Articles | Volume 15, issue 5
https://doi.org/10.5194/acp-15-2367-2015
© Author(s) 2015. 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-15-2367-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
04 Mar 2015
Research article |
| 04 Mar 2015
Kerb and urban increment of highly time-resolved trace elements in PM10, PM2.5 and PM1.0 winter aerosol in London during ClearfLo 2012
S. Visser
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
J. G. Slowik
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
P. Zotter
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
now at: Lucerne School of Engineering and Architecture, Bioenergy Research, Lucerne University of Applied Sciences and Arts, Horw, Switzerland
N. Bukowiecki
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
R. Dressler
Laboratory of Radiochemistry and Environmental Chemistry, Paul Scherrer Institute, Villigen, Switzerland
U. Flechsig
Swiss Light Source, Paul Scherrer Institute, Villigen, Switzerland
HASYLAB, DESY Photon Science, Hamburg, Germany
now at: European XFEL, Hamburg, Germany
D. C. Green
School of Biomedical Sciences, King's College London, London, UK
A. H. Tremper
School of Biomedical Sciences, King's College London, London, UK
D. E. Young
School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UK
now at: Department of Environmental Toxicology, University of California, Davis, CA, USA
P. I. Williams
National Centre for Atmospheric Science, University of Manchester, Manchester, UK
School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UK
J. D. Allan
National Centre for Atmospheric Science, University of Manchester, Manchester, UK
School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, UK
S. C. Herndon
Aerodyne Research, Inc., Billerica, MA, USA
L. R. Williams
Aerodyne Research, Inc., Billerica, MA, USA
Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA
now at: Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
A. Detournay
Centre for Ecology and Hydrology, Penicuik, Midlothian, UK
J. F. Barlow
Department of Meteorology, University of Reading, Reading, UK
C. H. Halios
Department of Meteorology, University of Reading, Reading, UK
Z. L. Fleming
Department of Chemistry, University of Leicester, Leicester, UK
National Centre for Atmospheric Science, University of Manchester, Manchester, UK
U. Baltensperger
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
A. S. H. Prévôt
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Arto Heitto, Cheng Wu, Diego Aliaga, Luis Blacutt, Xuemeng Chen, Yvette Gramlich, Liine Heikkinen, Wei Huang, Radovan Krejci, Paolo Laj, Isabel Moreno, Karine Sellegri, Fernando Velarde, Kay Weinhold, Alfred Wiedensohler, Qiaozhi Zha, Federico Bianchi, Marcos Andrade, Kari E. J. Lehtinen, Claudia Mohr, and Taina Yli-Juuti
EGUsphere, https://doi.org/10.5194/egusphere-2023-526, https://doi.org/10.5194/egusphere-2023-526, 2023
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Particle growth at Chacaltaya station in Bolivia was simulated based on measured vapor concentrations and ambient conditions. Major contributors to the simulated growth were low volatile organic compounds (LVOC). Also sulfuric acid had major role when volcanic activity was occurring in the area. This study provides insight on nanoparticle growth at this high-altitude Southern Hemispheric site and hence contributes to building the knowledge on early growth of atmospheric particles.
Qiaozhi Zha, Wei Huang, Diego Aliaga, Otso Peräkylä, Liine Heikkinen, Alkuin Maximilian Koenig, Cheng Wu, Joonas Enroth, Yvette Gramlich, Jing Cai, Samara Carbone, Armin Hansel, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, Victoria Sinclair, Radovan Krejci, Marcos Andrade, Claudia Mohr, and Federico Bianchi
Atmos. Chem. Phys., 23, 4559–4576, https://doi.org/10.5194/acp-23-4559-2023, https://doi.org/10.5194/acp-23-4559-2023, 2023
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We investigate the chemical composition of atmospheric cluster ions from January to May 2018 at the high-altitude research station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes. With state-of-the-art mass spectrometers and air mass history analysis, the measured cluster ions exhibited distinct diurnal and seasonal patterns, some of which contributed to new particle formation. Our study will improve the understanding of atmospheric ions and their role in high-altitude new particle formation.
Tara I. Yacovitch, Christoph Dyroff, Joseph R. Roscioli, Conner Daube, J. Barry McManus, and Scott C. Herndon
Atmos. Meas. Tech., 16, 1915–1921, https://doi.org/10.5194/amt-16-1915-2023, https://doi.org/10.5194/amt-16-1915-2023, 2023
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Ethylene oxide is a toxic, carcinogenic compound used in the medical and bulk sterilization industry. Here we describe a precise and fast laser-based ethylene oxide monitor. We report months-long concentrations at a Massachusetts site, and we show how they suggest a potential emission source 35 km away. This source, and another, is confirmed by driving the instrument downwind of the sites, where concentrations were tens to tens of thousands of times greater than background levels.
John W. Halfacre, Jordan Stewart, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Michael Flynn, Stephen J. Andrews, Steven S. Brown, Patrick R. Veres, and Pete M. Edwards
Atmos. Meas. Tech., 16, 1407–1429, https://doi.org/10.5194/amt-16-1407-2023, https://doi.org/10.5194/amt-16-1407-2023, 2023
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This study details a new sampling method for the optical detection of hydrogen chloride (HCl). HCl is an important atmospheric reservoir for chlorine atoms, which can affect nitrogen oxide cycling and the lifetimes of volatile organic compounds and ozone. However, HCl has a high affinity for interacting with surfaces, thereby preventing fast, quantitative measurements. The sampling technique in this study minimizes these surface interactions and provides a high-quality measurement of HCl.
Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, and Claudia Mohr
Atmos. Meas. Tech., 16, 1147–1165, https://doi.org/10.5194/amt-16-1147-2023, https://doi.org/10.5194/amt-16-1147-2023, 2023
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We introduce the offline application of FIGAERO-CIMS by analyzing Teflon and quartz filter samples that were collected at a typical urban site in Beijing with the deposition time varying from 30 min to 24 h. This method provides a feasible, simple, and quantitative way to investigate the molecular composition and volatility of OA compounds by using FIGAERO-CIMS to analyze offline samples.
Liine Heikkinen, Daniel G. Partridge, Wei Huang, Sara Blichner, Rahul Ranjan, Emanuele Tovazzi, Tuukka Petäjä, Claudia Mohr, and Ilona Riipinen
EGUsphere, https://doi.org/10.5194/egusphere-2023-164, https://doi.org/10.5194/egusphere-2023-164, 2023
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The organic vapor condensation with water vapor (co-condensation) is modeled in this work over the boreal forest environment because the forest air is rich in naturally emitted organic vapors. The simulations show that the number of cloud droplets can enhance by 20 % if the co-condensation process is considered. The enhancements are particularly high if the air contains small, naturally produced particles. Such conditions are most frequently met in Spring in the boreal forest.
