Articles | Volume 12, issue 24
https://doi.org/10.5194/acp-12-11795-2012
© Author(s) 2012. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-12-11795-2012
© Author(s) 2012. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
17 Dec 2012
Research article |
| 17 Dec 2012
Analysis of secondary organic aerosol formation and aging using positive matrix factorization of high-resolution aerosol mass spectra: application to the dodecane low-NOx system
J. S. Craven
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California, USA
L. D. Yee
Division of Engineering and Applied Science, California Institute of Technology, Pasadena, California, USA
School of Chemical and Biomolecular Engineering and School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, USA
M. R. Canagaratna
Aerodyne Research, Inc., Billerica, Massachusetts, USA
C. L. Loza
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California, USA
K. A. Schilling
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California, USA
R. L. N. Yatavelli
Department of Atmospheric Sciences, University of Washington, Seattle, Washington, USA
current address: Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Colorado, USA
J. A. Thornton
Department of Atmospheric Sciences, University of Washington, Seattle, Washington, USA
P. J. Ziemann
Air Pollution Research Center, Department of Environmental Sciences, and Environmental Toxicology Graduate Program, University of California, Riverside, California, USA
R. C. Flagan
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California, USA
Division of Engineering and Applied Science, California Institute of Technology, Pasadena, California, USA
J. H. Seinfeld
Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California, USA
Division of Engineering and Applied Science, California Institute of Technology, Pasadena, California, USA
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
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Attachment rate coefficients between ions and charged aerosol particles determine their lifetimes and may also influence cloud dynamics and aerosol processing. Here we present novel experiments that measure ion–aerosol attachment rate coefficients for multiply charged aerosol particles under atmospheric conditions in the CERN CLOUD chamber. Our results provide experimental discrimination between various theoretical models.
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Daniel John Katz, Aroob Abdelhamid, Harald Stark, Manjula R. Canagaratna, Douglas R. Worsnop, and Eleanor C. Browne
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Atmos. Chem. Phys., 23, 5233–5249, https://doi.org/10.5194/acp-23-5233-2023, https://doi.org/10.5194/acp-23-5233-2023, 2023
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Substantial advances have been made in recent years toward detecting and quantifying methane super-emitters from space. However, such advances have rarely been expanded to measure the global methane pledge because large-scale swaths and high-resolution sampling have not been coordinated. Here we present a versatile spaceborne architecture that can juggle planet-scale and plant-level methane retrievals, challenge official emission reports, and remain relevant for stereoscopic measurements.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Siegfried Schobesberger, Emma L. D'Ambro, Lejish Vettikkat, Ben H. Lee, Qiaoyun Peng, David M. Bell, John E. Shilling, Manish Shrivastava, Mikhail Pekour, Jerome Fast, and Joel A. Thornton
Atmos. Meas. Tech., 16, 247–271, https://doi.org/10.5194/amt-16-247-2023, https://doi.org/10.5194/amt-16-247-2023, 2023
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We present a new, highly sensitive technique for measuring atmospheric ammonia, an important trace gas that is emitted mainly by agriculture. We deployed the instrument on an aircraft during research flights over rural Oklahoma. Due to its fast response, we could analyze correlations with turbulent winds and calculate ammonia emissions from nearby areas at 1 to 2 km resolution. We observed high spatial variability and point sources that are not resolved in the US National Emissions Inventory.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Benjamin Sapper, Daven Henze, Manjula Canagaratna, and Harald Stark
EGUsphere, https://doi.org/10.5194/egusphere-2022-1221, https://doi.org/10.5194/egusphere-2022-1221, 2022
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Positive Matrix Factorization (PMF) has been used by atmospheric scientists to extract underlying factors present in large datasets. This paper presents a new technique for weighted PMF that drastically reduces the computational costs of previously developed algorithms. We use this technique to deliver interpretative factors and solution diagnostics from an atmospheric chemistry dataset.
Alfred W. Mayhew, Ben H. Lee, Joel A. Thornton, Thomas J. Bannan, James Brean, James R. Hopkins, James D. Lee, Beth S. Nelson, Carl Percival, Andrew R. Rickard, Marvin D. Shaw, Peter M. Edwards, and Jaqueline F. Hamilton
Atmos. Chem. Phys., 22, 14783–14798, https://doi.org/10.5194/acp-22-14783-2022, https://doi.org/10.5194/acp-22-14783-2022, 2022
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Isoprene nitrates are chemical species commonly found in the atmosphere that are important for their impacts on air quality and climate. This paper compares 3 different representations of the chemistry of isoprene nitrates in computational models highlighting cases where the choice of chemistry included has significant impacts on the concentration and composition of the modelled nitrates. Calibration of mass spectrometers is also shown to be an important factor when analysing isoprene nitrates.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Shenglun Wu, Hyung Joo Lee, Andrea Anderson, Shang Liu, Toshihiro Kuwayama, John H. Seinfeld, and Michael J. Kleeman
Atmos. Chem. Phys., 22, 4929–4949, https://doi.org/10.5194/acp-22-4929-2022, https://doi.org/10.5194/acp-22-4929-2022, 2022
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An ozone control experiment usually conducted in the laboratory was installed in a trailer and moved to the outdoor environment to directly confirm that we are controlling the right sources in order to lower ambient ozone concentrations. Adding small amounts of precursor oxides of nitrogen and volatile organic compounds to ambient air showed that the highest ozone concentrations are best controlled by reducing concentrations of oxides of nitrogen. The results confirm satellite measurements.
Sophia M. Charan, Yuanlong Huang, Reina S. Buenconsejo, Qi Li, David R. Cocker III, and John H. Seinfeld
Atmos. Chem. Phys., 22, 917–928, https://doi.org/10.5194/acp-22-917-2022, https://doi.org/10.5194/acp-22-917-2022, 2022
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In this study, we investigate the secondary organic aerosol formation potential of decamethylcyclopentasiloxane (D5), which is used as a tracer for volatile chemical products and measured in high concentrations both outdoors and indoors. By performing experiments in different types of reactors, we find that D5’s aerosol formation is highly dependent on OH, and, at low OH concentrations or exposures, D5 forms little aerosol. We also reconcile results from other studies.
Arto Heitto, Kari Lehtinen, Tuukka Petäjä, Felipe Lopez-Hilfiker, Joel A. Thornton, Markku Kulmala, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 155–171, https://doi.org/10.5194/acp-22-155-2022, https://doi.org/10.5194/acp-22-155-2022, 2022
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For atmospheric aerosol particles to take part in cloud formation, they need to be at least a few tens of nanometers in diameter. By using a particle condensation model, we investigated how two types of chemical reactions, oligomerization and decomposition, of organic molecules inside the particle may affect the growth of secondary aerosol particles to these sizes. We show that the effect is potentially significant, which highlights the importance of increasing understanding of these processes.
Elyse A. Pennington, Karl M. Seltzer, Benjamin N. Murphy, Momei Qin, John H. Seinfeld, and Havala O. T. Pye
Atmos. Chem. Phys., 21, 18247–18261, https://doi.org/10.5194/acp-21-18247-2021, https://doi.org/10.5194/acp-21-18247-2021, 2021
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Volatile chemical products (VCPs) are commonly used consumer and industrial items that contribute to the formation of atmospheric aerosol. We implemented the emissions and chemistry of VCPs in a regional-scale model and compared predictions with measurements made in Los Angeles. Our results reduced model bias and suggest that VCPs may contribute up to half of anthropogenic secondary organic aerosol in Los Angeles and are an important source of human-influenced particular matter in urban areas.
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.
Linhui Jiang, Yan Xia, Lu Wang, Xue Chen, Jianjie Ye, Tangyan Hou, Liqiang Wang, Yibo Zhang, Mengying Li, Zhen Li, Zhe Song, Yaping Jiang, Weiping Liu, Pengfei Li, Daniel Rosenfeld, John H. Seinfeld, and Shaocai Yu
Atmos. Chem. Phys., 21, 16985–17002, https://doi.org/10.5194/acp-21-16985-2021, https://doi.org/10.5194/acp-21-16985-2021, 2021
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This paper establishes a bottom-up approach to reveal a unique pattern of urban on-road vehicle emissions at a spatial resolution 1–3 orders of magnitude higher than current inventories. The results show that the hourly average on-road vehicle emissions of CO, NOx, HC, and PM2.5 are 74 kg, 40 kg, 8 kg, and 2 kg, respectively. Integrating our traffic-monitoring-based approach with urban measurements, we could address major data gaps between urban air pollutant emissions and concentrations.
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.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
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To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6835–6850, https://doi.org/10.5194/amt-14-6835-2021, https://doi.org/10.5194/amt-14-6835-2021, 2021
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Iodide-adduct chemical ionization mass spectrometry (I-CIMS) has been widely used to analyze airborne organics. In this study, I-CIMS sensitivities of isomers within a formula are found to generally vary by 1 and up to 2 orders of magnitude. Comparisons between measured and predicted moles, obtained using a voltage-scanning calibration approach, show that predictions for individual compounds or formulas might carry high uncertainty, yet the summed moles of analytes agree reasonably well.
Chenyang Bi, Jordan E. Krechmer, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 6551–6560, https://doi.org/10.5194/amt-14-6551-2021, https://doi.org/10.5194/amt-14-6551-2021, 2021
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Calibration techniques have been recently developed to log-linearly correlate analyte sensitivity with CIMS operating conditions particularly for compounds without authentic standards. In this work, we examine the previously ignored bias in the log-linear-based calibration method and estimate an average bias of 30 %, with 1 order of magnitude for less sensitive compounds in some circumstances. A step-by-step guide was provided to reduce and even remove the bias.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Weimeng Kong, Stavros Amanatidis, Huajun Mai, Changhyuk Kim, Benjamin C. Schulze, Yuanlong Huang, Gregory S. Lewis, Susanne V. Hering, John H. Seinfeld, and Richard C. Flagan
Atmos. Meas. Tech., 14, 5429–5445, https://doi.org/10.5194/amt-14-5429-2021, https://doi.org/10.5194/amt-14-5429-2021, 2021
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We present the design, modeling, and experimental characterization of the nano-scanning electrical mobility spectrometer (nSEMS), a recently developed instrument that probes particle physical properties in the 1.5–25 nm range. The nSEMS has proven to be extremely powerful in examining atmospheric nucleation and the subsequent growth of nanoparticles in the CERN CLOUD experiment, which provides a valuable asset to study atmospheric nanoparticles and to evaluate their impact on climate.
