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.
Kristian J. Kiland, Kevin L. Marroquin, Natalie R. Smith, Shaun Xu, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Meas. Tech., 15, 5545–5561, https://doi.org/10.5194/amt-15-5545-2022, https://doi.org/10.5194/amt-15-5545-2022, 2022
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Information on the viscosity of secondary organic aerosols is needed when making air quality, climate, and atmospheric chemistry predictions. Viscosity depends on temperature, so we developed a new method for measuring the temperature-dependent viscosity of small samples. As an application of the method, we measured the viscosity of farnesene secondary organic aerosol at different temperatures.
Alexandra L. Klodt, Marley Adamek, Monica Dibley, Sergey A. Nizkorodov, and Rachel E. O'Brien
Atmos. Chem. Phys., 22, 10155–10171, https://doi.org/10.5194/acp-22-10155-2022, https://doi.org/10.5194/acp-22-10155-2022, 2022
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We investigated photochemistry of a secondary organic aerosol under three different conditions: in a dilute aqueous solution mimicking cloud droplets, in a solution of concentrated ammonium sulfate mimicking deliquesced aerosol, and in an organic matrix mimicking dry organic aerosol. We find that rate and mechanisms of photochemistry depend sensitively on these conditions, suggesting that the same organic aerosol compounds will degrade at different rates depending on their local environment.
Fabian Mahrt, Long Peng, Julia Zaks, Yuanzhou Huang, Paul E. Ohno, Natalie R. Smith, Florence K. A. Gregson, Yiming Qin, Celia L. Faiola, Scot T. Martin, Sergey A. Nizkorodov, Markus Ammann, and Allan K. Bertram
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-331, https://doi.org/10.5194/acp-2022-331, 2022
Revised manuscript accepted for ACP
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The number of condensed phases in mixtures of different secondary organic aerosol (SOA) types determines their impact on air quality and climate. Here we observe the number of phases in individual particles that contain mixtures of two different types of SOA. We find that SOA mixtures can form one- or two-phase particles, depending on the difference in the average oxygen-to-carbon (O / C) ratios of the two SOA types mixed.
Matthew L. Dawson, Christian Guzman, Jeffrey H. Curtis, Mario Acosta, Shupeng Zhu, Donald Dabdub, Andrew Conley, Matthew West, Nicole Riemer, and Oriol Jorba
Geosci. Model Dev., 15, 3663–3689, https://doi.org/10.5194/gmd-15-3663-2022, https://doi.org/10.5194/gmd-15-3663-2022, 2022
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Progress in identifying complex, mixed-phase physicochemical processes has resulted in an advanced understanding of the evolution of atmospheric systems but has also introduced a level of complexity that few atmospheric models were designed to handle. We present a flexible treatment for multiphase chemical processes for models of diverse scale, from box up to global models. This enables users to build a customized multiphase mechanism that is accessible to a much wider community.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
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Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
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Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper 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.
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., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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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 of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213, https://doi.org/10.5194/acp-21-10199-2021, https://doi.org/10.5194/acp-21-10199-2021, 2021
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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 in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
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., 21, 8531–8555, https://doi.org/10.5194/acp-21-8531-2021, https://doi.org/10.5194/acp-21-8531-2021, 2021
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We present a comprehensive characterization of water-soluble organic carbon (WSOC) in seasonal snow of northwestern China. We applied complementary multimodal 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 a model simulation and showed the profound influences of WSOC on the energy budget of midlatitude seasonal snowpack.
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.
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.
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.
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.