Samuel J. Cliff, Will Drysdale, James D. Lee, Carole Helfter, Eiko Nemitz, Stefan Metzger, and Janet F. Barlow
Atmos. Chem. Phys., 23, 2315–2330, https://doi.org/10.5194/acp-23-2315-2023, https://doi.org/10.5194/acp-23-2315-2023, 2023
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Emissions of nitrogen oxides (NOx) to the atmosphere are an ongoing air quality issue. This study directly measures emissions of NOx and carbon dioxide from a tall tower in central London during the coronavirus pandemic. It was found that transport NOx emissions had reduced by >73 % since 2017 as a result of air quality policy and reduced congestion during coronavirus restrictions. During this period, central London was thought to be dominated by point-source heat and power generation emissions.
Wiebke Scholz, Jiali Shen, Diego Aliaga, Cheng Wu, Samara Carbone, Isabel Moreno, Qiaozhi Zha, Wei Huang, Liine Heikkinen, Jean Luc Jaffrezo, Gaelle Uzu, Eva Partoll, Markus Leiminger, Fernando Velarde, Paolo Laj, Patrick Ginot, Paolo Artaxo, Alfred Wiedensohler, Markku Kulmala, Claudia Mohr, Marcos Andrade, Victoria Sinclair, Federico Bianchi, and Armin Hansel
Atmos. Chem. Phys., 23, 895–920, https://doi.org/10.5194/acp-23-895-2023, https://doi.org/10.5194/acp-23-895-2023, 2023
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Dimethyl sulfide (DMS), emitted from the ocean, is the most abundant biogenic sulfur emission into the atmosphere. OH radicals, among others, can oxidize DMS to sulfuric and methanesulfonic acid, which are relevant for aerosol formation. We quantified DMS and nearly all DMS oxidation products with novel mass spectrometric instruments for gas and particle phase at the high mountain station Chacaltaya (5240 m a.s.l.) in the Bolivian Andes in free tropospheric air after long-range transport.
Lu Xu, Matthew M. Coggon, Chelsea E. Stockwell, Jessica B. Gilman, Michael A. Robinson, Martin Breitenlechner, Aaron Lamplugh, John D. Crounse, Paul O. Wennberg, J. Andrew Neuman, Gordon A. Novak, Patrick R. Veres, Steven S. Brown, and Carsten Warneke
Atmos. Meas. Tech., 15, 7353–7373, https://doi.org/10.5194/amt-15-7353-2022, https://doi.org/10.5194/amt-15-7353-2022, 2022
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We describe the development and operation of a chemical ionization mass spectrometer using an ammonium–water cluster (NH4+·H2O) as a reagent ion. NH4+·H2O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH4+ produced via ligand-switching reactions. The instrumental sensitivities of analytes depend on the binding energy of the analyte–NH4+ cluster; sensitivities can be estimated using voltage scanning.
Yandong Tong, Lu Qi, Giulia Stefenelli, Dongyu Simon Wang, Francesco Canonaco, Urs Baltensperger, André Stephan Henry Prévôt, and Jay Gates Slowik
Atmos. Meas. Tech., 15, 7265–7291, https://doi.org/10.5194/amt-15-7265-2022, https://doi.org/10.5194/amt-15-7265-2022, 2022
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We present a method for positive matrix factorisation (PMF) analysis on a single dataset that includes measurements from both EESI-TOF and AMS in Zurich, Switzerland. For the first time, we resolved and quantified secondary organic aerosol (SOA) sources. Meanwhile, we also determined the retrieved EESI-TOF factor-dependent sensitivities. This method provides a framework for exploiting semi-quantitative, high-resolution instrumentation for quantitative source apportionment.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Marta Via, Gang Chen, Francesco Canonaco, Kaspar R. Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, Cristina Marin, Colin O'Dowd, Jurgita Ovadnevaite, Jean-Eudes Petit, Michael Pikridas, Véronique Riffault, Jean Sciare, Jay G. Slowik, Leïla Simon, Jeni Vasilescu, Yunjiang Zhang, Olivier Favez, André S. H. Prévôt, Andrés Alastuey, and María Cruz Minguillón
Atmos. Meas. Tech., 15, 5479–5495, https://doi.org/10.5194/amt-15-5479-2022, https://doi.org/10.5194/amt-15-5479-2022, 2022
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This work presents the differences resulting from two techniques (rolling and seasonal) of the positive matrix factorisation model that can be run for organic aerosol source apportionment. The current state of the art suggests that the rolling technique is more accurate, but no proof of its effectiveness has been provided yet. This paper tackles this issue in the context of a synthetic dataset and a multi-site real-world comparison.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Yutong Liang, Christos Stamatis, Edward C. Fortner, Rebecca A. Wernis, Paul Van Rooy, Francesca Majluf, Tara I. Yacovitch, Conner Daube, Scott C. Herndon, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 22, 9877–9893, https://doi.org/10.5194/acp-22-9877-2022, https://doi.org/10.5194/acp-22-9877-2022, 2022
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This article reports the measurements of organic compounds emitted from western US wildfires. We identified and quantified 240 particle-phase compounds and 72 gas-phase compounds emitted in wildfire and related the emissions to the modified combustion efficiency. Higher emissions of diterpenoids and monoterpenes were observed, likely due to distillation from unburned heated vegetation. Our results can benefit future source apportionment and modeling studies as well as exposure assessments.
Will S. Drysdale, Adam R. Vaughan, Freya A. Squires, Sam J. Cliff, Stefan Metzger, David Durden, Natchaya Pingintha-Durden, Carole Helfter, Eiko Nemitz, C. Sue B. Grimmond, Janet Barlow, Sean Beevers, Gregor Stewart, David Dajnak, Ruth M. Purvis, and James D. Lee
Atmos. Chem. Phys., 22, 9413–9433, https://doi.org/10.5194/acp-22-9413-2022, https://doi.org/10.5194/acp-22-9413-2022, 2022
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Measurements of NOx emissions are important for a good understanding of air quality. While there are many direct measurements of NOx concentration, there are very few measurements of its emission. Measurements of emissions provide constraints on emissions inventories and air quality models. This article presents measurements of NOx emission from the BT Tower in central London in 2017 and compares them with inventories, finding that they underestimate by a factor of ∼1.48.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
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We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 15, 3747–3760, https://doi.org/10.5194/amt-15-3747-2022, https://doi.org/10.5194/amt-15-3747-2022, 2022
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Real-time detection of both the gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analyes.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
Linyu Gao, Junwei Song, Claudia Mohr, Wei Huang, Magdalena Vallon, Feng Jiang, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, https://doi.org/10.5194/acp-22-6001-2022, 2022
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We study secondary organic aerosol (SOA) from β-caryophyllene (BCP) ozonolysis with and without nitrogen oxides over 213–313 K in the simulation chamber. The yields and the rate constants were determined at 243–313 K. Chemical compositions varied at different temperatures, indicating a strong impact on the BCP ozonolysis pathways. This work helps to better understand the SOA from BCP ozonolysis for conditions representative of the real atmosphere from the boundary layer to the upper troposphere.