Louise N. Jensen, Manjula R. Canagaratna, Kasper Kristensen, Lauriane L. J. Quéléver, Bernadette Rosati, Ricky Teiwes, Marianne Glasius, Henrik B. Pedersen, Mikael Ehn, and Merete Bilde
Atmos. Chem. Phys., 21, 11545–11562, https://doi.org/10.5194/acp-21-11545-2021, https://doi.org/10.5194/acp-21-11545-2021, 2021
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This work targets the chemical composition of α-pinene-derived secondary organic aerosol (SOA) formed in the temperature range from -15 to 20°C. Experiments were conducted in an atmospheric simulation chamber. Positive matrix factorization analysis of data obtained by a high-resolution time-of-flight aerosol mass spectrometer shows that the elemental aerosol composition is controlled by the initial α-pinene concentration and temperature during SOA formation.
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.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Stavros Amanatidis, Yuanlong Huang, Buddhi Pushpawela, Benjamin C. Schulze, Christopher M. Kenseth, Ryan X. Ward, John H. Seinfeld, Susanne V. Hering, and Richard C. Flagan
Atmos. Meas. Tech., 14, 4507–4516, https://doi.org/10.5194/amt-14-4507-2021, https://doi.org/10.5194/amt-14-4507-2021, 2021
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We assess the performance of a highly portable mobility analyzer, the Spider DMA, in measuring ambient aerosol particle size distributions, with specific attention to its moderate sizing resolution (R=3). Long-term field testing showed excellent correlation with a conventional mobility analyzer (R=10) over the 17–500 nm range, suggesting that moderate resolution may be sufficient to obtain key properties of ambient size distributions, enabling smaller instruments and better counting statistics.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Stephanie L. Shaw, Eric S. Edgerton, Taekyu Joo, Nga L. Ng, and Ann M. Dillner
Atmos. Meas. Tech., 14, 4355–4374, https://doi.org/10.5194/amt-14-4355-2021, https://doi.org/10.5194/amt-14-4355-2021, 2021
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Infrared spectrometry can be applied in routine monitoring of atmospheric particles to give comprehensive characterization of the organic material by bond rather than species. Using this technique, the concentrations of particle organic material were found to decrease 2011–2016 in the southeastern US, driven by a decline in highly aged material, concurrent with declining anthropogenic emissions. However, an increase was observed in the fraction of more moderately aged organic matter.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 14, 3895–3907, https://doi.org/10.5194/amt-14-3895-2021, https://doi.org/10.5194/amt-14-3895-2021, 2021
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Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Mutian Ma, Laura-Hélèna Rivellini, YuXi Cui, Megan D. Willis, Rio Wilkie, Jonathan P. D. Abbatt, Manjula R. Canagaratna, Junfeng Wang, Xinlei Ge, and Alex K. Y. Lee
Atmos. Meas. Tech., 14, 2799–2812, https://doi.org/10.5194/amt-14-2799-2021, https://doi.org/10.5194/amt-14-2799-2021, 2021
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Chemical characterization of organic coatings is important to advance our understanding of the physio-chemical properties and atmospheric processing of black carbon (BC) particles. This work develops two approaches to improve the elemental analysis of oxygenated organic coatings using a soot-particle aerosol mass spectrometer. Analyzing ambient data with the new approaches indicated that secondary organics that coated on BC were likely less oxygenated compared to those externally mixed with BC.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Dana L. McGuffin, Yuanlong Huang, Richard C. Flagan, Tuukka Petäjä, B. Erik Ydstie, and Peter J. Adams
Geosci. Model Dev., 14, 1821–1839, https://doi.org/10.5194/gmd-14-1821-2021, https://doi.org/10.5194/gmd-14-1821-2021, 2021
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Atmospheric particle formation, emissions, and growth process rates are significant sources of uncertainty in predicting climate change. We aim to reduce that uncertainty by using measurements from several ground-based sites across Europe. We developed an estimation technique to adapt the governing process rates so model–measurement bias decays. The estimation framework developed has potential to improve model predictions while providing insight into the underlying atmospheric particle physics.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
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.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys., 20, 15513–15535, https://doi.org/10.5194/acp-20-15513-2020, https://doi.org/10.5194/acp-20-15513-2020, 2020
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This paper presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modeling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas–particle partitioning, and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Liqiang Wang, Shaocai Yu, Pengfei Li, Xue Chen, Zhen Li, Yibo Zhang, Mengying Li, Khalid Mehmood, Weiping Liu, Tianfeng Chai, Yannian Zhu, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 20, 14787–14800, https://doi.org/10.5194/acp-20-14787-2020, https://doi.org/10.5194/acp-20-14787-2020, 2020
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The Chinese government has made major strides in curbing anthropogenic emissions. In this study, we constrain a state-of-the-art CTM by a reliable data assimilation method with extensive chemical and meteorological observations. This comprehensive technical design provides a crucial advance in isolating the influences of emission changes and meteorological perturbations over the Yangtze River Delta (YRD) from 2016 to 2019, thus establishing the first map of the PM2.5 mitigation across the YRD.
Brigitte Rooney, Yuan Wang, Jonathan H. Jiang, Bin Zhao, Zhao-Cheng Zeng, and John H. Seinfeld
Atmos. Chem. Phys., 20, 14597–14616, https://doi.org/10.5194/acp-20-14597-2020, https://doi.org/10.5194/acp-20-14597-2020, 2020
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Wildfires have become increasingly prevalent. Intense smoke consisting of particulate matter (PM) leads to an increased risk of morbidity and mortality. The record-breaking Camp Fire ravaged Northern California for two weeks in 2018. Here, we employ a comprehensive chemical transport model along with ground-based and satellite observations to characterize the PM concentrations across Northern California and to investigate the pollution sensitivity predictions to key parameters of the model.
Sophia M. Charan, Reina S. Buenconsejo, and John H. Seinfeld
Atmos. Chem. Phys., 20, 13167–13190, https://doi.org/10.5194/acp-20-13167-2020, https://doi.org/10.5194/acp-20-13167-2020, 2020
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In urban areas, the emissions from volatile chemical products may be responsible for the formation of as much particulate matter as motor vehicles. Since exposure to particulate matter is a public health crisis, understanding its formation is critical. In this work, we investigate the secondary organic aerosol formation potential of benzyl alcohol, an important compound that is representative of some of these new emission sources, and find that more particulate matter forms than is expected.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Archit Mehra, Jordan E. Krechmer, Andrew Lambe, Chinmoy Sarkar, Leah Williams, Farzaneh Khalaj, Alex Guenther, John Jayne, Hugh Coe, Douglas Worsnop, Celia Faiola, and Manjula Canagaratna
Atmos. Chem. Phys., 20, 10953–10965, https://doi.org/10.5194/acp-20-10953-2020, https://doi.org/10.5194/acp-20-10953-2020, 2020
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Emissions of volatile organic compounds (VOCs) from plants are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Real plant emissions are much more diverse than the few proxies widely used for studies of plant SOA. Here we present the first study of SOA from Californian sage plants and the oxygenated monoterpenes representing their major emissions. We identify SOA products and show the importance of the formation of highly oxygenated organic molecules and oligomers.
Archit Mehra, Yuwei Wang, Jordan E. Krechmer, Andrew Lambe, Francesca Majluf, Melissa A. Morris, Michael Priestley, Thomas J. Bannan, Daniel J. Bryant, Kelly L. Pereira, Jacqueline F. Hamilton, Andrew R. Rickard, Mike J. Newland, Harald Stark, Philip Croteau, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, Lin Wang, and Hugh Coe
Atmos. Chem. Phys., 20, 9783–9803, https://doi.org/10.5194/acp-20-9783-2020, https://doi.org/10.5194/acp-20-9783-2020, 2020
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Aromatic volatile organic compounds (VOCs) emitted from anthropogenic activity are important for tropospheric ozone and secondary organic aerosol (SOA) formation. Here we present a detailed chemical characterisation of SOA from four C9-aromatic isomers and a polycyclic aromatic hydrocarbon (PAH). We identify and compare their oxidation products in the gas and particle phases, showing the different relative importance of oxidation pathways and proportions of highly oxygenated organic molecules.
Yuwei Wang, Archit Mehra, Jordan E. Krechmer, Gan Yang, Xiaoyu Hu, Yiqun Lu, Andrew Lambe, Manjula Canagaratna, Jianmin Chen, Douglas Worsnop, Hugh Coe, and Lin Wang
Atmos. Chem. Phys., 20, 9563–9579, https://doi.org/10.5194/acp-20-9563-2020, https://doi.org/10.5194/acp-20-9563-2020, 2020
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A series of OH-initiated oxidation experiments of trimethylbenzene were investigated in the absence and presence of NOx. Many C9 products with 1–11 oxygen atoms and C18 products presumably formed from dimerization of C9 peroxy radicals were observed, hinting at the extensive existence of autoxidation and accretion reaction pathways. The presence of NOx would suppress the formation of highly oxygenated C18 molecules and enhance the formation of organonitrates and even dinitrate compounds.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Ryan Schmedding, Quazi Z. Rasool, Yue Zhang, Havala O. T. Pye, Haofei Zhang, Yuzhi Chen, Jason D. Surratt, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Allen H. Goldstein, and William Vizuete
Atmos. Chem. Phys., 20, 8201–8225, https://doi.org/10.5194/acp-20-8201-2020, https://doi.org/10.5194/acp-20-8201-2020, 2020
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Accurate model prediction of aerosol concentrations is a known challenge. It is assumed in many modeling systems that aerosols are in a homogeneously mixed phase state. It has been observed that aerosols do phase separate and can form a highly viscous organic shell with an aqueous core impacting the formation processes of aerosols. This work is a model implementation to determine an aerosol's phase state using glass transition temperature and aerosol composition.
Angela Buchholz, Arttu Ylisirniö, Wei Huang, Claudia Mohr, Manjula Canagaratna, Douglas R. Worsnop, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 20, 7693–7716, https://doi.org/10.5194/acp-20-7693-2020, https://doi.org/10.5194/acp-20-7693-2020, 2020
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To understand the role of aerosol particles in the atmosphere, it is necessary to know their detailed chemical composition and physical properties, especially volatility. The thermal desorption data from FIGAERO–CIMS provides both but are difficult to analyse. With positive matrix factorisation, we can separate instrument background from the real signal. Compounds can be classified by their apparent volatility, and the contribution of thermal decomposition in the instrument can be identified.
