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An interactive open-access journal of the European Geosciences Union
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Volume 16, issue 19
Atmos. Chem. Phys., 16, 12767–12792, 2016
https://doi.org/10.5194/acp-16-12767-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-12767-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 16, 12767–12792, 2016
https://doi.org/10.5194/acp-16-12767-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-12767-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
Research article 13 Oct 2016
Research article | 13 Oct 2016
Discontinuities in hygroscopic growth below and above water saturation for laboratory surrogates of oligomers in organic atmospheric aerosols
Natasha Hodas et al.
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Amy P. Sullivan, Natasha Hodas, Barbara J. Turpin, Kate Skog, Frank N. Keutsch, Stefania Gilardoni, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Maria Cristina Facchini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Eiko Nemitz, Marsailidh M. Twigg, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 8095–8108, https://doi.org/10.5194/acp-16-8095-2016, https://doi.org/10.5194/acp-16-8095-2016, 2016
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This paper presents the results from our measurements and approach for the investigation of aqueous secondary organic aerosol (aqSOA) formation in the ambient atmosphere. When local aqSOA formation was observed, a correlation of water-soluble organic carbon with organic aerosol, aerosol liquid water, relative humidity, and aerosol nitrate was found. Key factors of local aqSOA production include air mass stagnation, formation of local nitrate overnight, and significant amounts of ammonia.
N. Hodas, A. Zuend, W. Mui, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 15, 5027–5045, https://doi.org/10.5194/acp-15-5027-2015, https://doi.org/10.5194/acp-15-5027-2015, 2015
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-973, https://doi.org/10.5194/acp-2020-973, 2020
Preprint under review for ACP
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction (RF) of •OH among detected radicals, but negatively correlated with the RF of C-centered radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1000, https://doi.org/10.5194/acp-2020-1000, 2020
Preprint under review for ACP
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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 and either adsorption or desorption can be the controlling process. 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.
Hoi Ki Lam, Rongshuang Xu, Jack Choczynski, James F. Davies, Dongwan Ham, Mijung Song, Andreas Zuend, Wentao Li, Ying-Lung Steve Tse, and Man Nin Chan
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-900, https://doi.org/10.5194/acp-2020-900, 2020
Preprint under review for ACP
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This work demonstrates that organic compounds present at or near the surface of aerosols can be subjected to oxidation initiated by gas-phase oxidants, such as hydroxyl radicals (OH). The reactivity is sensitive to their surface concentrations, which are determined by the phase separation behavior. This results of this work emphasize the effects of phase separation and potentially distinct aerosol morphologies on the chemical transformation of atmospheric aerosols.
Dana L. McGuffin, Yuanlong Huang, Richard C. Flagan, Tuukka Petäjä, B. Erik Ydstie, and Peter J. Adams
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-281, https://doi.org/10.5194/gmd-2020-281, 2020
Preprint under review for GMD
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus Petters
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-768, https://doi.org/10.5194/acp-2020-768, 2020
Preprint under review for ACP
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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 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.
Weigang Wang, Ting Lei, Andreas Zuend, Hang Su, Yafang Cheng, Yajun Shi, Maofa Ge, and Mingyuan Liu
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-632, https://doi.org/10.5194/acp-2020-632, 2020
Preprint under review for ACP
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Aerosol mixing state regulates the interactions between water molecules and particles and thus controls the aerosol activation and hygroscopic growth, which thereby influences the visibility degradation, cloud formation, and its radiative forcing. However, there are only very few studies attempting to investigate their interactions with water molecules. Here, we investigated the effect of organic coatings on the hygroscopic behavior of the inorganic core.
Liqiang Wang, Shaocai Yu, Pengfei Li, Xue Chen, Zhen Li, Yibo Zhang, Mengying Li, Khalid Mehmood, Weiping Liu, Tianfeng Chai, Yannian Zhu, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-510, https://doi.org/10.5194/acp-2020-510, 2020
Revised manuscript accepted for ACP
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The China government has made major strides in curbing anthropogenic emissions. In this study, we constrain a state-of-the-art CTM by a reliable data assimilation method with extensive chemical and meteorological observations. This comprehensive technical design provides a crucial advance in isolating the influences of emission changes and meteorological perturbations over the Yangtze River Delta (YRD) from 2016 to 2019, thus establishing the first map of the PM2.5 mitigation across the YRD.
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.
Brigitte Rooney, Yuan Wang, Jonathan H. Jiang, Bin Zhao, Zhao-Cheng Zeng, and John H. Seinfeld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-541, https://doi.org/10.5194/acp-2020-541, 2020
Revised manuscript accepted for ACP
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Wildfires have become increasingly prevalent. Intense smoke consisting of particulate matter (PM) leads to an increased risk of morbidity and mortality. The record-breaking Camp Fire ravaged northern California for two weeks in 2018. Here, we employ a comprehensive chemical transport model along with ground-based and satellite observations to characterize the PM concentrations across northern California and to investigate the pollution sensitivity predictions to key parameters of the model.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-536, https://doi.org/10.5194/acp-2020-536, 2020
Preprint under review for ACP
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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.
Alexander B. MacDonald, Ali Hossein Mardi, Hossein Dadashazar, Mojtaba Azadi Aghdam, Ewan Crosbie, Haflidi H. Jonsson, Richard C. Flagan, John H. Seinfeld, and Armin Sorooshian
Atmos. Chem. Phys., 20, 7645–7665, https://doi.org/10.5194/acp-20-7645-2020, https://doi.org/10.5194/acp-20-7645-2020, 2020
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Understanding how humans affect Earth's climate requires understanding of how particles in the air affect the number concentration of droplets in a cloud (Nd). We use the air-equivalent mass concentration of different chemical species contained in cloud water to predict Nd. In this study we found that the prediction of Nd is (1) best described by total sulfate; (2) improved when considering up to five species; and (3) dependent on factors like turbulence, smoke presence, and in-cloud height.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Sophia M. Charan, Reina S. Buenconsejo, and John H. Seinfeld
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-492, https://doi.org/10.5194/acp-2020-492, 2020
Revised manuscript accepted for ACP
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In urban areas, the emissions from volatile chemical products may be responsible for the formation of as much particulate matter as motor vehicles. Since exposure to particulate matter is a public health crisis, understanding its formation is critical. In this work we investigate the secondary organic aerosol formation potential of benzyl alcohol, an important compound that is representative of some of these new emission sources, and find that more particulate matter forms than is expected.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Natalie R. Gervasi, David O. Topping, and Andreas Zuend
Atmos. Chem. Phys., 20, 2987–3008, https://doi.org/10.5194/acp-20-2987-2020, https://doi.org/10.5194/acp-20-2987-2020, 2020
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Organic aerosols have been shown to exist often in a semi-solid or amorphous, glassy state. Highly viscous particles behave differently than their well-mixed liquid analogues with consequences for a variety of aerosol processes. Here, we introduce a new predictive mixture viscosity model called AIOMFAC-VISC. It enables us to predict the viscosity of aqueous organic mixtures as a function of temperature and chemical composition, covering the full range of liquid, semi-solid, and glassy states.
Khalid Mehmood, Yujie Wu, Liqiang Wang, Shaocai Yu, Pengfei Li, Xue Chen, Zhen Li, Yibo Zhang, Mengying Li, Weiping Liu, Yuesi Wang, Zirui Liu, Yannian Zhu, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 20, 2419–2443, https://doi.org/10.5194/acp-20-2419-2020, https://doi.org/10.5194/acp-20-2419-2020, 2020
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We selected June 2014 as our study period, which exhibited a complete evolution process of open biomass burning (OBB) dominated by open crop straw burning (OCSB) over central and eastern China (CEC). We established a constraining method that integrates ground-based PM2.5 measurements with the two-way coupled WRF-CMAQ model to derive optimal OBB emissions. It was found that these emissions could allow the model to reproduce meteorological and chemical fields over CEC during the study period.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-55, https://doi.org/10.5194/acp-2020-55, 2020
Revised manuscript accepted for ACP
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This manuscript presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modelling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas-particle partitioning and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Kyle Gorkowski, Thomas C. Preston, and Andreas Zuend
Atmos. Chem. Phys., 19, 13383–13407, https://doi.org/10.5194/acp-19-13383-2019, https://doi.org/10.5194/acp-19-13383-2019, 2019
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We present the new Binary Activity Thermodynamics (BAT) model, which is a water-sensitive reduced-complexity organic aerosol thermodynamics model. It can use bulk properties like O : C, molar mass, and RH to predict organic activity coefficients and water uptake behavior. We show applications in RH-dependent organic co-condensation, liquid–liquid phase separation, and Kohler curve predictions, and we validate the BAT model against laboratory measurements.
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.
