Articles | Volume 20, issue 20
Atmos. Chem. Phys., 20, 12163–12176, 2020
https://doi.org/10.5194/acp-20-12163-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Atmos. Chem. Phys., 20, 12163–12176, 2020
https://doi.org/10.5194/acp-20-12163-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
27 Oct 2020
Research article
| 27 Oct 2020
Drivers of cloud droplet number variability in the summertime in the southeastern United States
Aikaterini Bougiatioti et al.
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Irini Tsiodra, Georgios Grivas, Kalliopi Tavernaraki, Aikaterini Bougiatioti, Maria Apostolaki, Despina Paraskevopoulou, Alexandra Gogou, Constantine Parinos, Konstantina Oikonomou, Maria Tsagkaraki, Pavlos Zarmpas, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 21, 17865–17883, https://doi.org/10.5194/acp-21-17865-2021, https://doi.org/10.5194/acp-21-17865-2021, 2021
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We analyze observations from year-long measurements at Athens, Greece. Nighttime wintertime PAH levels are 4 times higher than daytime, and wintertime values are 15 times higher than summertime. Biomass burning aerosol during wintertime pollution events is responsible for these significant wintertime enhancements and accounts for 43 % of the population exposure to PAH carcinogenic risk. Biomass burning poses additional health risks beyond those associated with the high PM levels that develop.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203, https://doi.org/10.5194/acp-19-6185-2019, https://doi.org/10.5194/acp-19-6185-2019, 2019
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We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
Nikos Kalivitis, Veli-Matti Kerminen, Giorgos Kouvarakis, Iasonas Stavroulas, Evaggelia Tzitzikalaki, Panayiotis Kalkavouras, Nikos Daskalakis, Stelios Myriokefalitakis, Aikaterini Bougiatioti, Hanna E. Manninen, Pontus Roldin, Tuukka Petäjä, Michael Boy, Markku Kulmala, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 2671–2686, https://doi.org/10.5194/acp-19-2671-2019, https://doi.org/10.5194/acp-19-2671-2019, 2019
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New particle formation (NPF) is an important source of atmospheric aerosols. For the Mediterranean atmosphere, only few studies exist. In this study we present one of the longest series of NPF by analyzing 10 years of data from Crete, Greece. NPF took place on 27 % of the available days; it was more frequent in spring and less so in late summer. Model simulations showed that NPF in the subtropical environment may differ greatly from that in the boreal environment.
Iasonas Stavroulas, Aikaterini Bougiatioti, Georgios Grivas, Despina Paraskevopoulou, Maria Tsagkaraki, Pavlos Zarmpas, Eleni Liakakou, Evangelos Gerasopoulos, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 901–919, https://doi.org/10.5194/acp-19-901-2019, https://doi.org/10.5194/acp-19-901-2019, 2019
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Over the last few years, many cities in Greece have suffered from significant air quality deterioration events during wintertime. Driven by such observations, we studied the variability and main sources of submicron particulate matter in Athens, Greece, as a large part of the population in this region is exposed to high levels, which sometimes exceed legislative limit values. It was found that such events are mostly associated with combustion sources used for domestic heating during winter.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Panayiotis Kalkavouras, Elissavet Bossioli, Spiros Bezantakos, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Giorgos Kouvarakis, Anna P. Protonotariou, Aggeliki Dandou, George Biskos, Nikolaos Mihalopoulos, Athanasios Nenes, and Maria Tombrou
Atmos. Chem. Phys., 17, 175–192, https://doi.org/10.5194/acp-17-175-2017, https://doi.org/10.5194/acp-17-175-2017, 2017
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Concentrations of chemically and size-resolved submicron aerosol particles along with concentrations of gases and meteorological variables were measured at Santorini and Finokalia (central and southern Aegean Sea) during the Etesians. Particle nucleation bursts were recorded. The NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number by 12 %.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Aikaterini Bougiatioti, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, Panagiotis Kokkalis, George Biskos, Nikolaos Mihalopoulos, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 16, 7389–7409, https://doi.org/10.5194/acp-16-7389-2016, https://doi.org/10.5194/acp-16-7389-2016, 2016
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BBOA from long-range transport exhibits increased CCN concentrations for particles larger than 100 nm. At the same time the hygroscopicity parameter decreased for all particle sizes, as sub-100 nm particles appear to be richer in less hygroscopic organic material, while larger particles become less hygroscopic due to condensation of less hygroscopic gaseous compounds. Finally, atmospheric processing of freshly emitted BBOA to more oxidized organic aerosol can result in a 2-fold increase of κ.
Aikaterini Bougiatioti, Panayiota Nikolaou, Iasonas Stavroulas, Giorgos Kouvarakis, Rodney Weber, Athanasios Nenes, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, https://doi.org/10.5194/acp-16-4579-2016, 2016
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Atmospheric aerosols and relevant parameters were measured in the eastern Mediterranean during summer and fall 2012. Submicron aerosol water can contribute up to 33 % of total mass, and 27.5 % of this can be associated with organics. Using these data, the pH of the submicron aerosols was calculated to be highly acidic, varying from 0.5 to 2.8 and independently of air masses origin. Such pH values could increase nutrient availability and thus sea water productivity of the Mediterranean Sea.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
N. Kalivitis, V.-M. Kerminen, G. Kouvarakis, I. Stavroulas, A. Bougiatioti, A. Nenes, H. E. Manninen, T. Petäjä, M. Kulmala, and N. Mihalopoulos
Atmos. Chem. Phys., 15, 9203–9215, https://doi.org/10.5194/acp-15-9203-2015, https://doi.org/10.5194/acp-15-9203-2015, 2015
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Cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is presented, and this is the first direct evidence of CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the active NPF period.
K. M. Cerully, A. Bougiatioti, J. R. Hite Jr., H. Guo, L. Xu, N. L. Ng, R. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, https://doi.org/10.5194/acp-15-8679-2015, 2015
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The hygroscopicity of SE US aerosol is mostly water-soluble, with a hygroscopicity that is insensitive to partial volatilization in a thermodenuder.
The most and least oxidized components of the aerosol are the most hygroscopic of organic constituents.
No clear relationship was found between organic aerosol hygroscopicity and oxygen-to-carbon ratio.
The aerosol factors covary in a way that induces the observed diurnal invariance in total organic hygroscopicity.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-658, https://doi.org/10.5194/acp-2022-658, 2022
Preprint under review for ACP
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Emily D. Lenhardt, Lan Gao, Jens Redemann, Feng Xu, Sharon P. Burton, Brian Cairns, Ian Chang, Richard A. Ferrare, Chris A. Hostetler, Pablo E. Saide, Calvin Howes, Yohei Shinozuka, Snorre Stamnes, Mary Kacarab, Amie Dobracki, Jenny Wong, Steffen Freitag, and Athanasios Nenes
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-262, https://doi.org/10.5194/amt-2022-262, 2022
Preprint under review for AMT
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Small atmospheric particles, such as smoke from wildfires or pollutants from human activities, impact cloud properties, and clouds have a strong influence on climate change. To better understand the distributions of these particles, we develop relationships to derive their concentrations from remote sensing measurements from an instrument called a lidar. Our method is reliable for smoke particles, and similar steps can be taken to develop similar relationships for other particle types.
Hannah Carolin Frostenberg, André Welti, Mikael Luhr, Julien Savre, Erik S. Thomson, and Luisa Ickes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-696, https://doi.org/10.5194/acp-2022-696, 2022
Preprint under review for ACP
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Observations show that ice nucleating particle concentrations (INPCs) have a large variety and follow log-normal distributions for a given temperature. We introduce a new immersion freezing parameterization that applies this log-normal behavior: INPCs are drawn randomly from a temperature-dependent log-normal distribution. We show that the ice content of the modeled Arctic stratocumulus cloud is highly sensitive to the probability to draw high INPCs.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-498, https://doi.org/10.5194/acp-2022-498, 2022
Preprint under review for ACP
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In this study, we present an intercomparison study of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, Maria Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-551, https://doi.org/10.5194/acp-2022-551, 2022
Revised manuscript under review for ACP
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Ice formation is enabled by Ice Nucleating Particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that additionally to k-feldspar dust mineral that is globally the most important INP precursor, quartz, which is abundant in mineral dust, can be regionally significant, affecting different cloud level regimes (low-level clouds) than K-feldspar (mid-level clouds).
Christian Tatzelt, Silvia Henning, André Welti, Andrea Baccarini, Markus Hartmann, Martin Gysel-Beer, Manuela van Pinxteren, Robin L. Modini, Julia Schmale, and Frank Stratmann
Atmos. Chem. Phys., 22, 9721–9745, https://doi.org/10.5194/acp-22-9721-2022, https://doi.org/10.5194/acp-22-9721-2022, 2022
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We present the abundance and origin of cloud-relevant aerosol particles in the preindustral-like conditions of the Southern Ocean (SO) during austral summer. Cloud condensation nuclei (CCN) and ice-nucleating particles (INP) were measured during a circum-Antarctic scientific cruise with in situ instrumentation and offline filter measurements, respectively. Transport processes were found to play an equally important role as local sources for both the CCN and INP population of the SO.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, Sebastian Eastham, Christina J. Williamson, Agnieszka Kupc, and Charles A. Brock
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-487, https://doi.org/10.5194/acp-2022-487, 2022
Revised manuscript under review for ACP
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Particle number concentrations and size distributions in the stratosphere are studied through model simulations and comparisons with measurements. The nucleation scheme used in most of the solar geoengineering modeling studies over-predicts the nucleation rates and particle number concentrations in the stratosphere. The model based on updated nucleation schemes captures reasonably well some aspects of particle size distributions but misses some features. The possible reasons are discussed.
Caroline Dang, Michal Segal-Rozenhaimer, Haochi Che, Lu Zhang, Paola Formenti, Jonathan Taylor, Amie Dobracki, Sara Purdue, Pui-Shan Wong, Athanasios Nenes, Arthur Sedlacek III, Hugh Coe, Jens Redemann, Paquita Zuidema, Steven Howell, and James Haywood
Atmos. Chem. Phys., 22, 9389–9412, https://doi.org/10.5194/acp-22-9389-2022, https://doi.org/10.5194/acp-22-9389-2022, 2022
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Transmission electron microscopy was used to analyze aged African smoke particles and how the smoke interacts with the marine atmosphere. We found that the volatility of organic aerosol increases with biomass burning plume age, that black carbon is often mixed with potassium salts and that the marine atmosphere can incorporate Na and Cl into smoke particles. Marine salts are more processed when mixed with smoke plumes, and there are interesting Cl-rich yet Na-absent marine particles.
Lu Zhang, Michal Segal-Rozenhaimer, Haochi Che, Caroline Dang, Arthur J. Sedlacek III, Ernie R. Lewis, Amie Dobracki, Jenny P. S. Wong, Paola Formenti, Steven G. Howell, and Athanasios Nenes
Atmos. Chem. Phys., 22, 9199–9213, https://doi.org/10.5194/acp-22-9199-2022, https://doi.org/10.5194/acp-22-9199-2022, 2022
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Widespread biomass burning (BB) events occur annually in Africa and contribute ~ 1 / 3 of global BB emissions, which contain a large family of light-absorbing organics, known as brown carbon (BrC), whose absorption of incident radiation is difficult to estimate, leading to large uncertainties in the global radiative forcing estimation. This study quantifies the BrC absorption of aged BB particles and highlights the potential presence of absorbing iron oxides in this climatically important region.
Pamela Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-309, https://doi.org/10.5194/acp-2022-309, 2022
Revised manuscript accepted for ACP
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources, but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Kun Zhang, Zhiqiang Liu, Xiaojuan Zhang, Qing Li, Andrew Jensen, Wen Tan, Ling Huang, Yangjun Wang, Joost de Gouw, and Li Li
Atmos. Chem. Phys., 22, 4853–4866, https://doi.org/10.5194/acp-22-4853-2022, https://doi.org/10.5194/acp-22-4853-2022, 2022
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A significant increase in O3 concentrations was found during the lockdown period of COVID-19 in most areas of China. By field measurements coupled with machine learning, an observation-based model (OBM) and sensitivity analysis, we found the changes in the NOx / VOC ratio were a key reason for the significant rise in O3. To restrain O3 pollution, more efforts should be devoted to the control of anthropogenic OVOCs, alkenes and aromatics.
Stelios Myriokefalitakis, Elisa Bergas-Massó, María Gonçalves-Ageitos, Carlos Pérez García-Pando, Twan van Noije, Philippe Le Sager, Akinori Ito, Eleni Athanasopoulou, Athanasios Nenes, Maria Kanakidou, Maarten C. Krol, and Evangelos Gerasopoulos
Geosci. Model Dev., 15, 3079–3120, https://doi.org/10.5194/gmd-15-3079-2022, https://doi.org/10.5194/gmd-15-3079-2022, 2022
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We here describe the implementation of atmospheric multiphase processes in the EC-Earth Earth system model. We provide global budgets of oxalate, sulfate, and iron-containing aerosols, along with an analysis of the links among atmospheric composition, aqueous-phase processes, and aerosol dissolution, supported by comparison to observations. This work is a first step towards an interactive calculation of the deposition of bioavailable atmospheric iron coupled to the model’s ocean component.
Adam T. Ahern, Frank Erdesz, Nicholas L. Wagner, Charles A. Brock, Ming Lyu, Kyra Slovacek, Richard H. Moore, Elizabeth B. Wiggins, and Daniel M. Murphy
Atmos. Meas. Tech., 15, 1093–1105, https://doi.org/10.5194/amt-15-1093-2022, https://doi.org/10.5194/amt-15-1093-2022, 2022
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Particles in the atmosphere play a significant role in climate change by scattering light back into space, reducing the amount of energy available to be absorbed by greenhouse gases. We built a new instrument to measure what direction light is scattered by particles, e.g., wildfire smoke. This is important because, depending on the angle of the sun, some particles scatter light into space (cooling the planet), but some light is also scattered towards the Earth (not cooling the planet).
Paraskevi Georgakaki, Georgia Sotiropoulou, Étienne Vignon, Anne-Claire Billault-Roux, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 22, 1965–1988, https://doi.org/10.5194/acp-22-1965-2022, https://doi.org/10.5194/acp-22-1965-2022, 2022
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The modelling study focuses on the importance of ice multiplication processes in orographic mixed-phase clouds, which is one of the least understood cloud types in the climate system. We show that the consideration of ice seeding and secondary ice production through ice–ice collisional breakup is essential for correct predictions of precipitation in mountainous terrain, with important implications for radiation processes.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
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Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Irini Tsiodra, Georgios Grivas, Kalliopi Tavernaraki, Aikaterini Bougiatioti, Maria Apostolaki, Despina Paraskevopoulou, Alexandra Gogou, Constantine Parinos, Konstantina Oikonomou, Maria Tsagkaraki, Pavlos Zarmpas, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 21, 17865–17883, https://doi.org/10.5194/acp-21-17865-2021, https://doi.org/10.5194/acp-21-17865-2021, 2021
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We analyze observations from year-long measurements at Athens, Greece. Nighttime wintertime PAH levels are 4 times higher than daytime, and wintertime values are 15 times higher than summertime. Biomass burning aerosol during wintertime pollution events is responsible for these significant wintertime enhancements and accounts for 43 % of the population exposure to PAH carcinogenic risk. Biomass burning poses additional health risks beyond those associated with the high PM levels that develop.
Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
Atmos. Chem. Phys., 21, 17687–17714, https://doi.org/10.5194/acp-21-17687-2021, https://doi.org/10.5194/acp-21-17687-2021, 2021
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Aerosol–cloud interactions constitute the most uncertain contribution to climate change. The uptake kinetics of water by aerosol is a central process of cloud droplet formation, yet its molecular-scale mechanism is unknown. We use molecular simulations to study this process for phase-separated organic particles. Our results explain the increased cloud condensation activity of such particles and can be generalized over various compositions, thus possibly serving as a basis for future models.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Markus Hartmann, Xianda Gong, Simonas Kecorius, Manuela van Pinxteren, Teresa Vogl, André Welti, Heike Wex, Sebastian Zeppenfeld, Hartmut Herrmann, Alfred Wiedensohler, and Frank Stratmann
Atmos. Chem. Phys., 21, 11613–11636, https://doi.org/10.5194/acp-21-11613-2021, https://doi.org/10.5194/acp-21-11613-2021, 2021
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Ice-nucleating particles (INPs) are not well characterized in the Arctic despite their importance for the Arctic energy budget. Little is known about their nature (mineral or biological) and sources (terrestrial or marine, long-range transport or local). We find indications that, at the beginning of the melt season, a local, biogenic, probably marine source is likely, but significant enrichment of INPs has to take place from the ocean to the aerosol phase.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078, https://doi.org/10.5194/acp-21-11069-2021, https://doi.org/10.5194/acp-21-11069-2021, 2021
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Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 9741–9760, https://doi.org/10.5194/acp-21-9741-2021, https://doi.org/10.5194/acp-21-9741-2021, 2021
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Mixed-phase clouds are a large source of uncertainty in projections of the Arctic climate. This is partly due to the poor representation of the cloud ice formation processes. Implementing a parameterization for ice multiplication due to mechanical breakup upon collision of two ice particles in a high-resolution model improves cloud ice phase representation; however, cloud liquid remains overestimated.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech., 14, 4517–4542, https://doi.org/10.5194/amt-14-4517-2021, https://doi.org/10.5194/amt-14-4517-2021, 2021
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Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Amy Hrdina, Jennifer G. Murphy, Anna Gannet Hallar, John C. Lin, Alexander Moravek, Ryan Bares, Ross C. Petersen, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Munkh Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 21, 8111–8126, https://doi.org/10.5194/acp-21-8111-2021, https://doi.org/10.5194/acp-21-8111-2021, 2021
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Wintertime air pollution in the Salt Lake Valley is primarily composed of ammonium nitrate, which is formed when gas-phase ammonia and nitric acid react. The major point in this work is that the chemical composition of snow tells a very different story to what we measured in the atmosphere. With the dust–sea salt cations observed in PM2.5 and particle sizing data, we can estimate how much nitric acid may be lost to dust–sea salt that is not accounted for and how much more PM2.5 this could form.
Caroline C. Womack, Katherine M. Manfred, Nicholas L. Wagner, Gabriela Adler, Alessandro Franchin, Kara D. Lamb, Ann M. Middlebrook, Joshua P. Schwarz, Charles A. Brock, Steven S. Brown, and Rebecca A. Washenfelder
Atmos. Chem. Phys., 21, 7235–7252, https://doi.org/10.5194/acp-21-7235-2021, https://doi.org/10.5194/acp-21-7235-2021, 2021
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Microscopic particles interact with sunlight and affect the earth's climate in ways that are not fully understood. Aerosols from wildfire smoke present particular challenges due to their complexity in shape and composition. We demonstrate that we can experimentally measure aerosol optical properties for many types of smoke particles, using measurements of smoke from controlled burns, but that the method does not work well for smoke with high soot content.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Jack J. Lin, Kamal Raj R, Stella Wang, Esko Kokkonen, Mikko-Heikki Mikkelä, Samuli Urpelainen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 4709–4727, https://doi.org/10.5194/acp-21-4709-2021, https://doi.org/10.5194/acp-21-4709-2021, 2021
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We used surface-sensitive X-ray photoelectron spectroscopy (XPS) to study laboratory-generated nanoparticles of atmospheric interest at 0–16 % relative humidity. XPS gives direct information about changes in the chemical state from the binding energies of probed elements. Our results indicate water adsorption and associated chemical changes at the particle surfaces well below deliquescence, with distinct features for different particle components and implications for atmospheric chemistry.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894, https://doi.org/10.5194/acp-21-2881-2021, https://doi.org/10.5194/acp-21-2881-2021, 2021
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This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563, https://doi.org/10.5194/acp-21-1507-2021, https://doi.org/10.5194/acp-21-1507-2021, 2021
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Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771, https://doi.org/10.5194/acp-21-755-2021, https://doi.org/10.5194/acp-21-755-2021, 2021
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Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
Megan S. Claflin, Demetrios Pagonis, Zachary Finewax, Anne V. Handschy, Douglas A. Day, Wyatt L. Brown, John T. Jayne, Douglas R. Worsnop, Jose L. Jimenez, Paul J. Ziemann, Joost de Gouw, and Brian M. Lerner
Atmos. Meas. Tech., 14, 133–152, https://doi.org/10.5194/amt-14-133-2021, https://doi.org/10.5194/amt-14-133-2021, 2021
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We have developed a field-deployable gas chromatograph with thermal desorption preconcentration and detector switching between two high-resolution mass spectrometers for in situ measurements of volatile organic compounds (VOCs). This system combines chromatography with both proton transfer and electron ionization to offer fast time response and continuous molecular speciation. This technique was applied during the 2018 ATHLETIC campaign to characterize VOC emissions in an indoor environment.
André Welti, Kimmo Korhonen, Pasi Miettinen, Ana A. Piedehierro, Yrjö Viisanen, Annele Virtanen, and Ari Laaksonen
Atmos. Meas. Tech., 13, 7059–7067, https://doi.org/10.5194/amt-13-7059-2020, https://doi.org/10.5194/amt-13-7059-2020, 2020
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We describe a modification of the SPectrometer for Ice Nuclei (SPIN) chamber to study ice nucleation at low temperatures, relevant for ice formation in cirrus clouds. Validation experiments of homogeneous freezing of aqueous ammonium sulfate droplets and heterogeneous ice nucleation on silver iodide particles are included to demonstrate the advantages of the modified SPIN chamber for the investigation of ice nucleation in the extended temperature range.
André Welti, E. Keith Bigg, Paul J. DeMott, Xianda Gong, Markus Hartmann, Mike Harvey, Silvia Henning, Paul Herenz, Thomas C. J. Hill, Blake Hornblow, Caroline Leck, Mareike Löffler, Christina S. McCluskey, Anne Marie Rauker, Julia Schmale, Christian Tatzelt, Manuela van Pinxteren, and Frank Stratmann
Atmos. Chem. Phys., 20, 15191–15206, https://doi.org/10.5194/acp-20-15191-2020, https://doi.org/10.5194/acp-20-15191-2020, 2020
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Ship-based measurements of maritime ice nuclei concentrations encompassing all oceans are compiled. From this overview it is found that maritime ice nuclei concentrations are typically 10–100 times lower than over continents, while concentrations are surprisingly similar in different oceanic regions. The analysis of the influence of ship emissions shows no effect on the data, making ship-based measurements an efficient strategy for the large-scale exploration of ice nuclei concentrations.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099, https://doi.org/10.5194/acp-20-15079-2020, https://doi.org/10.5194/acp-20-15079-2020, 2020
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Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Agnieszka Kupc, Christina J. Williamson, Anna L. Hodshire, Jan Kazil, Eric Ray, T. Paul Bui, Maximilian Dollner, Karl D. Froyd, Kathryn McKain, Andrew Rollins, Gregory P. Schill, Alexander Thames, Bernadett B. Weinzierl, Jeffrey R. Pierce, and Charles A. Brock
Atmos. Chem. Phys., 20, 15037–15060, https://doi.org/10.5194/acp-20-15037-2020, https://doi.org/10.5194/acp-20-15037-2020, 2020
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Tropical upper troposphere over the Atlantic and Pacific oceans is a major source region of new particles. These particles are associated with the outflow from deep convection. We investigate the processes that govern the formation of these particles and their initial growth and show that none of the formation schemes commonly used in global models are consistent with observations. Using newer schemes indicates that organic compounds are likely important as nucleating and initial growth agents.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
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Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
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We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Hans-Christian Clemen, Johannes Schneider, Thomas Klimach, Frank Helleis, Franziska Köllner, Andreas Hünig, Florian Rubach, Stephan Mertes, Heike Wex, Frank Stratmann, André Welti, Rebecca Kohl, Fabian Frank, and Stephan Borrmann
Atmos. Meas. Tech., 13, 5923–5953, https://doi.org/10.5194/amt-13-5923-2020, https://doi.org/10.5194/amt-13-5923-2020, 2020
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We improved the efficiency of a single-particle mass spectrometer with a newly developed aerodynamic lens system, delayed ion extraction, and better electric shielding. The new components result in significantly improved particle analysis and sample statistics. This is particularly important for measurements of low-number-density particles, such as ice-nucleating particles, and for aircraft-based measurements at high altitudes or where high temporal and spatial resolution is required.
James M. Roberts, Chelsea E. Stockwell, Robert J. Yokelson, Joost de Gouw, Yong Liu, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, Kyle J. Zarzana, Steven S. Brown, Cristina Santin, Stefan H. Doerr, and Carsten Warneke
Atmos. Chem. Phys., 20, 8807–8826, https://doi.org/10.5194/acp-20-8807-2020, https://doi.org/10.5194/acp-20-8807-2020, 2020
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We measured total reactive nitrogen, Nr, in lab fires from western North American fuels, along with measurements of individual nitrogen compounds. We measured the amount of N that gets converted to inactive compounds (avg. 70 %), and the amount that is accounted for by individual species (85 % of remaining N). We provide guidelines for how the reactive nitrogen is distributed among individual compounds such as NOx and ammonia. This will help estimates and predictions of wildfire emissions.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
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.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Mary Kacarab, K. Lee Thornhill, Amie Dobracki, Steven G. Howell, Joseph R. O'Brien, Steffen Freitag, Michael R. Poellot, Robert Wood, Paquita Zuidema, Jens Redemann, and Athanasios Nenes
Atmos. Chem. Phys., 20, 3029–3040, https://doi.org/10.5194/acp-20-3029-2020, https://doi.org/10.5194/acp-20-3029-2020, 2020
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We find that extensive biomass burning aerosol plumes from southern Africa can profoundly influence clouds in the southeastern Atlantic. Concurrent variations in vertical velocity, however, are found to magnify the relationship between boundary layer aerosol and the cloud droplet number. Neglecting these covariances may strongly bias the sign and magnitude of aerosol impacts on the cloud droplet number.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Arnaldo Negron, Natasha DeLeon-Rodriguez, Samantha M. Waters, Luke D. Ziemba, Bruce Anderson, Michael Bergin, Konstantinos T. Konstantinidis, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1817–1838, https://doi.org/10.5194/acp-20-1817-2020, https://doi.org/10.5194/acp-20-1817-2020, 2020
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Airborne biological particles impact human health, cloud formation, and ecosystems, but few techniques are available to characterize their atmospheric abundance. Combining a newly developed high-volume sampling/flow cytometry technique together with an laser-induced fluorescence instrument, we detect a highly dynamic bioaerosol community over urban Atlanta, composed of pollen, fungi, and bacteria with low and high nucleic acid content.
Georgia Sotiropoulou, Sylvia Sullivan, Julien Savre, Gary Lloyd, Thomas Lachlan-Cope, Annica M. L. Ekman, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1301–1316, https://doi.org/10.5194/acp-20-1301-2020, https://doi.org/10.5194/acp-20-1301-2020, 2020
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Arctic clouds constitute a large source of uncertainty in predictions of future climate. Observations indicate that the number concentration of cloud ice crystals exceeds the concentration of aerosols that can act as ice-nucleating particles (INPs). We show that ice multiplication due to mechanical break-up upon collisions between the few primary ice crystals (formed from INPs) can explain the discrepancy. Including a description of the process in climate models can improve cloud representation.
Alexander Moravek, Jennifer G. Murphy, Amy Hrdina, John C. Lin, Christopher Pennell, Alessandro Franchin, Ann M. Middlebrook, Dorothy L. Fibiger, Caroline C. Womack, Erin E. McDuffie, Randal Martin, Kori Moore, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 15691–15709, https://doi.org/10.5194/acp-19-15691-2019, https://doi.org/10.5194/acp-19-15691-2019, 2019
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Ammonium nitrate is a major component of fine particulate matter of wintertime air pollution in the Great Salt Lake Region (UT, USA). We investigate the sources of ammonia in the region by using aircraft observations and comparing them to modelled ammonia mixing ratios based on emission inventory estimates. The results suggest that ammonia emissions are underestimated, specifically in regions with high agricultural activity, while ammonia in Salt Lake City is mainly of local origin.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, https://doi.org/10.5194/acp-19-14607-2019, 2019
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
Karl D. Froyd, Daniel M. Murphy, Charles A. Brock, Pedro Campuzano-Jost, Jack E. Dibb, Jose-Luis Jimenez, Agnieszka Kupc, Ann M. Middlebrook, Gregory P. Schill, Kenneth L. Thornhill, Christina J. Williamson, James C. Wilson, and Luke D. Ziemba
Atmos. Meas. Tech., 12, 6209–6239, https://doi.org/10.5194/amt-12-6209-2019, https://doi.org/10.5194/amt-12-6209-2019, 2019
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Single-particle mass spectrometer (SPMS) instruments characterize the composition of individual aerosol particles in real time. We present a new method that combines SPMS composition with independently measured particle size distributions to determine absolute number, surface area, volume, and mass concentrations of mineral dust, biomass burning, sea salt, and other climate-relevant atmospheric particle types, with a fast time response applicable to aircraft sampling.