Alexander B. MacDonald, Ali Hossein Mardi, Hossein Dadashazar, Mojtaba Azadi Aghdam, Ewan Crosbie, Haflidi H. Jonsson, Richard C. Flagan, John H. Seinfeld, and Armin Sorooshian
Atmos. Chem. Phys., 20, 7645–7665, https://doi.org/10.5194/acp-20-7645-2020, https://doi.org/10.5194/acp-20-7645-2020, 2020
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Understanding how humans affect Earth's climate requires understanding of how particles in the air affect the number concentration of droplets in a cloud (Nd). We use the air-equivalent mass concentration of different chemical species contained in cloud water to predict Nd. In this study we found that the prediction of Nd is (1) best described by total sulfate; (2) improved when considering up to five species; and (3) dependent on factors like turbulence, smoke presence, and in-cloud height.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Ziyue Li, Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Jiumeng Liu, John E. Shilling, Joel A. Thornton, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 2489–2512, https://doi.org/10.5194/acp-20-2489-2020, https://doi.org/10.5194/acp-20-2489-2020, 2020
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We discuss the development and application of a robust clustering method for the interpretation of compound-specific organic aerosol thermal desorption profiles. We demonstrate the utility of clustering for analysis and interpretation of the composition and volatility of secondary organic aerosol. We show that the thermal desorption profiles are represented by only 9–13 distinct clusters, with the number of clusters obtained dependent on the precursor and formation conditions.
Khalid Mehmood, Yujie Wu, Liqiang Wang, Shaocai Yu, Pengfei Li, Xue Chen, Zhen Li, Yibo Zhang, Mengying Li, Weiping Liu, Yuesi Wang, Zirui Liu, Yannian Zhu, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 20, 2419–2443, https://doi.org/10.5194/acp-20-2419-2020, https://doi.org/10.5194/acp-20-2419-2020, 2020
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We selected June 2014 as our study period, which exhibited a complete evolution process of open biomass burning (OBB) dominated by open crop straw burning (OCSB) over central and eastern China (CEC). We established a constraining method that integrates ground-based PM2.5 measurements with the two-way coupled WRF-CMAQ model to derive optimal OBB emissions. It was found that these emissions could allow the model to reproduce meteorological and chemical fields over CEC during the study period.
Abigail R. Koss, Manjula R. Canagaratna, Alexander Zaytsev, Jordan E. Krechmer, Martin Breitenlechner, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joseph R. Roscioli, Frank N. Keutsch, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 1021–1041, https://doi.org/10.5194/acp-20-1021-2020, https://doi.org/10.5194/acp-20-1021-2020, 2020
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Oxidation chemistry of organic compounds in the atmosphere produces a diverse spectrum of products. This diversity is difficult to represent in air quality and climate models, and in laboratory experiments it results in large and complex datasets. This work evaluates several methods to simplify the chemistry of oxidation systems in environmental chambers, including positive matrix factorization, hierarchical clustering analysis, and gamma kinetics parameterization.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
Brett B. Palm, Xiaoxi Liu, Jose L. Jimenez, and Joel A. Thornton
Atmos. Meas. Tech., 12, 5829–5844, https://doi.org/10.5194/amt-12-5829-2019, https://doi.org/10.5194/amt-12-5829-2019, 2019
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We introduce a coaxial, low-pressure ion–molecule reaction (IMR) region for iodide-adduct chemical ionization mass spectrometry, designed to decrease the effects of IMR wall interactions with organic/inorganic gases. This IMR has 3–10 times shorter delay times than previous IMRs. We introduce a conceptual framework for understanding and subtracting the background signal due to analyte molecules interacting with IMR walls. This framework can be applied to other tubing and instrument systems.
Xuan Zhang, Haofei Zhang, Wen Xu, Xiaokang Wu, Geoffrey S. Tyndall, John J. Orlando, John T. Jayne, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Meas. Tech., 12, 5535–5545, https://doi.org/10.5194/amt-12-5535-2019, https://doi.org/10.5194/amt-12-5535-2019, 2019
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We develop a new technique to characterize organic nitrates as intact molecules in atmospheric aerosols, and we apply this technique to identify hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.
Masayuki Takeuchi and Nga L. Ng
Atmos. Chem. Phys., 19, 12749–12766, https://doi.org/10.5194/acp-19-12749-2019, https://doi.org/10.5194/acp-19-12749-2019, 2019
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Organic nitrate is ubiquitous in the atmosphere and impacts the formation of aerosol and ozone, two leading air pollutants of concern worldwide. We conducted a comprehensive laboratory study to investigate the hydrolysis process of organic nitrate aerosol formed from monoterpenes, which are important reactive chemicals emitted by plants. Our results provide experimentally constrained parameters required to assess the role of organic nitrate in the formation of the air pollutants of our concern.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Felipe D. Lopez-Hilfiker, Veronika Pospisilova, Wei Huang, Markus Kalberer, Claudia Mohr, Giulia Stefenelli, Joel A. Thornton, Urs Baltensperger, Andre S. H. Prevot, and Jay G. Slowik
Atmos. Meas. Tech., 12, 4867–4886, https://doi.org/10.5194/amt-12-4867-2019, https://doi.org/10.5194/amt-12-4867-2019, 2019
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We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer (EESI-TOF), which provides real-time, near-molecular measurements of organic aerosol at atmospherically relevant concentrations, addressing a critical gap in existing measurement capabilities. Successful deployments of the EESI-TOF for laboratory measurements, ground-based ambient sampling, and aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.
Emma L. D'Ambro, Siegfried Schobesberger, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Ben H. Lee, Jiumeng Liu, Alla Zelenyuk, David Bell, Christopher D. Cappa, Taylor Helgestad, Ziyue Li, Alex Guenther, Jian Wang, Matthew Wise, Ryan Caylor, Jason D. Surratt, Theran Riedel, Noora Hyttinen, Vili-Taneli Salo, Galib Hasan, Theo Kurtén, John E. Shilling, and Joel A. Thornton
Atmos. Chem. Phys., 19, 11253–11265, https://doi.org/10.5194/acp-19-11253-2019, https://doi.org/10.5194/acp-19-11253-2019, 2019
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Isoprene is the most abundantly emitted reactive organic gas globally, and thus it is important to understand its fate and role in aerosol formation and growth. A major product of its oxidation is an epoxydiol, IEPOX, which can be efficiently taken up by acidic aerosol to generate substantial amounts of secondary organic aerosol (SOA). We present chamber experiments exploring the properties of IEPOX SOA and reconcile discrepancies between field, laboratory, and model studies of this process.
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.
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.
Brigitte Rooney, Ran Zhao, Yuan Wang, Kelvin H. Bates, Ajay Pillarisetti, Sumit Sharma, Seema Kundu, Tami C. Bond, Nicholas L. Lam, Bora Ozaltun, Li Xu, Varun Goel, Lauren T. Fleming, Robert Weltman, Simone Meinardi, Donald R. Blake, Sergey A. Nizkorodov, Rufus D. Edwards, Ankit Yadav, Narendra K. Arora, Kirk R. Smith, and John H. Seinfeld
Atmos. Chem. Phys., 19, 7719–7742, https://doi.org/10.5194/acp-19-7719-2019, https://doi.org/10.5194/acp-19-7719-2019, 2019
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Approximately 3 billion people worldwide cook with solid fuels, such as wood, charcoal, and agricultural residues, that are often combusted in inefficient cookstoves. Here, we simulate the distribution of the two major health-damaging outdoor pollution species (PM2.5 and O3) using state-of-the-science emissions databases and atmospheric chemical transport models to estimate the impact of household combustion on ambient air quality in India.
Rebecca H. Schwantes, Sophia M. Charan, Kelvin H. Bates, Yuanlong Huang, Tran B. Nguyen, Huajun Mai, Weimeng Kong, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 19, 7255–7278, https://doi.org/10.5194/acp-19-7255-2019, https://doi.org/10.5194/acp-19-7255-2019, 2019
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Oxidation of isoprene, the dominant non-methane biogenic volatile organic compound emitted into the atmosphere, is a significant source of secondary organic aerosol (SOA). Here formation of SOA from isoprene oxidation by the hydroxyl radical (OH) under high-NO conditions is measured. This work improves our understanding of isoprene SOA formation by demonstrating that low-volatility compounds formed under high-NO conditions produce significantly more aerosol than previously thought.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671, https://doi.org/10.5194/amt-12-1659-2019, https://doi.org/10.5194/amt-12-1659-2019, 2019
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Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298, https://doi.org/10.5194/acp-19-2283-2019, https://doi.org/10.5194/acp-19-2283-2019, 2019
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We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
Theo Kurtén, Noora Hyttinen, Emma Louise D'Ambro, Joel Thornton, and Nønne Lyng Prisle
Atmos. Chem. Phys., 18, 17589–17600, https://doi.org/10.5194/acp-18-17589-2018, https://doi.org/10.5194/acp-18-17589-2018, 2018
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We use COSMO-RS to compute saturation vapor pressures for two products of isoprene photo-oxidation and compare the results to measurements. COSMO-RS is an attractive option for calculating properties of molecules, as it is based on quantum mechanics and requires few fitting parameters. However, we show that the default implementation of this method suffers from errors related to both conformational sampling and intramolecular hydrogen bonding. We propose solutions to these problems.
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.
Siegfried Schobesberger, Emma L. D'Ambro, Felipe D. Lopez-Hilfiker, Claudia Mohr, and Joel A. Thornton
Atmos. Chem. Phys., 18, 14757–14785, https://doi.org/10.5194/acp-18-14757-2018, https://doi.org/10.5194/acp-18-14757-2018, 2018
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Current mass spectrometers allow us to measure the composition of individual organic molecules in aerosol particles, as well as how they evaporate from the particles when those are slowly heated up to 200 °C. We have developed a detailed computer model to simulate the physical and chemical processes that underlie that evaporation and thus help us understand important aerosol properties. Among other factors, we discuss the roles of vapor pressures, and accretion and decomposition reactions.
Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
Atmos. Meas. Tech., 11, 5087–5104, https://doi.org/10.5194/amt-11-5087-2018, https://doi.org/10.5194/amt-11-5087-2018, 2018
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The sources and atmospheric chemistry of gas-phase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. We evaluated the use of SF6− as a sensitive and selective chemical ionization reagent ion for real-time measurements of gas-phase organic acids at a rural site in Yorkville, Georgia. We found that ambient concentrations of organic acids ranged from a few ppt to several ppb, and are dependent on ambient temperature.