Hoi Ki Lam, Sze Man Shum, James F. Davies, Mijung Song, Andreas Zuend, and Man Nin Chan
Atmos. Chem. Phys., 19, 9581–9593, https://doi.org/10.5194/acp-19-9581-2019, https://doi.org/10.5194/acp-19-9581-2019, 2019
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We show the presence of dissolved inorganic salts could reduce the overall heterogeneous reactivity of organic compounds with gas–phase OH radicals at the surface by lowering the surface concentration of organic compounds. Until recently, the kinetic parameters reported in the literature were mostly measured based on experiments with pure organic particles. The lifetime of organic compounds or chemical tracers against heterogeneous OH reaction in the atmosphere could be longer than expected.
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.
Rebecca H. Schwantes, Sophia M. Charan, Kelvin H. Bates, Yuanlong Huang, Tran B. Nguyen, Huajun Mai, Weimeng Kong, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 19, 7255–7278, https://doi.org/10.5194/acp-19-7255-2019, https://doi.org/10.5194/acp-19-7255-2019, 2019
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Oxidation of isoprene, the dominant non-methane biogenic volatile organic compound emitted into the atmosphere, is a significant source of secondary organic aerosol (SOA). Here formation of SOA from isoprene oxidation by the hydroxyl radical (OH) under high-NO conditions is measured. This work improves our understanding of isoprene SOA formation by demonstrating that low-volatility compounds formed under high-NO conditions produce significantly more aerosol than previously thought.
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.
James F. Davies, Andreas Zuend, and Kevin R. Wilson
Atmos. Chem. Phys., 19, 2933–2946, https://doi.org/10.5194/acp-19-2933-2019, https://doi.org/10.5194/acp-19-2933-2019, 2019
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The formation of cloud droplets involves the condensation of water onto preexisting particles in the atmosphere. The efficiency of this process depends on the nature of the particles, and recent work has shown that organic-rich particles may exhibit a suppressed surface tension that promotes the formation of cloud droplets. In this technical note, we discuss the mechanism for this and highlight the evolution of surface tension as the key factor in the extent of surface effects.
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.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
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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.
Ting Lei, Andreas Zuend, Yafang Cheng, Hang Su, Weigang Wang, and Maofa Ge
Atmos. Chem. Phys., 18, 1045–1064, https://doi.org/10.5194/acp-18-1045-2018, https://doi.org/10.5194/acp-18-1045-2018, 2018
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Measurements and thermodynamic equilibrium predictions for organic–inorganic aerosols related to components from biomass burning emissions demonstrate a diversity of hygroscopic growth and shrinking behavior, which we observed using a hygroscopicity tandem differential mobility analyzer (HTDMA). Controlled laboratory experiments with single solutes and/or with mixed organic–inorganic systems of known phase state will be useful to constrain model parameters of thermodynamic equilibrium models.
Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, António Dias, Neil M. Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, and Peter H. McMurry
Atmos. Chem. Phys., 18, 845–863, https://doi.org/10.5194/acp-18-845-2018, https://doi.org/10.5194/acp-18-845-2018, 2018
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A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
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.
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.
Rebecca H. Schwantes, Katherine A. Schilling, Renee C. McVay, Hanna Lignell, Matthew M. Coggon, Xuan Zhang, Paul O. Wennberg, and John H. Seinfeld
Atmos. Chem. Phys., 17, 3453–3474, https://doi.org/10.5194/acp-17-3453-2017, https://doi.org/10.5194/acp-17-3453-2017, 2017
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Toluene, one of the principle aromatic compounds present in the atmosphere, is oxidized by OH to produce cresol and other products. Here later-generation low-volatility oxygenated products from cresol oxidation by OH are detected in the gas and particle phases. This work identifies a simple and significant mechanism for toluene secondary organic aerosol formation through the cresol pathway. Likely the phenolic pathway of other aromatic compounds is also important for secondary organic aerosol.
Yuanlong Huang, Matthew M. Coggon, Ran Zhao, Hanna Lignell, Michael U. Bauer, Richard C. Flagan, and John H. Seinfeld
Atmos. Meas. Tech., 10, 839–867, https://doi.org/10.5194/amt-10-839-2017, https://doi.org/10.5194/amt-10-839-2017, 2017
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We report on the development of a new laminar flow tube reactor for the study of gas-phase atmospheric chemistry and secondary organic aerosol formation. The present paper is devoted to the design and fluid dynamical characterization of the reactor. The results of gas and particle residence time distribution experiments in the reactor, together with an evaluation of the effect of non-isothermal conditions, are reported.
Theodora Nah, Renee C. McVay, Jeffrey R. Pierce, John H. Seinfeld, and Nga L. Ng
Atmos. Chem. Phys., 17, 2297–2310, https://doi.org/10.5194/acp-17-2297-2017, https://doi.org/10.5194/acp-17-2297-2017, 2017
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We present a model framework that accounts for coagulation in chamber studies where high seed aerosol surface area concentrations are used. The uncertainties in the calculated SOA mass concentrations and yields between four different particle-wall loss correction methods over the series of α-pinene ozonolysis experiments are also assessed. We show that SOA mass yields calculated by the four methods can deviate significantly in studies where high seed aerosol surface area concentrations are used.
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.
Theodora Nah, Renee C. McVay, Xuan Zhang, Christopher M. Boyd, John H. Seinfeld, and Nga L. Ng
Atmos. Chem. Phys., 16, 9361–9379, https://doi.org/10.5194/acp-16-9361-2016, https://doi.org/10.5194/acp-16-9361-2016, 2016
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The influence of seed aerosol surface area and oxidation rate on SOA formation in α-pinene ozonolysis is studied. SOA growth rate and mass yields are independent of seed surface area, consistent with the condensation of SOA-forming vapors being dominated by quasi-equilibrium growth. Faster α-pinene oxidation rates and higher SOA mass yields are observed at increasing O3 concentrations, indicating that a faster α-pinene oxidation rate leads to rapidly produced SOA-forming oxidation products.
Amy P. Sullivan, Natasha Hodas, Barbara J. Turpin, Kate Skog, Frank N. Keutsch, Stefania Gilardoni, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Maria Cristina Facchini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Eiko Nemitz, Marsailidh M. Twigg, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 8095–8108, https://doi.org/10.5194/acp-16-8095-2016, https://doi.org/10.5194/acp-16-8095-2016, 2016
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This paper presents the results from our measurements and approach for the investigation of aqueous secondary organic aerosol (aqSOA) formation in the ambient atmosphere. When local aqSOA formation was observed, a correlation of water-soluble organic carbon with organic aerosol, aerosol liquid water, relative humidity, and aerosol nitrate was found. Key factors of local aqSOA production include air mass stagnation, formation of local nitrate overnight, and significant amounts of ammonia.
Alessandro Franchin, Andy Downard, Juha Kangasluoma, Tuomo Nieminen, Katrianne Lehtipalo, Gerhard Steiner, Hanna E. Manninen, Tuukka Petäjä, Richard C. Flagan, and Markku Kulmala
Atmos. Meas. Tech., 9, 2709–2720, https://doi.org/10.5194/amt-9-2709-2016, https://doi.org/10.5194/amt-9-2709-2016, 2016
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High transmission efficiency is key for classifying and counting atmospheric aerosol below 10 nm. We developed a new high-transmission inlet for the Caltech nano-radial DMA (nRDMA) and successfully deployed the nRDMA, equipped with the new inlet, in chamber measurements, using a particle size magnifier (PSM) and a booster CPC as a counter. With this setup, we were able to measure size distributions of ions between 1.3 and 6 nm in mobility diameter.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
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
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
Renee C. McVay, Xuan Zhang, Bernard Aumont, Richard Valorso, Marie Camredon, Yuyi S. La, Paul O. Wennberg, and John H. Seinfeld
Atmos. Chem. Phys., 16, 2785–2802, https://doi.org/10.5194/acp-16-2785-2016, https://doi.org/10.5194/acp-16-2785-2016, 2016
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Secondary organic aerosol (SOA) affects climate change, human health, and cloud formation. We examine SOA formation from the biogenic hydrocarbon α-pinene and observe unexpected experimental results that run contrary to model predictions. Various processes are explored via modeling to rationalize the observations. The paper identifies the importance of further constraining via experiments various steps in the chemical mechanism in order to accurately predict SOA worldwide.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Atmos. Chem. Phys., 16, 2309–2322, https://doi.org/10.5194/acp-16-2309-2016, https://doi.org/10.5194/acp-16-2309-2016, 2016
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Multi-generational chemistry schemes applied in regional models do not increase secondary organic aerosol (SOA) mass production relative to traditional "two-product" schemes when both models are fitted to the same chamber data. The multi-generational chemistry schemes do change the predicted composition of SOA and the source attribution of SOA.
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.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
G. Gržinić, T. Bartels-Rausch, T. Berkemeier, A. Türler, and M. Ammann
Atmos. Chem. Phys., 15, 13615–13625, https://doi.org/10.5194/acp-15-13615-2015, https://doi.org/10.5194/acp-15-13615-2015, 2015
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The heterogeneous loss of dinitrogen pentoxide (N2O5) to citric acid aerosol, a proxy for highly oxygenated secondary organic aerosol, is shown to be substantially lower than to other aqueous organic aerosol proxies investigated previously. This is attributed to the widely changing viscosity within the atmospherically relevant humidity range. It may explain some of the unexpectedly low loss rates of N2O5 to aerosol particles derived from field studies.
A. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
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).
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Geosci. Model Dev., 8, 2553–2567, https://doi.org/10.5194/gmd-8-2553-2015, https://doi.org/10.5194/gmd-8-2553-2015, 2015
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Multi-generational oxidation of organic vapors can significantly alter the mass, chemical composition and properties of secondary organic aerosol (SOA). Here, we implement a semi-explicit, constrained multi-generational oxidation model of Cappa and Wilson (2012) in a 3-D air quality model. When compared with results from a current-generation SOA model, we predict similar mass concentrations of SOA but a different chemical composition. O:C ratios of SOA are in line with those measured globally.
M. J. Alvarado, C. R. Lonsdale, R. J. Yokelson, S. K. Akagi, H. Coe, J. S. Craven, E. V. Fischer, G. R. McMeeking, J. H. Seinfeld, T. Soni, J. W. Taylor, D. R. Weise, and C. E. Wold
Atmos. Chem. Phys., 15, 6667–6688, https://doi.org/10.5194/acp-15-6667-2015, https://doi.org/10.5194/acp-15-6667-2015, 2015
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Being able to understand and simulate the chemical evolution of biomass burning smoke plumes under a wide variety of conditions is a critical part of forecasting the impact of these fires on air quality, atmospheric composition, and climate. Here we use an improved model of this chemistry to simulate the evolution of ozone and secondary organic aerosol within a young biomass burning smoke plume from the Williams prescribed burn in chaparral, which was sampled over California in November 2009.
E. Jung, B. A. Albrecht, H. H. Jonsson, Y.-C. Chen, J. H. Seinfeld, A. Sorooshian, A. R. Metcalf, S. Song, M. Fang, and L. M. Russell
Atmos. Chem. Phys., 15, 5645–5658, https://doi.org/10.5194/acp-15-5645-2015, https://doi.org/10.5194/acp-15-5645-2015, 2015
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To study the effect of giant cloud condensation nuclei (GCCN) on precipitation processes in stratocumulus clouds, 1-10 µm diameter salt particles were released from an aircraft while flying near the cloud top off the central coast of California. The analyses suggest that GCCN result in a four-fold increase in the cloud base rainfall rate and depletion of the cloud water due to rainout.
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
N. Hodas, A. Zuend, W. Mui, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 15, 5027–5045, https://doi.org/10.5194/acp-15-5027-2015, https://doi.org/10.5194/acp-15-5027-2015, 2015
X. Zhang, R. H. Schwantes, R. C. McVay, H. Lignell, M. M. Coggon, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 15, 4197–4214, https://doi.org/10.5194/acp-15-4197-2015, https://doi.org/10.5194/acp-15-4197-2015, 2015
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We present an experimental protocol to constrain the nature of organic vapor--wall deposition in Teflon chambers and develop an empirical model to predict the wall-induced deposition rate of intermediate/semi/non-volatility organic vapors in chambers.
G. Ganbavale, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 15, 447–493, https://doi.org/10.5194/acp-15-447-2015, https://doi.org/10.5194/acp-15-447-2015, 2015
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This study presents a new, improved parameterisation of the temperature dependence of activity coefficients implemented in the AIOMFAC group-contribution model. The AIOMFAC model with the improved parameterisation is applicable for a large variety of aqueous organic as well as water-free organic solutions of relevance for atmospheric aerosols. The new model parameters were determined based on published and new thermodynamic equilibrium data covering a temperature range from ~190 to 440 K.
T. B. Nguyen, J. D. Crounse, R. H. Schwantes, A. P. Teng, K. H. Bates, X. Zhang, J. M. St. Clair, W. H. Brune, G. S. Tyndall, F. N. Keutsch, J. H. Seinfeld, and P. O. Wennberg
Atmos. Chem. Phys., 14, 13531–13549, https://doi.org/10.5194/acp-14-13531-2014, https://doi.org/10.5194/acp-14-13531-2014, 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.
T. Lei, A. Zuend, W. G. Wang, Y. H. Zhang, and M. F. Ge
Atmos. Chem. Phys., 14, 11165–11183, https://doi.org/10.5194/acp-14-11165-2014, https://doi.org/10.5194/acp-14-11165-2014, 2014
J. D. Fast, J. Allan, R. Bahreini, J. Craven, L. Emmons, R. Ferrare, P. L. Hayes, A. Hodzic, J. Holloway, C. Hostetler, J. L. Jimenez, H. Jonsson, S. Liu, Y. Liu, A. Metcalf, A. Middlebrook, J. Nowak, M. Pekour, A. Perring, L. Russell, A. Sedlacek, J. Seinfeld, A. Setyan, J. Shilling, M. Shrivastava, S. Springston, C. Song, R. Subramanian, J. W. Taylor, V. Vinoj, Q. Yang, R. A. Zaveri, and Q. Zhang
Atmos. Chem. Phys., 14, 10013–10060, https://doi.org/10.5194/acp-14-10013-2014, https://doi.org/10.5194/acp-14-10013-2014, 2014
G. Ganbavale, C. Marcolli, U. K. Krieger, A. Zuend, G. Stratmann, and T. Peter
Atmos. Chem. Phys., 14, 9993–10012, https://doi.org/10.5194/acp-14-9993-2014, https://doi.org/10.5194/acp-14-9993-2014, 2014
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
R. A. Zaveri, R. C. Easter, J. E. Shilling, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, https://doi.org/10.5194/acp-14-5153-2014, 2014
T. B. Nguyen, M. M. Coggon, K. H. Bates, X. Zhang, R. H. Schwantes, K. A. Schilling, C. L. Loza, R. C. Flagan, P. O. Wennberg, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 3497–3510, https://doi.org/10.5194/acp-14-3497-2014, https://doi.org/10.5194/acp-14-3497-2014, 2014
R. Zhang, T. Duhl, M. T. Salam, J. M. House, R. C. Flagan, E. L. Avol, F. D. Gilliland, A. Guenther, S. H. Chung, B. K. Lamb, and T. M. VanReken
Biogeosciences, 11, 1461–1478, https://doi.org/10.5194/bg-11-1461-2014, https://doi.org/10.5194/bg-11-1461-2014, 2014
J. J. Ensberg, P. L. Hayes, J. L. Jimenez, J. B. Gilman, W. C. Kuster, J. A. de Gouw, J. S. Holloway, T. D. Gordon, S. Jathar, A. L. Robinson, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, https://doi.org/10.5194/acp-14-2383-2014, 2014
X. Zhang, R. H. Schwantes, M. M. Coggon, C. L. Loza, K. A. Schilling, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1733–1753, https://doi.org/10.5194/acp-14-1733-2014, https://doi.org/10.5194/acp-14-1733-2014, 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
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
L. D. Yee, J. S. Craven, C. L. Loza, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 11121–11140, https://doi.org/10.5194/acp-13-11121-2013, https://doi.org/10.5194/acp-13-11121-2013, 2013
A. Wonaschütz, M. Coggon, A. Sorooshian, R. Modini, A. A. Frossard, L. Ahlm, J. Mülmenstädt, G. C. Roberts, L. M. Russell, S. Dey, F. J. Brechtel, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 9819–9835, https://doi.org/10.5194/acp-13-9819-2013, https://doi.org/10.5194/acp-13-9819-2013, 2013
L. D. Yee, K. E. Kautzman, C. L. Loza, K. A. Schilling, M. M. Coggon, P. S. Chhabra, M. N. Chan, A. W. H. Chan, S. P. Hersey, J. D. Crounse, P. O. Wennberg, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 8019–8043, https://doi.org/10.5194/acp-13-8019-2013, https://doi.org/10.5194/acp-13-8019-2013, 2013
H. Jiang, H. Liao, H. O. T. Pye, S. Wu, L. J. Mickley, J. H. Seinfeld, and X. Y. Zhang
Atmos. Chem. Phys., 13, 7937–7960, https://doi.org/10.5194/acp-13-7937-2013, https://doi.org/10.5194/acp-13-7937-2013, 2013
T. Berkemeier, A. J. Huisman, M. Ammann, M. Shiraiwa, T. Koop, and U. Pöschl
Atmos. Chem. Phys., 13, 6663–6686, https://doi.org/10.5194/acp-13-6663-2013, https://doi.org/10.5194/acp-13-6663-2013, 2013
A. J. Huisman, U. K. Krieger, A. Zuend, C. Marcolli, and T. Peter
Atmos. Chem. Phys., 13, 6647–6662, https://doi.org/10.5194/acp-13-6647-2013, https://doi.org/10.5194/acp-13-6647-2013, 2013
X. Zhang and J. H. Seinfeld
Atmos. Chem. Phys., 13, 5907–5926, https://doi.org/10.5194/acp-13-5907-2013, https://doi.org/10.5194/acp-13-5907-2013, 2013
T. R. Duhl, R. Zhang, A. Guenther, S. H. Chung, M. T. Salam, J. M. House, R. C. Flagan, E. L. Avol, F. D. Gilliland, B. K. Lamb, T. M. VanReken, Y. Zhang, and E. Salathé
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmdd-6-2325-2013, https://doi.org/10.5194/gmdd-6-2325-2013, 2013
Revised manuscript not accepted
C. D. Cappa, X. Zhang, C. L. Loza, J. S. Craven, L. D. Yee, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 1591–1606, https://doi.org/10.5194/acp-13-1591-2013, https://doi.org/10.5194/acp-13-1591-2013, 2013
J. S. Craven, L. D. Yee, N. L. Ng, M. R. Canagaratna, C. L. Loza, K. A. Schilling, R. L. N. Yatavelli, J. A. Thornton, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 12, 11795–11817, https://doi.org/10.5194/acp-12-11795-2012, https://doi.org/10.5194/acp-12-11795-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
The ice-nucleating activity of Arctic sea surface microlayer samples and marine algal cultures
Comparing secondary organic aerosol (SOA) volatility distributions derived from isothermal SOA particle evaporation data and FIGAERO–CIMS measurements