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)
Chemical characteristics and sources of PM2.5 in Hohhot, a semi-arid city in northern China: insight from the COVID-19 lockdown
The positive effect of formaldehyde on the photocatalytic renoxification of nitrate on TiO2 particles
Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical
A comprehensive study on hygroscopic behaviour and nitrate depletion of NaNO3 and dicarboxylic acid mixtures: implications for nitrate depletion in tropospheric aerosols
Secondary organic aerosols from OH oxidation of cyclic volatile methyl siloxanes as an important Si source in the atmosphere
Effects of OH radical and SO2 concentrations on photochemical reactions of mixed anthropogenic organic gases
Effects of the sample matrix on the photobleaching and photodegradation of toluene-derived secondary organic aerosol compounds
Functionality-based formation of secondary organic aerosol from m-xylene photooxidation
Chemical composition of secondary organic aerosol particles formed from mixtures of anthropogenic and biogenic precursors
A novel pathway of atmospheric sulfate formation through carbonate radicals
A sulfuric acid nucleation potential model for the atmosphere
Optical and chemical properties and oxidative potential of aqueous-phase products from OH and 3C∗-initiated photooxidation of eugenol
The relationship between PM2.5 and anticyclonic wave activity during summer over the United States
Not All Types of Secondary Organic Aerosol Mix: Two Phases Observed When Mixing Different Secondary Organic Aerosol Types
The influence of the addition of a reactive low SOA yield VOC on the volatility of particles formed from photo-oxidation of anthropogenic – biogenic mixtures
Measurement Report: A new coupled method of pH titration and size-resolved analysis to identify the structure, aging, and source of water-soluble organic carbon
Iron from coal combustion particles dissolves much faster than mineral dust under simulated atmospheric acidic conditions
Cellulose in atmospheric particulate matter at rural and urban sites across France and Switzerland
Kinetics, SOA yields, and chemical composition of secondary organic aerosol from β-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K
Chemical transformation of α-pinene-derived organosulfate via heterogeneous OH oxidation: implications for sources and environmental fates of atmospheric organosulfates
Aqueous chemical bleaching of 4-nitrophenol brown carbon by hydroxyl radicals; products, mechanism, and light absorption
Significant formation of sulfate aerosols contributed by the heterogeneous drivers of dust surface
Secondary organic aerosol formation from camphene oxidation: measurements and modeling
Technical note: Real-time diagnosis of the hygroscopic growth micro-dynamics of nanoparticles with Fourier transform infrared spectroscopy
Single-particle Raman spectroscopy for studying physical and chemical processes of atmospheric particles
Are reactive oxygen species (ROS) a suitable metric to predict toxicity of carbonaceous aerosol particles?
Secondary organic aerosol and organic nitrogen yields from the nitrate radical (NO3) oxidation of alpha-pinene from various RO2 fates
Secondary organic aerosol formation from the oxidation of decamethylcyclopentasiloxane at atmospherically relevant OH concentrations
Aqueous secondary organic aerosol formation from the direct photosensitized oxidation of vanillin in the absence and presence of ammonium nitrate
Chamber investigation of the formation and transformation of secondary organic aerosol in mixtures of biogenic and anthropogenic volatile organic compounds
Evolution of volatility and composition in sesquiterpene-mixed and α-pinene secondary organic aerosol particles during isothermal evaporation
Potential new tracers and their mass fraction in the emitted PM10 from the burning of household waste in stoves
Synergetic effects of NH3 and NOx on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation
Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature
Technical note: Adsorption and desorption equilibria from statistical thermodynamics and rates from transition state theory
Nighttime chemistry of biomass burning emissions in urban areas: A dual mobile chamber study
Formation and evolution of secondary organic aerosols derived from urban-lifestyle sources: vehicle exhaust and cooking emissions
Mass spectral characterization of secondary organic aerosol from urban cooking and vehicular sources
An organic crystalline state in ageing atmospheric aerosol proxies: spatially resolved structural changes in levitated fatty acid particles
Photolytically induced changes in composition and volatility of biogenic secondary organic aerosol from nitrate radical oxidation during night-to-day transition
The driving factors of new particle formation and growth in the polluted boundary layer
Exploring the composition and volatility of secondary organic aerosols in mixed anthropogenic and biogenic precursor systems
Acidity and the multiphase chemistry of atmospheric aqueous particles and clouds
Chemical composition, optical properties, and oxidative potential of water- and methanol-soluble organic compounds emitted from the combustion of biomass materials and coal
Photodegradation of atmospheric chromophores: changes in oxidation state and photochemical reactivity
Temperature and volatile organic compound concentrations as controlling factors for chemical composition of α-pinene-derived secondary organic aerosol
Tracer-based source apportioning of atmospheric organic carbon and the influence of anthropogenic emissions on secondary organic aerosol formation in Hong Kong
Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air
Characterization of primary and aged wood burning and coal combustion organic aerosols in an environmental chamber and its implications for atmospheric aerosols
Revisiting the reaction of dicarbonyls in aerosol proxy solutions containing ammonia: the case of butenedial
Haijun Zhou, Tao Liu, Bing Sun, Yongli Tian, Xingjun Zhou, Feng Hao, Xi Chun, Zhiqiang Wan, Peng Liu, Jingwen Wang, and Dagula Du
Atmos. Chem. Phys., 22, 12153–12166, https://doi.org/10.5194/acp-22-12153-2022, https://doi.org/10.5194/acp-22-12153-2022, 2022
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A single year’s offline measurement was conducted in Hohhot to reveal the chemical characteristics and sources of PM2.5 in a semi-arid region. We believe that our study makes a significant contribution to the literature because relatively few studies have focused on the chemical composition and sources of PM2.5 with offline measurements. A knowledge gap exists concerning how chemical composition and sources respond to implemented control measures for aerosols, particularly in a semi-arid region.