Lu Xu, Havala O. T. Pye, Jia He, Yunle Chen, Benjamin N. Murphy, and Nga Lee Ng
Atmos. Chem. Phys., 18, 12613–12637, https://doi.org/10.5194/acp-18-12613-2018, https://doi.org/10.5194/acp-18-12613-2018, 2018
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In this study, we integrate lab-in-the-field experiments, extensive ambient ground measurements, and state-of-the-art modeling to constrain the concentration of organic aerosol from biogenic monoterpenes and sesquiterpenes. Further, we show that the organic aerosol from the investigated sources accounts for roughly 20 % of the World Health Organization PM2.5 standard in the southeastern US.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
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.
Yue Zhang, Shachi Katira, Andrew Lee, Andrew T. Lambe, Timothy B. Onasch, Wen Xu, William A. Brooks, Manjula R. Canagaratna, Andrew Freedman, John T. Jayne, Doug R. Worsnop, Paul Davidovits, David Chandler, and Charles E. Kolb
Atmos. Meas. Tech., 11, 3479–3490, https://doi.org/10.5194/amt-11-3479-2018, https://doi.org/10.5194/amt-11-3479-2018, 2018
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We have adopted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols at submicron sizes and relatively low mass concentrations. Aerosol particles are deposited in the form of a thin film with interdigitated electrodes using electrostatic precipitation. Broadband dielectric spectroscopy is used to measure the kinetically controlled glass transition temperatures of glycerol and citric acid aerosols with three atmospheric relevant cooling rates.
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.
Riinu Ots, Mathew R. Heal, Dominique E. Young, Leah R. Williams, James D. Allan, Eiko Nemitz, Chiara Di Marco, Anais Detournay, Lu Xu, Nga L. Ng, Hugh Coe, Scott C. Herndon, Ian A. Mackenzie, David C. Green, Jeroen J. P. Kuenen, Stefan Reis, and Massimo Vieno
Atmos. Chem. Phys., 18, 4497–4518, https://doi.org/10.5194/acp-18-4497-2018, https://doi.org/10.5194/acp-18-4497-2018, 2018
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The main hypothesis of this paper is that people who live in large cities in the UK disobey the
smoke control lawas it has not been actively enforced for decades now. However, the use of wood in residential heating has increased, partly due to renewable energy targets, but also for discretionary (i.e. pleasant fireplaces) reasons. Our study is based mainly in London, but similar struggles with urban air quality due to residential wood and coal burning are seen in other major European cities.
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.
Jingyi Li, Jingqiu Mao, Arlene M. Fiore, Ronald C. Cohen, John D. Crounse, Alex P. Teng, Paul O. Wennberg, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Jeff Peischl, Ilana B. Pollack, Thomas B. Ryerson, Patrick Veres, James M. Roberts, J. Andrew Neuman, John B. Nowak, Glenn M. Wolfe, Thomas F. Hanisco, Alan Fried, Hanwant B. Singh, Jack Dibb, Fabien Paulot, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2341–2361, https://doi.org/10.5194/acp-18-2341-2018, https://doi.org/10.5194/acp-18-2341-2018, 2018
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We present the first comprehensive model evaluation of summertime reactive oxidized nitrogen using a high-resolution chemistry–climate model with up-to-date isoprene oxidation chemistry, along with a series of observations from aircraft campaigns and ground measurement networks from 2004 to 2013 over the Southeast US. We investigate the impact of NOx emission reductions on changes in reactive nitrogen speciation and export efficiency as well as ozone in the past and future decade.
Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, António Dias, Neil M. Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, and Peter H. McMurry
Atmos. Chem. Phys., 18, 845–863, https://doi.org/10.5194/acp-18-845-2018, https://doi.org/10.5194/acp-18-845-2018, 2018
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A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
Yunjiang Zhang, Lili Tang, Philip L. Croteau, Olivier Favez, Yele Sun, Manjula R. Canagaratna, Zhuang Wang, Florian Couvidat, Alexandre Albinet, Hongliang Zhang, Jean Sciare, André S. H. Prévôt, John T. Jayne, and Douglas R. Worsnop
Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, https://doi.org/10.5194/acp-17-14501-2017, 2017
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We conducted the first field measurements of non-refractory fine aerosols (NR-PM2.5) in a megacity of eastern China using a PM2.5-ACSM along with a PM1-ACSM measurement. Inter-comparisons demonstrated that the NR-PM2.5 components can be characterized. Substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm, with sulfate and SOA being the two largest contributors. The impacts of aerosol water driven by secondary inorganic aerosols on SOA formation were explored.
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.
Ryan Thalman, Suzane S. de Sá, Brett B. Palm, Henrique M. J. Barbosa, Mira L. Pöhlker, M. Lizabeth Alexander, Joel Brito, Samara Carbone, Paulo Castillo, Douglas A. Day, Chongai Kuang, Antonio Manzi, Nga Lee Ng, Arthur J. Sedlacek III, Rodrigo Souza, Stephen Springston, Thomas Watson, Christopher Pöhlker, Ulrich Pöschl, Meinrat O. Andreae, Paulo Artaxo, Jose L. Jimenez, Scot T. Martin, and Jian Wang
Atmos. Chem. Phys., 17, 11779–11801, https://doi.org/10.5194/acp-17-11779-2017, https://doi.org/10.5194/acp-17-11779-2017, 2017
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Particle hygroscopicity, mixing state, and the hygroscopicity of organic components were characterized in central Amazonia for 1 year; their seasonal and diel variations were driven by a combination of primary emissions, photochemical oxidation, and boundary layer development. The relationship between the hygroscopicity of organic components and their oxidation level was examined, and the results help to reconcile the differences among the relationships observed in previous studies.
Yue Zhao, Jeremy K. Chan, Felipe D. Lopez-Hilfiker, Megan A. McKeown, Emma L. D'Ambro, Jay G. Slowik, Jeffrey A. Riffell, and Joel A. Thornton
Atmos. Meas. Tech., 10, 3609–3625, https://doi.org/10.5194/amt-10-3609-2017, https://doi.org/10.5194/amt-10-3609-2017, 2017
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We present a novel atmospheric pressure electrospray chemical ionization (ESCI) source that can generate intense and stable currents of several specific reagent ions using a range of salt solutions prepared in methanol. We couple the ESCI source to a high-resolution time-of-flight mass spectrometer (HRToF-MS) and assess instrument performance through calibrations using different gas standards and measurements of organic mixtures formed by ozonolysis of α-pinene.
Wing Y. Tuet, Yunle Chen, Shierly Fok, Julie A. Champion, and Nga L. Ng
Atmos. Chem. Phys., 17, 11423–11440, https://doi.org/10.5194/acp-17-11423-2017, https://doi.org/10.5194/acp-17-11423-2017, 2017
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Exposure to secondary organic aerosols (SOAs) may have cardiopulmonary health implications. Alveolar macrophages were exposed to various SOA systems and reactive oxygen and nitrogen species production and cytokine secretion was measured post-exposure. Results from this study show that the chemical structure of SOA products may be important for determining cellular responses and demonstrate that the health effects of SOA are important to consider for the health implications of ambient aerosols.
Benjamin N. Murphy, Matthew C. Woody, Jose L. Jimenez, Ann Marie G. Carlton, Patrick L. Hayes, Shang Liu, Nga L. Ng, Lynn M. Russell, Ari Setyan, Lu Xu, Jeff Young, Rahul A. Zaveri, Qi Zhang, and Havala O. T. Pye
Atmos. Chem. Phys., 17, 11107–11133, https://doi.org/10.5194/acp-17-11107-2017, https://doi.org/10.5194/acp-17-11107-2017, 2017
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We incorporate recent findings about the behavior of organic pollutants in urban airsheds into the Community Multiscale Air Quality (CMAQ) model to refine predictions of organic particulate pollution in the United States. The new techniques, which account for the volatility and ongoing chemistry of airborne organic compounds, substantially reduce biases, particularly in the winter time and near emission sources.
Andrew Lambe, Paola Massoli, Xuan Zhang, Manjula Canagaratna, John Nowak, Conner Daube, Chao Yan, Wei Nie, Timothy Onasch, John Jayne, Charles Kolb, Paul Davidovits, Douglas Worsnop, and William Brune
Atmos. Meas. Tech., 10, 2283–2298, https://doi.org/10.5194/amt-10-2283-2017, https://doi.org/10.5194/amt-10-2283-2017, 2017
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This work enables the study of NOx-influenced secondary organic aerosol formation chemistry in oxidation flow reactors to an extent that was not previously possible. The method uses reactions of exited oxygen O(1D) radicals (formed from ozone photolysis at 254 nm or nitrous oxide photolysis at 185 nm) with nitrous oxide (N2O) to produce NO. We demonstrate proof of concept using chemical ionization mass spectrometer measurements to detect gas-phase oxidation products of isoprene and α -pinene.
Rebecca H. Schwantes, Katherine A. Schilling, Renee C. McVay, Hanna Lignell, Matthew M. Coggon, Xuan Zhang, Paul O. Wennberg, and John H. Seinfeld
Atmos. Chem. Phys., 17, 3453–3474, https://doi.org/10.5194/acp-17-3453-2017, https://doi.org/10.5194/acp-17-3453-2017, 2017
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Toluene, one of the principle aromatic compounds present in the atmosphere, is oxidized by OH to produce cresol and other products. Here later-generation low-volatility oxygenated products from cresol oxidation by OH are detected in the gas and particle phases. This work identifies a simple and significant mechanism for toluene secondary organic aerosol formation through the cresol pathway. Likely the phenolic pathway of other aromatic compounds is also important for secondary organic aerosol.
Yuanlong Huang, Matthew M. Coggon, Ran Zhao, Hanna Lignell, Michael U. Bauer, Richard C. Flagan, and John H. Seinfeld
Atmos. Meas. Tech., 10, 839–867, https://doi.org/10.5194/amt-10-839-2017, https://doi.org/10.5194/amt-10-839-2017, 2017
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We report on the development of a new laminar flow tube reactor for the study of gas-phase atmospheric chemistry and secondary organic aerosol formation. The present paper is devoted to the design and fluid dynamical characterization of the reactor. The results of gas and particle residence time distribution experiments in the reactor, together with an evaluation of the effect of non-isothermal conditions, are reported.