Laboratory studies of fresh and aged biomass burning aerosol emitted from east African biomass fuels – Part 1: Optical properties
Enhanced growth rate of atmospheric particles from sulfuric acid
Composition and volatility of secondary organic aerosol (SOA) formed from oxidation of real tree emissions compared to simplified volatile organic compound (VOC) systems
Effects of SO2 on optical properties of secondary organic aerosol generated from photooxidation of toluene under different relative humidity conditions
Influence of the dry aerosol particle size distribution and morphology on the cloud condensation nuclei activation. An experimental and theoretical investigation
Experimental investigation into the volatilities of highly oxygenated organic molecules (HOMs)
Detection of tar brown carbon with a single particle soot photometer (SP2)
Complex refractive indices and single-scattering albedo of global dust aerosols in the shortwave spectrum and relationship to size and iron content
Technical note: Frenkel, Halsey and Hill analysis of water on clay minerals: toward closure between cloud condensation nuclei activity and water adsorption
Liquid–liquid phase separation and viscosity within secondary organic aerosol generated from diesel fuel vapors
Laboratory study of the heterogeneous ice nucleation on black-carbon-containing aerosol
Specifying the light-absorbing properties of aerosol particles in fresh snow samples, collected at the Environmental Research Station Schneefernerhaus (UFS), Zugspitze
Optimization of process models for determining volatility distribution and viscosity of organic aerosols from isothermal particle evaporation data
Inversely modeling homogeneous H2SO4 − H2O nucleation rate in exhaust-related conditions
The importance of crystalline phases in ice nucleation by volcanic ash
Heterogeneous ice nucleation properties of natural desert dust particles coated with a surrogate of secondary organic aerosol
Cloud condensation nuclei activity of six pollenkitts and the influence of their surface activity
Links of climate variability in Arctic sea ice, Eurasian teleconnection pattern and summer surface ozone pollution in North China
The effect of hydrophobic glassy organic material on the cloud condensation nuclei activity of particles with different morphologies
Technical note: The role of evolving surface tension in the formation of cloud droplets
Physical properties of secondary photochemical aerosol from OH oxidation of a cyclic siloxane
Cloud droplet activation of secondary organic aerosol is mainly controlled by molecular weight, not water solubility
Production of particulate brown carbon during atmospheric aging of residential wood-burning emissions
Evaluating the performance of two surface layer schemes for the momentum and heat exchange processes during severe haze pollution in Jing-Jin-Ji in eastern China
Measured particle water uptake enhanced by co-condensing vapours
Cloud droplet activation of black carbon particles coated with organic compounds of varying solubility
Measurement and modeling of the multiwavelength optical properties of uncoated flame-generated soot
Liquid–liquid phase separation in organic particles containing one and two organic species: importance of the average O : C
Establishing the impact of model surfactants on cloud condensation nuclei activity of sea spray aerosol mimics
Morphological transformation of soot: investigation of microphysical processes during the condensation of sulfuric acid and limonene ozonolysis product vapors
Experimental study of H2SO4 aerosol nucleation at high ionization levels
Determination of the refractive index of insoluble organic extracts from atmospheric aerosol over the visible wavelength range using optical tweezers
Hygroscopic behavior of atmospheric aerosols containing nitrate salts and water-soluble organic acids
Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China
Investigating biomass burning aerosol morphology using a laser imaging nephelometer
Resolving nanoparticle growth mechanisms from size- and time-dependent growth rate analysis
A detailed characterization of the Saharan dust collected during the Fennec campaign in 2011: in situ ground-based and laboratory measurements
Hygroscopicity of organic surrogate compounds from biomass burning and their effect on the efflorescence of ammonium sulfate in mixed aerosol particles
New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model
The role of ions in new particle formation in the CLOUD chamber
Potential influences of neglecting aerosol effects on the NCEP GFS precipitation forecast
Emission characteristics of refractory black carbon aerosols from fresh biomass burning: a perspective from laboratory experiments
Re-evaluating black carbon in the Himalayas and the Tibetan Plateau: concentrations and deposition
Leipzig Ice Nucleation chamber Comparison (LINC): intercomparison of four online ice nucleation counters
Water uptake by fresh Indonesian peat burning particles is limited by water-soluble organic matter
A complete parameterisation of the relative humidity and wavelength dependence of the refractive index of hygroscopic inorganic aerosol particles
The effect of hydroxyl functional groups and molar mass on the viscosity of non-crystalline organic and organic–water particles
Diffusivity measurements of volatile organics in levitated viscous aerosol particles
Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
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The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
Olli-Pekka Tikkanen, Angela Buchholz, Arttu Ylisirniö, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 20, 10441–10458, https://doi.org/10.5194/acp-20-10441-2020, https://doi.org/10.5194/acp-20-10441-2020, 2020
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We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
Damon M. Smith, Marc N. Fiddler, Rudra P. Pokhrel, and Solomon Bililign
Atmos. Chem. Phys., 20, 10149–10168, https://doi.org/10.5194/acp-20-10149-2020, https://doi.org/10.5194/acp-20-10149-2020, 2020
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Biomass burning aerosol can scatter and absorb light, contributing to the cooling or warming of the planet. The scattering and absorption properties (optical properties) change as aerosol ages and interacts with atmospheric gases. Optical properties also depend on burning conditions, fuel type, and morphology. Africa is a major source of biomass burning aerosols, but there are very few laboratory studies. This study focuses on the optical properties of aerosols from east African biomass fuels.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
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.
Wenyu Zhang, Weigang Wang, Junling Li, Chao Peng, Kun Li, Li Zhou, Bo Shi, Yan Chen, Mingyuan Liu, and Maofa Ge
Atmos. Chem. Phys., 20, 4477–4492, https://doi.org/10.5194/acp-20-4477-2020, https://doi.org/10.5194/acp-20-4477-2020, 2020
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We investigated the effect of SO2 under different humidities on optical properties of toluene-derived SOA under four conditions with CRDs and PAX at 532 and 375 nm, respectively. Our results showed that SO2 under different humidities can change the refractive complex index of toluene SOA by influencing the multiphase processes and altering the aerosol chemical compositions. Different atmospheric conditions could affect the properties of toluene SOA, as well as the global radiative balance.
Junteng Wu, Alessandro Faccinetto, Symphorien Grimonprez, Sébastien Batut, Jérôme Yon, Pascale Desgroux, and Denis Petitprez
Atmos. Chem. Phys., 20, 4209–4225, https://doi.org/10.5194/acp-20-4209-2020, https://doi.org/10.5194/acp-20-4209-2020, 2020
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Soot particles released during anthropogenic activities may lead to positive direct or negative indirect climate forcing depending on their aging in the atmosphere. The latter occurs whenever soot particles act as cloud condensation nuclei (CCN) and trigger the formation of persistent clouds. Herein, we investigate the impact of the size distribution and morphology of freshly emitted soot particles on their aging process and propose a model to quantitatively predict their efficiency as CCN.
Otso Peräkylä, Matthieu Riva, Liine Heikkinen, Lauriane Quéléver, Pontus Roldin, and Mikael Ehn
Atmos. Chem. Phys., 20, 649–669, https://doi.org/10.5194/acp-20-649-2020, https://doi.org/10.5194/acp-20-649-2020, 2020
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Highly oxygenated organic molecules have been suggested to form a large part of secondary organic aerosol. However, with their exotic structures, their volatilities are not well known, making their exact role in particle formation hard to assess. In laboratory experiments, we found the volatility of HOMs formed in the ozonolysis of the monoterpene alpha-pinene to be in the middle of earlier estimates. The volatilities of HOMs could be well explained in terms of their molecular formulae.