Yuhan Liu, Xuejiao Wang, Jing Shang, Weiwei Xu, Mengshuang Sheng, and Chunxiang Ye
Atmos. Chem. Phys., 22, 11347–11358, https://doi.org/10.5194/acp-22-11347-2022, https://doi.org/10.5194/acp-22-11347-2022, 2022
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In this study, the influence of HCHO on renoxification on nitrate-doped TiO2 particles is investigated by using an experimental chamber. Mass NOx release is suggested to follow the NO−3-NO3·-HNO3-NOx pathway, with HCHO involved in the transformation of NO3· to HNO3 through hydrogen abstraction. Our proposed reaction mechanism by which HCHO promotes photocatalytic renoxification is helpful for deeply understanding the atmospheric photochemical processes and nitrogen cycling.
Yindong Guo, Hongru Shen, Iida Pullinen, Hao Luo, Sungah Kang, Luc Vereecken, Hendrik Fuchs, Mattias Hallquist, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, Defeng Zhao, and Thomas F. Mentel
Atmos. Chem. Phys., 22, 11323–11346, https://doi.org/10.5194/acp-22-11323-2022, https://doi.org/10.5194/acp-22-11323-2022, 2022
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The oxidation of limonene, a common volatile emitted by trees and chemical products, by NO3, a nighttime oxidant, forms many highly oxygenated organic molecules (HOM), including C10-30 compounds. Most of the HOM are second-generation organic nitrates, in which carbonyl-substituted C10 nitrates accounted for a major fraction. Their formation can be explained by chemistry of peroxy radicals. HOM, especially low-volatile ones, play an important role in nighttime new particle formation and growth.
Shuaishuai Ma, Qiong Li, and Yunhong Zhang
Atmos. Chem. Phys., 22, 10955–10970, https://doi.org/10.5194/acp-22-10955-2022, https://doi.org/10.5194/acp-22-10955-2022, 2022
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The nitrate phase state can play a critical role in determining the occurrence and extent of nitrate depletion in internally mixed NaNO3–DCA particles, which may be instructive for relevant aerosol reaction systems. Besides, organic acids have a potential to deplete nitrate based on the comprehensive consideration of acidity, particle-phase state, droplet water activity, and HNO3 gas-phase diffusion.
Chong Han, Hongxing Yang, Kun Li, Patrick Lee, John Liggio, Amy Leithead, and Shao-Meng Li
Atmos. Chem. Phys., 22, 10827–10839, https://doi.org/10.5194/acp-22-10827-2022, https://doi.org/10.5194/acp-22-10827-2022, 2022
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We presented yields and compositions of Si-containing SOAs generated from the reaction of cVMSs (D3–D6) with OH radicals. NOx played a negative role in cVMS SOA formation, while ammonium sulfate seeds enhanced D3–D5 SOA yields at short photochemical ages under high-NOx conditions. The aerosol mass spectra confirmed that the components of cVMS SOAs significantly relied on OH exposure. A global cVMS-derived SOA source strength was estimated in order to understand SOA formation potentials of cVMSs.
Junling Li, Kun Li, Hao Zhang, Xin Zhang, Yuanyuan Ji, Wanghui Chu, Yuxue Kong, Yangxi Chu, Yanqin Ren, Yujie Zhang, Haijie Zhang, Rui Gao, Zhenhai Wu, Fang Bi, Xuan Chen, Xuezhong Wang, Weigang Wang, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 22, 10489–10504, https://doi.org/10.5194/acp-22-10489-2022, https://doi.org/10.5194/acp-22-10489-2022, 2022
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Ozone formation is enhanced by higher OH concentration and higher temperature but is influenced little by SO2. SO2 can largely enhance the particle formation. Organo-sulfates and organo-nitrates are detected in the formed particles, and the presence of SO2 can promote the formation of organo-sulfates. The results provide a scientific basis for systematically evaluating the effects of SO2, OH concentration, and temperature on the oxidation of mixed organic gases in the atmosphere.
Alexandra L. Klodt, Marley Adamek, Monica Dibley, Sergey A. Nizkorodov, and Rachel E. O'Brien
Atmos. Chem. Phys., 22, 10155–10171, https://doi.org/10.5194/acp-22-10155-2022, https://doi.org/10.5194/acp-22-10155-2022, 2022
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We investigated photochemistry of a secondary organic aerosol under three different conditions: in a dilute aqueous solution mimicking cloud droplets, in a solution of concentrated ammonium sulfate mimicking deliquesced aerosol, and in an organic matrix mimicking dry organic aerosol. We find that rate and mechanisms of photochemistry depend sensitively on these conditions, suggesting that the same organic aerosol compounds will degrade at different rates depending on their local environment.