Theodora Nah, Renee C. McVay, Jeffrey R. Pierce, John H. Seinfeld, and Nga L. Ng
Atmos. Chem. Phys., 17, 2297–2310, https://doi.org/10.5194/acp-17-2297-2017, https://doi.org/10.5194/acp-17-2297-2017, 2017
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We present a model framework that accounts for coagulation in chamber studies where high seed aerosol surface area concentrations are used. The uncertainties in the calculated SOA mass concentrations and yields between four different particle-wall loss correction methods over the series of α-pinene ozonolysis experiments are also assessed. We show that SOA mass yields calculated by the four methods can deviate significantly in studies where high seed aerosol surface area concentrations are used.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Wing Y. Tuet, Yunle Chen, Lu Xu, Shierly Fok, Dong Gao, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 17, 839–853, https://doi.org/10.5194/acp-17-839-2017, https://doi.org/10.5194/acp-17-839-2017, 2017
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Secondary organic aerosols (SOA) comprise a significant fraction of particulate matter (PM) and may have health implications. The water-soluble oxidative potentials of various SOA systems were determined using dithiothreitol consumption. Results from this study demonstrate that precursor identity was more influential than reaction condition in determining SOA oxidative potential and highlight a need to consider SOA contributions from anthropogenic hydrocarbons to PM-induced health effects.
Provat K. Saha, Andrey Khlystov, Khairunnisa Yahya, Yang Zhang, Lu Xu, Nga L. Ng, and Andrew P. Grieshop
Atmos. Chem. Phys., 17, 501–520, https://doi.org/10.5194/acp-17-501-2017, https://doi.org/10.5194/acp-17-501-2017, 2017
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.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
Neha Sareen, Annmarie G. Carlton, Jason D. Surratt, Avram Gold, Ben Lee, Felipe D. Lopez-Hilfiker, Claudia Mohr, Joel A. Thornton, Zhenfa Zhang, Yong B. Lim, and Barbara J. Turpin
Atmos. Chem. Phys., 16, 14409–14420, https://doi.org/10.5194/acp-16-14409-2016, https://doi.org/10.5194/acp-16-14409-2016, 2016
Xuan Zhang, Jordan E. Krechmer, Michael Groessl, Wen Xu, Stephan Graf, Michael Cubison, John T. Jayne, Jose L. Jimenez, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Chem. Phys., 16, 12945–12959, https://doi.org/10.5194/acp-16-12945-2016, https://doi.org/10.5194/acp-16-12945-2016, 2016
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We develop a novel two-dimensional space to probe the molecular composition of atmospheric organic aerosols.
Natasha Hodas, Andreas Zuend, Katherine Schilling, Thomas Berkemeier, Manabu Shiraiwa, Richard C. Flagan, and John H. Seinfeld
Atmos. Chem. Phys., 16, 12767–12792, https://doi.org/10.5194/acp-16-12767-2016, https://doi.org/10.5194/acp-16-12767-2016, 2016
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Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic-inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. This work explores the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
Javier Sanchez, David J. Tanner, Dexian Chen, L. Gregory Huey, and Nga L. Ng
Atmos. Meas. Tech., 9, 3851–3861, https://doi.org/10.5194/amt-9-3851-2016, https://doi.org/10.5194/amt-9-3851-2016, 2016
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HO2 radicals play an important role in tropospheric chemistry. Here we propose a new direct method for measuring HO2 radicals in the atmosphere using bromide anion chemical ionization mass spectrometry. Ambient measurements in Atlanta are presented. Instrument performance parameters: sensitivity, lower detection limit, and time resolution are discussed. We demonstrate that the technique provides excellent selectivity and is suitable for in situ ground-based HO2 measurements.
Theodora Nah, Renee C. McVay, Xuan Zhang, Christopher M. Boyd, John H. Seinfeld, and Nga L. Ng
Atmos. Chem. Phys., 16, 9361–9379, https://doi.org/10.5194/acp-16-9361-2016, https://doi.org/10.5194/acp-16-9361-2016, 2016
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The influence of seed aerosol surface area and oxidation rate on SOA formation in α-pinene ozonolysis is studied. SOA growth rate and mass yields are independent of seed surface area, consistent with the condensation of SOA-forming vapors being dominated by quasi-equilibrium growth. Faster α-pinene oxidation rates and higher SOA mass yields are observed at increasing O3 concentrations, indicating that a faster α-pinene oxidation rate leads to rapidly produced SOA-forming oxidation products.
Hilkka Timonen, Mike Cubison, Minna Aurela, David Brus, Heikki Lihavainen, Risto Hillamo, Manjula Canagaratna, Bettina Nekat, Rolf Weller, Douglas Worsnop, and Sanna Saarikoski
Atmos. Meas. Tech., 9, 3263–3281, https://doi.org/10.5194/amt-9-3263-2016, https://doi.org/10.5194/amt-9-3263-2016, 2016
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The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power (m∕Δm50 ∼ 500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements and ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results.
Jordan E. Krechmer, Michael Groessl, Xuan Zhang, Heikki Junninen, Paola Massoli, Andrew T. Lambe, Joel R. Kimmel, Michael J. Cubison, Stephan Graf, Ying-Hsuan Lin, Sri H. Budisulistiorini, Haofei Zhang, Jason D. Surratt, Richard Knochenmuss, John T. Jayne, Douglas R. Worsnop, Jose-Luis Jimenez, and Manjula R. Canagaratna
Atmos. Meas. Tech., 9, 3245–3262, https://doi.org/10.5194/amt-9-3245-2016, https://doi.org/10.5194/amt-9-3245-2016, 2016
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.
Alessandro Franchin, Andy Downard, Juha Kangasluoma, Tuomo Nieminen, Katrianne Lehtipalo, Gerhard Steiner, Hanna E. Manninen, Tuukka Petäjä, Richard C. Flagan, and Markku Kulmala
Atmos. Meas. Tech., 9, 2709–2720, https://doi.org/10.5194/amt-9-2709-2016, https://doi.org/10.5194/amt-9-2709-2016, 2016
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High transmission efficiency is key for classifying and counting atmospheric aerosol below 10 nm. We developed a new high-transmission inlet for the Caltech nano-radial DMA (nRDMA) and successfully deployed the nRDMA, equipped with the new inlet, in chamber measurements, using a particle size magnifier (PSM) and a booster CPC as a counter. With this setup, we were able to measure size distributions of ions between 1.3 and 6 nm in mobility diameter.
Riinu Ots, Dominique E. Young, Massimo Vieno, Lu Xu, Rachel E. Dunmore, James D. Allan, Hugh Coe, Leah R. Williams, Scott C. Herndon, Nga L. Ng, Jacqueline F. Hamilton, Robert Bergström, Chiara Di Marco, Eiko Nemitz, Ian A. Mackenzie, Jeroen J. P. Kuenen, David C. Green, Stefan Reis, and Mathew R. Heal
Atmos. Chem. Phys., 16, 6453–6473, https://doi.org/10.5194/acp-16-6453-2016, https://doi.org/10.5194/acp-16-6453-2016, 2016
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This study investigates the contribution of diesel vehicle emissions to organic aerosol formation and particulate matter concentrations in London. Comparisons of simulated pollutant concentrations with observations show good agreement and give confidence in the skill of the model applied. The contribution of diesel vehicle emissions, which are currently not included in official emissions inventories, is demonstrated to be substantial, indicating that more research on this topic is required.
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.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
Felipe D. Lopez-Hilfiker, Siddarth Iyer, Claudia Mohr, Ben H. Lee, Emma L. D'Ambro, Theo Kurtén, and Joel A. Thornton
Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, https://doi.org/10.5194/amt-9-1505-2016, 2016
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We present the maximum sensitivity of a TOF-CIMS using the collision limit and iodide adducts. We also present an ion adduct declustering scanning procedure which determines the effective binding energies of the detected ion adducts and therefore their approximate sensitivity. The combination of declustering scanning and the collision limit provides an approximate calibration for many compounds in the mass spectrum which would otherwise be impossible to obtain by traditional methods.
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
Rajan K. Chakrabarty, Madhu Gyawali, Reddy L. N. Yatavelli, Apoorva Pandey, Adam C. Watts, Joseph Knue, Lung-Wen A. Chen, Robert R. Pattison, Anna Tsibart, Vera Samburova, and Hans Moosmüller
Atmos. Chem. Phys., 16, 3033–3040, https://doi.org/10.5194/acp-16-3033-2016, https://doi.org/10.5194/acp-16-3033-2016, 2016
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Brown carbon aerosols dominate particulate emissions from the burning of Alaskan and Siberian peatlands. They physically occur as amorphous "tar balls" with negligible black carbon mixing. They absorb very strongly in the shorter visible wavelengths, characterized by a mean Ångström coefficient of ≈ 9. These aerosols could result in a net warming of the atmosphere, provided the albedo of the underlying surface is greater than 0.6.
Christopher D. Cappa, Shantanu H. Jathar, Michael J. Kleeman, Kenneth S. Docherty, Jose L. Jimenez, John H. Seinfeld, and Anthony S. Wexler
Atmos. Chem. Phys., 16, 3041–3059, https://doi.org/10.5194/acp-16-3041-2016, https://doi.org/10.5194/acp-16-3041-2016, 2016
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Losses of vapors to walls of chambers can negatively bias SOA formation measurements, consequently leading to low predicted SOA concentrations in air quality models. Here, we show that accounting for such vapor losses leads to substantial increases in the predicted amount of SOA formed from VOCs and to notable increases in the O : C atomic ratio in two US regions. Comparison with a variety of observational data suggests generally improved model performance when vapor wall losses are accounted for.
Renee C. McVay, Xuan Zhang, Bernard Aumont, Richard Valorso, Marie Camredon, Yuyi S. La, Paul O. Wennberg, and John H. Seinfeld
Atmos. Chem. Phys., 16, 2785–2802, https://doi.org/10.5194/acp-16-2785-2016, https://doi.org/10.5194/acp-16-2785-2016, 2016
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Secondary organic aerosol (SOA) affects climate change, human health, and cloud formation. We examine SOA formation from the biogenic hydrocarbon α-pinene and observe unexpected experimental results that run contrary to model predictions. Various processes are explored via modeling to rationalize the observations. The paper identifies the importance of further constraining via experiments various steps in the chemical mechanism in order to accurately predict SOA worldwide.