Joel C. Corbin and Martin Gysel-Beer
Atmos. Chem. Phys., 19, 15673–15690, https://doi.org/10.5194/acp-19-15673-2019, https://doi.org/10.5194/acp-19-15673-2019, 2019
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We review the literature to refine the definition of "tar balls" (or tar particles). Then, using a marine-engine data set, we show that a standard SP2 can identify tar particles in two ways, as evaporating and non-incandescing (30 % of tar particles by number) or incandescing particles which scatter more light than soot at incandescence (70 % of tar particles by number). To our knowledge, no other technique can provide in situ, real-time evidence for the presence of tar particles in an aerosol.
Claudia Di Biagio, Paola Formenti, Yves Balkanski, Lorenzo Caponi, Mathieu Cazaunau, Edouard Pangui, Emilie Journet, Sophie Nowak, Meinrat O. Andreae, Konrad Kandler, Thuraya Saeed, Stuart Piketh, David Seibert, Earle Williams, and Jean-François Doussin
Atmos. Chem. Phys., 19, 15503–15531, https://doi.org/10.5194/acp-19-15503-2019, https://doi.org/10.5194/acp-19-15503-2019, 2019
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This paper presents a new dataset of laboratory measurements of the shortwave (SW) spectral complex refractive index and single-scattering albedo (SSA) for global mineral dust aerosols of varying origin and composition. Our results show that the dust refractive index and SSA vary strongly from source to source, mostly due to particle iron content changes. We recommend that source-dependent values of the SW spectral refractive index and SSA be used in models and remote sensing applications.
Courtney D. Hatch, Paul R. Tumminello, Megan A. Cassingham, Ann L. Greenaway, Rebecca Meredith, and Matthew J. Christie
Atmos. Chem. Phys., 19, 13581–13589, https://doi.org/10.5194/acp-19-13581-2019, https://doi.org/10.5194/acp-19-13581-2019, 2019
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Atmospheric mineral dust has been identified as an important contributor to cloud formation and cloud properties that influence the Earth's climate, yet experimental measurements of climate model parameters currently disagree. This study demonstrates current best practices for analyzing water adsorption measurements, resulting in significantly improved agreement among experimental practices. As such, more accurate parameters can be used to improve simulations of aerosol climate effects.
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
Leonid Nichman, Martin Wolf, Paul Davidovits, Timothy B. Onasch, Yue Zhang, Doug R. Worsnop, Janarjan Bhandari, Claudio Mazzoleni, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 12175–12194, https://doi.org/10.5194/acp-19-12175-2019, https://doi.org/10.5194/acp-19-12175-2019, 2019
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Previous studies showed widespread ice nucleation activity of soot. In this systematic study we investigated the factors that affect the heterogeneous ice nucleation activity of soot surrogates in the cirrus cloud regime. Our observations are consistent with an ice nucleation mechanism of pore condensation followed by freezing. The results show significant variations in ice nucleation activity as a function of size, morphology, and surface chemistry of the black-carbon-containing particles.
Martin Schnaiter, Claudia Linke, Inas Ibrahim, Alexei Kiselev, Fritz Waitz, Thomas Leisner, Stefan Norra, and Till Rehm
Atmos. Chem. Phys., 19, 10829–10844, https://doi.org/10.5194/acp-19-10829-2019, https://doi.org/10.5194/acp-19-10829-2019, 2019
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When combustion particles are deposited to the ground, they darken Earth's snow and ice surfaces by even tiny quantities. This darkening reduces the back reflection of sunlight and induces an additional climate warming. Particles from fresh snow samples were investigated according to their light absorption strength. Enhanced absorption was found in the snow that cannot fully be attributed to combustion particles. Dust and biogenic matter are likely the cause of this additional snow darkening.
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.
Miska Olin, Jenni Alanen, Marja R. T. Palmroth, Topi Rönkkö, and Miikka Dal Maso
Atmos. Chem. Phys., 19, 6367–6388, https://doi.org/10.5194/acp-19-6367-2019, https://doi.org/10.5194/acp-19-6367-2019, 2019
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The mechanism for new particle formation (NPF) in vehicle exhaust is currently unknown. This study focuses on determining the NPF rate in vehicle exhaust caused by sulfuric acid, which is the most promising candidate involved in the NPF process. The NPF rate function obtained in this study helps in examining the NPF mechanism in exhaust plumes, and it can also be used to improve air quality models. The results also imply that the NPF process cannot be fully explained by sulfuric acid only.
Elena C. Maters, Donald B. Dingwell, Corrado Cimarelli, Dirk Müller, Thomas F. Whale, and Benjamin J. Murray
Atmos. Chem. Phys., 19, 5451–5465, https://doi.org/10.5194/acp-19-5451-2019, https://doi.org/10.5194/acp-19-5451-2019, 2019
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This experimental study investigates the influence of volcanic ash chemical composition, crystallinity, and mineralogy on its ability to promote freezing of supercooled water. The results indicate that crystals in ash play a key role in this process and suggest that feldspars and perhaps pyroxenes in ash may be highly ice-active. These findings contribute to improving understanding of the potential of ash emissions from different explosive eruptions to impact ice formation in the atmosphere.
Zamin A. Kanji, Ryan C. Sullivan, Monika Niemand, Paul J. DeMott, Anthony J. Prenni, Cédric Chou, Harald Saathoff, and Ottmar Möhler
Atmos. Chem. Phys., 19, 5091–5110, https://doi.org/10.5194/acp-19-5091-2019, https://doi.org/10.5194/acp-19-5091-2019, 2019
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The ice nucleation ability of two natural desert dusts coated with a proxy of secondary organic aerosol is presented for temperatures and relative humidity conditions relevant for mixed-phase clouds. We find that at the tested conditions, there is no effect on the ice nucleation ability of the particles due to the organic coating. Furthermore, the two dust samples do not show variability within measurement uncertainty. Particle size and surface area may play a role in any difference observed.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
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We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Zhicong Yin, Huijun Wang, Yuyan Li, Xiaohui Ma, and Xinyu Zhang
Atmos. Chem. Phys., 19, 3857–3871, https://doi.org/10.5194/acp-19-3857-2019, https://doi.org/10.5194/acp-19-3857-2019, 2019
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Summer surface ozone pollution has rapidly intensified recently, damaging human and ecosystem health. This study aims to examine the large-scale atmospheric circulations associated with the interannual variation in summer surface O3 pollution in North China based on long-term meteorological observations. The impacts of Arctic sea ice were also revealed. The outcomes may provide a basis for understanding the interannual variation of 03 pollution and its seasonal to interannual prediction.
Ankit Tandon, Nicholas E. Rothfuss, and Markus D. Petters
Atmos. Chem. Phys., 19, 3325–3339, https://doi.org/10.5194/acp-19-3325-2019, https://doi.org/10.5194/acp-19-3325-2019, 2019
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Organic compounds may form a barrier to condensation. Such barriers have been hypothesized to prevent water and other substances from mixing with salt cores. This will hinder the particles' ability to aid cloud formation of < 100 nm particles. Here we perform experiments encasing particles in plastic shells akin to water bottles. Against expectations, the plastic shell did not alter the droplet activation behavior of the encased particles. Water appears to readily permeate the plastic shell.
James F. Davies, Andreas Zuend, and Kevin R. Wilson
Atmos. Chem. Phys., 19, 2933–2946, https://doi.org/10.5194/acp-19-2933-2019, https://doi.org/10.5194/acp-19-2933-2019, 2019
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The formation of cloud droplets involves the condensation of water onto preexisting particles in the atmosphere. The efficiency of this process depends on the nature of the particles, and recent work has shown that organic-rich particles may exhibit a suppressed surface tension that promotes the formation of cloud droplets. In this technical note, we discuss the mechanism for this and highlight the evolution of surface tension as the key factor in the extent of surface effects.
Nathan J. Janechek, Rachel F. Marek, Nathan Bryngelson, Ashish Singh, Robert L. Bullard, William H. Brune, and Charles O. Stanier
Atmos. Chem. Phys., 19, 1649–1664, https://doi.org/10.5194/acp-19-1649-2019, https://doi.org/10.5194/acp-19-1649-2019, 2019
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Cyclic volatile methyl siloxanes (cVMSs) are widely used chemicals in personal care products which can undergo oxidation to generate secondary organic aerosol. In this work, cVMS oxidation aerosols were generated using a photochemical chamber and the physical properties characterized. The aerosol yield, volatility, hygroscopicity, morphology, elemental composition, and proposed parameters for treatment as secondary organic aerosol in atmospheric models are provided.
Jian Wang, John E. Shilling, Jiumeng Liu, Alla Zelenyuk, David M. Bell, Markus D. Petters, Ryan Thalman, Fan Mei, Rahul A. Zaveri, and Guangjie Zheng
Atmos. Chem. Phys., 19, 941–954, https://doi.org/10.5194/acp-19-941-2019, https://doi.org/10.5194/acp-19-941-2019, 2019
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Earlier studies showed organic hygroscopicity increases with oxidation level. Such increases have been attributed to higher water solubility for more oxidized organics. By systematically varying the water content of activating droplets, we show that for secondary organic aerosols, essentially all organics are dissolved at the point of droplet activation. Therefore, the organic hygroscopicity is not limited by solubility but is dictated mainly by the molecular weight of organic species.