Simonas Kecorius, Teresa Vogl, Pauli Paasonen, Janne Lampilahti, Daniel Rothenberg, Heike Wex, Sebastian Zeppenfeld, Manuela van Pinxteren, Markus Hartmann, Silvia Henning, Xianda Gong, Andre Welti, Markku Kulmala, Frank Stratmann, Hartmut Herrmann, and Alfred Wiedensohler
Atmos. Chem. Phys., 19, 14339–14364, https://doi.org/10.5194/acp-19-14339-2019, https://doi.org/10.5194/acp-19-14339-2019, 2019
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Arctic sea-ice retreat, atmospheric new particle formation (NPF), and aerosol–cloud interaction may all be linked via a positive feedback mechanism. Understanding the sources of cloud condensation nuclei (CCN) is an important piece in the Arctic amplification puzzle. We show that Arctic newly formed particles do not have to grow beyond the Aitken mode to act as CCN. This is important, because NPF occurrence in the Arctic is expected to increase, making it a significant contributor to CCN budget.
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
Eleni Marinou, Matthias Tesche, Athanasios Nenes, Albert Ansmann, Jann Schrod, Dimitra Mamali, Alexandra Tsekeri, Michael Pikridas, Holger Baars, Ronny Engelmann, Kalliopi-Artemis Voudouri, Stavros Solomos, Jean Sciare, Silke Groß, Florian Ewald, and Vassilis Amiridis
Atmos. Chem. Phys., 19, 11315–11342, https://doi.org/10.5194/acp-19-11315-2019, https://doi.org/10.5194/acp-19-11315-2019, 2019
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We assess the feasibility of ground-based and spaceborne lidars to retrieve profiles of cloud-relevant aerosol concentrations and ice-nucleating particles. The retrieved profiles are in good agreement with airborne in situ measurements. Our methodology will be applied to satellite observations in the future so as to provide a global 3D product of cloud-relevant properties.
André Welti, Ulrike Lohmann, and Zamin A. Kanji
Atmos. Chem. Phys., 19, 10901–10918, https://doi.org/10.5194/acp-19-10901-2019, https://doi.org/10.5194/acp-19-10901-2019, 2019
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The ice nucleation ability of singly immersed feldspar particles in suspended water droplets relevant for ice crystal formation under mixed-phase cloud conditions is presented. The effects of particle size, crystal structure, trace metal and mineralogical composition are discussed by testing up to five different diameters in the submicron range and nine different feldspar samples at conditions relevant for ice nucleation in mixed-phase clouds.
Erin E. McDuffie, Caroline C. Womack, Dorothy L. Fibiger, William P. Dube, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Joel A. Thornton, Alexander Moravek, Jennifer G. Murphy, Munkhbayar Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 19, 9287–9308, https://doi.org/10.5194/acp-19-9287-2019, https://doi.org/10.5194/acp-19-9287-2019, 2019
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Populated mountain basins, including the Salt Lake Valley (SLV) in Utah, suffer from wintertime stagnation events that trap emissions near the surface and cause fine particulate matter (PM2.5) concentrations to reach unhealthy levels. Previously limited by a lack of nighttime measurements, this study uses 2017 UWFPS aircraft campaign data, in combination with a box model, to show that nitrogen chemistry above the surface at night is a major source of PM2.5 during a wintertime event in the SLV.
Xin Chen, Dylan B. Millet, Hanwant B. Singh, Armin Wisthaler, Eric C. Apel, Elliot L. Atlas, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, John D. Crounse, Joost A. de Gouw, Frank M. Flocke, Alan Fried, Brian G. Heikes, Rebecca S. Hornbrook, Tomas Mikoviny, Kyung-Eun Min, Markus Müller, J. Andrew Neuman, Daniel W. O'Sullivan, Jeff Peischl, Gabriele G. Pfister, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Stephen R. Shertz, Chelsea R. Thompson, Victoria Treadaway, Patrick R. Veres, James Walega, Carsten Warneke, Rebecca A. Washenfelder, Petter Weibring, and Bin Yuan
Atmos. Chem. Phys., 19, 9097–9123, https://doi.org/10.5194/acp-19-9097-2019, https://doi.org/10.5194/acp-19-9097-2019, 2019
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Volatile organic compounds (VOCs) affect air quality and modify the lifetimes of other pollutants. We combine a high-resolution 3-D atmospheric model with an ensemble of aircraft observations to perform an integrated analysis of the VOC budget over North America. We find that biogenic emissions provide the main source of VOC reactivity even in most major cities. Our findings point to key gaps in current models related to oxygenated VOCs and to the distribution of VOCs in the free troposphere.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Benjamin L. Deming, Demetrios Pagonis, Xiaoxi Liu, Douglas A. Day, Ranajit Talukdar, Jordan E. Krechmer, Joost A. de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 12, 3453–3461, https://doi.org/10.5194/amt-12-3453-2019, https://doi.org/10.5194/amt-12-3453-2019, 2019
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Losses or measurement delays of gas-phase compounds sampled through tubing are important to atmospheric science. Here we characterize 14 tubing materials by measuring the effects on step changes in organic compound concentration. We find that polymeric tubings exhibit absorptive partitioning behaviour while glass and metal tubings show adsorptive partitioning. Adsorptive materials impart complex humidity, concentration, and VOC–VOC interaction dependencies that absorptive tubings do not.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Charles A. Brock, Christina Williamson, Agnieszka Kupc, Karl D. Froyd, Frank Erdesz, Nicholas Wagner, Matthews Richardson, Joshua P. Schwarz, Ru-Shan Gao, Joseph M. Katich, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Jose L. Jimenez, Bernadett Weinzierl, Maximilian Dollner, ThaoPaul Bui, and Daniel M. Murphy
Atmos. Meas. Tech., 12, 3081–3099, https://doi.org/10.5194/amt-12-3081-2019, https://doi.org/10.5194/amt-12-3081-2019, 2019
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From 2016 to 2018 a NASA aircraft profiled the atmosphere from 180 m to ~12 km from the Arctic to the Antarctic over both the Pacific and Atlantic oceans. This program, ATom, sought to sample atmospheric chemical composition to compare with global climate models. We describe the how measurements of particulate matter were made during ATom, and show that the instrument performance was excellent. Data from this project can be used with confidence to evaluate models and compare with satellites.
Jenny P. S. Wong, Maria Tsagkaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 19, 7319–7334, https://doi.org/10.5194/acp-19-7319-2019, https://doi.org/10.5194/acp-19-7319-2019, 2019
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Biomass burning is a major source of light-absorbing organic species in atmospheric aerosols, and it can play an important role in climate and atmospheric chemistry. Through a combination of laboratory experiments and field observations, this work demonstrated that the light absorption properties of aged biomass burning organic aerosols are dominated by high-molecular-weight compounds. In addition, we found that total hydrated sugars may be a robust tracer for aged biomass burning aerosols.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203, https://doi.org/10.5194/acp-19-6185-2019, https://doi.org/10.5194/acp-19-6185-2019, 2019
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We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
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.
Daniel M. Murphy, Karl D. Froyd, Huisheng Bian, Charles A. Brock, Jack E. Dibb, Joshua P. DiGangi, Glenn Diskin, Maximillian Dollner, Agnieszka Kupc, Eric M. Scheuer, Gregory P. Schill, Bernadett Weinzierl, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 19, 4093–4104, https://doi.org/10.5194/acp-19-4093-2019, https://doi.org/10.5194/acp-19-4093-2019, 2019
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We present the first data on the concentration of sea-salt aerosol throughout most of the depth of the troposphere and a wide range of latitudes. Sea-salt concentrations in the upper troposphere are very small. This puts stringent limits on how sea-salt aerosol affects halogen and nitric acid chemistry there. With a widely distributed source, sea-salt aerosol provides an excellent test of wet scavenging and vertical transport of aerosols in chemical transport models.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Nikos Kalivitis, Veli-Matti Kerminen, Giorgos Kouvarakis, Iasonas Stavroulas, Evaggelia Tzitzikalaki, Panayiotis Kalkavouras, Nikos Daskalakis, Stelios Myriokefalitakis, Aikaterini Bougiatioti, Hanna E. Manninen, Pontus Roldin, Tuukka Petäjä, Michael Boy, Markku Kulmala, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 2671–2686, https://doi.org/10.5194/acp-19-2671-2019, https://doi.org/10.5194/acp-19-2671-2019, 2019
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New particle formation (NPF) is an important source of atmospheric aerosols. For the Mediterranean atmosphere, only few studies exist. In this study we present one of the longest series of NPF by analyzing 10 years of data from Crete, Greece. NPF took place on 27 % of the available days; it was more frequent in spring and less so in late summer. Model simulations showed that NPF in the subtropical environment may differ greatly from that in the boreal environment.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Iasonas Stavroulas, Aikaterini Bougiatioti, Georgios Grivas, Despina Paraskevopoulou, Maria Tsagkaraki, Pavlos Zarmpas, Eleni Liakakou, Evangelos Gerasopoulos, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 901–919, https://doi.org/10.5194/acp-19-901-2019, https://doi.org/10.5194/acp-19-901-2019, 2019
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Over the last few years, many cities in Greece have suffered from significant air quality deterioration events during wintertime. Driven by such observations, we studied the variability and main sources of submicron particulate matter in Athens, Greece, as a large part of the population in this region is exposed to high levels, which sometimes exceed legislative limit values. It was found that such events are mostly associated with combustion sources used for domestic heating during winter.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Hongyu Guo, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 17307–17323, https://doi.org/10.5194/acp-18-17307-2018, https://doi.org/10.5194/acp-18-17307-2018, 2018
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Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
Alessandro Franchin, Dorothy L. Fibiger, Lexie Goldberger, Erin E. McDuffie, Alexander Moravek, Caroline C. Womack, Erik T. Crosman, Kenneth S. Docherty, William P. Dube, Sebastian W. Hoch, Ben H. Lee, Russell Long, Jennifer G. Murphy, Joel A. Thornton, Steven S. Brown, Munkhbayar Baasandorj, and Ann M. Middlebrook
Atmos. Chem. Phys., 18, 17259–17276, https://doi.org/10.5194/acp-18-17259-2018, https://doi.org/10.5194/acp-18-17259-2018, 2018
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We present the results of aerosol and trace gas measurements from airborne and ground-based platforms. The measurements took place in January–February 2017 in northern Utah as part of the Utah Winter Fine Particulate Study (UWFPS). We characterized the chemical composition of PM1 on a regional scale, also probing the vertical dimension. We used a thermodynamic model to study the effectiveness of limiting total ammonium or total nitrate as a strategy to control aerosol concentrations.
Sylvia C. Sullivan, Christian Barthlott, Jonathan Crosier, Ilya Zhukov, Athanasios Nenes, and Corinna Hoose
Atmos. Chem. Phys., 18, 16461–16480, https://doi.org/10.5194/acp-18-16461-2018, https://doi.org/10.5194/acp-18-16461-2018, 2018
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Ice crystal formation in clouds can occur via thermodynamic nucleation, but also via mechanical collisions between pre-existing crystals or co-existing droplets. When descriptions of this mechanical ice generation are implemented into the COSMO weather model, we find that the contributions to crystal number from thermodynamic and mechanical processes are of the same order. Mechanical ice generation also intensifies differences in precipitation intensity between dynamic and quiescent regions.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, https://doi.org/10.5194/bg-15-6659-2018, 2018
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The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Kyle J. Zarzana, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, William P. Dubé, Robert J. Yokelson, Carsten Warneke, Joost A. de Gouw, James M. Roberts, and Steven S. Brown
Atmos. Chem. Phys., 18, 15451–15470, https://doi.org/10.5194/acp-18-15451-2018, https://doi.org/10.5194/acp-18-15451-2018, 2018
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Emissions of glyoxal and methylglyoxal from fuels common to the western United States were measured using cavity-enhanced spectroscopy, which provides a more selective measurement of those compounds than was previously available. Primary emissions of glyoxal were lower than previously reported and showed variability between the different fuel groups. However, emissions of glyoxal relative to formaldehyde were constant across almost all the fuel groups at 6 %–7 %.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Sarah Grawe, Stefanie Augustin-Bauditz, Hans-Christian Clemen, Martin Ebert, Stine Eriksen Hammer, Jasmin Lubitz, Naama Reicher, Yinon Rudich, Johannes Schneider, Robert Staacke, Frank Stratmann, André Welti, and Heike Wex
Atmos. Chem. Phys., 18, 13903–13923, https://doi.org/10.5194/acp-18-13903-2018, https://doi.org/10.5194/acp-18-13903-2018, 2018
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In this study, coal fly ash particles immersed in supercooled cloud droplets were analyzed concerning their freezing behavior. Additionally, physico-chemical particle properties (morphology, chemical composition, crystallography) were investigated. In combining both aspects, components that potentially contribute to the observed freezing behavior of the ash could be identified. Interactions at the particle-water interface, that depend on suspension time and influence freezing, are discussed.
Petros Vasilakos, Armistead Russell, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys., 18, 12765–12775, https://doi.org/10.5194/acp-18-12765-2018, https://doi.org/10.5194/acp-18-12765-2018, 2018
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In this work, we investigated the role of emission reductions on aerosol acidity and particulate nitrate. We found that models exhibit positive biases in pH predictions, attributed to very high levels of crustal elements (Mg, Ca, K) in model simulations, which in turn led to an increasing aerosol pH trend over the past decade and allowed nitrate to become an important component of aerosol, which is inconsistent with the measurements, highlighting the importance of accurate pH prediction.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Kanako Sekimoto, Abigail R. Koss, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Carsten Warneke, Robert J. Yokelson, James M. Roberts, and Joost de Gouw
Atmos. Chem. Phys., 18, 9263–9281, https://doi.org/10.5194/acp-18-9263-2018, https://doi.org/10.5194/acp-18-9263-2018, 2018
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We found that on average 85 % of the VOC emissions from biomass burning across various fuels representative of the western US (including various coniferous and chaparral fuels) can be explained using only two emission profiles: (i) a high-temperature pyrolysis profile and (ii) a low-temperature pyrolysis profile. The high-temperature profile is quantitatively similar between different fuel types (r2 > 0.84), and likewise for the low-temperature profile.
Christina Williamson, Agnieszka Kupc, James Wilson, David W. Gesler, J. Michael Reeves, Frank Erdesz, Richard McLaughlin, and Charles A. Brock
Atmos. Meas. Tech., 11, 3491–3509, https://doi.org/10.5194/amt-11-3491-2018, https://doi.org/10.5194/amt-11-3491-2018, 2018
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We describe the operating principle, design and performance of the Nucleation Mode Aerosol Size Spectrometer (NMASS), an instrument composed of 5 condensation particle counters measuring size selected particle concentrations between 3 and 60 nm. An inversion to recover size distributions from the data is evaluated. Calibrations of a 2-NMASS system for measuring size distributions on the NASA Atmospheric Tomography Mission, and examples of its in-flight performance are presented.