Andrew J. Lindsay, Daniel C. Anderson, Rebecca A. Wernis, Yutong Liang, Allen H. Goldstein, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Ed C. Fortner, Philip L. Croteau, Francesca Majluf, Jordan E. Krechmer, Tara I. Yacovitch, Walter B. Knighton, and Ezra C. Wood
Atmos. Chem. Phys., 22, 4909–4928, https://doi.org/10.5194/acp-22-4909-2022, https://doi.org/10.5194/acp-22-4909-2022, 2022
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Wildfire smoke dramatically impacts air quality and often has elevated concentrations of ozone. We present measurements of ozone and its precursors at a rural site periodically impacted by wildfire smoke. Measurements of total peroxy radicals, key ozone precursors that have been studied little within wildfires, compare well with chemical box model predictions. Our results indicate no serious issues with using current chemistry mechanisms to model chemistry in aged wildfire plumes.
Chenjie Yu, Dantong Liu, Kang Hu, Ping Tian, Yangzhou Wu, Delong Zhao, Huihui Wu, Dawei Hu, Wenbo Guo, Qiang Li, Mengyu Huang, Deping Ding, and James D. Allan
Atmos. Chem. Phys., 22, 4375–4391, https://doi.org/10.5194/acp-22-4375-2022, https://doi.org/10.5194/acp-22-4375-2022, 2022
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In this study, we applied a new technique to investigate the aerosol properties on both a mass and number basis and CCN abilities in Beijing suburban regions. The size-resolved aerosol chemical compositions and CCN activation measurement enable a detailed analysis of BC-containing particle hygroscopicity and its size-dependent contribution to the CCN activation. The results presented in this study will affect future models and human health studies.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
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Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
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.
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.
Dawei Hu, M. Rami Alfarra, Kate Szpek, Justin M. Langridge, Michael I. Cotterell, Claire Belcher, Ian Rule, Zixia Liu, Chenjie Yu, Yunqi Shao, Aristeidis Voliotis, Mao Du, Brett Smith, Greg Smallwood, Prem Lobo, Dantong Liu, Jim M. Haywood, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 21, 16161–16182, https://doi.org/10.5194/acp-21-16161-2021, https://doi.org/10.5194/acp-21-16161-2021, 2021
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Here, we developed new techniques for investigating these properties in the laboratory and applied these to BC and BrC from different sources, including diesel exhaust, inverted propane flame and wood combustion. These have allowed us to quantify the changes in shape and chemical composition of different soots according to source and variables such as the moisture content of wood.
Mariam Fawaz, Anita Avery, Timothy B. Onasch, Leah R. Williams, and Tami C. Bond
Atmos. Chem. Phys., 21, 15605–15618, https://doi.org/10.5194/acp-21-15605-2021, https://doi.org/10.5194/acp-21-15605-2021, 2021
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Biomass burning is responsible for 90 % of the emissions of primary organic aerosols to the atmosphere. Emissions from biomass burning sources are considered chaotic. In this work, we developed a controlled experimental approach to understand the controlling factors in emission. Our results showed that emissions are repeatable and deterministic and that emissions from wood can be constrained.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Benjamin Sumlin, Edward Fortner, Andrew Lambe, Nishit J. Shetty, Conner Daube, Pai Liu, Francesca Majluf, Scott Herndon, and Rajan K. Chakrabarty
Atmos. Chem. Phys., 21, 11843–11856, https://doi.org/10.5194/acp-21-11843-2021, https://doi.org/10.5194/acp-21-11843-2021, 2021
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We present a comparison of the changes to light absorption behavior and chemical composition of wildfire smoke particles from day- and nighttime oxidation processes and discuss the results within the context of previous laboratory findings.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
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.
Zainab Bibi, Hugh Coe, James Brooks, Paul I. Williams, Ernesto Reyes-Villegas, Michael Priestley, Carl J. Percival, and James D. Allan
Atmos. Chem. Phys., 21, 10763–10777, https://doi.org/10.5194/acp-21-10763-2021, https://doi.org/10.5194/acp-21-10763-2021, 2021
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We are presenting a new method to apportion black carbon/soot into multiple sources through the inclusion of fullerene and metal data into HR-SP-AMS factorisation. While this itself would be considered a technical development, we can present a budget of contributions to measured BC during the event studied, including the conclusion that fireworks contributed little compared to the bonfire, traffic, and domestic wood-burning emissions.
Evelyn Freney, Karine Sellegri, Alessia Nicosia, Leah R. Williams, Matteo Rinaldi, Jonathan T. Trueblood, André S. H. Prévôt, Melilotus Thyssen, Gérald Grégori, Nils Haëntjens, Julie Dinasquet, Ingrid Obernosterer, France Van Wambeke, Anja Engel, Birthe Zäncker, Karine Desboeufs, Eija Asmi, Hilkka Timonen, and Cécile Guieu
Atmos. Chem. Phys., 21, 10625–10641, https://doi.org/10.5194/acp-21-10625-2021, https://doi.org/10.5194/acp-21-10625-2021, 2021
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In this work, we present observations of the organic aerosol content in primary sea spray aerosols (SSAs) continuously generated along a 5-week cruise in the Mediterranean. This information is combined with seawater biogeochemical properties also measured continuously along the ship track to develop a number of parametrizations that can be used in models to determine SSA organic content in oligotrophic waters that represent 60 % of the oceans from commonly measured seawater variables.
James M. Cash, Ben Langford, Chiara Di Marco, Neil J. Mullinger, James Allan, Ernesto Reyes-Villegas, Ruthambara Joshi, Mathew R. Heal, W. Joe F. Acton, C. Nicholas Hewitt, Pawel K. Misztal, Will Drysdale, Tuhin K. Mandal, Shivani, Ranu Gadi, Bhola Ram Gurjar, and Eiko Nemitz
Atmos. Chem. Phys., 21, 10133–10158, https://doi.org/10.5194/acp-21-10133-2021, https://doi.org/10.5194/acp-21-10133-2021, 2021
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We present the first real-time composition of submicron particulate matter (PM1) in Old Delhi using high-resolution aerosol mass spectrometry. Seasonal analysis shows peak concentrations occur during the post-monsoon, and novel-tracers reveal the largest sources are a combination of local open and regional crop residue burning. Strong links between increased chloride aerosol concentrations and burning sources of PM1 suggest burning sources are responsible for the post-monsoon chloride peak.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Huihui Wu, Jonathan W. Taylor, Justin M. Langridge, Chenjie Yu, James D. Allan, Kate Szpek, Michael I. Cotterell, Paul I. Williams, Michael Flynn, Patrick Barker, Cathryn Fox, Grant Allen, James Lee, and Hugh Coe
Atmos. Chem. Phys., 21, 9417–9440, https://doi.org/10.5194/acp-21-9417-2021, https://doi.org/10.5194/acp-21-9417-2021, 2021
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Seasonal biomass burning over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important climate impacts but are poorly constrained. We conducted in situ airborne measurements to investigate the evolution of smoke aerosol properties in this region. We observed absorption enhancement for both black carbon and brown carbon after emission, which provides new field results and constraints on aerosol parameterizations for future climate models.