Yixin Li, Jiayun Zhao, Mario Gomez-Hernandez, Michael Lavallee, Natalie M. Johnson, and Renyi Zhang
Atmos. Chem. Phys., 22, 9843–9857, https://doi.org/10.5194/acp-22-9843-2022, https://doi.org/10.5194/acp-22-9843-2022, 2022
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Here we elucidate the production of COOs and their roles in SOA and brown carbon formation from m-xylene oxidation by simultaneously monitoring the evolution of gas-phase products and aerosol properties in an environmental chamber. A kinetic framework is developed to predict SOA production from the concentrations and uptake coefficients for COOs. This functionality-based approach reproduces SOA formation from m-xylene oxidation well and is applicable to VOC oxidation for other species.
Yunqi Shao, Aristeidis Voliotis, Mao Du, Yu Wang, Kelly Pereira, Jacqueline Hamilton, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 9799–9826, https://doi.org/10.5194/acp-22-9799-2022, https://doi.org/10.5194/acp-22-9799-2022, 2022
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This study explored the chemical properties of secondary organic aerosol (SOA) that formed from photo-oxidation of single and mixed biogenic and anthropogenic precursors. We showed that SOA chemical properties in a mixed vapour system are mainly affected by the
higher-yield precursor's oxidation products and products from
cross-product formation. This study also identifies potential tracer compounds in a mixed vapour system that might be used in SOA source attribution in future ambient studies.
Yangyang Liu, Yue Deng, Jiarong Liu, Xiaozhong Fang, Tao Wang, Kejian Li, Kedong Gong, Aziz U. Bacha, Iqra Nabi, Qiuyue Ge, Xiuhui Zhang, Christian George, and Liwu Zhang
Atmos. Chem. Phys., 22, 9175–9197, https://doi.org/10.5194/acp-22-9175-2022, https://doi.org/10.5194/acp-22-9175-2022, 2022
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Both CO2 and carbonate salt work as the precursor of carbonate radicals, which largely promotes sulfate formation during the daytime. This study provides the first indication that the carbonate radical not only plays a role as an intermediate in tropospheric anion chemistry but also as a strong oxidant for the surface processing of trace gas in the atmosphere. CO2, carbponate radicals, and sulfate receive attention from those looking at the environment, atmosphere, aerosol, and photochemistry.
Jack S. Johnson and Coty N. Jen
Atmos. Chem. Phys., 22, 8287–8297, https://doi.org/10.5194/acp-22-8287-2022, https://doi.org/10.5194/acp-22-8287-2022, 2022
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Sulfuric acid nucleation forms particles in Earth's atmosphere that influence cloud formation and climate. This study introduces the Nucleation Potential Model, which simplifies the diverse reactions between sulfuric acid and numerous precursor gases to predict nucleation rates. Results show that the model is capable of estimating the potency and concentration of mixtures of precursor gases from laboratory and field observations and can be used to model nucleation across diverse environments.
Xudong Li, Ye Tao, Longwei Zhu, Shuaishuai Ma, Shipeng Luo, Zhuzi Zhao, Ning Sun, Xinlei Ge, and Zhaolian Ye
Atmos. Chem. Phys., 22, 7793–7814, https://doi.org/10.5194/acp-22-7793-2022, https://doi.org/10.5194/acp-22-7793-2022, 2022
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This work has, for the first time, investigated the optical and chemical properties and oxidative potential of aqueous-phase photooxidation products of eugenol (a biomass-burning-emitted compound) and elucidated the interplay among these properties. Large mass yields exceeding 100 % were found, and the aqueous processing is a source of BrC (likely relevant with humic-like substances). We also show that aqueous processing can produce species that are more toxic than that of its precursor.
Ye Wang, Natalie Mahowald, Peter Hess, Wenxiu Sun, and Gang Chen
Atmos. Chem. Phys., 22, 7575–7592, https://doi.org/10.5194/acp-22-7575-2022, https://doi.org/10.5194/acp-22-7575-2022, 2022
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PM2.5 is positively related to anticyclonic wave activity (AWA) changes close to the observing sites. Changes between current and future climates in AWA can explain up to 75 % of PM2.5 variability at some stations using a linear regression model. Our analysis indicates that higher PM2.5 concentrations occur when a positive AWA anomaly is prominent, which could be critical for understanding how pollutants respond to changing atmospheric circulation and for developing robust pollution projections.
Fabian Mahrt, Long Peng, Julia Zaks, Yuanzhou Huang, Paul E. Ohno, Natalie R. Smith, Florence K. A. Gregson, Yiming Qin, Celia L. Faiola, Scot T. Martin, Sergey A. Nizkorodov, Markus Ammann, and Allan K. Bertram
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-331, https://doi.org/10.5194/acp-2022-331, 2022
Revised manuscript accepted for ACP
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The number of condensed phases in mixtures of different secondary organic aerosol (SOA) types determines their impact on air quality and climate. Here we observe the number of phases in individual particles that contain mixtures of two different types of SOA. We find that SOA mixtures can form one- or two-phase particles, depending on the difference in the average oxygen-to-carbon (O / C) ratios of the two SOA types mixed.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-312, https://doi.org/10.5194/acp-2022-312, 2022
Revised manuscript accepted for ACP
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture are contributing significantly to the signal, suggesting interactions can be important.