Si-Wan Kim, Vijay Natraj, Seoyoung Lee, Hyeong-Ahn Kwon, Rokjin Park, Joost de Gouw, Gregory Frost, Jhoon Kim, Jochen Stutz, Michael Trainer, Catalina Tsai, and Carsten Warneke
Atmos. Chem. Phys., 18, 7639–7655, https://doi.org/10.5194/acp-18-7639-2018, https://doi.org/10.5194/acp-18-7639-2018, 2018
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Formaldehyde (HCHO) is a hazardous air pollutant and is associated with tropospheric ozone production. HCHO has been monitored from space. In this study, to acquire high-quality satellite-based HCHO observations, we utilize fine-resolution atmospheric chemistry model results as an input to the computer code for satellite retrievals over the Los Angeles Basin. Our study indicates that the use of fine-resolution profile shapes helps to identify HCHO plumes from space.
Chelsea E. Stockwell, Agnieszka Kupc, Bartłomiej Witkowski, Ranajit K. Talukdar, Yong Liu, Vanessa Selimovic, Kyle J. Zarzana, Kanako Sekimoto, Carsten Warneke, Rebecca A. Washenfelder, Robert J. Yokelson, Ann M. Middlebrook, and James M. Roberts
Atmos. Meas. Tech., 11, 2749–2768, https://doi.org/10.5194/amt-11-2749-2018, https://doi.org/10.5194/amt-11-2749-2018, 2018
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This work investigates the total conversion of particle-bound nitrogen and organic carbon across platinum and molybdenum catalysts followed by NO–O3 chemiluminescence and nondispersive infrared CO2 detection. We show the instrument is an accurate particle mass measurement method and demonstrate its ability to calibrate particle mass measurement instrumentation through comparisons with a calibrated particle-into-liquid sampler coupled to an electrospray ionization source of a mass spectrometer.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
André Welti, Konrad Müller, Zoë L. Fleming, and Frank Stratmann
Atmos. Chem. Phys., 18, 5307–5320, https://doi.org/10.5194/acp-18-5307-2018, https://doi.org/10.5194/acp-18-5307-2018, 2018
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We report on ambient concentrations of ice nuclei, measured on the Cabo Verde islands. Concentrations are found to exponentially increase by 7 orders of magnitude from −5 to −38 °C. At each temperature, the frequency distribution of observed concentrations can be described by a lognormal distribution, typical for random dilution of substances during transport. Random dilution is found to account for larger fluctuations in IN concentration than seasonal changes and changes in air mass origin.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Non-methane organic gases (NMOGs) were detected by proton-transfer-reaction mass spectrometry (PTR-ToF) during an extensive laboratory characterization of wildfire emissions. Identifications for PTR-ToF ion masses are proposed and supported by a combination of techniques. Overall excellent agreement with other instrumentation is shown. Scalable emission factors and ratios are reported for many newly reported reactive species. An analysis of chemical characteristics is presented.
Vanessa Selimovic, Robert J. Yokelson, Carsten Warneke, James M. Roberts, Joost de Gouw, James Reardon, and David W. T. Griffith
Atmos. Chem. Phys., 18, 2929–2948, https://doi.org/10.5194/acp-18-2929-2018, https://doi.org/10.5194/acp-18-2929-2018, 2018
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We burned fuels representing western US wildfires in large-scale laboratory simulations to generate relevant emissions as confirmed by lab–field comparison. We report emission factors (EFs) for light scattering and absorption and BC along with SSA at 870 and 401 nm and AAE. We report EF for 22 trace gases that are major inorganic and organic emissions from flaming and smoldering. We report trace gas EF for species rarely (NH3) or not yet measured (e.g., HONO, acetic acid) for real US wildfires.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Eric Edgerton, Karsten Baumann, Philip A. Feiner, David O. Miller, William H. Brune, Abigail R. Koss, Joost A. de Gouw, Pawel K. Misztal, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 18, 2601–2614, https://doi.org/10.5194/acp-18-2601-2018, https://doi.org/10.5194/acp-18-2601-2018, 2018
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Observations of increased ozone on hotter days are widely reported, but the mechanisms driving this relationship remain uncertain. We use measurements from the rural southeastern United States to study how temperature affects ozone production. We find that changing NOx emissions, most likely from soil microbes, can be a major driver of increased ozone with temperature in the continental background. These findings suggest that ozone will increase with temperature under a wide range of conditions.
Catalina Tsai, Max Spolaor, Santo Fedele Colosimo, Olga Pikelnaya, Ross Cheung, Eric Williams, Jessica B. Gilman, Brian M. Lerner, Robert J. Zamora, Carsten Warneke, James M. Roberts, Ravan Ahmadov, Joost de Gouw, Timothy Bates, Patricia K. Quinn, and Jochen Stutz
Atmos. Chem. Phys., 18, 1977–1996, https://doi.org/10.5194/acp-18-1977-2018, https://doi.org/10.5194/acp-18-1977-2018, 2018
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Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH). Vertical HONO fluxes, observed in the snow-free, wintertime Uintah Basin, Utah, USA, show that chemical formation of HONO on the ground closes the HONO budget. Under high NOx conditions, HONO formation is most likely due to photo-enhanced conversion of NO2 on the ground. Under moderate to low NO2 conditions, photolysis of HNO3 on the ground seems to be the most likely source of HONO.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Agnieszka Kupc, Christina Williamson, Nicholas L. Wagner, Mathews Richardson, and Charles A. Brock
Atmos. Meas. Tech., 11, 369–383, https://doi.org/10.5194/amt-11-369-2018, https://doi.org/10.5194/amt-11-369-2018, 2018
Demetrios Pagonis, Jordan E. Krechmer, Joost de Gouw, Jose L. Jimenez, and Paul J. Ziemann
Atmos. Meas. Tech., 10, 4687–4696, https://doi.org/10.5194/amt-10-4687-2017, https://doi.org/10.5194/amt-10-4687-2017, 2017
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Laboratory studies were conducted to investigate gas-wall partitioning of atmospheric organic compounds in Teflon tubing and inside an instrument used to monitor concentrations. Rapid partitioning caused time delays in instrument response that vary with tubing length and diameter, flow rate, and compound volatility. Tubing delay times of seconds to hours were described using a model that also included effects of instrument surfaces. The results can enable better design of air sampling systems.
Robert C. Rhew, Malte Julian Deventer, Andrew A. Turnipseed, Carsten Warneke, John Ortega, Steve Shen, Luis Martinez, Abigail Koss, Brian M. Lerner, Jessica B. Gilman, James N. Smith, Alex B. Guenther, and Joost A. de Gouw
Atmos. Chem. Phys., 17, 13417–13438, https://doi.org/10.5194/acp-17-13417-2017, https://doi.org/10.5194/acp-17-13417-2017, 2017
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Alkenes emanate from both natural and anthropogenic sources and can contribute to atmospheric ozone production. This study measured
lightalkene (ethene, propene and butene) fluxes from a ponderosa pine forest using a novel relaxed eddy accumulation method, revealing much larger emissions than previously estimated and accounting for a significant fraction of OH reactivity. Emissions have a diurnal cycle related to sunlight and temperature, and the forest canopy appears to be the source.
Jin Liao, Charles A. Brock, Daniel M. Murphy, Donna T. Sueper, André Welti, and Ann M. Middlebrook
Atmos. Meas. Tech., 10, 3801–3820, https://doi.org/10.5194/amt-10-3801-2017, https://doi.org/10.5194/amt-10-3801-2017, 2017
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The Aerodyne aerosol mass spectrometer (AMS) has emerged as a widely used method for measuring the real-time, submicron, nonrefractory aerosol composition. A large uncertainty in accurate measurements with the AMS (the collection efficiency due to particle bounce) is evaluated in this paper using in situ measurements of particle light scattering. Current calculations of the collection efficiency reasonably predict this effect in acidic environments, resulting in more confidence for AMS results.
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.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
Shantanu H. Jathar, Christopher Heppding, Michael F. Link, Delphine K. Farmer, Ali Akherati, Michael J. Kleeman, Joost A. de Gouw, Patrick R. Veres, and James M. Roberts
Atmos. Chem. Phys., 17, 8959–8970, https://doi.org/10.5194/acp-17-8959-2017, https://doi.org/10.5194/acp-17-8959-2017, 2017
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Our work makes novel emissions measurements of isocyanic acid, a toxic gas, from a modern-day diesel engine and finds that diesel engines emit isocyanic acid but the emissions control devices do not enhance or destroy the isocyanic acid. Air quality model calculations suggest that diesel engines are possibly important sources of isocyanic acid in urban environments although the isocyanic acid levels are ten times lower than levels linked to adverse human health effects.
Khairunnisa Yahya, Timothy Glotfelty, Kai Wang, Yang Zhang, and Athanasios Nenes
Geosci. Model Dev., 10, 2333–2363, https://doi.org/10.5194/gmd-10-2333-2017, https://doi.org/10.5194/gmd-10-2333-2017, 2017
Caroline C. Womack, J. Andrew Neuman, Patrick R. Veres, Scott J. Eilerman, Charles A. Brock, Zachary C. J. Decker, Kyle J. Zarzana, William P. Dube, Robert J. Wild, Paul J. Wooldridge, Ronald C. Cohen, and Steven S. Brown
Atmos. Meas. Tech., 10, 1911–1926, https://doi.org/10.5194/amt-10-1911-2017, https://doi.org/10.5194/amt-10-1911-2017, 2017
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The accurate detection of reactive nitrogen species (NOy) is key to understanding tropospheric ozone production. Typically, NOy is detected by thermal conversion to NO2, followed by NO2 detection. Here, we assess the conversion efficiency of several NOy species to NO2 in a thermal dissociation cavity ring-down spectrometer and discuss how this conversion efficiency is affected by certain experimental conditions, such as oven residence time, and interferences from non-NOy species.
Petros Vasilakos, Yong-Ηa Kim, Jeffrey R. Pierce, Sotira Yiacoumi, Costas Tsouris, and Athanasios Nenes
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2017-96, https://doi.org/10.5194/gmd-2017-96, 2017
Revised manuscript not accepted
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Radioactive charging can significantly impact the way radioactive aerosols behave, and as a result their lifetime, but such effects are neglected in predictive model studies of radioactive plumes. We extend a well-established model that simulates the evolution of atmospheric particulate matter to account for radioactive charging effects in an accurate and computationally efficient way. It is shown that radioactivity can strongly impact the deposition patterns of aerosol.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Bin Yuan, Matthew M. Coggon, Abigail R. Koss, Carsten Warneke, Scott Eilerman, Jeff Peischl, Kenneth C. Aikin, Thomas B. Ryerson, and Joost A. de Gouw
Atmos. Chem. Phys., 17, 4945–4956, https://doi.org/10.5194/acp-17-4945-2017, https://doi.org/10.5194/acp-17-4945-2017, 2017
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In this study, we measured emissions of volatile organic compounds (VOCs) from concentrated animal feeding operations (CAFOs) using both mobile laboratory and aircraft measurements. We will use this data set to investigate chemical compositions of VOC emissions and sources apportionment for these VOC emissions in different facilities.
Chelsea R. Thompson, Paul B. Shepson, Jin Liao, L. Greg Huey, Chris Cantrell, Frank Flocke, and John Orlando
Atmos. Chem. Phys., 17, 3401–3421, https://doi.org/10.5194/acp-17-3401-2017, https://doi.org/10.5194/acp-17-3401-2017, 2017
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The generally accepted mechanism leading to ozone depletion events in the Arctic assumes efficient gas-phase recycling of bromine atoms, such that the rate of ozone depletion has often been estimated as the rate that Br atoms regenerate through gas-phase BrO + BrO and BrO + ClO reactions. Using a large suite of data from the OASIS2009 campaign, our modeling results show that the gas-phase regeneration of Br is less efficient than expected and that heterogeneous recycling on surfaces is critical.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
Luisa Ickes, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 17, 1713–1739, https://doi.org/10.5194/acp-17-1713-2017, https://doi.org/10.5194/acp-17-1713-2017, 2017
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The goal of this study is to find a parameterization scheme for general circulation models to describe immersion freezing with the ability to shift and adjust the slope of the freezing curve compared to homogeneous freezing to match experimental data. We investigated how accurate different formulations of classical nucleation theory reproduce measured immersion freezing curves for different mineral dust types.
Anusha P. S. Hettiyadura, Thilina Jayarathne, Karsten Baumann, Allen H. Goldstein, Joost A. de Gouw, Abigail Koss, Frank N. Keutsch, Kate Skog, and Elizabeth A. Stone
Atmos. Chem. Phys., 17, 1343–1359, https://doi.org/10.5194/acp-17-1343-2017, https://doi.org/10.5194/acp-17-1343-2017, 2017
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Organosulfates are components of secondary organic aerosol (SOA) formed in the presence of sulfate. Herein, their abundance, identity, and potential to form as sampling artifacts were studied in Centreville, AL, USA. The 10 most abundant signals accounted for 58–78 % of the total, with at least 20–200 other species accounting for the remainder. These major species were largely associated with biogenic gases, like isoprene and monoterpenes, and are proposed targets for future standard development.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313, https://doi.org/10.5194/amt-10-291-2017, https://doi.org/10.5194/amt-10-291-2017, 2017
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Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107, https://doi.org/10.5194/amt-10-83-2017, https://doi.org/10.5194/amt-10-83-2017, 2017
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The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Panayiotis Kalkavouras, Elissavet Bossioli, Spiros Bezantakos, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Giorgos Kouvarakis, Anna P. Protonotariou, Aggeliki Dandou, George Biskos, Nikolaos Mihalopoulos, Athanasios Nenes, and Maria Tombrou
Atmos. Chem. Phys., 17, 175–192, https://doi.org/10.5194/acp-17-175-2017, https://doi.org/10.5194/acp-17-175-2017, 2017
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Concentrations of chemically and size-resolved submicron aerosol particles along with concentrations of gases and meteorological variables were measured at Santorini and Finokalia (central and southern Aegean Sea) during the Etesians. Particle nucleation bursts were recorded. The NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number by 12 %.
Stelios Myriokefalitakis, Athanasios Nenes, Alex R. Baker, Nikolaos Mihalopoulos, and Maria Kanakidou
Biogeosciences, 13, 6519–6543, https://doi.org/10.5194/bg-13-6519-2016, https://doi.org/10.5194/bg-13-6519-2016, 2016
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The global atmospheric cycle of P is simulated accounting for natural and anthropogenic sources, acid dissolution of dust aerosol and changes in atmospheric acidity. Simulations show that P-containing dust dissolution flux may have increased in the last 150 years but is expected to decrease in the future, and biological particles are important carriers of bioavailable P to the ocean. These insights to the P cycle have important implications for marine ecosystem responses to climate change.