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.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Atmos. Chem. Phys., 16, 2309–2322, https://doi.org/10.5194/acp-16-2309-2016, https://doi.org/10.5194/acp-16-2309-2016, 2016
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Multi-generational chemistry schemes applied in regional models do not increase secondary organic aerosol (SOA) mass production relative to traditional "two-product" schemes when both models are fitted to the same chamber data. The multi-generational chemistry schemes do change the predicted composition of SOA and the source attribution of SOA.
Y. S. La, M. Camredon, P. J. Ziemann, R. Valorso, A. Matsunaga, V. Lannuque, J. Lee-Taylor, A. Hodzic, S. Madronich, and B. Aumont
Atmos. Chem. Phys., 16, 1417–1431, https://doi.org/10.5194/acp-16-1417-2016, https://doi.org/10.5194/acp-16-1417-2016, 2016
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The potential impact of chamber walls on the loss of gaseous organic species and secondary organic aerosol (SOA) formation has been explored using the GECKO-A modeling tool, which explicitly represents SOA formation and gas-wall partitioning. The model was compared with 41 smog chamber experiments of SOA formation under OH oxidation of alkane and alkene serie. The organic vapor loss to the chamber walls is found to affect SOA yields as well as the composition of the gas and the particle phase.
T. P. Riedel, Y.-H. Lin, Z. Zhang, K. Chu, J. A. Thornton, W. Vizuete, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 16, 1245–1254, https://doi.org/10.5194/acp-16-1245-2016, https://doi.org/10.5194/acp-16-1245-2016, 2016
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IEPOX, a photooxidation product of isoprene, contributes to ambient secondary organic aerosol concentrations. Controlled atmospheric chamber experiments and modeling are used to extract formation rate information of chemical species that contribute to IEPOX-derived secondary organic aerosol.
L. Xu, L. R. Williams, D. E. Young, J. D. Allan, H. Coe, P. Massoli, E. Fortner, P. Chhabra, S. Herndon, W. A. Brooks, J. T. Jayne, D. R. Worsnop, A. C. Aiken, S. Liu, K. Gorkowski, M. K. Dubey, Z. L. Fleming, S. Visser, A. S. H. Prévôt, and N. L. Ng
Atmos. Chem. Phys., 16, 1139–1160, https://doi.org/10.5194/acp-16-1139-2016, https://doi.org/10.5194/acp-16-1139-2016, 2016
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We investigate the spatial distribution of submicron aerosol in the greater London area as part of the Clean Air for London (ClearfLo) project in winter 2012. Although the concentrations of organic aerosol (OA) are similar between a rural and an urban site, the OA sources are different. We also examine the volatility of submicron aerosol at the rural site and find that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon.
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.
M. D. Petters, S. M. Kreidenweis, and P. J. Ziemann
Geosci. Model Dev., 9, 111–124, https://doi.org/10.5194/gmd-9-111-2016, https://doi.org/10.5194/gmd-9-111-2016, 2016
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Organic particles suspended in air serve as nucleation seeds for droplets in atmospheric clouds. Over time their chemical composition changes towards more functionalized compounds. This work presents a model that can predict an organic compounds' ability promote the nucleation of cloud drops from its functional group composition. Hydroxyl, carboxyl, aldehyde, hydroperoxide, carbonyl, and ether moieties promote droplet nucleation. Methylene and nitrate moieties inhibit droplet nucleation.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
D. M. Lienhard, A. J. Huisman, U. K. Krieger, Y. Rudich, C. Marcolli, B. P. Luo, D. L. Bones, J. P. Reid, A. T. Lambe, M. R. Canagaratna, P. Davidovits, T. B. Onasch, D. R. Worsnop, S. S. Steimer, T. Koop, and T. Peter
Atmos. Chem. Phys., 15, 13599–13613, https://doi.org/10.5194/acp-15-13599-2015, https://doi.org/10.5194/acp-15-13599-2015, 2015
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New data of water diffusivity in secondary organic aerosol (SOA) material and organic/inorganic model mixtures is presented over an extensive temperature range. Our data suggest that water diffusion in SOA is sufficiently fast so that it is unlikely to have significant consequences on the direct climatic effect under tropospheric conditions. Glass formation in SOA is unlikely to restrict homogeneous ice nucleation.
V. Crenn, J. Sciare, P. L. Croteau, S. Verlhac, R. Fröhlich, C. A. Belis, W. Aas, M. Äijälä, A. Alastuey, B. Artiñano, D. Baisnée, N. Bonnaire, M. Bressi, M. Canagaratna, F. Canonaco, C. Carbone, F. Cavalli, E. Coz, M. J. Cubison, J. K. Esser-Gietl, D. C. Green, V. Gros, L. Heikkinen, H. Herrmann, C. Lunder, M. C. Minguillón, G. Močnik, C. D. O'Dowd, J. Ovadnevaite, J.-E. Petit, E. Petralia, L. Poulain, M. Priestman, V. Riffault, A. Ripoll, R. Sarda-Estève, J. G. Slowik, A. Setyan, A. Wiedensohler, U. Baltensperger, A. S. H. Prévôt, J. T. Jayne, and O. Favez
Atmos. Meas. Tech., 8, 5063–5087, https://doi.org/10.5194/amt-8-5063-2015, https://doi.org/10.5194/amt-8-5063-2015, 2015
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A large intercomparison study of 13 Q-ACSM was conducted for a 3-week period in the region of Paris to evaluate the performance of this instrument and to monitor the major NR-PM1 chemical components. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were found to be 9, 15, 19, 28, and 36% for NR-PM1, NO3, OM, SO4, and NH4, respectively. Some recommendations regarding best calibration practices, standardized data processing and data treatment are also provided.
S. Visser, J. G. Slowik, M. Furger, P. Zotter, N. Bukowiecki, F. Canonaco, U. Flechsig, K. Appel, D. C. Green, A. H. Tremper, D. E. Young, P. I. Williams, J. D. Allan, H. Coe, L. R. Williams, C. Mohr, L. Xu, N. L. Ng, E. Nemitz, J. F. Barlow, C. H. Halios, Z. L. Fleming, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11291–11309, https://doi.org/10.5194/acp-15-11291-2015, https://doi.org/10.5194/acp-15-11291-2015, 2015
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Trace element measurements in three particle size ranges (PM10-2.5, PM2.5-1.0 and PM1.0-0.3) were performed with 2h time resolution at kerbside, urban background and rural sites during the ClearfLo winter 2012 campaign in London. The environment-dependent variability of emissions was characterized using the Multilinear Engine implementation of the positive matrix factorization model. A total of nine different factors were resolved from local, regional and natural origin.
A. Kürten, S. Münch, L. Rondo, F. Bianchi, J. Duplissy, T. Jokinen, H. Junninen, N. Sarnela, S. Schobesberger, M. Simon, M. Sipilä, J. Almeida, A. Amorim, J. Dommen, N. M. Donahue, E. M. Dunne, R. C. Flagan, A. Franchin, J. Kirkby, A. Kupc, V. Makhmutov, T. Petäjä, A. P. Praplan, F. Riccobono, G. Steiner, A. Tomé, G. Tsagkogeorgas, P. E. Wagner, D. Wimmer, U. Baltensperger, M. Kulmala, D. R. Worsnop, and J. Curtius
Atmos. Chem. Phys., 15, 10701–10721, https://doi.org/10.5194/acp-15-10701-2015, https://doi.org/10.5194/acp-15-10701-2015, 2015
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New particle formation (NPF) is an important atmospheric process. At cold temperatures in the upper troposphere the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system are thought to be important for NPF. Sulfuric acid monomer (H2SO4) and sulfuric acid dimer ((H2SO4)2) concentrations were measured between 208 and 248K for these systems and dimer evaporation rates were derived. These data will help to better understand and predict binary and ternary nucleation at low temperatures.
S. H. Jathar, C. D. Cappa, A. S. Wexler, J. H. Seinfeld, and M. J. Kleeman
Geosci. Model Dev., 8, 2553–2567, https://doi.org/10.5194/gmd-8-2553-2015, https://doi.org/10.5194/gmd-8-2553-2015, 2015
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Multi-generational oxidation of organic vapors can significantly alter the mass, chemical composition and properties of secondary organic aerosol (SOA). Here, we implement a semi-explicit, constrained multi-generational oxidation model of Cappa and Wilson (2012) in a 3-D air quality model. When compared with results from a current-generation SOA model, we predict similar mass concentrations of SOA but a different chemical composition. O:C ratios of SOA are in line with those measured globally.
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.
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
C. M. Boyd, J. Sanchez, L. Xu, A. J. Eugene, T. Nah, W. Y. Tuet, M. I. Guzman, and N. L. Ng
Atmos. Chem. Phys., 15, 7497–7522, https://doi.org/10.5194/acp-15-7497-2015, https://doi.org/10.5194/acp-15-7497-2015, 2015
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Laboratory chamber studies were conducted to investigate the formation of secondary organic aerosol from β-pinene oxidation by nitrate radicals. These experiments probed the effects of peroxy radical fate and relative humidity on the mass and chemical composition of secondary organic aerosol formed from nighttime chemistry. Results from this study were used to evaluate the contributions of NO3+monoterpene reaction to ambient organic aerosol recently measured in the southeastern United States.
L. Xu, S. Suresh, H. Guo, R. J. Weber, and N. L. Ng
Atmos. Chem. Phys., 15, 7307–7336, https://doi.org/10.5194/acp-15-7307-2015, https://doi.org/10.5194/acp-15-7307-2015, 2015
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Year-long comprehensive characterization of ambient aerosol was performed in both rural and urban sites in the southeastern US as part of Southeastern Center of Air Pollution and Epidemiology (SCAPE) study and Southeastern Oxidant and Aerosol Study (SOAS). Three independent methods were applied to estimate the concentration of particle-phase organic nitrates. The spatial distribution of organic aerosol is investigated by comparing simultaneous HR-ToF-AMS and ACSM measurements at different sites.