Yuanyuan Qin, Juanjuan Qin, Xiaobo Wang, Kang Xiao, Ting Qi, Yuwei Gao, Xueming Zhou, Shaoxuan Shi, Jingnan Li, Jingsi Gao, Ziyin Zhang, Jihua Tan, Yang Zhang, and Rongzhi Chen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-321, https://doi.org/10.5194/acp-2022-321, 2022
Revised manuscript accepted for ACP
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Deep interrogation of water-soluble organic carbon (WSOC) in aerosols is critical and challenging because WSOC is involved in many key particle-associated chemical reactions. This work examined how the chemical structure (distribution of functional groups) and optical properties (UV/fluorescence properties) of WSOC were affected by pH and particle size. We found that the pH-dependent and particle size-dependent behaviors could effectively reveal the structure, aging, and source of aerosol WSOC.
Clarissa Baldo, Akinori Ito, Michael D. Krom, Weijun Li, Tim Jones, Nick Drake, Konstantin Ignatyev, Nicholas Davidson, and Zongbo Shi
Atmos. Chem. Phys., 22, 6045–6066, https://doi.org/10.5194/acp-22-6045-2022, https://doi.org/10.5194/acp-22-6045-2022, 2022
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High ionic strength relevant to the aerosol-water enhanced proton-promoted dissolution of iron in coal fly ash (up to 7 times) but suppressed oxalate-promoted dissolution at low pH (< 3). Fe in coal fly ash dissolved up to 7 times faster than in Saharan dust at low pH. A global model with the updated dissolution rates of iron in coal fly ash suggested a larger contribution of pyrogenic dissolved Fe over regions with a strong impact from fossil fuel combustions.
Adam Brighty, Véronique Jacob, Gaëlle Uzu, Lucille Borlaza, Sébastien Conil, Christoph Hueglin, Stuart K. Grange, Olivier Favez, Cécile Trébuchon, and Jean-Luc Jaffrezo
Atmos. Chem. Phys., 22, 6021–6043, https://doi.org/10.5194/acp-22-6021-2022, https://doi.org/10.5194/acp-22-6021-2022, 2022
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With an revised analytical method and long-term sampling strategy, we have been able to elucidate much more information about atmospheric plant debris, a poorly understood class of particulate matter. We found weaker seasonal patterns at urban locations compared to rural locations and significant interannual variability in concentrations between previous years and 2020, during the COVID-19 pandemic. This suggests a possible man-made influence on plant debris concentration and source strength.
Linyu Gao, Junwei Song, Claudia Mohr, Wei Huang, Magdalena Vallon, Feng Jiang, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, https://doi.org/10.5194/acp-22-6001-2022, 2022
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We study secondary organic aerosol (SOA) from β-caryophyllene (BCP) ozonolysis with and without nitrogen oxides over 213–313 K in the simulation chamber. The yields and the rate constants were determined at 243–313 K. Chemical compositions varied at different temperatures, indicating a strong impact on the BCP ozonolysis pathways. This work helps to better understand the SOA from BCP ozonolysis for conditions representative of the real atmosphere from the boundary layer to the upper troposphere.
Rongshuang Xu, Sze In Madeleine Ng, Wing Sze Chow, Yee Ka Wong, Yuchen Wang, Donger Lai, Zhongping Yao, Pui-Kin So, Jian Zhen Yu, and Man Nin Chan
Atmos. Chem. Phys., 22, 5685–5700, https://doi.org/10.5194/acp-22-5685-2022, https://doi.org/10.5194/acp-22-5685-2022, 2022
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To date, while over a hundred organosulfates (OSs) have been detected in atmospheric aerosols, many of them are still unidentified, with unknown precursors and formation processes. We found the heterogeneous OH oxidation of an α-pinene-derived organosulfate (C10H17O5SNa, αpOS-249, αpOS-249) can proceed at an efficient rate and transform into more oxygenated OSs, which have been commonly detected in atmospheric aerosols and α-pinene-derived SOA in chamber studies.
Bartłomiej Witkowski, Priyanka Jain, and Tomasz Gierczak
Atmos. Chem. Phys., 22, 5651–5663, https://doi.org/10.5194/acp-22-5651-2022, https://doi.org/10.5194/acp-22-5651-2022, 2022
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This article describes a comprehensive investigation of the aqueous oxidation of 4-nitrophenol (4NP) by hydroxyl radicals (OH). The reaction was carried out in a laboratory photoreactor. We report the formation of key intermediates under different pH conditions and the evolution of the light absorption of the reaction solution. The results provide new insights into the formation and removal (chemical bleaching) of light-absorbing organic aerosols (atmospheric brown carbon).