Yvonne Boose, André Welti, James Atkinson, Fabiola Ramelli, Anja Danielczok, Heinz G. Bingemer, Michael Plötze, Berko Sierau, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 15075–15095, https://doi.org/10.5194/acp-16-15075-2016, https://doi.org/10.5194/acp-16-15075-2016, 2016
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We compare the immersion freezing behavior of four airborne to 11 surface-collected dust samples to investigate the role of different minerals for atmospheric ice nucleation on desert dust. We find that present K-feldspars dominate at T > 253 K, while quartz does at colder temperatures, and surface-collected dust samples are not necessarily representative for airborne dust. For improved ice cloud prediction, modeling of quartz and feldspar emission and transport are key.
Glenn M. Wolfe, Margaret R. Marvin, Sandra J. Roberts, Katherine R. Travis, and Jin Liao
Geosci. Model Dev., 9, 3309–3319, https://doi.org/10.5194/gmd-9-3309-2016, https://doi.org/10.5194/gmd-9-3309-2016, 2016
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The Framework for 0-D Atmospheric Modeling (F0AM) is a new, user-friendly platform for simulation of atmospheric chemistry systems. It incorporates a suite of commonly used mechanisms and is adaptable to photochemical chambers, Lagrangian plumes, and steady-state or time-varying diurnal cycles. We provide a detailed model description, demonstrate several common applications, and highlight some of the advantages and challenges of the 0-D box modeling approach.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Baban Nagare, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8899–8914, https://doi.org/10.5194/acp-16-8899-2016, https://doi.org/10.5194/acp-16-8899-2016, 2016
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The relative importance of contact freezing and immersion freezing at mixed-phase cloud temperatures is the subject of debate. We performed experiments using continuous-flow diffusion chambers to compare the freezing efficiency of ice-nucleating particles for both these nucleation modes. Silver iodide, kaolinite and Arizona Test Dust were used as ice-nucleating particles. We could not confirm the dominance of contact freezing over immersion freezing for our experimental conditions.
Claudia Marcolli, Baban Nagare, André Welti, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8915–8937, https://doi.org/10.5194/acp-16-8915-2016, https://doi.org/10.5194/acp-16-8915-2016, 2016
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Silver iodide is one of the best-investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Nevertheless, many open questions remain. This paper gives an overview of silver iodide as an ice nucleus and tries to identify the factors that influence the ice nucleation ability of silver iodide.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Abigail R. Koss, Carsten Warneke, Bin Yuan, Matthew M. Coggon, Patrick R. Veres, and Joost A. de Gouw
Atmos. Meas. Tech., 9, 2909–2925, https://doi.org/10.5194/amt-9-2909-2016, https://doi.org/10.5194/amt-9-2909-2016, 2016
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Using laboratory and field experiments, we have explored how the technique of NO+ chemical ionization mass spectrometry can be used to measure volatile organic compounds (VOCs) in the troposphere. Results include the design and operation of the instrument, an evaluation of the technique’s utility for atmospheric measurement, and a guide for data interpretation. Use of this technique will improve our understanding of VOC chemistry.
Sarvesh Garimella, Thomas Bjerring Kristensen, Karolina Ignatius, Andre Welti, Jens Voigtländer, Gourihar R. Kulkarni, Frank Sagan, Gregory Lee Kok, James Dorsey, Leonid Nichman, Daniel Alexander Rothenberg, Michael Rösch, Amélie Catharina Ruth Kirchgäßner, Russell Ladkin, Heike Wex, Theodore W. Wilson, Luis Antonio Ladino, Jon P. D. Abbatt, Olaf Stetzer, Ulrike Lohmann, Frank Stratmann, and Daniel James Cziczo
Atmos. Meas. Tech., 9, 2781–2795, https://doi.org/10.5194/amt-9-2781-2016, https://doi.org/10.5194/amt-9-2781-2016, 2016
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The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nuclei counter manufactured by Droplet Measurement Technologies in Boulder, CO. This study characterizes the SPIN chamber, reporting data from laboratory measurements and quantifying uncertainties. Overall, we report that the SPIN is able to reproduce previous CFDC ice nucleation measurements.
Bin Yuan, Abigail Koss, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Harald Stark, and Joost A. de Gouw
Atmos. Meas. Tech., 9, 2735–2752, https://doi.org/10.5194/amt-9-2735-2016, https://doi.org/10.5194/amt-9-2735-2016, 2016
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We present the development of a hydronium (H3O+) time of flight chemical ionization mass spectrometer (H3O+ ToF-CIMS). We characterize the humidity dependence of the reagent ions and VOC signals in details. The low mass cutoff issue of RF-only quadrupole leads to unusual humidity dependence of reagent ions. The new H3O+ ToF-CIMS was successfully deployed on the NOAA WP-3D research aircraft for the SONGNEX campaign in 2015 and some initial results from the SONGNEX campaign are presented.
Paul S. Romer, Kaitlin C. Duffey, Paul J. Wooldridge, Hannah M. Allen, Benjamin R. Ayres, Steven S. Brown, William H. Brune, John D. Crounse, Joost de Gouw, Danielle C. Draper, Philip A. Feiner, Juliane L. Fry, Allen H. Goldstein, Abigail Koss, Pawel K. Misztal, Tran B. Nguyen, Kevin Olson, Alex P. Teng, Paul O. Wennberg, Robert J. Wild, Li Zhang, and Ronald C. Cohen
Atmos. Chem. Phys., 16, 7623–7637, https://doi.org/10.5194/acp-16-7623-2016, https://doi.org/10.5194/acp-16-7623-2016, 2016
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The lifetime of nitrogen oxides (NOx) is evaluated by analysis of field measurements from the southeastern United States. At warm temperatures in the daytime boundary layer, NOx interconverts rapidly with both PAN and alkyl and multifunctional nitrates (RONO2), and the relevant lifetime is the combined lifetime of these three classes. We find that the production of RONO2, followed by hydrolysis to produce nitric acid, is the dominant pathway for NOx removal in an isoprene dominated forest.
Amber M. Ortega, Patrick L. Hayes, Zhe Peng, Brett B. Palm, Weiwei Hu, Douglas A. Day, Rui Li, Michael J. Cubison, William H. Brune, Martin Graus, Carsten Warneke, Jessica B. Gilman, William C. Kuster, Joost de Gouw, Cándido Gutiérrez-Montes, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 7411–7433, https://doi.org/10.5194/acp-16-7411-2016, https://doi.org/10.5194/acp-16-7411-2016, 2016
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An oxidation flow reactor (OFR) was deployed to study secondary organic aerosol (SOA) formation and aging of urban emissions at a wide range of OH exposures during the CalNex campaign in Pasadena, CA, in 2010. Results include linking SOA formation to short-lived reactive compounds, similar elemental composition of reactor-aged emissions to atmospheric aging, changes in OA mass due to condensation of oxidized gas-phase species and heterogeneous oxidation of particle-phase species.
Aikaterini Bougiatioti, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, Panagiotis Kokkalis, George Biskos, Nikolaos Mihalopoulos, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 16, 7389–7409, https://doi.org/10.5194/acp-16-7389-2016, https://doi.org/10.5194/acp-16-7389-2016, 2016
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BBOA from long-range transport exhibits increased CCN concentrations for particles larger than 100 nm. At the same time the hygroscopicity parameter decreased for all particle sizes, as sub-100 nm particles appear to be richer in less hygroscopic organic material, while larger particles become less hygroscopic due to condensation of less hygroscopic gaseous compounds. Finally, atmospheric processing of freshly emitted BBOA to more oxidized organic aerosol can result in a 2-fold increase of κ.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Alexis R. Attwood, Andreas Beyersdorf, Pedro Campuzano-Jost, Annmarie G. Carlton, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Nga L. Ng, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Rebecca A. Washenfelder, Andre Welti, Lu Xu, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 4987–5007, https://doi.org/10.5194/acp-16-4987-2016, https://doi.org/10.5194/acp-16-4987-2016, 2016
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Microscopic pollution particles make the atmosphere look hazy and also cool the earth by sending sunlight back to space. When the air is moist, these particles swell with water and scatter even more sunlight. We showed that particles formed from organic material – which dominates particulate pollution in the southeastern U.S. – does not take up water very effectively, toward the low end of most previous studies. We also found a better way to mathematically describe this swelling process.
Charles A. Brock, Nicholas L. Wagner, Bruce E. Anderson, Andreas Beyersdorf, Pedro Campuzano-Jost, Douglas A. Day, Glenn S. Diskin, Timothy D. Gordon, Jose L. Jimenez, Daniel A. Lack, Jin Liao, Milos Z. Markovic, Ann M. Middlebrook, Anne E. Perring, Matthews S. Richardson, Joshua P. Schwarz, Andre Welti, Luke D. Ziemba, and Daniel M. Murphy
Atmos. Chem. Phys., 16, 5009–5019, https://doi.org/10.5194/acp-16-5009-2016, https://doi.org/10.5194/acp-16-5009-2016, 2016
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Two research aircraft made dozens of vertical profiles over rural areas in the southeastern US in summer 2013. These measurements show that, in addition to how much pollution was present and how moist the atmosphere was, the size of the pollutant particles affected how much sunlight was reflected back to space. These measurements will help climate modelers determine which characteristics of pollution are important to predict with accuracy.
Aikaterini Bougiatioti, Panayiota Nikolaou, Iasonas Stavroulas, Giorgos Kouvarakis, Rodney Weber, Athanasios Nenes, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, https://doi.org/10.5194/acp-16-4579-2016, 2016
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Atmospheric aerosols and relevant parameters were measured in the eastern Mediterranean during summer and fall 2012. Submicron aerosol water can contribute up to 33 % of total mass, and 27.5 % of this can be associated with organics. Using these data, the pH of the submicron aerosols was calculated to be highly acidic, varying from 0.5 to 2.8 and independently of air masses origin. Such pH values could increase nutrient availability and thus sea water productivity of the Mediterranean Sea.
Christopher R. Hoyle, Clare S. Webster, Harald E. Rieder, Athanasios Nenes, Emanuel Hammer, Erik Herrmann, Martin Gysel, Nicolas Bukowiecki, Ernest Weingartner, Martin Steinbacher, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4043–4061, https://doi.org/10.5194/acp-16-4043-2016, https://doi.org/10.5194/acp-16-4043-2016, 2016
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A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from the high-altitude site Jungfraujoch. It is found that cloud droplet formation at the Jungfraujoch is predominantly controlled by the number concentration of aerosol particles. A statistical model based on only the number of particles larger than 80nm can explain 79 % of the observed variance in droplet numbers.
Yong-ha Kim, Sotira Yiacoumi, Athanasios Nenes, and Costas Tsouris
Atmos. Chem. Phys., 16, 3449–3462, https://doi.org/10.5194/acp-16-3449-2016, https://doi.org/10.5194/acp-16-3449-2016, 2016
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Three microphysical approaches are proposed to incorporate mutual effects of particle charging and coagulation in predictions of transient charge and size distributions of atmospheric particles, including radioactive aerosols. The three approaches have different levels of complexities and are applicable to various laboratory and field atmospheric studies. Also, these approaches can be easily incorporated into aerosol transport models at different scales to account for particle charging effects.
Sylvia C. Sullivan, Ricardo Morales Betancourt, Donifan Barahona, and Athanasios Nenes
Atmos. Chem. Phys., 16, 2611–2629, https://doi.org/10.5194/acp-16-2611-2016, https://doi.org/10.5194/acp-16-2611-2016, 2016
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We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
efficiency of various INP.
The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
Bin Yuan, John Liggio, Jeremy Wentzell, Shao-Meng Li, Harald Stark, James M. Roberts, Jessica Gilman, Brian Lerner, Carsten Warneke, Rui Li, Amy Leithead, Hans D. Osthoff, Robert Wild, Steven S. Brown, and Joost A. de Gouw
Atmos. Chem. Phys., 16, 2139–2153, https://doi.org/10.5194/acp-16-2139-2016, https://doi.org/10.5194/acp-16-2139-2016, 2016
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We describe high-resolution measurements of nitrated phenols using a time-of-flight chemical ionization mass spectrometer (ToF-CIMS). Strong diurnal profiles were observed for nitrated phenols, with concentration maxima at night. Box model simulations were able to reproduce the measured nitrated phenols.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738, https://doi.org/10.5194/acp-16-715-2016, https://doi.org/10.5194/acp-16-715-2016, 2016
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Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
R. J. Wild, P. M. Edwards, T. S. Bates, R. C. Cohen, J. A. de Gouw, W. P. Dubé, J. B. Gilman, J. Holloway, J. Kercher, A. R. Koss, L. Lee, B. M. Lerner, R. McLaren, P. K. Quinn, J. M. Roberts, J. Stutz, J. A. Thornton, P. R. Veres, C. Warneke, E. Williams, C. J. Young, B. Yuan, K. J. Zarzana, and S. S. Brown
Atmos. Chem. Phys., 16, 573–583, https://doi.org/10.5194/acp-16-573-2016, https://doi.org/10.5194/acp-16-573-2016, 2016
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High wintertime ozone levels have been observed in the Uintah Basin, Utah, a sparsely populated rural region with intensive oil and gas operations. The reactive nitrogen budget plays an important role in tropospheric ozone formation, and we find that nighttime chemistry has a large effect on its partitioning. Much of the oxidation of reactive nitrogen during a high-ozone year occurred via heterogeneous uptake onto aerosol at night, keeping NOx at concentrations comparable to a low-ozone year.
J. B. Gilman, B. M. Lerner, W. C. Kuster, P. D. Goldan, C. Warneke, P. R. Veres, J. M. Roberts, J. A. de Gouw, I. R. Burling, and R. J. Yokelson
Atmos. Chem. Phys., 15, 13915–13938, https://doi.org/10.5194/acp-15-13915-2015, https://doi.org/10.5194/acp-15-13915-2015, 2015
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A comprehensive suite of instruments was used to quantify the emissions of over 200 organic and inorganic gases from 56 laboratory burns of 18 different biomass fuel types common in the southeastern, southwestern, or northern United States. Emission ratios relative to carbon monoxide (CO) are used to characterize the composition of gases emitted by mass; OH reactivity; and potential secondary organic aerosol (SOA) precursors for the three different U.S. fuel regions presented here.