Nivedita K. Kumar, Joel C. Corbin, Emily A. Bruns, Dario Massabó, Jay G. Slowik, Luka Drinovec, Griša Močnik, Paolo Prati, Athanasia Vlachou, Urs Baltensperger, Martin Gysel, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 17843–17861, https://doi.org/10.5194/acp-18-17843-2018, https://doi.org/10.5194/acp-18-17843-2018, 2018
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It is clear that considerable uncertainties still exist in understanding the magnitude of aerosol absorption on a global scale and its contribution to global warming. This manuscript provides a comprehensive assessment of the optical absorption by organic aerosols (brown carbon) from residential wood combustion as a function of atmospheric aging.
Yue Peng, Hong Wang, Yubin Li, Changwei Liu, Tianliang Zhao, Xiaoye Zhang, Zhiqiu Gao, Tong Jiang, Huizheng Che, and Meng Zhang
Atmos. Chem. Phys., 18, 17421–17435, https://doi.org/10.5194/acp-18-17421-2018, https://doi.org/10.5194/acp-18-17421-2018, 2018
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Two surface layer schemes are evaluated in eastern China based on observational flux data. The results indicate that the Li scheme better describes regional atmosphere stratification compared with the MM5 scheme, especially for the transition stage from unstable to stable atmosphere conditions, corresponding to PM2.5 accumulation. Our research suggests the potential improved possibilities for severe haze prediction in eastern China by coupling Li online into atmosphere chemical models.
Dawei Hu, David Topping, and Gordon McFiggans
Atmos. Chem. Phys., 18, 14925–14937, https://doi.org/10.5194/acp-18-14925-2018, https://doi.org/10.5194/acp-18-14925-2018, 2018
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Co-condensation of inorganic or organic vapours on growing droplets could significantly enhance both CCN and cloud droplet number concentration, thereby influencing climate. Until now, there has been very few direct observational evidence of this process. We exposed involatile inorganic particles to a moist atmosphere containing a controlled amount of an organic semi-volatile vapour. We measured a much greater growth of the particles than if they had only been exposed to water vapour.
Maryam Dalirian, Arttu Ylisirniö, Angela Buchholz, Daniel Schlesinger, Johan Ström, Annele Virtanen, and Ilona Riipinen
Atmos. Chem. Phys., 18, 12477–12489, https://doi.org/10.5194/acp-18-12477-2018, https://doi.org/10.5194/acp-18-12477-2018, 2018
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Atmospheric black carbon (BC) particles are a concern due to their impact on air quality and climate. Their net climate effect is, however, still uncertain. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of BC particles, in pure state or coated by various organic species. Our results show that existing theories have potential in describing the CCN activation of atmospheric BC mixed with soluble pollutants.
Sara D. Forestieri, Taylor M. Helgestad, Andrew T. Lambe, Lindsay Renbaum-Wolff, Daniel A. Lack, Paola Massoli, Eben S. Cross, Manvendra K. Dubey, Claudio Mazzoleni, Jason S. Olfert, Arthur J. Sedlacek III, Andrew Freedman, Paul Davidovits, Timothy B. Onasch, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 12141–12159, https://doi.org/10.5194/acp-18-12141-2018, https://doi.org/10.5194/acp-18-12141-2018, 2018
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We characterized optical properties of flame-derived black carbon particles and interpret our observations through the use of Mie theory and Rayleigh–Debye–Gans theory. We determined that the mass absorption coefficient is independent of particle collapse and use this to derive theory- and wavelength-specific refractive indices for black carbon (BC). We demonstrate the inadequacy of Mie theory and suggest an alternative approach for atmospheric models to better represent light absorption by BC.
Mijung Song, Suhan Ham, Ryan J. Andrews, Yuan You, and Allan K. Bertram
Atmos. Chem. Phys., 18, 12075–12084, https://doi.org/10.5194/acp-18-12075-2018, https://doi.org/10.5194/acp-18-12075-2018, 2018
Sara D. Forestieri, Sean M. Staudt, Thomas M. Kuborn, Katharine Faber, Christopher R. Ruehl, Timothy H. Bertram, and Christopher D. Cappa
Atmos. Chem. Phys., 18, 10985–11005, https://doi.org/10.5194/acp-18-10985-2018, https://doi.org/10.5194/acp-18-10985-2018, 2018
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Our work establishes how surface tension reduction influences droplet growth and activation of simple sea spray mimics (NaCl coated with fatty acids). Fatty acids can substantially reduce droplet surface tension near activation but have limited impact on activation. Coating of NaCl by palmitic acid (a wax) impedes water uptake, but this impedance is removed if oleic acid (a liquid) is mixed in. The properties that surface-active compounds need to impact activation are theoretically examined.
Xiangyu Pei, Mattias Hallquist, Axel C. Eriksson, Joakim Pagels, Neil M. Donahue, Thomas Mentel, Birgitta Svenningsson, William Brune, and Ravi Kant Pathak
Atmos. Chem. Phys., 18, 9845–9860, https://doi.org/10.5194/acp-18-9845-2018, https://doi.org/10.5194/acp-18-9845-2018, 2018
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The findings in this study show that morphological transformation of soot occurs via two key complementary and sequential processes, i.e., void filling in the particle and its diameter growth. To quantify the state of morphological transformation, i.e., the utilization of material for filling and growth during the condensation processes, a framework was developed which can further be utilized to quantify the effect of condensed material on the optical and hygroscopic properties of soot.
Maja Tomicic, Martin Bødker Enghoff, and Henrik Svensmark
Atmos. Chem. Phys., 18, 5921–5930, https://doi.org/10.5194/acp-18-5921-2018, https://doi.org/10.5194/acp-18-5921-2018, 2018
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A supernova within a distance of about 100 pc from the Earth would increase the cosmic ray flux and thereby the atmospheric ionization. We study the impact of high ion concentrations on aerosol nucleation through experiments. The measurements show that nucleation increases by up to an order of magnitude when the ionization increases from background to supernova levels under fixed concentrations of the nucleating gas. This suggests that a supernova could influence the atmospheric microphysics.
Rosalie H. Shepherd, Martin D. King, Amelia A. Marks, Neil Brough, and Andrew D. Ward
Atmos. Chem. Phys., 18, 5235–5252, https://doi.org/10.5194/acp-18-5235-2018, https://doi.org/10.5194/acp-18-5235-2018, 2018
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The refractive index of atmospheric extracts sourced from urban (London), remote (Antarctica), and woodsmoke aerosol was determined by applying optical trapping simultaneously with Mie spectroscopy. In addition, owing to the absorbing nature of woodsmoke and an aqueous humic acid aerosol extract, the absorption Ångström exponent could be determined.The refractive index and absorption Ångström exponent were then applied in a top-of-the-atmosphere albedo radiation transfer model.
Bo Jing, Zhen Wang, Fang Tan, Yucong Guo, Shengrui Tong, Weigang Wang, Yunhong Zhang, and Maofa Ge
Atmos. Chem. Phys., 18, 5115–5127, https://doi.org/10.5194/acp-18-5115-2018, https://doi.org/10.5194/acp-18-5115-2018, 2018
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The nitrate/organic acid mixed aerosols exhibit varying phase behavior and hygroscopic growth depending upon the type of components in the particles. Our results reveal that the coexisting organic acid has considerable impacts on the phase and morphology of nitrate particles in the low and medium RH range, which thus result in obvious enhancement or suppression of water uptake with increasing RH. This new information provided here has important implications for atmospheric chemistry.
Jie Chen, Zhijun Wu, Stefanie Augustin-Bauditz, Sarah Grawe, Markus Hartmann, Xiangyu Pei, Zirui Liu, Dongsheng Ji, and Heike Wex
Atmos. Chem. Phys., 18, 3523–3539, https://doi.org/10.5194/acp-18-3523-2018, https://doi.org/10.5194/acp-18-3523-2018, 2018
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The ice nucleation activity of urban aerosols in the atmosphere of Beijing was detected in this study. Results showed that ice-nucleating particle (INP) concentrations were not influenced by the highly variable numbers of atmospheric particles, both in mass and particle number concentrations, implying that INP concentrations might not be influenced directly by anthropogenic activities, at least not down to roughly −25 °C and maybe even below.