Tao Wang, Yangyang Liu, Hanyun Cheng, Zhenzhen Wang, Hongbo Fu, Jianmin Chen, and Liwu Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-227, https://doi.org/10.5194/acp-2022-227, 2022
Revised manuscript accepted for ACP
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This study compared the gas-phase, aqueous-phase and heterogeneous SO2 oxidation pathways by combining laboratory work with modeling study. The heterogeneous chemistry, particularly that induced by the dust surface drivers, presents positive implications for the removal of airborne SO2 and formation of sulfate aerosols. This work highlighted the atmospheric significance of dust-driven chemistry and suggested a comparison model to evaluate the following heterogeneous laboratory research.
Qi Li, Jia Jiang, Isaac K. Afreh, Kelley C. Barsanti, and David R. Cocker III
Atmos. Chem. Phys., 22, 3131–3147, https://doi.org/10.5194/acp-22-3131-2022, https://doi.org/10.5194/acp-22-3131-2022, 2022
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Chamber-derived secondary organic aerosol (SOA) yields from camphene are reported for the first time. The role of peroxy radicals (RO2) was investigated using chemically detailed box models. We observed higher SOA yields (up to 64 %) in the experiments with added NOx than without due to the formation of highly oxygenated organic molecules (HOMs) when
NOx is present. This work can improve the representation of camphene in air quality models and provide insights into other monoterpene studies.
Xiuli Wei, Haosheng Dai, Huaqiao Gui, Jiaoshi Zhang, Yin Cheng, Jie Wang, Yixin Yang, Youwen Sun, and Jianguo Liu
Atmos. Chem. Phys., 22, 3097–3109, https://doi.org/10.5194/acp-22-3097-2022, https://doi.org/10.5194/acp-22-3097-2022, 2022
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We demonstrated the usage of the Fourier transform infrared (FTIR) spectroscopic technique to characterize in real time the hygroscopic growth properties of nanoparticles and their phase transition micro-dynamics at the molecular level. We first realize real-time measurements of water content and dry nanoparticle mass to characterize hygroscopic growth factors. We then identify in real time the hydration interactions and the dynamic hygroscopic growth process of the functional groups.
Zhancong Liang, Yangxi Chu, Masao Gen, and Chak K. Chan
Atmos. Chem. Phys., 22, 3017–3044, https://doi.org/10.5194/acp-22-3017-2022, https://doi.org/10.5194/acp-22-3017-2022, 2022
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The properties and fate of individual airborne particles can be significantly different, leading to distinct environmental impacts (e.g., climate and human health). While many instruments only analyze an ensemble of these particles, single-particle Raman spectroscopy enables unambiguous characterization of individual particles. This paper comprehensively reviews the applications of such a technique in studying atmospheric particles, especially for their physicochemical processing.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
Atmos. Chem. Phys., 22, 1467–1482, https://doi.org/10.5194/acp-22-1467-2022, https://doi.org/10.5194/acp-22-1467-2022, 2022
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The main nighttime sink of α-pinene, a hydrocarbon abundantly emitted by plants, is reaction with NO3 to form nitrooxy peroxy radicals (nRO2). Using uniquely designed chamber experiments, we show that this reaction is a major source of organic aerosol when nRO2 reacts with other nRO2 and forms a nitrooxy hydroperoxide when nRO2 reacts with HO2. Under ambient conditions these pathways are key loss processes of atmospheric reactive nitrogen in areas with mixed biogenic and anthropogenic influence.
Sophia M. Charan, Yuanlong Huang, Reina S. Buenconsejo, Qi Li, David R. Cocker III, and John H. Seinfeld
Atmos. Chem. Phys., 22, 917–928, https://doi.org/10.5194/acp-22-917-2022, https://doi.org/10.5194/acp-22-917-2022, 2022
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In this study, we investigate the secondary organic aerosol formation potential of decamethylcyclopentasiloxane (D5), which is used as a tracer for volatile chemical products and measured in high concentrations both outdoors and indoors. By performing experiments in different types of reactors, we find that D5’s aerosol formation is highly dependent on OH, and, at low OH concentrations or exposures, D5 forms little aerosol. We also reconcile results from other studies.