B. R. Ayres, H. M. Allen, D. C. Draper, S. S. Brown, R. J. Wild, J. L. Jimenez, D. A. Day, P. Campuzano-Jost, W. Hu, J. de Gouw, A. Koss, R. C. Cohen, K. C. Duffey, P. Romer, K. Baumann, E. Edgerton, S. Takahama, J. A. Thornton, B. H. Lee, F. D. Lopez-Hilfiker, C. Mohr, P. O. Wennberg, T. B. Nguyen, A. Teng, A. H. Goldstein, K. Olson, and J. L. Fry
Atmos. Chem. Phys., 15, 13377–13392, https://doi.org/10.5194/acp-15-13377-2015, https://doi.org/10.5194/acp-15-13377-2015, 2015
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This paper reports atmospheric gas- and aerosol-phase field measurements from the southeastern United States in summer 2013 to demonstrate that the oxidation of biogenic volatile organic compounds by nitrate radical produces a substantial amount of secondary organic aerosol in this region. This process, driven largely by monoterpenes, results in a comparable aerosol nitrate production rate to inorganic nitrate formation by heterogeneous uptake of HNO3 onto dust particles.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
F. Xiong, K. M. McAvey, K. A. Pratt, C. J. Groff, M. A. Hostetler, M. A. Lipton, T. K. Starn, J. V. Seeley, S. B. Bertman, A. P. Teng, J. D. Crounse, T. B. Nguyen, P. O. Wennberg, P. K. Misztal, A. H. Goldstein, A. B. Guenther, A. R. Koss, K. F. Olson, J. A. de Gouw, K. Baumann, E. S. Edgerton, P. A. Feiner, L. Zhang, D. O. Miller, W. H. Brune, and P. B. Shepson
Atmos. Chem. Phys., 15, 11257–11272, https://doi.org/10.5194/acp-15-11257-2015, https://doi.org/10.5194/acp-15-11257-2015, 2015
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Hydroxynitrates from isoprene oxidation were quantified both in the laboratory and through field studies. The yield of hydroxynitrates 9(+4/-3)% derived from chamber experiments was applied in a zero-dimensional model to simulate the production and loss of isoprene hydroxynitrates in an ambient environment during the 2013 Southern Oxidant and Aerosol Study (SOAS). NOx was determined to be the limiting factor for the formation of isoprene hydroxynitrates during SOAS.
C. Huang, H. L. Wang, L. Li, Q. Wang, Q. Lu, J. A. de Gouw, M. Zhou, S. A. Jing, J. Lu, and C. H. Chen
Atmos. Chem. Phys., 15, 11081–11096, https://doi.org/10.5194/acp-15-11081-2015, https://doi.org/10.5194/acp-15-11081-2015, 2015
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SOA formations from vehicle exhausts and gas evaporation contribute 40% and 60% of total organic aerosols observed in summer and winter in urban Shanghai. Diesel vehicles, which accounted for less than 20% of vehicle kilometers of travel, contribute the most to vehicular POA emissions and SOA production in urban Shanghai. Intermediate-volatile organic compounds (IVOCs) in vehicle exhausts contribute greatly to SOA formation in the urban atmosphere of China.
P. S. Kim, D. J. Jacob, J. A. Fisher, K. Travis, K. Yu, L. Zhu, R. M. Yantosca, M. P. Sulprizio, J. L. Jimenez, P. Campuzano-Jost, K. D. Froyd, J. Liao, J. W. Hair, M. A. Fenn, C. F. Butler, N. L. Wagner, T. D. Gordon, A. Welti, P. O. Wennberg, J. D. Crounse, J. M. St. Clair, A. P. Teng, D. B. Millet, J. P. Schwarz, M. Z. Markovic, and A. E. Perring
Atmos. Chem. Phys., 15, 10411–10433, https://doi.org/10.5194/acp-15-10411-2015, https://doi.org/10.5194/acp-15-10411-2015, 2015
L. Lee, P. J. Wooldridge, J. deGouw, S. S. Brown, T. S. Bates, P. K. Quinn, and R. C. Cohen
Atmos. Chem. Phys., 15, 9313–9325, https://doi.org/10.5194/acp-15-9313-2015, https://doi.org/10.5194/acp-15-9313-2015, 2015
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Secondary organic aerosol affects both the environment and human health. We characterized the aerosol composition in Uintah Basin by measuring the concentration of nitrooxy group moiety which is produced through chemical interaction of volatile organic compounds and NOx emitted largely from local human activity. We found nitrooxy compounds to be a persistent, if not dominant, portion of fine aerosol mass. Similar results may be expected from emissions due to traffic in cities.
N. Kalivitis, V.-M. Kerminen, G. Kouvarakis, I. Stavroulas, A. Bougiatioti, A. Nenes, H. E. Manninen, T. Petäjä, M. Kulmala, and N. Mihalopoulos
Atmos. Chem. Phys., 15, 9203–9215, https://doi.org/10.5194/acp-15-9203-2015, https://doi.org/10.5194/acp-15-9203-2015, 2015
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Cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is presented, and this is the first direct evidence of CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the active NPF period.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. M. Cerully, A. Bougiatioti, J. R. Hite Jr., H. Guo, L. Xu, N. L. Ng, R. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, https://doi.org/10.5194/acp-15-8679-2015, 2015
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The hygroscopicity of SE US aerosol is mostly water-soluble, with a hygroscopicity that is insensitive to partial volatilization in a thermodenuder.
The most and least oxidized components of the aerosol are the most hygroscopic of organic constituents.
No clear relationship was found between organic aerosol hygroscopicity and oxygen-to-carbon ratio.
The aerosol factors covary in a way that induces the observed diurnal invariance in total organic hygroscopicity.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
P. R. Veres, J. M. Roberts, R. J. Wild, P. M. Edwards, S. S. Brown, T. S. Bates, P. K. Quinn, J. E. Johnson, R. J. Zamora, and J. de Gouw
Atmos. Chem. Phys., 15, 8101–8114, https://doi.org/10.5194/acp-15-8101-2015, https://doi.org/10.5194/acp-15-8101-2015, 2015
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In this paper laboratory work is documented establishing iodide ion chemical ionization mass spectrometry (I- CIMS) as a sensitive method for the unambiguous detection of peroxynitric acid (HO2NO2; PNA). A dynamic calibration source for HO2NO2, HO2, and HONO was developed and calibrated using a novel total NOy detector (NOy CaRDS). The ambient observations of HO2NO2 using I- CIMS made during the 2013 and 2014 Uintah Basin Wintertime Ozone Study (UBWOS) are presented.
Y. Shinozuka, A. D. Clarke, A. Nenes, A. Jefferson, R. Wood, C. S. McNaughton, J. Ström, P. Tunved, J. Redemann, K. L. Thornhill, R. H. Moore, T. L. Lathem, J. J. Lin, and Y. J. Yoon
Atmos. Chem. Phys., 15, 7585–7604, https://doi.org/10.5194/acp-15-7585-2015, https://doi.org/10.5194/acp-15-7585-2015, 2015
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
S. Myriokefalitakis, N. Daskalakis, N. Mihalopoulos, A. R. Baker, A. Nenes, and M. Kanakidou
Biogeosciences, 12, 3973–3992, https://doi.org/10.5194/bg-12-3973-2015, https://doi.org/10.5194/bg-12-3973-2015, 2015
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The global atmospheric cycle of Fe is simulated accounting for natural and combustion sources, proton- and organic ligand-promoted Fe dissolution from dust aerosol and changes in anthropogenic emissions, and thus in atmospheric acidity. Simulations show that Fe dissolution may have increased in the last 150 years and is expected to decrease due to air pollution regulations. Reductions in dissolved-Fe deposition can further limit the primary productivity over high-nutrient-low-chlorophyll water.
N. L. Wagner, C. A. Brock, W. M. Angevine, A. Beyersdorf, P. Campuzano-Jost, D. Day, J. A. de Gouw, G. S. Diskin, T. D. Gordon, M. G. Graus, J. S. Holloway, G. Huey, J. L. Jimenez, D. A. Lack, J. Liao, X. Liu, M. Z. Markovic, A. M. Middlebrook, T. Mikoviny, J. Peischl, A. E. Perring, M. S. Richardson, T. B. Ryerson, J. P. Schwarz, C. Warneke, A. Welti, A. Wisthaler, L. D. Ziemba, and D. M. Murphy
Atmos. Chem. Phys., 15, 7085–7102, https://doi.org/10.5194/acp-15-7085-2015, https://doi.org/10.5194/acp-15-7085-2015, 2015
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This paper investigates the summertime vertical profile of aerosol over the southeastern US using in situ measurements collected from aircraft. We use a vertical mixing model and measurements of CO to predict the vertical profile of aerosol that we would expect from vertical mixing alone and compare with the observed aerosol profile. We found a modest enhancement of aerosol in the cloudy transition layer during shallow cumulus convection and attribute the enhancement to local aerosol formation.
D. B. Millet, M. Baasandorj, D. K. Farmer, J. A. Thornton, K. Baumann, P. Brophy, S. Chaliyakunnel, J. A. de Gouw, M. Graus, L. Hu, A. Koss, B. H. Lee, F. D. Lopez-Hilfiker, J. A. Neuman, F. Paulot, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, B. J. Williams, and J. Xu
Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, https://doi.org/10.5194/acp-15-6283-2015, 2015
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Formic acid (HCOOH) is an abundant atmospheric acid that affects precipitation chemistry and acidity. HCOOH measurements over the USA are 2-3× larger than can be explained by known sources and sinks, revealing a key gap in current understanding. Observations indicate a large biogenic source plus chemical production across a range of precursors. Model simulations cannot capture the HCOOH diurnal amplitude or nocturnal profile, implying a deposition bias and possibly even larger missing source.
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
A. R. Koss, J. de Gouw, C. Warneke, J. B. Gilman, B. M. Lerner, M. Graus, B. Yuan, P. Edwards, S. S. Brown, R. Wild, J. M. Roberts, T. S. Bates, and P. K. Quinn
Atmos. Chem. Phys., 15, 5727–5741, https://doi.org/10.5194/acp-15-5727-2015, https://doi.org/10.5194/acp-15-5727-2015, 2015
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Extraction of natural gas and oil is associated with a range of possible atmospheric environmental issues. Here we present an analysis of gas-phase hydrocarbon measurements taken in an oil and natural gas extraction area in Utah during a period of high wintertime ozone. We are able to constrain important chemical parameters related to emission sources and rates, hydrocarbon photochemistry, and VOC composition.
K. R. Baker, A. G. Carlton, T. E. Kleindienst, J. H. Offenberg, M. R. Beaver, D. R. Gentner, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, J. B. Gilman, J. A. de Gouw, M. C. Woody, H. O. T. Pye, J. T. Kelly, M. Lewandowski, M. Jaoui, P. S. Stevens, W. H. Brune, Y.-H. Lin, C. L. Rubitschun, and J. D. Surratt
Atmos. Chem. Phys., 15, 5243–5258, https://doi.org/10.5194/acp-15-5243-2015, https://doi.org/10.5194/acp-15-5243-2015, 2015
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This work details the evaluation of PM2.5 carbon, VOC precursors, and OH estimated by the CMAQ photochemical transport model using routine and special measurements from the 2010 CalNex field study. Here, CMAQ and most recent emissions inventory (2011 NEI) are used to generate model PM2.5 OC estimates that are examined in novel ways including primary vs. secondary formation, fossil vs. contemporary carbon, OH and HO2 evaluation, and the relationship between key VOC precursors and SOC tracers.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, https://doi.org/10.5194/acp-15-2775-2015, 2015
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We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
N. Hiranuma, S. Augustin-Bauditz, H. Bingemer, C. Budke, J. Curtius, A. Danielczok, K. Diehl, K. Dreischmeier, M. Ebert, F. Frank, N. Hoffmann, K. Kandler, A. Kiselev, T. Koop, T. Leisner, O. Möhler, B. Nillius, A. Peckhaus, D. Rose, S. Weinbruch, H. Wex, Y. Boose, P. J. DeMott, J. D. Hader, T. C. J. Hill, Z. A. Kanji, G. Kulkarni, E. J. T. Levin, C. S. McCluskey, M. Murakami, B. J. Murray, D. Niedermeier, M. D. Petters, D. O'Sullivan, A. Saito, G. P. Schill, T. Tajiri, M. A. Tolbert, A. Welti, T. F. Whale, T. P. Wright, and K. Yamashita
Atmos. Chem. Phys., 15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, https://doi.org/10.5194/acp-15-2489-2015, 2015
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Seventeen ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of illite NX. All data showed a similar temperature trend, but the measured ice nucleation activity was on average smaller for the wet suspended samples and higher for the dry-dispersed aerosol samples at high temperatures. A continued investigation and collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
C. Warneke, P. Veres, S. M. Murphy, J. Soltis, R. A. Field, M. G. Graus, A. Koss, S.-M. Li, R. Li, B. Yuan, J. M. Roberts, and J. A. de Gouw
Atmos. Meas. Tech., 8, 411–420, https://doi.org/10.5194/amt-8-411-2015, https://doi.org/10.5194/amt-8-411-2015, 2015
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
L. Lee, P. J. Wooldridge, J. B. Gilman, C. Warneke, J. de Gouw, and R. C. Cohen
Atmos. Chem. Phys., 14, 12441–12454, https://doi.org/10.5194/acp-14-12441-2014, https://doi.org/10.5194/acp-14-12441-2014, 2014
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Alkyl nitrate formation is known to be an important sink of NOx in a wide range of environments. In a study in the Uintah basin in 2012, we find that formation of these compounds represents a more rapid NOx (NO + NO2) sink than does nitric acid formation. This rapid formation is in large part due to the low mean temperature (~0°C) during the study and is consistent with laboratory observations.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
R. Li, C. Warneke, M. Graus, R. Field, F. Geiger, P. R. Veres, J. Soltis, S.-M. Li, S. M. Murphy, C. Sweeney, G. Pétron, J. M. Roberts, and J. de Gouw
Atmos. Meas. Tech., 7, 3597–3610, https://doi.org/10.5194/amt-7-3597-2014, https://doi.org/10.5194/amt-7-3597-2014, 2014
C. Warneke, F. Geiger, P. M. Edwards, W. Dube, G. Pétron, J. Kofler, A. Zahn, S. S. Brown, M. Graus, J. B. Gilman, B. M. Lerner, J. Peischl, T. B. Ryerson, J. A. de Gouw, and J. M. Roberts
Atmos. Chem. Phys., 14, 10977–10988, https://doi.org/10.5194/acp-14-10977-2014, https://doi.org/10.5194/acp-14-10977-2014, 2014
R. Morales Betancourt and A. Nenes
Geosci. Model Dev., 7, 2345–2357, https://doi.org/10.5194/gmd-7-2345-2014, https://doi.org/10.5194/gmd-7-2345-2014, 2014
W. Ait-Helal, A. Borbon, S. Sauvage, J. A. de Gouw, A. Colomb, V. Gros, F. Freutel, M. Crippa, C. Afif, U. Baltensperger, M. Beekmann, J.-F. Doussin, R. Durand-Jolibois, I. Fronval, N. Grand, T. Leonardis, M. Lopez, V. Michoud, K. Miet, S. Perrier, A. S. H. Prévôt, J. Schneider, G. Siour, P. Zapf, and N. Locoge
Atmos. Chem. Phys., 14, 10439–10464, https://doi.org/10.5194/acp-14-10439-2014, https://doi.org/10.5194/acp-14-10439-2014, 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
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, https://doi.org/10.5194/gmd-7-1733-2014, 2014
B. Gantt, J. He, X. Zhang, Y. Zhang, and A. Nenes