Katherine M. Manfred, Rebecca A. Washenfelder, Nicholas L. Wagner, Gabriela Adler, Frank Erdesz, Caroline C. Womack, Kara D. Lamb, Joshua P. Schwarz, Alessandro Franchin, Vanessa Selimovic, Robert J. Yokelson, and Daniel M. Murphy
Atmos. Chem. Phys., 18, 1879–1894, https://doi.org/10.5194/acp-18-1879-2018, https://doi.org/10.5194/acp-18-1879-2018, 2018
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In this study, we use a new laser imaging nephelometer to measure the bulk aerosol scattering phase function for biomass burning aerosol from controlled fires. By comparing measurements to models for spherical and fractal particles, we demonstrate that the dominant morphology varies by fuel type. This instrument has unique capabilities to directly measure how morphology affects optical properties, and can be used in the future for important validations of remote sensing retrievals.
Lukas Pichelstorfer, Dominik Stolzenburg, John Ortega, Thomas Karl, Harri Kokkola, Anton Laakso, Kari E. J. Lehtinen, James N. Smith, Peter H. McMurry, and Paul M. Winkler
Atmos. Chem. Phys., 18, 1307–1323, https://doi.org/10.5194/acp-18-1307-2018, https://doi.org/10.5194/acp-18-1307-2018, 2018
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Quantification of new particle formation as a source of atmospheric aerosol is clearly of importance for climate and health aspects. In our new study we developed two analysis methods that allow retrieval of nanoparticle growth dynamics at much higher precision than it was possible so far. Our results clearly demonstrate that growth rates show much more variation than is currently known and suggest that the Kelvin effect governs growth in the sub-10 nm size range.
Adriana Rocha-Lima, J. Vanderlei Martins, Lorraine A. Remer, Martin Todd, John H. Marsham, Sebastian Engelstaedter, Claire L. Ryder, Carolina Cavazos-Guerra, Paulo Artaxo, Peter Colarco, and Richard Washington
Atmos. Chem. Phys., 18, 1023–1043, https://doi.org/10.5194/acp-18-1023-2018, https://doi.org/10.5194/acp-18-1023-2018, 2018
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We present results of ground-based measurements and subsequent laboratory analysis of Sahara dust samples collected in Algeria and Mauritania during the Fennec campaign in 2011. The results show that the sampled dust has low absorption characteristics and exhibits a distinct spectral bow-like shape. We find distinctive differences in the composition and optical characteristics of the dust from the two sites, corroborating with other studies that not all Saharan dust is the same.
Ting Lei, Andreas Zuend, Yafang Cheng, Hang Su, Weigang Wang, and Maofa Ge
Atmos. Chem. Phys., 18, 1045–1064, https://doi.org/10.5194/acp-18-1045-2018, https://doi.org/10.5194/acp-18-1045-2018, 2018
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Measurements and thermodynamic equilibrium predictions for organic–inorganic aerosols related to components from biomass burning emissions demonstrate a diversity of hygroscopic growth and shrinking behavior, which we observed using a hygroscopicity tandem differential mobility analyzer (HTDMA). Controlled laboratory experiments with single solutes and/or with mixed organic–inorganic systems of known phase state will be useful to constrain model parameters of thermodynamic equilibrium models.
Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, António Dias, Neil M. Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, and Peter H. McMurry
Atmos. Chem. Phys., 18, 845–863, https://doi.org/10.5194/acp-18-845-2018, https://doi.org/10.5194/acp-18-845-2018, 2018
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A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
Mengjiao Jiang, Jinqin Feng, Zhanqing Li, Ruiyu Sun, Yu-Tai Hou, Yuejian Zhu, Bingcheng Wan, Jianping Guo, and Maureen Cribb
Atmos. Chem. Phys., 17, 13967–13982, https://doi.org/10.5194/acp-17-13967-2017, https://doi.org/10.5194/acp-17-13967-2017, 2017
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Aerosol–cloud interactions have been recognized as playing an important role in precipitation. As a benchmark evaluation of model results that exclude aerosol effects, the operational precipitation forecast (before any aerosol effects included) is evaluated using multiple datasets with the goal of determining if there is any link between the model bias and aerosol loading. The forecast model overestimates light and underestimates heavy rain. Aerosols suppress light rain and enhance heavy rain.
Xiaole Pan, Yugo Kanaya, Fumikazu Taketani, Takuma Miyakawa, Satoshi Inomata, Yuichi Komazaki, Hiroshi Tanimoto, Zhe Wang, Itsushi Uno, and Zifa Wang
Atmos. Chem. Phys., 17, 13001–13016, https://doi.org/10.5194/acp-17-13001-2017, https://doi.org/10.5194/acp-17-13001-2017, 2017
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Characteristics of refractory black carbon (rBC) from open biomass burning (OBB) have a great impact on regional pollution and climate, in particular in East Asia. However, experimental study on characteristics of rBC from agricultural residue burning in East China was limited. This study performed laboratory experiments: we found that emission of rBC is highly related to flaming burning, and non-rBC to smoldering burning. Rapid condensation of semi-volatile organics resulted in coated rBC.
Chaoliu Li, Fangping Yan, Shichang Kang, Pengfei Chen, Xiaowen Han, Zhaofu Hu, Guoshuai Zhang, Ye Hong, Shaopeng Gao, Bin Qu, Zhejing Zhu, Jiwei Li, Bing Chen, and Mika Sillanpää
Atmos. Chem. Phys., 17, 11899–11912, https://doi.org/10.5194/acp-17-11899-2017, https://doi.org/10.5194/acp-17-11899-2017, 2017
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In this study, we found, due to contribution of carbonates, previously reported BC concentration in atmosphere of the Himalayas and Tibetan Plateau (HTP) were overestimated by around 39–52 %. Meanwhile, we found BC deposition of lake cores overestimated the atmospheric deposition of BC in the HTP; BC depositions of glacier region reflected actual values of 17.9 ± 5.3 mg m−2 a−1. The above results are critical for studying atmospheric distribution and chemical transport of BC in and around the HTP.
Monika Burkert-Kohn, Heike Wex, André Welti, Susan Hartmann, Sarah Grawe, Lisa Hellner, Paul Herenz, James D. Atkinson, Frank Stratmann, and Zamin A. Kanji
Atmos. Chem. Phys., 17, 11683–11705, https://doi.org/10.5194/acp-17-11683-2017, https://doi.org/10.5194/acp-17-11683-2017, 2017
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Several instruments can investigate properties of ice-nucleating particles (INPs), which are crucial to understanding ice cloud formation. We intercompare four online ice nucleation counters and reasonable agreement is found when the same ice nucleation mode is tested. A variable scaling factor was necessary to reconcile condensation freezing results with immersion freezing. Factors related to instrumental setup and aerosol generation are discussed to explain observed differences.
Jing Chen, Sri Hapsari Budisulistiorini, Masayuki Itoh, Wen-Chien Lee, Takuma Miyakawa, Yuichi Komazaki, Liu Dong Qing Yang, and Mikinori Kuwata
Atmos. Chem. Phys., 17, 11591–11604, https://doi.org/10.5194/acp-17-11591-2017, https://doi.org/10.5194/acp-17-11591-2017, 2017
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We report size-dependent water uptake by fresh Indonesian peat burning particles and discuss relationship between water uptake and chemical characteristics. Fresh peat burning particles are almost non-hygroscopic, as determined by both the water-soluble organic fraction and the difference in κ of slightly and highly water-soluble fractions. This work experimentally validates the reference for κ of OA-dominated particles, thus contributing to more accurate estimation of aerosol climate impacts.
Michael I. Cotterell, Rose E. Willoughby, Bryan R. Bzdek, Andrew J. Orr-Ewing, and Jonathan P. Reid
Atmos. Chem. Phys., 17, 9837–9851, https://doi.org/10.5194/acp-17-9837-2017, https://doi.org/10.5194/acp-17-9837-2017, 2017
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The optical properties of aerosols are required to analyse measurements of aerosol properties, estimate radiative forcing and interpret remote sensing retrievals. We provide comprehensive data sets of the refractive indices of the most important inorganic aerosol constituents, reporting parameterisations for the wavelength and relative humidity dependencies for each system. We assess the accuracy of this study, made on single trapped particles, against previous less comprehensive data sets.
James W. Grayson, Erin Evoy, Mijung Song, Yangxi Chu, Adrian Maclean, Allena Nguyen, Mary Alice Upshur, Marzieh Ebrahimi, Chak K. Chan, Franz M. Geiger, Regan J. Thomson, and Allan K. Bertram
Atmos. Chem. Phys., 17, 8509–8524, https://doi.org/10.5194/acp-17-8509-2017, https://doi.org/10.5194/acp-17-8509-2017, 2017
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The viscosities of four polyols and three saccharides mixed with water were determined. The results from the polyol studies suggest viscosity increases by 1–2 orders of magnitude with the addition of an OH functional group to a carbon backbone. The results from the saccharide studies suggest that the viscosity of highly oxidized compounds is strongly dependent on molar mass and oligomerization of highly oxidized compounds in atmospheric SOM could lead to large increases in viscosity.
