhen Zhao, Amara L. Holder, Michael D. Hays, Xi Chen, Guofeng Shen, James J. Jetter, Wyatt M. Champion, and Qin'geng Wang
Atmos. Chem. Phys., 20, 14077–14090, https://doi.org/10.5194/acp-20-14077-2020, https://doi.org/10.5194/acp-20-14077-2020, 2020
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This study investigated the composition, structures, and light absorption of N-containing aromatic compounds (NACs) in PM2.5 emitted from burning red oak and charcoal in a variety of cookstoves. The results suggest that the identified NACs might have substantial fractions remaining in the gas phase. In comparison to other sources, cookstove emissions from red oak or charcoal fuels did not exhibit unique NAC structural features but had distinct NAC composition.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1018, https://doi.org/10.5194/acp-2020-1018, 2020
Revised manuscript accepted for ACP
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by Chemical Mass Balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Yujue Wang, Min Hu, Nan Xu, Yanhong Qin, Zhijun Wu, Liwu Zeng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 20, 13721–13734, https://doi.org/10.5194/acp-20-13721-2020, https://doi.org/10.5194/acp-20-13721-2020, 2020
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Field straw residue burning is a widespread type of biomass burning in Asia, while its emissions are poorly understood. In this study, we designed lab-controlled experiments to comprehensively investigate the emission factors, chemical compositions and light absorption properties of both water-soluble and water-insoluble carbonaceous aerosols emitted from straw burning. The results clearly highlight the significant influences of burning conditions and combustion efficiency on the emissions.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
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We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Clarissa Baldo, Paola Formenti, Sophie Nowak, Servanne Chevaillier, Mathieu Cazaunau, Edouard Pangui, Claudia Di Biagio, Jean-Francois Doussin, Konstantin Ignatyev, Pavla Dagsson-Waldhauserova, Olafur Arnalds, A. Robert MacKenzie, and Zongbo Shi
Atmos. Chem. Phys., 20, 13521–13539, https://doi.org/10.5194/acp-20-13521-2020, https://doi.org/10.5194/acp-20-13521-2020, 2020
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We showed that Icelandic dust has a fundamentally different chemical and mineralogical composition from low-latitude dust. In particular, magnetite is as high as 1 %–2 % of the total dust mass. Our results suggest that Icelandic dust may have an important impact on the radiation balance in the subpolar and polar regions.
Sophia M. Charan, Reina S. Buenconsejo, and John H. Seinfeld
Atmos. Chem. Phys., 20, 13167–13190, https://doi.org/10.5194/acp-20-13167-2020, https://doi.org/10.5194/acp-20-13167-2020, 2020
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In urban areas, the emissions from volatile chemical products may be responsible for the formation of as much particulate matter as motor vehicles. Since exposure to particulate matter is a public health crisis, understanding its formation is critical. In this work, we investigate the secondary organic aerosol formation potential of benzyl alcohol, an important compound that is representative of some of these new emission sources, and find that more particulate matter forms than is expected.
Kasper Kristensen, Louise N. Jensen, Lauriane L. J. Quéléver, Sigurd Christiansen, Bernadette Rosati, Jonas Elm, Ricky Teiwes, Henrik B. Pedersen, Marianne Glasius, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 20, 12549–12567, https://doi.org/10.5194/acp-20-12549-2020, https://doi.org/10.5194/acp-20-12549-2020, 2020
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Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, https://doi.org/10.5194/acp-20-11387-2020, 2020
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In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Young-Chul Song, Ariana G. Bé, Scot T. Martin, Franz M. Geiger, Allan K. Bertram, Regan J. Thomson, and Mijung Song
Atmos. Chem. Phys., 20, 11263–11273, https://doi.org/10.5194/acp-20-11263-2020, https://doi.org/10.5194/acp-20-11263-2020, 2020
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We report the liquid–liquid phase separation (LLPS) of organic aerosol consisting of α-pinene- and β-caryophyllene-derived ozonolysis products and commercial organic compounds. As compositional complexity increased from one to two organic species, LLPS occurred over a wider range of average O : C values (increasing from 0.44 to 0.67). These results provide further evidence that LLPS is likely frequent in organic aerosol particles in the troposphere, even in the absence of inorganic salt.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-924, https://doi.org/10.5194/acp-2020-924, 2020
Revised manuscript accepted for ACP
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Functional group composition of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Peng Zhang, Tianzeng Chen, Jun Liu, Guangyan Xu, Qingxin Ma, Biwu Chu, Wanqi Sun, and Hong He
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-929, https://doi.org/10.5194/acp-2020-929, 2020
Revised manuscript accepted for ACP
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This work highlights the opposing effects of primary and secondary H2SO4 on both SOA formation and constitutes. Our findings revealed that a substantial increase in secondary H2SO4 particles promoted the SOA formation of ethyl methacrylate with increasing SO2 in the absence of seed particles. However, increased primary H2SO4 with seed acidity enhanced ethyl methacrylate uptake, but reduced its SOA formation in the presence of seed particles.