Atmos. Chem. Phys., 14, 7485–7497, https://doi.org/10.5194/acp-14-7485-2014, https://doi.org/10.5194/acp-14-7485-2014, 2014
G. Drozd, J. Woo, S. A. K. Häkkinen, A. Nenes, and V. F. McNeill
Atmos. Chem. Phys., 14, 5205–5215, https://doi.org/10.5194/acp-14-5205-2014, https://doi.org/10.5194/acp-14-5205-2014, 2014
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen
Atmos. Meas. Tech., 7, 1377–1384, https://doi.org/10.5194/amt-7-1377-2014, https://doi.org/10.5194/amt-7-1377-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
R. Morales Betancourt and A. Nenes
Atmos. Chem. Phys., 14, 4809–4826, https://doi.org/10.5194/acp-14-4809-2014, https://doi.org/10.5194/acp-14-4809-2014, 2014
K. C. Wells, D. B. Millet, K. E. Cady-Pereira, M. W. Shephard, D. K. Henze, N. Bousserez, E. C. Apel, J. de Gouw, C. Warneke, and H. B. Singh
Atmos. Chem. Phys., 14, 2555–2570, https://doi.org/10.5194/acp-14-2555-2014, https://doi.org/10.5194/acp-14-2555-2014, 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
A. M. Ortega, D. A. Day, M. J. Cubison, W. H. Brune, D. Bon, J. A. de Gouw, and J. L. Jimenez
Atmos. Chem. Phys., 13, 11551–11571, https://doi.org/10.5194/acp-13-11551-2013, https://doi.org/10.5194/acp-13-11551-2013, 2013
S. S. Brown, W. P. Dubé, R. Bahreini, A. M. Middlebrook, C. A. Brock, C. Warneke, J. A. de Gouw, R. A. Washenfelder, E. Atlas, J. Peischl, T. B. Ryerson, J. S. Holloway, J. P. Schwarz, R. Spackman, M. Trainer, D. D. Parrish, F. C. Fehshenfeld, and A. R. Ravishankara
Atmos. Chem. Phys., 13, 11317–11337, https://doi.org/10.5194/acp-13-11317-2013, https://doi.org/10.5194/acp-13-11317-2013, 2013
Z. A. Kanji, A. Welti, C. Chou, O. Stetzer, and U. Lohmann
Atmos. Chem. Phys., 13, 9097–9118, https://doi.org/10.5194/acp-13-9097-2013, https://doi.org/10.5194/acp-13-9097-2013, 2013
M. Trail, A. P. Tsimpidi, P. Liu, K. Tsigaridis, Y. Hu, A. Nenes, and A. G. Russell
Geosci. Model Dev., 6, 1429–1445, https://doi.org/10.5194/gmd-6-1429-2013, https://doi.org/10.5194/gmd-6-1429-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 2013
R. H. Moore, V. A. Karydis, S. L. Capps, T. L. Lathem, and A. Nenes
Atmos. Chem. Phys., 13, 4235–4251, https://doi.org/10.5194/acp-13-4235-2013, https://doi.org/10.5194/acp-13-4235-2013, 2013
R. A. Washenfelder, J. M. Flores, C. A. Brock, S. S. Brown, and Y. Rudich
Atmos. Meas. Tech., 6, 861–877, https://doi.org/10.5194/amt-6-861-2013, https://doi.org/10.5194/amt-6-861-2013, 2013
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756, https://doi.org/10.5194/acp-13-2735-2013, https://doi.org/10.5194/acp-13-2735-2013, 2013
D. A. Lack, R. Bahreini, J. M. Langridge, J. B. Gilman, and A. M. Middlebrook
Atmos. Chem. Phys., 13, 2415–2422, https://doi.org/10.5194/acp-13-2415-2013, https://doi.org/10.5194/acp-13-2415-2013, 2013
M. Frosch, M. Bilde, A. Nenes, A. P. Praplan, Z. Jurányi, J. Dommen, M. Gysel, E. Weingartner, and U. Baltensperger
Atmos. Chem. Phys., 13, 2283–2297, https://doi.org/10.5194/acp-13-2283-2013, https://doi.org/10.5194/acp-13-2283-2013, 2013
Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
R. J. Yokelson, I. R. Burling, J. B. Gilman, C. Warneke, C. E. Stockwell, J. de Gouw, S. K. Akagi, S. P. Urbanski, P. Veres, J. M. Roberts, W. C. Kuster, J. Reardon, D. W. T. Griffith, T. J. Johnson, S. Hosseini, J. W. Miller, D. R. Cocker III, H. Jung, and D. R. Weise
Atmos. Chem. Phys., 13, 89–116, https://doi.org/10.5194/acp-13-89-2013, https://doi.org/10.5194/acp-13-89-2013, 2013
C. R. Lonsdale, R. G. Stevens, C. A. Brock, P. A. Makar, E. M. Knipping, and J. R. Pierce
Atmos. Chem. Phys., 12, 11519–11531, https://doi.org/10.5194/acp-12-11519-2012, https://doi.org/10.5194/acp-12-11519-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Measurement report: Increasing trend of atmospheric ion concentrations in the boreal forest
Vertical profiles of cloud condensation nuclei number concentration and its empirical estimate from aerosol optical properties over the North China Plain
Measurement report: The Urmia playa as a source of airborne dust and ice-nucleating particles – Part 1: Correlation between soils and airborne samples
Constraining the particle-scale diversity of black carbon light absorption using a unified framework
Survival probability of new atmospheric particles: closure between theory and measurements from 1.4 to 100 nm
Predicting atmospheric background number concentration of ice-nucleating particles in the Arctic
Different effects of anthropogenic emissions and aging processes on the mixing state of soot particles in the nucleation and accumulation modes
Fluorescence characteristics, absorption properties, and radiative effects of water-soluble organic carbon in seasonal snow across northeastern China
Measurement report: Size distributions of urban aerosols down to 1 nm from long-term measurements
Rapid reappearance of air pollution after cold air outbreaks in northern and eastern China
On the relation between apparent ion and total particle growth rates in the boreal forest and related chamber experiments
Assessment of NAAPS-RA performance in Maritime Southeast Asia during CAMP2Ex
Comparison of particle number size distribution trends in ground measurements and climate models
Aerosol size distribution changes in FIREX-AQ biomass burning plumes: the impact of plume concentration on coagulation and OA condensation/evaporation
Impact of water uptake and mixing state on submicron particle deposition in the human respiratory tract (HRT) based on explicit hygroscopicity measurements at HRT-like conditions
Parameterizations of size distribution and refractive index of biomass burning organic aerosol with black carbon content
Newly identified climatically and environmentally significant high-latitude dust sources
Airborne observations during KORUS-AQ show that aerosol optical depths are more spatially self-consistent than aerosol intensive properties
Using aircraft measurements to characterize subgrid-scale variability of aerosol properties near the Atmospheric Radiation Measurement Southern Great Plains site
Measurement report: A multi-year study on the impacts of Chinese New Year celebrations on air quality in Beijing, China
A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation: Insights from the MOSAiC expedition
An Evaluation of Biomass Burning Aerosol Mass, Extinction, and Size Distribution in GEOS using Observations from CAMP2Ex
Mixing state of black carbon at different atmospheres in north and southwest China
Columnar and surface urban aerosol in the Moscow megacity according to measurements and simulations with the COSMO-ART model
Vertical aerosol particle exchange in the marine boundary layer estimated from helicopter-borne measurements in the Azores region
Circum-Antarctic abundance and properties of CCN and INPs
The ice-nucleating activity of African mineral dust in the Caribbean boundary layer
Biomass burning and marine aerosol processing over the southeast Atlantic Ocean: a TEM single-particle analysis
Measurement report: Atmopsheric new particle formation in a peri-urban site in Lille, Northern France
Volatility parameterization of ambient organic aerosols at a rural site of the North China Plain
Juha Sulo, Janne Lampilahti, Xuemeng Chen, Jenni Kontkanen, Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Katrianne Lehtipalo
Atmos. Chem. Phys., 22, 15223–15242, https://doi.org/10.5194/acp-22-15223-2022, https://doi.org/10.5194/acp-22-15223-2022, 2022
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We measured atmospheric ion concentrations continuously in a boreal forest between 2005 and 2021 and observed an increasing interannual trend. The increase in cluster ion concentrations can be largely explained by an overall decreasing level of anthropogenic aerosols in the boreal forest. This suggests that the role of ions in atmospheric new particle formation may be more important in the future.
Rui Zhang, Yuying Wang, Zhanqing Li, Zhibin Wang, Russell R. Dickerson, Xinrong Ren, Hao He, Fei Wang, Ying Gao, Xi Chen, Jialu Xu, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 14879–14891, https://doi.org/10.5194/acp-22-14879-2022, https://doi.org/10.5194/acp-22-14879-2022, 2022
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Factors of cloud condensation nuclei number concentration (NCCN) profiles determined in the North China Plain include air mass sources, temperature structure, anthropogenic emissions, and terrain distribution. Cloud condensation nuclei (CCN) spectra suggest that the ability of aerosol activation into CCN is stronger in southeasterly than in northwesterly air masses and stronger in the free atmosphere than near the surface. A good method to parameterize NCCN from aerosol optical data is found.
Nikou Hamzehpour, Claudia Marcolli, Sara Pashai, Kristian Klumpp, and Thomas Peter
Atmos. Chem. Phys., 22, 14905–14930, https://doi.org/10.5194/acp-22-14905-2022, https://doi.org/10.5194/acp-22-14905-2022, 2022
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Playa surfaces in Iran that emerged through Lake Urmia (LU) desiccation have become a relevant dust source of regional relevance. Here, we identify highly erodible LU playa surfaces and determine their physicochemical properties and mineralogical composition and perform emulsion-freezing experiments with them. We find high ice nucleation activities (up to 250 K) that correlate positively with organic matter and clay content and negatively with pH, salinity, K-feldspars, and quartz.
Payton Beeler and Rajan K. Chakrabarty
Atmos. Chem. Phys., 22, 14825–14836, https://doi.org/10.5194/acp-22-14825-2022, https://doi.org/10.5194/acp-22-14825-2022, 2022
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Understanding and parameterizing the influences of black carbon (BC) particle morphology and compositional heterogeneity on its light absorption represent a fundamental problem. We develop scaling laws using a single unifying parameter that effectively encompasses large-scale diversity observed in BC light absorption on a per-particle basis. The laws help reconcile the disparities between field observations and model predictions. Our framework is packaged in an open-source Python application.
Runlong Cai, Chenjuan Deng, Dominik Stolzenburg, Chenxi Li, Junchen Guo, Veli-Matti Kerminen, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 22, 14571–14587, https://doi.org/10.5194/acp-22-14571-2022, https://doi.org/10.5194/acp-22-14571-2022, 2022
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The survival probability of new particles is the key parameter governing their influences on the atmosphere and climate, yet the knowledge of particle survival in the atmosphere is rather limited. We propose methods to compute the size-resolved particle survival probability and validate them using simulations and measurements from diverse environments. Using these methods, we could explain particle survival from the cluster size to the cloud condensation nuclei size.
Guangyu Li, Jörg Wieder, Julie T. Pasquier, Jan Henneberger, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 14441–14454, https://doi.org/10.5194/acp-22-14441-2022, https://doi.org/10.5194/acp-22-14441-2022, 2022
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The concentration of ice-nucleating particles (INPs) is atmospherically relevant for primary ice formation in clouds. In this work, from 12 weeks of field measurement data in the Arctic, we developed a new parameterization to predict INP concentrations applicable for pristine background conditions based only on temperature. The INP parameterization could improve the cloud microphysical representation in climate models, aiding in Arctic climate predictions.
Yuying Wang, Rong Hu, Qiuyan Wang, Zhanqing Li, Maureen Cribb, Yele Sun, Xiaorui Song, Yi Shang, Yixuan Wu, Xin Huang, and Yuxiang Wang
Atmos. Chem. Phys., 22, 14133–14146, https://doi.org/10.5194/acp-22-14133-2022, https://doi.org/10.5194/acp-22-14133-2022, 2022
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The mixing state of size-resolved soot particles and their influencing factors were investigated. The results suggest anthropogenic emissions and aging processes have diverse impacts on the mixing state of soot particles in different modes. Considering that the mixing state of soot particles is crucial to model aerosol absorption, this finding is important to study particle growth and the warming effect of black carbon aerosols.
Xiaoying Niu, Wei Pu, Pingqing Fu, Yang Chen, Yuxuan Xing, Dongyou Wu, Ziqi Chen, Tenglong Shi, Yue Zhou, Hui Wen, and Xin Wang
Atmos. Chem. Phys., 22, 14075–14094, https://doi.org/10.5194/acp-22-14075-2022, https://doi.org/10.5194/acp-22-14075-2022, 2022
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In this study, we do the first investigation of WSOC in seasonal snow of northeastern China. The results revealed the regional-specific compositions and sources of WSOC due to different natural environments and anthropogenic activities. The abundant concentrations of WSOC and its absorption properties contributed to a crucial impact on the snow albedo and radiative effect. We established that our study could raise awareness of carbon cycling processes, hydrological processes, and climate change.
Chenjuan Deng, Yiran Li, Chao Yan, Jin Wu, Runlong Cai, Dongbin Wang, Yongchun Liu, Juha Kangasluoma, Veli-Matti Kerminen, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 22, 13569–13580, https://doi.org/10.5194/acp-22-13569-2022, https://doi.org/10.5194/acp-22-13569-2022, 2022
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The size distributions of urban atmospheric particles convey important information on their origins and impacts. This study investigates the characteristics of typical particle size distributions and key gaseous precursors in the long term in urban Beijing. A fitting function is proposed to represent and help interpret size distribution including particles and gaseous precursors. In addition to NPF (new particle formation) as the major source, vehicles can emit sub-3 nm particles as well
Qian Liu, Guixing Chen, Lifang Sheng, and Toshiki Iwasaki
Atmos. Chem. Phys., 22, 13371–13388, https://doi.org/10.5194/acp-22-13371-2022, https://doi.org/10.5194/acp-22-13371-2022, 2022
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Air pollution can be cleaned up quickly by a cold air outbreak (CAO) but reappears after a CAO. By quantifying the CAO properties, we find the coldness and depth of the cold air mass are key factors affecting the rapid (slow) reappearance of air pollution through modulating the atmospheric boundary layer height and stability. We also find that the spatial pattern of CAO in high-latitude Eurasia a few days ahead can be recognized as a precursor for the reappearance of air pollution.