M. J. Alvarado, C. R. Lonsdale, R. J. Yokelson, S. K. Akagi, H. Coe, J. S. Craven, E. V. Fischer, G. R. McMeeking, J. H. Seinfeld, T. Soni, J. W. Taylor, D. R. Weise, and C. E. Wold
Atmos. Chem. Phys., 15, 6667–6688, https://doi.org/10.5194/acp-15-6667-2015, https://doi.org/10.5194/acp-15-6667-2015, 2015
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Being able to understand and simulate the chemical evolution of biomass burning smoke plumes under a wide variety of conditions is a critical part of forecasting the impact of these fires on air quality, atmospheric composition, and climate. Here we use an improved model of this chemistry to simulate the evolution of ozone and secondary organic aerosol within a young biomass burning smoke plume from the Williams prescribed burn in chaparral, which was sampled over California in November 2009.
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.
E. Jung, B. A. Albrecht, H. H. Jonsson, Y.-C. Chen, J. H. Seinfeld, A. Sorooshian, A. R. Metcalf, S. Song, M. Fang, and L. M. Russell
Atmos. Chem. Phys., 15, 5645–5658, https://doi.org/10.5194/acp-15-5645-2015, https://doi.org/10.5194/acp-15-5645-2015, 2015
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To study the effect of giant cloud condensation nuclei (GCCN) on precipitation processes in stratocumulus clouds, 1-10 µm diameter salt particles were released from an aircraft while flying near the cloud top off the central coast of California. The analyses suggest that GCCN result in a four-fold increase in the cloud base rainfall rate and depletion of the cloud water due to rainout.
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.
N. Hodas, A. Zuend, W. Mui, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 15, 5027–5045, https://doi.org/10.5194/acp-15-5027-2015, https://doi.org/10.5194/acp-15-5027-2015, 2015
X. Zhang, R. H. Schwantes, R. C. McVay, H. Lignell, M. M. Coggon, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 15, 4197–4214, https://doi.org/10.5194/acp-15-4197-2015, https://doi.org/10.5194/acp-15-4197-2015, 2015
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We present an experimental protocol to constrain the nature of organic vapor--wall deposition in Teflon chambers and develop an empirical model to predict the wall-induced deposition rate of intermediate/semi/non-volatility organic vapors in chambers.
S. Visser, J. G. Slowik, M. Furger, P. Zotter, N. Bukowiecki, R. Dressler, U. Flechsig, K. Appel, D. C. Green, A. H. Tremper, D. E. Young, P. I. Williams, J. D. Allan, S. C. Herndon, L. R. Williams, C. Mohr, L. Xu, N. L. Ng, A. Detournay, J. F. Barlow, C. H. Halios, Z. L. Fleming, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 2367–2386, https://doi.org/10.5194/acp-15-2367-2015, https://doi.org/10.5194/acp-15-2367-2015, 2015
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Ambient concentrations of trace elements with 2h time resolution were measured in three size ranges (PM10–2.5, PM2.5–1.0, PM1.0–0.3) at kerbside, urban background and rural sites in London during the ClearfLo (Clean Air for London) field campaign. Quantification of kerb and urban increments, and assessment of diurnal and weekly variability provided insight into sources governing urban air quality and the effects of urban micro-environments on human exposure.
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
P. S. Chhabra, A. T. Lambe, M. R. Canagaratna, H. Stark, J. T. Jayne, T. B. Onasch, P. Davidovits, J. R. Kimmel, and D. R. Worsnop
Atmos. Meas. Tech., 8, 1–18, https://doi.org/10.5194/amt-8-1-2015, https://doi.org/10.5194/amt-8-1-2015, 2015
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Authors of this publication used acetate chemical ionization mass spectrometry (acetate-CIMS) to measure experimental products of alpha-pinene and naphthalene oxidation formed in a flow reactor. Acetate-CIMS instrumentation is selective toward carboxylic acid compounds which are readily formed in atmospheric photooxidation processes. Spectral information was used to identify previously measured products of both systems and to estimate their volatilities.
T. B. Nguyen, J. D. Crounse, R. H. Schwantes, A. P. Teng, K. H. Bates, X. Zhang, J. M. St. Clair, W. H. Brune, G. S. Tyndall, F. N. Keutsch, J. H. Seinfeld, and P. O. Wennberg
Atmos. Chem. Phys., 14, 13531–13549, https://doi.org/10.5194/acp-14-13531-2014, https://doi.org/10.5194/acp-14-13531-2014, 2014
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 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
M. Shiraiwa, T. Berkemeier, K. A. Schilling-Fahnestock, J. H. Seinfeld, and U. Pöschl
Atmos. Chem. Phys., 14, 8323–8341, https://doi.org/10.5194/acp-14-8323-2014, https://doi.org/10.5194/acp-14-8323-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
A. Setyan, C. Song, M. Merkel, W. B. Knighton, T. B. Onasch, M. R. Canagaratna, D. R. Worsnop, A. Wiedensohler, J. E. Shilling, and Q. Zhang
Atmos. Chem. Phys., 14, 6477–6494, https://doi.org/10.5194/acp-14-6477-2014, https://doi.org/10.5194/acp-14-6477-2014, 2014
C. J. Gaston, J. A. Thornton, and N. L. Ng
Atmos. Chem. Phys., 14, 5693–5707, https://doi.org/10.5194/acp-14-5693-2014, https://doi.org/10.5194/acp-14-5693-2014, 2014
R. A. Zaveri, R. C. Easter, J. E. Shilling, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 5153–5181, https://doi.org/10.5194/acp-14-5153-2014, https://doi.org/10.5194/acp-14-5153-2014, 2014
M. Paglione, S. Saarikoski, S. Carbone, R. Hillamo, M. C. Facchini, E. Finessi, L. Giulianelli, C. Carbone, S. Fuzzi, F. Moretti, E. Tagliavini, E. Swietlicki, K. Eriksson Stenström, A. S. H. Prévôt, P. Massoli, M. Canaragatna, D. Worsnop, and S. Decesari
Atmos. Chem. Phys., 14, 5089–5110, https://doi.org/10.5194/acp-14-5089-2014, https://doi.org/10.5194/acp-14-5089-2014, 2014
S. Bleicher, J. C. Buxmann, R. Sander, T. P. Riedel, J. A. Thornton, U. Platt, and C. Zetzsch
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-10135-2014, https://doi.org/10.5194/acpd-14-10135-2014, 2014
Revised manuscript has not been submitted
T. P. Riedel, G. M. Wolfe, K. T. Danas, J. B. Gilman, W. C. Kuster, D. M. Bon, A. Vlasenko, S.-M. Li, E. J. Williams, B. M. Lerner, P. R. Veres, J. M. Roberts, J. S. Holloway, B. Lefer, S. S. Brown, and J. A. Thornton
Atmos. Chem. Phys., 14, 3789–3800, https://doi.org/10.5194/acp-14-3789-2014, https://doi.org/10.5194/acp-14-3789-2014, 2014
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. Lutz, M. Hallquist, D. Worsnop, and J. A. Thornton
Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, https://doi.org/10.5194/amt-7-983-2014, 2014
T. B. Nguyen, M. M. Coggon, K. H. Bates, X. Zhang, R. H. Schwantes, K. A. Schilling, C. L. Loza, R. C. Flagan, P. O. Wennberg, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 3497–3510, https://doi.org/10.5194/acp-14-3497-2014, https://doi.org/10.5194/acp-14-3497-2014, 2014
S. E. Pusede, D. R. Gentner, P. J. Wooldridge, E. C. Browne, A. W. Rollins, K.-E. Min, A. R. Russell, J. Thomas, L. Zhang, W. H. Brune, S. B. Henry, J. P. DiGangi, F. N. Keutsch, S. A. Harrold, J. A. Thornton, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, J. Sanders, X. Ren, T. C. VandenBoer, M. Z. Markovic, A. Guha, R. Weber, A. H. Goldstein, and R. C. Cohen
Atmos. Chem. Phys., 14, 3373–3395, https://doi.org/10.5194/acp-14-3373-2014, https://doi.org/10.5194/acp-14-3373-2014, 2014
R. Zhang, T. Duhl, M. T. Salam, J. M. House, R. C. Flagan, E. L. Avol, F. D. Gilliland, A. Guenther, S. H. Chung, B. K. Lamb, and T. M. VanReken
Biogeosciences, 11, 1461–1478, https://doi.org/10.5194/bg-11-1461-2014, https://doi.org/10.5194/bg-11-1461-2014, 2014
J. J. Ensberg, P. L. Hayes, J. L. Jimenez, J. B. Gilman, W. C. Kuster, J. A. de Gouw, J. S. Holloway, T. D. Gordon, S. Jathar, A. L. Robinson, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 2383–2397, https://doi.org/10.5194/acp-14-2383-2014, https://doi.org/10.5194/acp-14-2383-2014, 2014
P. Tiitta, V. Vakkari, P. Croteau, J. P. Beukes, P. G. van Zyl, M. Josipovic, A. D. Venter, K. Jaars, J. J. Pienaar, N. L. Ng, M. R. Canagaratna, J. T. Jayne, V.-M. Kerminen, H. Kokkola, M. Kulmala, A. Laaksonen, D. R. Worsnop, and L. Laakso
Atmos. Chem. Phys., 14, 1909–1927, https://doi.org/10.5194/acp-14-1909-2014, https://doi.org/10.5194/acp-14-1909-2014, 2014
X. Zhang, R. H. Schwantes, M. M. Coggon, C. L. Loza, K. A. Schilling, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1733–1753, https://doi.org/10.5194/acp-14-1733-2014, https://doi.org/10.5194/acp-14-1733-2014, 2014
R. L. N. Yatavelli, H. Stark, S. L. Thompson, J. R. Kimmel, M. J. Cubison, D. A. Day, P. Campuzano-Jost, B. B. Palm, A. Hodzic, J. A. Thornton, J. T. Jayne, D. R. Worsnop, and J. L. Jimenez
Atmos. Chem. Phys., 14, 1527–1546, https://doi.org/10.5194/acp-14-1527-2014, https://doi.org/10.5194/acp-14-1527-2014, 2014
C. L. Loza, J. S. Craven, L. D. Yee, M. M. Coggon, R. H. Schwantes, M. Shiraiwa, X. Zhang, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 1423–1439, https://doi.org/10.5194/acp-14-1423-2014, https://doi.org/10.5194/acp-14-1423-2014, 2014
A. L. Corrigan, L. M. Russell, S. Takahama, M. Äijälä, M. Ehn, H. Junninen, J. Rinne, T. Petäjä, M. Kulmala, A. L. Vogel, T. Hoffmann, C. J. Ebben, F. M. Geiger, P. Chhabra, J. H. Seinfeld, D. R. Worsnop, W. Song, J. Auld, and J. Williams
Atmos. Chem. Phys., 13, 12233–12256, https://doi.org/10.5194/acp-13-12233-2013, https://doi.org/10.5194/acp-13-12233-2013, 2013
B. Friedman, A. Zelenyuk, J. Beranek, G. Kulkarni, M. Pekour, A. Gannet Hallar, I. B. McCubbin, J. A. Thornton, and D. J Cziczo
Atmos. Chem. Phys., 13, 11839–11851, https://doi.org/10.5194/acp-13-11839-2013, https://doi.org/10.5194/acp-13-11839-2013, 2013
L. R. Williams, L. A. Gonzalez, J. Peck, D. Trimborn, J. McInnis, M. R. Farrar, K. D. Moore, J. T. Jayne, W. A. Robinson, D. K. Lewis, T. B. Onasch, M. R. Canagaratna, A. Trimborn, M. T. Timko, G. Magoon, R. Deng, D. Tang, E. de la Rosa Blanco, A. S. H. Prévôt, K. A. Smith, and D. R. Worsnop