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.
Dac-Loc Nguyen, Hendryk Czech, Simone M. Pieber, Jürgen Schnelle-Kreis, Martin Steinbacher, Jürgen Orasche, Stephan Henne, Olga B. Popovicheva, Gülcin Abbaszade, Guenter Engling, Nicolas Bukowiecki, Nhat-Anh Nguyen, Xuan-Anh Nguyen, and Ralf Zimmermann
Atmos. Chem. Phys., 21, 8293–8312, https://doi.org/10.5194/acp-21-8293-2021, https://doi.org/10.5194/acp-21-8293-2021, 2021
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Southeast Asia is well-known for emission-intense and recurring wildfires and after-harvest crop residue burning during the pre-monsoon season from February to April. We describe a biomass burning (BB) plume arriving at remote Pha Din meteorological station, outline its carbonaceous particulate matter (PM) constituents based on more than 50 target compounds and discuss possible BB sources. This study adds valuable information on chemical PM composition for a region with scarce data availability.
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).
Dianne Sanchez, Roger Seco, Dasa Gu, Alex Guenther, John Mak, Youngjae Lee, Danbi Kim, Joonyoung Ahn, Don Blake, Scott Herndon, Daun Jeong, John T. Sullivan, Thomas Mcgee, Rokjin Park, and Saewung Kim
Atmos. Chem. Phys., 21, 6331–6345, https://doi.org/10.5194/acp-21-6331-2021, https://doi.org/10.5194/acp-21-6331-2021, 2021
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We present observations of total reactive gases in a suburban forest observatory in the Seoul metropolitan area. The quantitative comparison with speciated trace gas observations illustrated significant underestimation in atmospheric reactivity from the speciated trace gas observational dataset. We present scientific discussion about potential causes.
Steven J. Campbell, Kate Wolfer, Battist Utinger, Joe Westwood, Zhi-Hui Zhang, Nicolas Bukowiecki, Sarah S. Steimer, Tuan V. Vu, Jingsha Xu, Nicholas Straw, Steven Thomson, Atallah Elzein, Yele Sun, Di Liu, Linjie Li, Pingqing Fu, Alastair C. Lewis, Roy M. Harrison, William J. Bloss, Miranda Loh, Mark R. Miller, Zongbo Shi, and Markus Kalberer
Atmos. Chem. Phys., 21, 5549–5573, https://doi.org/10.5194/acp-21-5549-2021, https://doi.org/10.5194/acp-21-5549-2021, 2021
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In this study, we quantify PM2.5 oxidative potential (OP), a metric widely suggested as a potential measure of particle toxicity, in Beijing in summer and winter using four acellular assays. We correlate PM2.5 OP with a comprehensive range of atmospheric and particle composition measurements, demonstrating inter-assay differences and seasonal variation of PM2.5 OP. Using multivariate statistical analysis, we highlight specific particle chemical components and sources that influence OP.
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.
Pamela S. Rickly, Lu Xu, John D. Crounse, Paul O. Wennberg, and Andrew W. Rollins
Atmos. Meas. Tech., 14, 2429–2439, https://doi.org/10.5194/amt-14-2429-2021, https://doi.org/10.5194/amt-14-2429-2021, 2021
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Key improvements have been made to an in situ laser-induced fluorescence instrument for measuring SO2 in polluted and pristine environments. Laser linewidth is reduced, rapid laser tuning is implemented, and fluorescence bandpass filters are optimized. These improvements have led to a 50 % reduction in instrument detection limit. The influence of aromatic compounds was also investigated and determined to not bias SO2 measurements.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697, https://doi.org/10.5194/gmd-14-1681-2021, https://doi.org/10.5194/gmd-14-1681-2021, 2021
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We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
Rosaria E. Pileci, Robin L. Modini, Michele Bertò, Jinfeng Yuan, Joel C. Corbin, Angela Marinoni, Bas Henzing, Marcel M. Moerman, Jean P. Putaud, Gerald Spindler, Birgit Wehner, Thomas Müller, Thomas Tuch, Arianna Trentini, Marco Zanatta, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Meas. Tech., 14, 1379–1403, https://doi.org/10.5194/amt-14-1379-2021, https://doi.org/10.5194/amt-14-1379-2021, 2021
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Black carbon (BC), which is an important constituent of atmospheric aerosols, remains difficult to quantify due to various limitations of available methods. This study provides an extensive comparison of co-located field measurements, applying two methods based on different principles. It was shown that both methods indeed quantify the same aerosol property – BC mass concentration. The level of agreement that can be expected was quantified, and some reasons for discrepancy were identified.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad El Haddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Meas. Tech., 14, 923–943, https://doi.org/10.5194/amt-14-923-2021, https://doi.org/10.5194/amt-14-923-2021, 2021
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Long-term ambient aerosol mass spectrometric data were analyzed with a statistical model (PMF) to obtain source contributions and fingerprints. The new aspects of this paper involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Jinfeng Yuan, Robin Lewis Modini, Marco Zanatta, Andreas B. Herber, Thomas Müller, Birgit Wehner, Laurent Poulain, Thomas Tuch, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 21, 635–655, https://doi.org/10.5194/acp-21-635-2021, https://doi.org/10.5194/acp-21-635-2021, 2021
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Black carbon (BC) aerosols contribute substantially to climate warming due to their unique light absorption capabilities. We performed field measurements at a central European background site in winter and found that variability in the absorption efficiency of BC particles is driven mainly by their internal mixing state. Our results suggest that, at this site, knowing the BC mixing state is sufficient to describe BC light absorption enhancements due to the lensing effect in good approximation.
Rutambhara Joshi, Dantong Liu, Eiko Nemitz, Ben Langford, Neil Mullinger, Freya Squires, James Lee, Yunfei Wu, Xiaole Pan, Pingqing Fu, Simone Kotthaus, Sue Grimmond, Qiang Zhang, Ruili Wu, Oliver Wild, Michael Flynn, Hugh Coe, and James Allan
Atmos. Chem. Phys., 21, 147–162, https://doi.org/10.5194/acp-21-147-2021, https://doi.org/10.5194/acp-21-147-2021, 2021
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Black carbon (BC) is a component of particulate matter which has significant effects on climate and human health. Sources of BC include biomass burning, transport, industry and domestic cooking and heating. In this study, we measured BC emissions in Beijing, finding a dominance of traffic emissions over all other sources. The quantitative method presented here has benefits for revising widely used emissions inventories and for understanding BC sources with impacts on air quality and climate.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
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.
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.