Loïc Gonzalez Carracedo, Katrianne Lehtipalo, Lauri R. Ahonen, Nina Sarnela, Sebastian Holm, Juha Kangasluoma, Markku Kulmala, Paul M. Winkler, and Dominik Stolzenburg
Atmos. Chem. Phys., 22, 13153–13166, https://doi.org/10.5194/acp-22-13153-2022, https://doi.org/10.5194/acp-22-13153-2022, 2022
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Fast nanoparticle growth is essential for the survival of new aerosol particles in the atmosphere and hence their contribution to the climate. We show that using naturally charged ions for growth calculations can cause a significant error. During the diurnal cycle, the importance of ion-induced and neutral nucleation varies, causing the ion population to have a slower measurable apparent growth. Results suggest that data from ion spectrometers need to be considered with great care below 3 nm.
Eva-Lou Edwards, Jeffrey S. Reid, Peng Xian, Sharon P. Burton, Anthony L. Cook, Ewan C. Crosbie, Marta A. Fenn, Richard A. Ferrare, Sean W. Freeman, John W. Hair, David B. Harper, Chris A. Hostetler, Claire E. Robinson, Amy Jo Scarino, Michael A. Shook, G. Alexander Sokolowsky, Susan C. van den Heever, Edward L. Winstead, Sarah Woods, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 22, 12961–12983, https://doi.org/10.5194/acp-22-12961-2022, https://doi.org/10.5194/acp-22-12961-2022, 2022
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This study compares NAAPS-RA model simulations of aerosol optical thickness (AOT) and extinction to those retrieved with a high spectral resolution lidar near the Philippines. Agreement for AOT was good, and extinction agreement was strongest below 1500 m. Substituting dropsonde relative humidities into NAAPS-RA did not drastically improve agreement, and we discuss potential reasons why. Accurately modeling future conditions in this region is crucial due to its susceptibility to climate change.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Ruiqi Man, Zhijun Wu, Taomou Zong, Aristeidis Voliotis, Yanting Qiu, Johannes Größ, Dominik van Pinxteren, Limin Zeng, Hartmut Herrmann, Alfred Wiedensohler, and Min Hu
Atmos. Chem. Phys., 22, 12387–12399, https://doi.org/10.5194/acp-22-12387-2022, https://doi.org/10.5194/acp-22-12387-2022, 2022
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Regional and total deposition doses for different age groups were quantified based on explicit hygroscopicity measurements. We found that particle hygroscopic growth led to a reduction (~24 %) in the total dose. The deposition rate of hygroscopic particles was higher in the daytime, while hydrophobic particles exhibited a higher rate at night and during rush hours. The results will deepen the understanding of the impact of hygroscopicity and the mixing state on deposition patterns in the lungs.
Biao Luo, Ye Kuang, Shan Huang, Qicong Song, Weiwei Hu, Wei Li, Yuwen Peng, Duohong Chen, Dingli Yue, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 22, 12401–12415, https://doi.org/10.5194/acp-22-12401-2022, https://doi.org/10.5194/acp-22-12401-2022, 2022
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We performed comprehensive analysis on biomass burning organic aerosol (BBOA) size distributions, as well as mass scattering and absorption efficiencies, with an improved method of on-line quantification of brown carbon absorptions. Both BBOA volume size distribution and retrieved refractive index depend highly on combustion conditions represented by the black carbon content, which has significant implications for BBOA climate effect simulations.
Outi Meinander, Pavla Dagsson-Waldhauserova, Pavel Amosov, Elena Aseyeva, Cliff Atkins, Alexander Baklanov, Clarissa Baldo, Sarah L. Barr, Barbara Barzycka, Liane G. Benning, Bojan Cvetkovic, Polina Enchilik, Denis Frolov, Santiago Gassó, Konrad Kandler, Nikolay Kasimov, Jan Kavan, James King, Tatyana Koroleva, Viktoria Krupskaya, Markku Kulmala, Monika Kusiak, Hanna K. Lappalainen, Michał Laska, Jerome Lasne, Marek Lewandowski, Bartłomiej Luks, James B. McQuaid, Beatrice Moroni, Benjamin Murray, Ottmar Möhler, Adam Nawrot, Slobodan Nickovic, Norman T. O’Neill, Goran Pejanovic, Olga Popovicheva, Keyvan Ranjbar, Manolis Romanias, Olga Samonova, Alberto Sanchez-Marroquin, Kerstin Schepanski, Ivan Semenkov, Anna Sharapova, Elena Shevnina, Zongbo Shi, Mikhail Sofiev, Frédéric Thevenet, Throstur Thorsteinsson, Mikhail Timofeev, Nsikanabasi Silas Umo, Andreas Uppstu, Darya Urupina, György Varga, Tomasz Werner, Olafur Arnalds, and Ana Vukovic Vimic
Atmos. Chem. Phys., 22, 11889–11930, https://doi.org/10.5194/acp-22-11889-2022, https://doi.org/10.5194/acp-22-11889-2022, 2022
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High-latitude dust (HLD) is a short-lived climate forcer, air pollutant, and nutrient source. Our results suggest a northern HLD belt at 50–58° N in Eurasia and 50–55° N in Canada and at >60° N in Eurasia and >58° N in Canada. Our addition to the previously identified global dust belt (GDB) provides crucially needed information on the extent of active HLD sources with both direct and indirect impacts on climate and environment in remote regions, which are often poorly understood and predicted.
Samuel E. LeBlanc, Michal Segal-Rozenhaimer, Jens Redemann, Connor Flynn, Roy R. Johnson, Stephen E. Dunagan, Robert Dahlgren, Jhoon Kim, Myungje Choi, Arlindo da Silva, Patricia Castellanos, Qian Tan, Luke Ziemba, Kenneth Lee Thornhill, and Meloë Kacenelenbogen
Atmos. Chem. Phys., 22, 11275–11304, https://doi.org/10.5194/acp-22-11275-2022, https://doi.org/10.5194/acp-22-11275-2022, 2022
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Airborne observations of atmospheric particles and pollution over Korea during a field campaign in May–June 2016 showed that the smallest atmospheric particles are present in the lowest 2 km of the atmosphere. The aerosol size is more spatially variable than optical thickness. We show this with remote sensing (4STAR), in situ (LARGE) observations, satellite measurements (GOCI), and modeled properties (MERRA-2), and it is contrary to the current understanding.
Jerome D. Fast, David M. Bell, Gourihar Kulkarni, Jiumeng Liu, Fan Mei, Georges Saliba, John E. Shilling, Kaitlyn Suski, Jason Tomlinson, Jian Wang, Rahul Zaveri, and Alla Zelenyuk
Atmos. Chem. Phys., 22, 11217–11238, https://doi.org/10.5194/acp-22-11217-2022, https://doi.org/10.5194/acp-22-11217-2022, 2022
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Recent aircraft measurements from the HI-SCALE campaign conducted over the Southern Great Plains (SGP) site in Oklahoma are used to quantify spatial variability of aerosol properties in terms of grid spacings typically used by weather and climate models. Surprisingly large horizontal gradients in aerosol properties were frequently observed in this rural area. This spatial variability can be used as an uncertainty range when comparing surface point measurements with model predictions.
Benjamin Foreback, Lubna Dada, Kaspar R. Daellenbach, Chao Yan, Lili Wang, Biwu Chu, Ying Zhou, Tom V. Kokkonen, Mona Kurppa, Rosaria E. Pileci, Yonghong Wang, Tommy Chan, Juha Kangasluoma, Lin Zhuohui, Yishou Guo, Chang Li, Rima Baalbaki, Joni Kujansuu, Xiaolong Fan, Zemin Feng, Pekka Rantala, Shahzad Gani, Federico Bianchi, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, Yongchun Liu, and Pauli Paasonen
Atmos. Chem. Phys., 22, 11089–11104, https://doi.org/10.5194/acp-22-11089-2022, https://doi.org/10.5194/acp-22-11089-2022, 2022
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This study analyzed air quality in Beijing during the Chinese New Year over 7 years, including data from a new in-depth measurement station. This is one of few studies to look at long-term impacts, including the outcome of firework restrictions starting in 2018. Results show that firework pollution has gone down since 2016, indicating a positive result from the restrictions. Results of this study may be useful in making future decisions about the use of fireworks to improve air quality.
Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall’Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-591, https://doi.org/10.5194/acp-2022-591, 2022
Revised manuscript accepted for ACP
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The Arctic is a unique environment that is warming faster than other locations on Earth. We evaluate measurements of aerosol particles, which can influence climate, over the central Arctic Ocean for a full year and compare the data to land-based measurement stations across the Arctic. Our measurements show that the central Arctic has similarities, but also distinct differences, from the stations further south. We note that this may change as the Arctic warms and sea ice continues to decline.
Allison B. Marquardt Collow, Virginie Buchard, Peter R. Colarco, Arlindo M. da Silva, Ravi Govindaraju, Edward P. Nowottnick, Sharon Burton, Richard Ferrare, Chris Hostetler, and Luke Ziemba
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-545, https://doi.org/10.5194/acp-2022-545, 2022
Revised manuscript accepted for ACP
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Biomass burning aerosol impacts aspects of the atmosphere and Earth system through radiative forcing, serving as cloud condensation nuclei, and air quality. Despite its importance, the representation of biomass burning aerosol is not always accurate in models. Field campaign observations from CAMP2Ex are used to evaluate the mass and extinction of aerosols in the GEOS model. Notable biases in the model illuminate areas of future development with GEOS and the underlying GOCART aerosol module.
Gang Zhao, Tianyi Tan, Shuya Hu, Zhuofei Du, Dongjie Shang, Zhijun Wu, Song Guo, Jing Zheng, Wenfei Zhu, Mengren Li, Limin Zeng, and Min Hu
Atmos. Chem. Phys., 22, 10861–10873, https://doi.org/10.5194/acp-22-10861-2022, https://doi.org/10.5194/acp-22-10861-2022, 2022
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Black carbon is the second strongest absorbing component in the atmosphere that exerts warming effects on climate. One critical challenge in quantifying the ambient black carbon's radiative effects is addressing the BC microphysical properties. In this study, the microphysical properties of the aged and fresh BC particles are synthetically analyzed under different atmospheres. The measurement results can be further used in models to help constrain the uncertainties of the BC radiative effects.
Natalia E. Chubarova, Heike Vogel, Elizaveta E. Androsova, Alexander A. Kirsanov, Olga B. Popovicheva, Bernhard Vogel, and Gdaliy S. Rivin
Atmos. Chem. Phys., 22, 10443–10466, https://doi.org/10.5194/acp-22-10443-2022, https://doi.org/10.5194/acp-22-10443-2022, 2022
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Effects of urban aerosol pollution in Moscow were analyzed using the COSMO-ART chemical transport model and intensive measurement campaigns. We show that urban aerosol comprises about 15–20% of columnar aerosol content, consisting mainly of fine aerosol mode. The black carbon (BC) fraction is about 5 %, depending on particle dispersion intensity (IPD). The BC fraction low value explains weak absorbing properties of the Moscow atmosphere. IPD also defines the daily cycle of urban aerosol species.
Janine Lückerath, Andreas Held, Holger Siebert, Michel Michalkow, and Birgit Wehner
Atmos. Chem. Phys., 22, 10007–10021, https://doi.org/10.5194/acp-22-10007-2022, https://doi.org/10.5194/acp-22-10007-2022, 2022
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Three different methods were applied to estimate the vertical aerosol particle flux in the marine boundary layer (MBL) and between the MBL and free troposphere. For the first time, aerosol fluxes derived from these three methods were estimated and compared using airborne aerosol measurements using data from the ACORES field campaign in the northeastern Atlantic Ocean in July 2017. The amount of fluxes was small and directed up and down for different cases, but the methods were applicable.
Christian Tatzelt, Silvia Henning, André Welti, Andrea Baccarini, Markus Hartmann, Martin Gysel-Beer, Manuela van Pinxteren, Robin L. Modini, Julia Schmale, and Frank Stratmann
Atmos. Chem. Phys., 22, 9721–9745, https://doi.org/10.5194/acp-22-9721-2022, https://doi.org/10.5194/acp-22-9721-2022, 2022
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We present the abundance and origin of cloud-relevant aerosol particles in the preindustral-like conditions of the Southern Ocean (SO) during austral summer. Cloud condensation nuclei (CCN) and ice-nucleating particles (INP) were measured during a circum-Antarctic scientific cruise with in situ instrumentation and offline filter measurements, respectively. Transport processes were found to play an equally important role as local sources for both the CCN and INP population of the SO.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
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The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
Caroline Dang, Michal Segal-Rozenhaimer, Haochi Che, Lu Zhang, Paola Formenti, Jonathan Taylor, Amie Dobracki, Sara Purdue, Pui-Shan Wong, Athanasios Nenes, Arthur Sedlacek III, Hugh Coe, Jens Redemann, Paquita Zuidema, Steven Howell, and James Haywood
Atmos. Chem. Phys., 22, 9389–9412, https://doi.org/10.5194/acp-22-9389-2022, https://doi.org/10.5194/acp-22-9389-2022, 2022
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Transmission electron microscopy was used to analyze aged African smoke particles and how the smoke interacts with the marine atmosphere. We found that the volatility of organic aerosol increases with biomass burning plume age, that black carbon is often mixed with potassium salts and that the marine atmosphere can incorporate Na and Cl into smoke particles. Marine salts are more processed when mixed with smoke plumes, and there are interesting Cl-rich yet Na-absent marine particles.
Suzanne Crumeyrolle, Jenni Kontkanen, Clémence Rose, Alejandra Velasquez Garcia, Eric Bourrianne, Maxime Catalfamo, Véronique Riffault, Emmanuel Tison, Joel Ferreira de Brito, Nicolas Visez, Nicolas Ferlay, Frédérique Auriol, and Isabelle Chiapello
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-436, https://doi.org/10.5194/acp-2022-436, 2022
Revised manuscript accepted for ACP
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Ultrafine particles (UFPs) are particles with an aerodynamic diameter of 100 nm or less, has negligible mass concentration but is the dominant contributor to the total particle number concentration. The present study aims to better understand the environmental factors favoring or inhibiting, atmospheric new particle formation (NPF) over Lille a large city North of France and to analyze the impact of such event on urban air quality using a long-term dataset (3 years).
Siman Ren, Lei Yao, Yuwei Wang, Gan Yang, Yiliang Liu, Yueyang Li, Yiqun Lu, Lihong Wang, and Lin Wang
Atmos. Chem. Phys., 22, 9283–9297, https://doi.org/10.5194/acp-22-9283-2022, https://doi.org/10.5194/acp-22-9283-2022, 2022
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We improved the empirical functions between volatility and chemical formulas of organic aerosols based on lab experiments and field observations. It was found that organic compounds in ambient aerosols can be divided into two groups according to their O / C ratios and that there should be specialized volatility parameterizations for different O / C organic compounds.