Beatrix Rosette Go Mabato, Yan Lyu, Yan Ji, Yong Jie Li, Dan Dan Huang, Xue Li, Theodora Nah, Chun Ho Lam, and Chak K. Chan
Atmos. Chem. Phys., 22, 273–293, https://doi.org/10.5194/acp-22-273-2022, https://doi.org/10.5194/acp-22-273-2022, 2022
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Biomass burning (BB) is a global phenomenon that releases large quantities of pollutants such as phenols and aromatic carbonyls into the atmosphere. These compounds can form secondary organic aerosols (SOAs) which play an important role in the Earth’s energy budget. In this work, we demonstrated that the direct irradiation of vanillin (VL) could generate aqueous SOA (aqSOA) such as oligomers. In the presence of nitrate, VL photo-oxidation can also form nitrated compounds.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, M. Rami Alfarra, Thomas J. Bannan, Dawei Hu, Kelly L. Pereira, Jaqueline F. Hamilton, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1080, https://doi.org/10.5194/acp-2021-1080, 2022
Revised manuscript accepted for ACP
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Mixing experiments are crucial and highly beneficial for our understanding on atmospheric chemical interactions. However, the interpretation quickly becomes complex and both the experimental design and evaluation needs to be scrutinised carefully. Advanced online and offline compositional measurements can reveal substantial additional information to aid in the interpretation of yield data, including components uniquely found in mixtures and property changes in the SOA formed from mixtures of VOC.
Zijun Li, Angela Buchholz, Arttu Ylisirniö, Luis Barreira, Liqing Hao, Siegfried Schobesberger, Taina Yli-Juuti, and Annele Virtanen
Atmos. Chem. Phys., 21, 18283–18302, https://doi.org/10.5194/acp-21-18283-2021, https://doi.org/10.5194/acp-21-18283-2021, 2021
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We compared the evolution of two types of secondary organic aerosol (SOA) particles during isothermal evaporation. The sesquiterpene SOA particles demonstrated higher resilience to evaporation than α-pinene SOA particles generated under comparable conditions. In-depth analysis showed that under high-relative-humidity conditions, particulate water drove the evolution of particulate constituents by reducing the particle viscosity and initiating chemical aqueous-phase processes.
András Hoffer, Ádám Tóth, Beatrix Jancsek-Turóczi, Attila Machon, Aida Meiramova, Attila Nagy, Luminita Marmureanu, and András Gelencsér
Atmos. Chem. Phys., 21, 17855–17864, https://doi.org/10.5194/acp-21-17855-2021, https://doi.org/10.5194/acp-21-17855-2021, 2021
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Due to the widespread use of plastics high amounts of waste are burned in households worldwide, emitting vast amounts of PM10 and PAHs into the atmosphere. In this work different types of common plastics were burned in the laboratory with a view to identifying potentially specific tracer compounds and determining their emission factors. The compounds found were also successfully identified in atmospheric PM10 samples, indicating their potential use as ambient tracers for illegal waste burning.
Shijie Liu, Dandan Huang, Yiqian Wang, Si Zhang, Xiaodi Liu, Can Wu, Wei Du, and Gehui Wang
Atmos. Chem. Phys., 21, 17759–17773, https://doi.org/10.5194/acp-21-17759-2021, https://doi.org/10.5194/acp-21-17759-2021, 2021
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A series of chamber experiments was performed to probe the individual and common effects of NH3 and NOx on toluene secondary organic aerosol (SOA) formation through OH photooxidation. The synergetic effects of NH3 and NOx on the toluene SOA concentration and optical absorption were observed. The higher-volatility products formed in the presence of NOx could precipitate into the particle phase when NH3 was added. The formation pathways of N-containing OAs through NOx or NH3 are also discussed.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Daniel A. Knopf and Markus Ammann
Atmos. Chem. Phys., 21, 15725–15753, https://doi.org/10.5194/acp-21-15725-2021, https://doi.org/10.5194/acp-21-15725-2021, 2021
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Adsorption on and desorption of gas molecules from solid or liquid surfaces or interfaces represent the initial interaction of gas-to-condensed-phase processes that can define the physicochemical evolution of the condensed phase. We apply a thermodynamic and microscopic treatment of these multiphase processes to evaluate how adsorption and desorption rates and surface accommodation depend on the choice of adsorption model and standard states with implications for desorption energy and lifetimes.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Zirui Zhang, Wenfei Zhu, Min Hu, Kefan Liu, Hui Wang, Rongzhi Tang, Ruizhe Shen, Ying Yu, Rui Tan, Kai Song, Yuanju Li, Wenbin Zhang, Zhou Zhang, Hongming Xu, Shijin Shuai, Shuangde Li, Yunfa Chen, Jiayun Li, Yuesi Wang, and Song Guo
Atmos. Chem. Phys., 21, 15221–15237, https://doi.org/10.5194/acp-21-15221-2021, https://doi.org/10.5194/acp-21-15221-2021, 2021
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We comprehensively investigated the mass growth potential, oxidation degree, formation pathway, and mass spectra features of typical urban-lifestyle secondary organic aerosols (SOAs) including vehicle SOAs and cooking SOAs. The mass spectra we acquired could provide necessary references to estimate the mass fractions of vehicle and cooking SOAs in the atmosphere, which would greatly decrease the uncertainty in air quality evaluation and health risk assessment in urban areas.