Jing Cai, Biwu Chu, Lei Yao, Chao Yan, Liine M. Heikkinen, Feixue Zheng, Chang Li, Xiaolong Fan, Shaojun Zhang, Daoyuan Yang, Yonghong Wang, Tom V. Kokkonen, Tommy Chan, Ying Zhou, Lubna Dada, Yongchun Liu, Hong He, Pauli Paasonen, Joni T. Kujansuu, Tuukka Petäjä, Claudia Mohr, Juha Kangasluoma, Federico Bianchi, Yele Sun, Philip L. Croteau, Douglas R. Worsnop, Veli-Matti Kerminen, Wei Du, Markku Kulmala, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 20, 12721–12740, https://doi.org/10.5194/acp-20-12721-2020, https://doi.org/10.5194/acp-20-12721-2020, 2020
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By applying both OA PMF and size PMF at the same urban measurement site in Beijing, similar particle source types, including vehicular emissions, cooking emissions and secondary formation-related sources, were resolved by both frameworks and agreed well. It is also found that in the absence of new particle formation, vehicular and cooking emissions dominate the particle number concentration, while secondary particulate matter governed PM2.5 mass during spring and summer in Beijing.
Nicole Biedermann, Elena Bykova, Wolfgang Morgenroth, Ilias Efthimiopoulos, Jan Mueller, Georg Spiekermann, Konstantin Glazyrin, Anna Pakhomova, Karen Appel, and Max Wilke
Eur. J. Mineral., 32, 575–586, https://doi.org/10.5194/ejm-32-575-2020, https://doi.org/10.5194/ejm-32-575-2020, 2020
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Carbonates play a key role in the chemistry and dynamics of our planet. The role of SrCO3 in the deep mantle has received little attention due to its low abundance. However, knowing the high-pressure phase behaviour of natural carbonates across its full compositional range is essential to evaluate effects of chemical substitution in the system of deep-Earth carbonates. We performed powder and single-crystal X-ray diffraction up to 49 GPa and observed a phase transition in SrCO3 at around 26 GPa.
Huihui Wu, Jonathan W. Taylor, Kate Szpek, Justin M. Langridge, Paul I. Williams, Michael Flynn, James D. Allan, Steven J. Abel, Joseph Pitt, Michael I. Cotterell, Cathryn Fox, Nicholas W. Davies, Jim Haywood, and Hugh Coe
Atmos. Chem. Phys., 20, 12697–12719, https://doi.org/10.5194/acp-20-12697-2020, https://doi.org/10.5194/acp-20-12697-2020, 2020
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Airborne measurements of highly aged biomass burning aerosols (BBAs) over the remote southeast Atlantic provide unique aerosol parameters for climate models. Our observations demonstrate the persistence of strongly absorbing BBAs across wide regions of the South Atlantic. We also found significant vertical variation in the single-scattering albedo of these BBAs, as a function of relative chemical composition and size. Aerosol properties in the marine BL are suggested to be separated from the FT.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Anna K. Tobler, Alicja Skiba, Dongyu S. Wang, Philip Croteau, Katarzyna Styszko, Jarosław Nęcki, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Meas. Tech., 13, 5293–5301, https://doi.org/10.5194/amt-13-5293-2020, https://doi.org/10.5194/amt-13-5293-2020, 2020
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Some quadrupole aerosol chemical speciation monitors (Q-ACSMs) have had issues with the quantification of particulate chloride, resulting in apparent negative chloride concentrations. We can show that this is due to the different behavior of Cl+ and HCl+, and we present a correction for the more accurate quantification of chloride. The correction can be applied to measurements in environments where the particulate chloride is dominated by NH4Cl.
Jonathan W. Taylor, Huihui Wu, Kate Szpek, Keith Bower, Ian Crawford, Michael J. Flynn, Paul I. Williams, James Dorsey, Justin M. Langridge, Michael I. Cotterell, Cathryn Fox, Nicholas W. Davies, Jim M. Haywood, and Hugh Coe
Atmos. Chem. Phys., 20, 11201–11221, https://doi.org/10.5194/acp-20-11201-2020, https://doi.org/10.5194/acp-20-11201-2020, 2020
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Every year, huge plumes of smoke hundreds of miles wide travel over the south Atlantic Ocean from fires in central and southern Africa. These plumes absorb the sun’s energy and warm the climate. We used airborne optical instrumentation to determine how absorbing the smoke was as well as the relative importance of black and brown carbon. We also tested different ways of simulating these properties that could be used in a climate model.
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.
María A. Burgos, Elisabeth Andrews, Gloria Titos, Angela Benedetti, Huisheng Bian, Virginie Buchard, Gabriele Curci, Zak Kipling, Alf Kirkevåg, Harri Kokkola, Anton Laakso, Julie Letertre-Danczak, Marianne T. Lund, Hitoshi Matsui, Gunnar Myhre, Cynthia Randles, Michael Schulz, Twan van Noije, Kai Zhang, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Junying Sun, Ernest Weingartner, and Paul Zieger
Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, https://doi.org/10.5194/acp-20-10231-2020, 2020
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We investigate how well models represent the enhancement in scattering coefficients due to particle water uptake, and perform an evaluation of several implementation schemes used in ten Earth system models. Our results show the importance of the parameterization of hygroscopicity and model chemistry as drivers of some of the observed diversity amongst model estimates. The definition of dry conditions and the phenomena taking place in this relative humidity range also impact the model evaluation.
Liwei Wang, Jay G. Slowik, Nidhi Tripathi, Deepika Bhattu, Pragati Rai, Varun Kumar, Pawan Vats, Rangu Satish, Urs Baltensperger, Dilip Ganguly, Neeraj Rastogi, Lokesh K. Sahu, Sachchida N. Tripathi, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 9753–9770, https://doi.org/10.5194/acp-20-9753-2020, https://doi.org/10.5194/acp-20-9753-2020, 2020
Paolo Laj, Alessandro Bigi, Clémence Rose, Elisabeth Andrews, Cathrine Lund Myhre, Martine Collaud Coen, Yong Lin, Alfred Wiedensohler, Michael Schulz, John A. Ogren, Markus Fiebig, Jonas Gliß, Augustin Mortier, Marco Pandolfi, Tuukka Petäja, Sang-Woo Kim, Wenche Aas, Jean-Philippe Putaud, Olga Mayol-Bracero, Melita Keywood, Lorenzo Labrador, Pasi Aalto, Erik Ahlberg, Lucas Alados Arboledas, Andrés Alastuey, Marcos Andrade, Begoña Artíñano, Stina Ausmeel, Todor Arsov, Eija Asmi, John Backman, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Sébastien Conil, Cedric Couret, Derek Day, Wan Dayantolis, Anna Degorska, Konstantinos Eleftheriadis, Prodromos Fetfatzis, Olivier Favez, Harald Flentje, Maria I. Gini, Asta Gregorič, Martin Gysel-Beer, A. Gannet Hallar, Jenny Hand, Andras Hoffer, Christoph Hueglin, Rakesh K. Hooda, Antti Hyvärinen, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Jeong Eun Kim, Giorgos Kouvarakis, Irena Kranjc, Radovan Krejci, Markku Kulmala, Casper Labuschagne, Hae-Jung Lee, Heikki Lihavainen, Neng-Huei Lin, Gunter Löschau, Krista Luoma, Angela Marinoni, Sebastiao Martins Dos Santos, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Nhat Anh Nguyen, Jakub Ondracek, Noemi Pérez, Maria Rita Perrone, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Natalia Prats, Anthony Prenni, Fabienne Reisen, Salvatore Romano, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Maik Schütze, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Martin Steinbacher, Junying Sun, Gloria Titos, Barbara Toczko, Thomas Tuch, Pierre Tulet, Peter Tunved, Ville Vakkari, Fernando Velarde, Patricio Velasquez, Paolo Villani, Sterios Vratolis, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Jesus Yus-Diez, Vladimir Zdimal, Paul Zieger, and Nadezda Zikova
Atmos. Meas. Tech., 13, 4353–4392, https://doi.org/10.5194/amt-13-4353-2020, https://doi.org/10.5194/amt-13-4353-2020, 2020
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The paper establishes the fiducial reference of the GAW aerosol network providing the fully characterized value chain to the provision of four climate-relevant aerosol properties from ground-based sites. Data from almost 90 stations worldwide are reported for a reference year, 2017, providing a unique and very robust view of the variability of these variables worldwide. Current gaps in the GAW network are analysed and requirements for the Global Climate Monitoring System are proposed.