Damon M. Smith, Tianqu Cui, Marc N. Fiddler, Rudra P. Pokhrel, Jason D. Surratt, and Solomon Bililign
Atmos. Chem. Phys., 20, 10169–10191, https://doi.org/10.5194/acp-20-10169-2020, https://doi.org/10.5194/acp-20-10169-2020, 2020
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Biomass fuels used for domestic purposes in east Africa produce a significant atmospheric burden of aerosols and volatile organic compounds. The chemical properties and composition of these aerosols have not been investigated in the laboratory. In this work methanol extracts from filter samples of aerosol collected from an indoor smog chamber were analyzed to determine the chemical composition and identify the light absorption properties of organic aerosol constituents.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
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Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Alexis Dépée, Pascal Lemaitre, Thomas Gelain, Marie Monier, and Andrea Flossmann
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-832, https://doi.org/10.5194/acp-2020-832, 2020
Revised manuscript accepted for ACP
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Present article describe a new In-Cloud Aerosol Scavenging Experiment (In-CASE) that has been conceived to measure the collection efficiency of submicron aerosol particles by cloud droplets. Present article focus on the influence of electrostatic effect on the collection efficiency.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
David O. De Haan, Lelia N. Hawkins, Kevin Jansen, Hannah G. Welsh, Raunak Pednekar, Alexia de Loera, Natalie G. Jimenez, Margaret A. Tolbert, Mathieu Cazaunau, Aline Gratien, Antonin Bergé, Edouard Pangui, Paola Formenti, and Jean-François Doussin
Atmos. Chem. Phys., 20, 9581–9590, https://doi.org/10.5194/acp-20-9581-2020, https://doi.org/10.5194/acp-20-9581-2020, 2020
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When exposed to glyoxal in chamber experiments, dry ammonium or methylammonium sulfate particles turn brown immediately and reversibly without increasing in size. Much less browning was observed on wet aerosol particles, and no browning was observed with sodium sulfate aerosol. While estimated dry aerosol light absorption caused by background glyoxal (70 ppt) is insignificant compared to that of secondary brown carbon overall, in polluted regions this process could be a source of brown carbon.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
Petroc D. Shelley, Thomas J. Bannan, Stephen D. Worrall, M. Rami Alfarra, Ulrich K. Krieger, Carl J. Percival, Arthur Garforth, and David Topping
Atmos. Chem. Phys., 20, 8293–8314, https://doi.org/10.5194/acp-20-8293-2020, https://doi.org/10.5194/acp-20-8293-2020, 2020
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The methods used to estimate the vapour pressures of compounds in the atmosphere typically perform poorly when applied to organic compounds found in the atmosphere. New measurements have been made and compared to previous experimental data and estimated values so that the limitations within the estimation methods can be identified and in the future be rectified.
Deep Sengupta, Vera Samburova, Chiranjivi Bhattarai, Adam C. Watts, Hans Moosmüller, and Andrey Y. Khlystov
Atmos. Chem. Phys., 20, 8227–8250, https://doi.org/10.5194/acp-20-8227-2020, https://doi.org/10.5194/acp-20-8227-2020, 2020
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This paper presents important results on the atmospheric chemistry of combustion emissions. Organic compounds from these emissions can contribute significantly to chemical and physical properties of atmospheric aerosols. In this paper, a detailed chemical analysis of gas- and particle-phase polar organic compounds from the laboratory combustion of globally important fuels is presented. The aging experiments were performed to understand the fate of biomass-burning organics in the atmosphere.
Junling Li, Weigang Wang, Kun Li, Wenyu Zhang, Chao Peng, Li Zhou, Bo Shi, Yan Chen, Mingyuan Liu, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 20, 8123–8137, https://doi.org/10.5194/acp-20-8123-2020, https://doi.org/10.5194/acp-20-8123-2020, 2020
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Long-chain alkanes (a large fraction of diesel fuel and its exhaust) are important potential contributors of SOA. Through the analysis of the components of formed SOA, we found that low-temperature conditions promote the oligomerization of n-dodecane, and the degree of oligomerization can reach tetramerization. The presence of the oligomers enhances the light extinction of the particles. UV-scattering particles in the boundary layer can accelerate photochemical reactions and haze production.
Minli Wang, Yiqun Chen, Heyun Fu, Xiaolei Qu, Bengang Li, Shu Tao, and Dongqiang Zhu
Atmos. Chem. Phys., 20, 7941–7954, https://doi.org/10.5194/acp-20-7941-2020, https://doi.org/10.5194/acp-20-7941-2020, 2020
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The mechanism and factors controlling the hygroscopicity of black-carbon-containing particles (BCPs) from different carbon sources are not well understood. We thoroughly characterized the chemical and compositional properties of 15 samples of BCPs from different sources (wood, herb, and soot) and further investigated their hygroscopicity. Depending on the carbon source, organic carbon and dissolved mineral contents were key determinants of the equilibrium and kinetics of water uptake by BCPs.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Gi Young Jeong
Atmos. Chem. Phys., 20, 7411–7428, https://doi.org/10.5194/acp-20-7411-2020, https://doi.org/10.5194/acp-20-7411-2020, 2020
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During long-range transport, mineral dust interacts with the atmosphere, biosphere, cryosphere, and pedosphere, influencing ecosystems, the atmospheric energy balance, and air quality. This study analyzed the mineral and chemical compositions of Asian dust samples collected during 14 years in Korea. The result showed mineralogical and geochemical variation depending on the dust migration path, fractionation, and atmospheric reactions as well as average properties.
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Short summary
We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
We have observed a strong effect of relative humidity on the composition of particulate matter...
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