Wenfei Zhu, Song Guo, Zirui Zhang, Hui Wang, Ying Yu, Zheng Chen, Ruizhe Shen, Rui Tan, Kai Song, Kefan Liu, Rongzhi Tang, Yi Liu, Shengrong Lou, Yuanju Li, Wenbin Zhang, Zhou Zhang, Shijin Shuai, Hongming Xu, Shuangde Li, Yunfa Chen, Min Hu, Francesco Canonaco, and Andre S. H. Prévôt
Atmos. Chem. Phys., 21, 15065–15079, https://doi.org/10.5194/acp-21-15065-2021, https://doi.org/10.5194/acp-21-15065-2021, 2021
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The experiments of primary emissions and secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicles) were conducted. The mass spectral features of primary organic aerosol (POA) and SOA were characterized by using a high-resolution time-of-flight aerosol mass spectrometer. This work, for the first time, establishes the vehicle and cooking SOA source profiles and can be further used as source constraints in the OA source apportionment in the ambient atmosphere.
Adam Milsom, Adam M. Squires, Jacob A. Boswell, Nicholas J. Terrill, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 21, 15003–15021, https://doi.org/10.5194/acp-21-15003-2021, https://doi.org/10.5194/acp-21-15003-2021, 2021
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Atmospheric aerosols can be solid, semi-solid or liquid. This phase state may impact key aerosol processes such as oxidation and water uptake, affecting cloud droplet formation and urban air pollution. We have observed a solid crystalline organic phase in a levitated proxy for cooking emissions, oleic acid. Spatially resolved structural changes were followed during ageing by X-ray scattering, revealing phase gradients, aggregate products and a markedly reduced ozonolysis reaction rate.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Tao Cao, Meiju Li, Chunlin Zou, Xingjun Fan, Jianzhong Song, Wanglu Jia, Chiling Yu, Zhiqiang Yu, and Ping'an Peng
Atmos. Chem. Phys., 21, 13187–13205, https://doi.org/10.5194/acp-21-13187-2021, https://doi.org/10.5194/acp-21-13187-2021, 2021
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Brown carbon (BrC) fractions derived from biomass burning and coal combustion including water- and methanol-soluble organic carbon were comprehensively characterized for their optical and chemical properties, as well as oxidative potential. Moreover, the key components or functional groups that were responsible for the reactive oxygen species (ROS) generation capacity of BrC were also discussed. These findings are useful for estimation of their environmental, climate, and health impacts.
Zhen Mu, Qingcai Chen, Lixin Zhang, Dongjie Guan, and Hao Li
Atmos. Chem. Phys., 21, 11581–11591, https://doi.org/10.5194/acp-21-11581-2021, https://doi.org/10.5194/acp-21-11581-2021, 2021
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Sunlight affects the life and chemical composition of atmospheric aerosols and thus alters air quality. This study demonstrated that the photo-aging process not only changed the chemical compositions of chromophoric aerosols but also changed the roles of the chromophoric organic matter in the photo-aging process of aerosol. This study adds to our understanding of how sunlight affects chromophoric aerosol aging.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
Yubo Cheng, Yiqiu Ma, and Di Hu
Atmos. Chem. Phys., 21, 10589–10608, https://doi.org/10.5194/acp-21-10589-2021, https://doi.org/10.5194/acp-21-10589-2021, 2021
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We conducted chemical characterization and source apportionment of PM2.5 in Hong Kong. Secondary formation was the leading contributor to organic carbon (OC) throughout the year. NOx processing played a key role in both daytime and nighttime secondary organic aerosol (SOA) production, and monoterpene SOA was the most abundant. Sulfate was positively related to total and secondary sulfate-related OC, and particle acidity was significantly correlated with SOC from aging of biomass burning.
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., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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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 of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
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Functional group compositions 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.
Jack C. Hensley, Adam W. Birdsall, Gregory Valtierra, Joshua L. Cox, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8809–8821, https://doi.org/10.5194/acp-21-8809-2021, https://doi.org/10.5194/acp-21-8809-2021, 2021
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We measured reactions of butenedial, an atmospheric dicarbonyl, in aqueous mixtures that mimic the conditions of aerosol particles. Major reaction products and rates were determined to assess their atmospheric relevance and to compare against other well-studied dicarbonyls. We suggest that the structure of the carbon backbone, not just the dominant functional group, plays a major role in dicarbonyl reactivity, influencing the fate and ability of dicarbonyls to produce brown carbon.
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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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