Jill S. Johnson, Leighton A. Regayre, Masaru Yoshioka, Kirsty J. Pringle, Steven T. Turnock, Jo Browse, David M. H. Sexton, John W. Rostron, Nick A. J. Schutgens, Daniel G. Partridge, Dantong Liu, James D. Allan, Hugh Coe, Aijun Ding, David D. Cohen, Armand Atanacio, Ville Vakkari, Eija Asmi, and Ken S. Carslaw
Atmos. Chem. Phys., 20, 9491–9524, https://doi.org/10.5194/acp-20-9491-2020, https://doi.org/10.5194/acp-20-9491-2020, 2020
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We use over 9000 monthly aggregated grid-box measurements of aerosol to constrain the uncertainty in the HadGEM3-UKCA climate model. Measurements of AOD, PM2.5, particle number concentrations, sulfate and organic mass concentrations are compared to 1 million
variantsof the model using an implausibility metric. Despite many compensating effects in the model, the procedure constrains the probability distributions of many parameters, and direct radiative forcing uncertainty is reduced by 34 %.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Martine Collaud Coen, Elisabeth Andrews, Andrés Alastuey, Todor Petkov Arsov, John Backman, Benjamin T. Brem, Nicolas Bukowiecki, Cédric Couret, Konstantinos Eleftheriadis, Harald Flentje, Markus Fiebig, Martin Gysel-Beer, Jenny L. Hand, András Hoffer, Rakesh Hooda, Christoph Hueglin, Warren Joubert, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Casper Labuschagne, Neng-Huei Lin, Yong Lin, Cathrine Lund Myhre, Krista Luoma, Hassan Lyamani, Angela Marinoni, Olga L. Mayol-Bracero, Nikos Mihalopoulos, Marco Pandolfi, Natalia Prats, Anthony J. Prenni, Jean-Philippe Putaud, Ludwig Ries, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Patrick Sheridan, James Patrick Sherman, Junying Sun, Gloria Titos, Elvis Torres, Thomas Tuch, Rolf Weller, Alfred Wiedensohler, Paul Zieger, and Paolo Laj
Atmos. Chem. Phys., 20, 8867–8908, https://doi.org/10.5194/acp-20-8867-2020, https://doi.org/10.5194/acp-20-8867-2020, 2020
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Long-term trends of aerosol radiative properties (52 stations) prove that aerosol load has significantly decreased over the last 20 years. Scattering trends are negative in Europe (EU) and North America (NA), not ss in Asia, and show a mix of positive and negative trends at polar stations. Absorption has mainly negative trends. The single scattering albedo has positive trends in Asia and eastern EU and negative in western EU and NA, leading to a global positive median trend of 0.02 % per year.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
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.
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
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.
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.
Andrew T. Lambe, Ezra C. Wood, Jordan E. Krechmer, Francesca Majluf, Leah R. Williams, Philip L. Croteau, Manuela Cirtog, Anaïs Féron, Jean-Eudes Petit, Alexandre Albinet, Jose L. Jimenez, and Zhe Peng
Atmos. Meas. Tech., 13, 2397–2411, https://doi.org/10.5194/amt-13-2397-2020, https://doi.org/10.5194/amt-13-2397-2020, 2020
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We present a new method to continuously generate N2O5 in the gas phase that is injected into a reactor where it decomposes to generate nitrate radicals (NO3). To assess the applicability of the method towards different chemical systems, we present experimental and model characterization of the integrated NO3 exposure and other metrics as a function of operating conditions. We demonstrate the method by characterizing secondary organic aerosol particles generated from the β-pinene + NO3 reaction.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
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We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
William T. Morgan, James D. Allan, Stéphane Bauguitte, Eoghan Darbyshire, Michael J. Flynn, James Lee, Dantong Liu, Ben Johnson, Jim Haywood, Karla M. Longo, Paulo E. Artaxo, and Hugh Coe
Atmos. Chem. Phys., 20, 5309–5326, https://doi.org/10.5194/acp-20-5309-2020, https://doi.org/10.5194/acp-20-5309-2020, 2020
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We flew a large atmospheric research aircraft across a number of different environments in the Amazon basin during the 2012 biomass burning season. Smoke from fires builds up and has a significant impact on weather, climate, health and natural ecosystems. Our goal was to quantify changes in the properties of the smoke emitted by fires as it is transported through the atmosphere. We found that the major control on the properties of the smoke was due to differences in the fires themselves.
Sobhan Kumar Kompalli, Surendran Nair Suresh Babu, Sreedharan Krishnakumari Satheesh, Krishnaswamy Krishna Moorthy, Trupti Das, Ramasamy Boopathy, Dantong Liu, Eoghan Darbyshire, James D. Allan, James Brooks, Michael J. Flynn, and Hugh Coe
Atmos. Chem. Phys., 20, 3965–3985, https://doi.org/10.5194/acp-20-3965-2020, https://doi.org/10.5194/acp-20-3965-2020, 2020
Adil Shah, Joseph R. Pitt, Hugo Ricketts, J. Brian Leen, Paul I. Williams, Khristopher Kabbabe, Martin W. Gallagher, and Grant Allen
Atmos. Meas. Tech., 13, 1467–1484, https://doi.org/10.5194/amt-13-1467-2020, https://doi.org/10.5194/amt-13-1467-2020, 2020
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Methane is a potent greenhouse gas, with large flux uncertainties from facility-scale sources, such as natural gas extraction infrastructure. A recently developed flux quantification method was successfully tested by flying an unmanned aerial vehicle (UAV) downwind of 22 controlled atmospheric methane releases. The UAVs were used to derive high-precision atmospheric methane measurements. The UAV methodology was successful in both detecting the release and providing a rough flux estimate.