Sandra Bastelberger, Ulrich K. Krieger, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 17, 8453–8471, https://doi.org/10.5194/acp-17-8453-2017, https://doi.org/10.5194/acp-17-8453-2017, 2017
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We present quantitative condensed-phase diffusivity measurements of a volatile organic (tetraethylene glycol) in highly viscous single aerosol particles (aqueous sucrose). The condensed-phase diffusivity exhibits a strong temperature and humidity dependence. Our results suggest that diffusion limitations of volatile organics in highly viscous organic aerosol may severely impact gas–particle partitioning under cold and dry conditions.
Cited articles
Altieri, K. E., Seitzinger, S. P., Carlton, A. G., Tuprin, B. J., Klein, G. C., and Marshall, A. G.: Oligomers formed through in-cloud methylglyoxal reactions: chemical composition, properties, and mechanisms investigated by ultra-high resolution FT-ICR mass spectrometry, Atmos. Environ., 42, 1476–1490, 2008.
Apelblat, A.: The vapour pressures of saturated aqueous solutions of potassium bromide, ammonium sulfate, copper(II) sulfate, iron(II) sulfate, and manganese(II) dichloride, at temperatures from 283 K to 308 K, J. Chem. Thermodyn., 25, 1513–1520, 1993.
Asa-Awuku, A., Sullivan, A. P., Hennigan, C. J., Weber, R. J., and Nenes, A.: Investigation of molar volume and surfactant characteristics of water-soluble organic compounds in biomass burning aerosol, Atmos. Chem. Phys., 8, 799–812, https://doi.org/10.5194/acp-8-799-2008, 2008.
Asa-Awuku, A., Engelhart, G. J., Lee, B. H., Pandis, S. N., and Nenes, A.: Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol, Atmos. Chem. Phys., 9, 795–812, https://doi.org/10.5194/acp-9-795-2009, 2009.
Ayranci, E. and Sahin, M.: Interactions of polyethylene glycols with water studied by measurements of density and sound velocity, J. Chem. Thermodyn., 40, 1200–1207, 2008.
Baltensperger, U., Kalberer, M., Dommen, J., Paulsen, D., Alfarra, M. R., Coe, H., Fisseha, R., Gascho, A., Gysel, M., Nyeki, S., Sax, M., Steinbacher, M., Prevot, A. S. H., Sjögren, S., Weingartner, E., and Zenobi, R.: Secondary organic aerosols from anthropogenic and biogenic precursors, Farraday Discuss., 130, 265–278, 2005.
Barsanti, K. C. and Pankow, J. F.: Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions-Part 1: Aldehydes and ketones, Atmos. Environ., 38, 4371–4382, 2004.
Barsanti, K. C. and Pankow, J. F.: Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions-2: Dialdehydes, methylglyoxal, and diketones, Atmos. Environ., 39, 6597–6607, 2005.
Barsanti, K. C. and Pankow, J. F.: Thermodynamics of the formation of atmospheric organic particulate matter by accretion reactions-Part 3: Carboxylic and dicarboxylic acids, Atmos. Environ., 40, 6676–6686, 2006.
Berkemeier, T., Shiraiwa, M., Pöschl, U., and Koop, T.: Competition between water uptake and ice nucleation by glassy organic aerosol particles, Atmos. Chem. Phys., 14, 12513–12531, https://doi.org/10.5194/acp-14-12513-2014, 2014.
Bertram, A. K., Martin, S. T., Hanna, S. J., Smith, M. L., Bodsworth, A., Chen, Q., Kuwata, M., Liu, A., You, Y., and Zorn, S. R.: Predicting the relative humidities of liquid-liquid phase separation, efflorescence, and deliquescence of mixed particles of ammonium sulfate, organic material, and water using the organic-to-sulfate mass ratio of the particle and the oxygen-to-carbon elemental ratio of the organic component, Atmos. Chem. Phys., 11, 10995–11006, https://doi.org/10.5194/acp-11-10995-2011, 2011.
Bilde, M. and Svenningsson, B.: CCN activation of slightly soluble organics: the importance of small amounts of inorganic salts and particle phase, Tellus B, 56, 128–134, 2004.
Bones, D. L., Reid, J. P., Lienhard, D. M., and Krieger, U. K.: Comparing the mechanism of water condensation and evaporation in glassy aerosol, P. Natl. Acad. Sci. USA, 109, 11613–11618, 2012.
Boucher, O., Randall, D., Artaxo, P., Bretherton, C., Feingold, G., Forster, P., Kerminen, V.-M., Kondo, Y., Liao, H., Lohman, U., Rasch, P., Satheesh, S. K., Sherwood, S., Stevens, B., and Zhang, X. Y.: Clouds and Aerosols, in: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Stocker, T. F., Qin, D., Plattner, G.-K., Tognor, M., Allen, S. K., Boschung, J., Nauels, A., Xia, Y., Bex, V., and Midgley, P. M., Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2013.
Brechtel, F. J. and Kreidenweis, S. M.: Predicting particle critical supersaturation from hygroscopic growth measurements in the humidified TDMA. Part II: Laboratory and ambient studies, J. Atmos. Sci., 57, 1872–1887, 2000.
Brooks, S. D., DeMott, P. J., and Kreidenweis, S. M.: Water uptake by particles containing humic materials with ammonium sulfate, Atmos. Environ., 38, 1859–1868, 2004.
Ciobanu, V. G., Marcolli, C., Krieger, U. K., Weers, U., and Peter, T.: Liquid-liquid phase separation in mixed organic/inorganic aerosol particles, J. Phys. Chem., 113, 10966–10978, 2009.
Ciobanu, V. G., Marcolli, C., Krieger, U. K., Zuend, A., and Peter, T.: Efflorescence of ammonium sulfate and coated ammonium sulfate particles: Evidence for surface nucleation, J. Phys. Chem. A, 114, 9486–9495, 2010.
Clegg, S. L. and Wexler, A. S.: Densities and Apparent Molar Volumes of Atmospherically Important Electrolyte Solutions. 1. The Solutes H2SO4, HNO3, HCl, Na2SO4, NaNO3, NaCl, (NH4)2SO4, NH4NO3, and NH4Cl from 0 to 50 °C, including extrapolations to very low temperature and to the pure liquid state, and NaHSO4, NaOH, and NH3 at 25 °C, J. Phys. Chem. A, 115, 3393–3460, 2011.
Denkenberger, K. A., Moffet, R. C., Holecek, J. C., Rebotier, T. P., and Prather, K. A.: Real-time, single-particle measurements of oligomers in aged ambient aerosol particles, Environ. Sci. Technol., 41, 5439–5446, 2007.
Dette, H. P., Qi, M., Scroder, D. C., Godt, A., and Koop, T.: Glass-forming properties of 3-methylbutane-1,2,3-tricarboxylic acid and its mixtures with water and pinonic acid, J. Phys. Chem. A, 118, 7024–7033, 2014.
Dow Chemical Company: Carbowax polyethylene glycols, Form No 118-01789-1011 AMS, 2011.
Dusek, U., Frank, G. P., Massling, A., Zeromskiene, K., Iinuma, Y., Schmid, O., Helas, G., Hennig, T., Wiedensohler, A., and Andreae, M. O.: Water uptake by biomass burning aerosol at sub- and supersaturated conditions: closure studies and implications for the role of organics, Atmos. Chem. Phys., 11, 9519–9532, https://doi.org/10.5194/acp-11-9519-2011, 2011.
Ekström, S., Nozière, B., Hultberg, M., Alsberg, T., Magnér, J., Nilsson, E. D., and Artaxo, P.: A possible role of ground-based microorganisms on cloud formation in the atmosphere, Biogeosciences, 7, 387–394, https://doi.org/10.5194/bg-7-387-2010, 2010.
Erdakos, G. B. and Pankow, J. F.: Gas/particle partitioning of neutral and ionizing compounds to single- and multi-phase aerosol particles. 2. Phase separation in liquid particulate matter containing both polar and low-polarity organic compounds, Atmos. Environ., 38, 1005–1013, 2004.
Facchini, M. C., Decesari, S., Mircea, M., Fuzzi, S., and Loglio, G.: Surface tension of atmospheric wet aerosol and cloud/fog droplets in relation to their organic carbon content and chemical composition, Atmos. Environ., 34, 4853–4857, 2000.
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Gao, Y. G., Chen, S. B., and Yu, L. E.: Efflorescence Relative Humidity for Ammonium Sulfate Particles. J. Phys. Chem. A, 110, 7602–7608, 2006.
Good, N., Topping, D. O., Allan, J. D., Flynn, M., Fuentes, E., Irwin, M., Williams, P. I., Coe, H., and McFiggans, G.: Consistency between parameterisations of aerosol hygroscopicity and CCN activity during the RHaMBLe discovery cruise, Atmos. Chem. Phys., 10, 3189–3203, https://doi.org/10.5194/acp-10-3189-2010, 2010.
Graber, T. A., Medina, H., Galleguillos, H. R., and Taboada, M. E.: Phase equilibrium and partition of iodide in a aqueous biphasic system formed by (NH4)2SO4
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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.
Discontinuities in apparent hygroscopicity below and above water saturation have been observed...
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