Atmos. Meas. Tech., 6, 3271–3280, https://doi.org/10.5194/amt-6-3271-2013, https://doi.org/10.5194/amt-6-3271-2013, 2013
L. D. Yee, J. S. Craven, C. L. Loza, K. A. Schilling, N. L. Ng, M. R. Canagaratna, P. J. Ziemann, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 11121–11140, https://doi.org/10.5194/acp-13-11121-2013, https://doi.org/10.5194/acp-13-11121-2013, 2013
A. Wonaschütz, M. Coggon, A. Sorooshian, R. Modini, A. A. Frossard, L. Ahlm, J. Mülmenstädt, G. C. Roberts, L. M. Russell, S. Dey, F. J. Brechtel, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 9819–9835, https://doi.org/10.5194/acp-13-9819-2013, https://doi.org/10.5194/acp-13-9819-2013, 2013
M. Dall'Osto, X. Querol, A. Alastuey, M. C. Minguillon, M. Alier, F. Amato, M. Brines, M. Cusack, J. O. Grimalt, A. Karanasiou, T. Moreno, M. Pandolfi, J. Pey, C. Reche, A. Ripoll, R. Tauler, B. L. Van Drooge, M. Viana, R. M. Harrison, J. Gietl, D. Beddows, W. Bloss, C. O'Dowd, D. Ceburnis, G. Martucci, N. L. Ng, D. Worsnop, J. Wenger, E. Mc Gillicuddy, J. Sodeau, R. Healy, F. Lucarelli, S. Nava, J. L. Jimenez, F. Gomez Moreno, B. Artinano, A. S. H. Prévôt, L. Pfaffenberger, S. Frey, F. Wilsenack, D. Casabona, P. Jiménez-Guerrero, D. Gross, and N. Cots
Atmos. Chem. Phys., 13, 8991–9019, https://doi.org/10.5194/acp-13-8991-2013, https://doi.org/10.5194/acp-13-8991-2013, 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
Y. J. Li, B. Y. L. Lee, J. Z. Yu, N. L. Ng, and C. K. Chan
Atmos. Chem. Phys., 13, 8739–8753, https://doi.org/10.5194/acp-13-8739-2013, https://doi.org/10.5194/acp-13-8739-2013, 2013
L. D. Yee, K. E. Kautzman, C. L. Loza, K. A. Schilling, M. M. Coggon, P. S. Chhabra, M. N. Chan, A. W. H. Chan, S. P. Hersey, J. D. Crounse, P. O. Wennberg, R. C. Flagan, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 8019–8043, https://doi.org/10.5194/acp-13-8019-2013, https://doi.org/10.5194/acp-13-8019-2013, 2013
H. Jiang, H. Liao, H. O. T. Pye, S. Wu, L. J. Mickley, J. H. Seinfeld, and X. Y. Zhang
Atmos. Chem. Phys., 13, 7937–7960, https://doi.org/10.5194/acp-13-7937-2013, https://doi.org/10.5194/acp-13-7937-2013, 2013
X. Zhang and J. H. Seinfeld
Atmos. Chem. Phys., 13, 5907–5926, https://doi.org/10.5194/acp-13-5907-2013, https://doi.org/10.5194/acp-13-5907-2013, 2013
T. R. Duhl, R. Zhang, A. Guenther, S. H. Chung, M. T. Salam, J. M. House, R. C. Flagan, E. L. Avol, F. D. Gilliland, B. K. Lamb, T. M. VanReken, Y. Zhang, and E. Salathé
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmdd-6-2325-2013, https://doi.org/10.5194/gmdd-6-2325-2013, 2013
Revised manuscript not accepted
J. E. Shilling, R. A. Zaveri, J. D. Fast, L. Kleinman, M. L. Alexander, M. R. Canagaratna, E. Fortner, J. M. Hubbe, J. T. Jayne, A. Sedlacek, A. Setyan, S. Springston, D. R. Worsnop, and Q. Zhang
Atmos. Chem. Phys., 13, 2091–2113, https://doi.org/10.5194/acp-13-2091-2013, https://doi.org/10.5194/acp-13-2091-2013, 2013
C. D. Cappa, X. Zhang, C. L. Loza, J. S. Craven, L. D. Yee, and J. H. Seinfeld
Atmos. Chem. Phys., 13, 1591–1606, https://doi.org/10.5194/acp-13-1591-2013, https://doi.org/10.5194/acp-13-1591-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
Enhanced Sulfate Formation in Mixed Biomass Burning and Sea-salt Particles Mediated by Photosensitization: Effects of Chloride and Nitrogen-containing Compounds
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photooxidation: Remarkably enhancing effects of seeds and ammonia
Atmospheric oxidation of 1,3-butadiene: influence of acidity and relative humidity on SOA composition and air toxic compounds
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Technical note: High-resolution analyses of concentrations and sizes of black carbon particles deposited on northwest Greenland over the past 350 years – Part 1. Continuous flow analysis of the SIGMA-D ice core using a Wide-Range Single-Particle Soot Photometer and a high-efficiency nebulizer
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
The impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
Technical note: In situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a quartz crystal microbalance with dissipation monitoring (QCM-D)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Impact of fossil and non-fossil fuel sources on the molecular compositions of water-soluble humic-like substances in PM2.5 at a suburban site of Yangtze River Delta, China
Technical note: Improved synthetic routes to cis- and trans-(2-methyloxirane-2,3-diyl)dimethanol (cis- and trans-β-isoprene epoxydiol)
Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2633, https://doi.org/10.5194/egusphere-2024-2633, 2024
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This study provided laboratory evidence that the photosensitizers in biomass burning extracts can enhance the sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air, with less contribution of direct photosensitization via triplets.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Si Zhang, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-2119, https://doi.org/10.5194/egusphere-2024-2119, 2024
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SOA from acetone photooxidation can be formed more readily on neutral aerosols than on acidic aerosols, while heterogeneous reaction of carbonyl with ammonium is only active on acidic aerosols in the presence of NH3, which produces light-absorbing N-containing compounds. Our work suggested that the heterogeneous oxidation of highly volatile VOC, for example acetone, is an importance source of SOA in the atmosphere, which should be accounted for in the future model studies.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof Rudzinski, Michael Lewandowski, Tadeusz Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
EGUsphere, https://doi.org/10.5194/egusphere-2024-2032, https://doi.org/10.5194/egusphere-2024-2032, 2024
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications to urban air quality. Health effects studies have focused on whole particulate matter but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
EGUsphere, https://doi.org/10.5194/egusphere-2024-1496, https://doi.org/10.5194/egusphere-2024-1496, 2024
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We developed a continuous flow analysis system to analyse an ice core from northwest Greenland, and coupled it with an improved BC measurement technique. This coupling allowed accurate high-resolution analyses of BC particles' size distributions and concentrations with diameters between 70 nm and 4 μm for the past 350 years. Our results provide crucial insights into BC's climatic effects. We also found that previous ice core studies substantially underestimated the BC mass concentrations.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
EGUsphere, https://doi.org/10.5194/egusphere-2024-905, https://doi.org/10.5194/egusphere-2024-905, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate & fructose) during humidity change & ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact on water uptake & chemical reactivity affecting atmospheric lifetimes, urban air quality (protecting harmful emissions from degradation and enabling their long-range transport) & climate (affecting cloud formation) with implications for human health.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing threats to human health and air quality. However, less is known about its emissions and health risks. Full-volatility organic species from incense-burning smoke are detected and quantified. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was a source of ice-nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible and therefore change cloud formation and properties. Our results show that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene). We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
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Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yihang Hong, Yu-Chi Lin, Mingyuan Yu, Hongxing Jiang, Zhineng Cheng, Rongshuang Xu, and Xiaoying Yang
Atmos. Chem. Phys., 23, 8305–8324, https://doi.org/10.5194/acp-23-8305-2023, https://doi.org/10.5194/acp-23-8305-2023, 2023
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The interaction between the sources and molecular compositions of humic-like substances (HULIS) at Nanjing, China, was explored. Significant fossil fuel source contributions to HULIS were found in the 14C results from biomass burnng and traffic emissions. Increasing biogenic secondary organic aerosol (SOA) products and anthropogenic aromatic compounds were detected in summer and winter, respectively.
Molly Frauenheim, Jason D. Surratt, Zhenfa Zhang, and Avram Gold
Atmos. Chem. Phys., 23, 7859–7866, https://doi.org/10.5194/acp-23-7859-2023, https://doi.org/10.5194/acp-23-7859-2023, 2023
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We report synthesis of the isoprene-derived photochemical oxidation products trans- and cis-β-epoxydiols in high overall yields from inexpensive, readily available starting compounds. Protection/deprotection steps or time-consuming purification is not required, and the reactions can be scaled up to gram quantities. The procedures provide accessibility of these important compounds to atmospheric chemistry laboratories with only basic capabilities in organic synthesis.
Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang
Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023, https://doi.org/10.5194/acp-23-7495-2023, 2023
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The results show that 14C elemental carbon (EC) was not only related to the isolation method but also to the types and proportions of the biomass sources in the sample. The hydropyrolysis (Hypy) method, which can be used to isolate a highly stable portion of ECHypy and avoid charring, is a more effective and stable approach for the matrix-independent 14C quantification of EC in aerosols, and the 13C–ECHypy and non-fossil ECHypy values of SRM1649b were –24.9 ‰ and 11 %, respectively.
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