Chenjie Yu, Dantong Liu, Kurtis Broda, Rutambhara Joshi, Jason Olfert, Yele Sun, Pingqing Fu, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 20, 3645–3661, https://doi.org/10.5194/acp-20-3645-2020, https://doi.org/10.5194/acp-20-3645-2020, 2020
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This study presents the first atmospheric application of a new morphology-independent measurement for the quantification of the mixing state of rBC-containing particles in urban Beijing as part of the UK–China APHH campaign. An inversion method has been applied for better quantification of rBC mixing state. The mass-resolved rBC mixing state information presented here has implications for detailed models of BC, its optical properties and its atmospheric life cycle.
Pragati Rai, Markus Furger, Jay G. Slowik, Francesco Canonaco, Roman Fröhlich, Christoph Hüglin, María Cruz Minguillón, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 1657–1674, https://doi.org/10.5194/acp-20-1657-2020, https://doi.org/10.5194/acp-20-1657-2020, 2020
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A source apportionment study of hourly resolved elements in PM10 measured at a traffic-influenced site in Härkingen, Switzerland, using positive matrix factorization (PMF) and multilinear engine-2 (ME-2) offered resolution of robust and unambiguous factor profiles and contributions. We show that the rotational control available in ME-2 provides a means for treating extreme events such as fireworks within a PMF analysis.
Jianhui Jiang, Sebnem Aksoyoglu, Imad El-Haddad, Giancarlo Ciarelli, Hugo A. C. Denier van der Gon, Francesco Canonaco, Stefania Gilardoni, Marco Paglione, María Cruz Minguillón, Olivier Favez, Yunjiang Zhang, Nicolas Marchand, Liqing Hao, Annele Virtanen, Kalliopi Florou, Colin O'Dowd, Jurgita Ovadnevaite, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 15247–15270, https://doi.org/10.5194/acp-19-15247-2019, https://doi.org/10.5194/acp-19-15247-2019, 2019
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We use an air quality model with a modified organic aerosol (OA) module based on chamber experiments to identify the OA sources and their contributions in Europe. Comparisons with long-term measurements at nine sites in 2011 show an improvement in OA simulation. Our results suggest that the biomass burning and biogenic emissions are the dominant sources in winter and summer, respectively. Contributions of diesel and gasoline vehicles are relatively small compared to a previous study in the US.
Giulia Stefenelli, Veronika Pospisilova, Felipe D. Lopez-Hilfiker, Kaspar R. Daellenbach, Christoph Hüglin, Yandong Tong, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 14825–14848, https://doi.org/10.5194/acp-19-14825-2019, https://doi.org/10.5194/acp-19-14825-2019, 2019
Leigh R. Crilley, Louisa J. Kramer, Bin Ouyang, Jun Duan, Wenqian Zhang, Shengrui Tong, Maofa Ge, Ke Tang, Min Qin, Pinhua Xie, Marvin D. Shaw, Alastair C. Lewis, Archit Mehra, Thomas J. Bannan, Stephen D. Worrall, Michael Priestley, Asan Bacak, Hugh Coe, James Allan, Carl J. Percival, Olalekan A. M. Popoola, Roderic L. Jones, and William J. Bloss
Atmos. Meas. Tech., 12, 6449–6463, https://doi.org/10.5194/amt-12-6449-2019, https://doi.org/10.5194/amt-12-6449-2019, 2019
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Nitrous acid (HONO) is key species for understanding tropospheric chemistry, yet accurate and precise measurements are challenging. Here we report an inter–comparison exercise of a number of instruments that measured HONO in a highly polluted location (Beijing). All instruments agreed on the temporal trends yet displayed divergence in absolute concentrations. The cause of this divergence was unclear, but it may in part be due to spatial variability in instrument location.
Jun Zhou, Miriam Elser, Ru-Jin Huang, Manuel Krapf, Roman Fröhlich, Deepika Bhattu, Giulia Stefenelli, Peter Zotter, Emily A. Bruns, Simone M. Pieber, Haiyan Ni, Qiyuan Wang, Yichen Wang, Yaqing Zhou, Chunying Chen, Mao Xiao, Jay G. Slowik, Samuel Brown, Laure-Estelle Cassagnes, Kaspar R. Daellenbach, Thomas Nussbaumer, Marianne Geiser, André S. H. Prévôt, Imad El-Haddad, Junji Cao, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 19, 14703–14720, https://doi.org/10.5194/acp-19-14703-2019, https://doi.org/10.5194/acp-19-14703-2019, 2019
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Reactive oxygen species (ROS) are believed to contribute to the adverse health effects of aerosols. We measured particle-bound ROS (PB-ROS) with an online instrument in two distinct environments, i.e., Beijing (China) and Bern (Switzerland). In both cities these exogenic ROS are predominantly related to secondary organic aerosol (SOA). PB-ROS content in SOA from various anthropogenic emission sources tested in the laboratory was comparable to that in the ambient measurements.
Xiaoli Shen, Heike Vogel, Bernhard Vogel, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, Thomas Leisner, André S. H. Prévôt, and Harald Saathoff
Atmos. Chem. Phys., 19, 13189–13208, https://doi.org/10.5194/acp-19-13189-2019, https://doi.org/10.5194/acp-19-13189-2019, 2019
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This study provides good insight into the chemical nature and complex origin of aerosols by combining comprehensive field observations and transport modelling. We suggest that factors related to topography, metrological conditions, local emissions, in situ formation and growth, regional transport, and the interaction of biogenic and anthropogenic compounds need to be considered for a comprehensive understanding of aerosol processes.
James Brooks, Dantong Liu, James D. Allan, Paul I. Williams, Jim Haywood, Ellie J. Highwood, Sobhan K. Kompalli, S. Suresh Babu, Sreedharan K. Satheesh, Andrew G. Turner, and Hugh Coe
Atmos. Chem. Phys., 19, 13079–13096, https://doi.org/10.5194/acp-19-13079-2019, https://doi.org/10.5194/acp-19-13079-2019, 2019
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Our study presents an analysis of the vertical and horizontal black carbon properties across northern India using aircraft measurements. The Indo-Gangetic Plain saw the greatest black carbon mass concentrations during the pre-monsoon season. Two black carbon modes were recorded: a small black carbon mode (traffic emissions) in the north-west and a moderately coated mode (solid-fuel emissions) in the Indo-Gangetic Plain. In the vertical profile, absorption properties increase with height.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
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.
Duncan Watson-Parris, Nick Schutgens, Carly Reddington, Kirsty J. Pringle, Dantong Liu, James D. Allan, Hugh Coe, Ken S. Carslaw, and Philip Stier
Atmos. Chem. Phys., 19, 11765–11790, https://doi.org/10.5194/acp-19-11765-2019, https://doi.org/10.5194/acp-19-11765-2019, 2019
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The vertical distribution of aerosol in the atmosphere affects its ability to act as cloud condensation nuclei and changes the amount of sunlight it absorbs or reflects. Common global measurements of aerosol provide no information about this vertical distribution. Using a global collection of in situ aircraft measurements to compare with an aerosol–climate model (ECHAM-HAM), we explore the key processes controlling this distribution and find that wet removal plays a key role.
Wei Huang, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 19, 11687–11700, https://doi.org/10.5194/acp-19-11687-2019, https://doi.org/10.5194/acp-19-11687-2019, 2019
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We investigate the molecular composition and volatility of oxygenated organic aerosol (OOA) particles in summer and winter in Stuttgart, Germany. OOA in summer is more influenced by biogenic emissions, while in winter biomass burning emissions are an important source. OOA in winter is also less volatile. Potential reasons are discussed in our paper. Our study shows the important contributions of nonfossil OA from biogenic and biomass burning even in an urban area with high traffic emissions.
Giulia Stefenelli, Jianhui Jiang, Amelie Bertrand, Emily A. Bruns, Simone M. Pieber, Urs Baltensperger, Nicolas Marchand, Sebnem Aksoyoglu, André S. H. Prévôt, Jay G. Slowik, and Imad El Haddad
Atmos. Chem. Phys., 19, 11461–11484, https://doi.org/10.5194/acp-19-11461-2019, https://doi.org/10.5194/acp-19-11461-2019, 2019
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Box model simulations, based on the volatility basis set approach, of smog chamber wood combustion experiments conducted at different temperatures (−10 °C, 2 °C, 15 °C), emission loads, combustion conditions (flaming and smoldering) and residential stoves fabricated in the last 2 decades. Novel parameterization methods based on a genetic algorithm approach allowed estimation of precursor class contributions to SOA and evaluation of the effect of emission variability on SOA yield predictions.
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.
Sanna Saarikoski, Leah R. Williams, Steven R. Spielman, Gregory S. Lewis, Arantzazu Eiguren-Fernandez, Minna Aurela, Susanne V. Hering, Kimmo Teinilä, Philip Croteau, John T. Jayne, Thorsten Hohaus, Douglas R. Worsnop, and Hilkka Timonen
Atmos. Meas. Tech., 12, 3907–3920, https://doi.org/10.5194/amt-12-3907-2019, https://doi.org/10.5194/amt-12-3907-2019, 2019
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An air-to-air ultrafine particle concentrator (Aerosol Dynamics Inc. concentrator; ADIc) has been tailored for the low (~ 0.08 L min−1) inlet flow of aerosol mass spectrometers, and it provides a factor of 8–21 enrichment in the concentration of particles. The ADIc was evaluated in laboratory and field measurements. The results showed that the concentration factor depends primarily on the ratio between the sample flow and the output flow and is independent of particle size above about 10 nm.
Nicholas W. Davies, Cathryn Fox, Kate Szpek, Michael I. Cotterell, Jonathan W. Taylor, James D. Allan, Paul I. Williams, Jamie Trembath, Jim M. Haywood, and Justin M. Langridge
Atmos. Meas. Tech., 12, 3417–3434, https://doi.org/10.5194/amt-12-3417-2019, https://doi.org/10.5194/amt-12-3417-2019, 2019
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This research project assesses biases in traditional, filter-based, aerosol absorption measurements by comparison to state-of-the-art, non-filter-based, or in situ, measurements. We assess biases in traditional absorption measurements for three main aerosol types, including dust and fresh and aged biomass burning aerosols. The main results of this study are that the traditional and state-of-the-art absorption measurements are well correlated and that biases in the former are up to 45 %.
Jessie M. Creamean, Claudia Mignani, Nicolas Bukowiecki, and Franz Conen
Atmos. Chem. Phys., 19, 8123–8140, https://doi.org/10.5194/acp-19-8123-2019, https://doi.org/10.5194/acp-19-8123-2019, 2019
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Aerosols that serve as seeds for cloud ice formation are important to study because they impact cloud radiative properties, lifetime, and precipitation formation. We present an investigation of ice-nucleating particles (INPs) from aerosol, rime, and snow samples collected in clear and cloudy conditions during winter storms in the Swiss Alsp. INPs were more abundant and effective when storms originated from the south. We use spectral characteristics to investigate warm versus cold mode INPs.
Lu Qi, Mindong Chen, Giulia Stefenelli, Veronika Pospisilova, Yandong Tong, Amelie Bertrand, Christoph Hueglin, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 8037–8062, https://doi.org/10.5194/acp-19-8037-2019, https://doi.org/10.5194/acp-19-8037-2019, 2019
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Current understanding of OA sources is limited by the chemical resolution of existing real-time measurement technology. We describe the first wintertime deployment of a novel extractive electrospray ionization time-of-flight mass spectrometer, which provides near-molecular OA measurements with high time resolution. We show that biomass combustion strongly influences winter OA. Via factor analysis, aging-dependent signatures and time contributions of biomass-combustion-derived OA are resolved.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Athanasia Vlachou, Anna Tobler, Houssni Lamkaddam, Francesco Canonaco, Kaspar R. Daellenbach, Jean-Luc Jaffrezo, María Cruz Minguillón, Marek Maasikmets, Erik Teinemaa, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 7279–7295, https://doi.org/10.5194/acp-19-7279-2019, https://doi.org/10.5194/acp-19-7279-2019, 2019
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The resolution of rotational ambiguity in positive matrix factorization (PMF) models is a major challenge. Here, we developed a method based on bootstrapping and correlations to extract environmentally meaningful solutions from PMF analysis based on offline aerosol mass spectrometry data. The method has been tested on a dataset that covers 1 full year of filter samples collected at three different sites in Estonia.
Dantong Liu, Rutambhara Joshi, Junfeng Wang, Chenjie Yu, James D. Allan, Hugh Coe, Michael J. Flynn, Conghui Xie, James Lee, Freya Squires, Simone Kotthaus, Sue Grimmond, Xinlei Ge, Yele Sun, and Pingqing Fu
Atmos. Chem. Phys., 19, 6749–6769, https://doi.org/10.5194/acp-19-6749-2019, https://doi.org/10.5194/acp-19-6749-2019, 2019
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This study provides source attribution and characterization of BC in the Beijing urban environment in both winter and summer. For the first time, the physically and chemically based source apportionments are compared to evaluate the primary source contribution and secondary processing of BC-containing particles. A method is proposed to isolate the BC from the transportation sector and coal combustion sources.
Kaspar R. Daellenbach, Ivan Kourtchev, Alexander L. Vogel, Emily A. Bruns, Jianhui Jiang, Tuukka Petäjä, Jean-Luc Jaffrezo, Sebnem Aksoyoglu, Markus Kalberer, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 5973–5991, https://doi.org/10.5194/acp-19-5973-2019, https://doi.org/10.5194/acp-19-5973-2019, 2019
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Here we present the molecular composition of the organic aerosol (OA) at an urban site in Central Europe (Zurich, Switzerland) and compare it to smog chamber wood smoke and ambient biogenic secondary OA (SOA) (Orbitrap analyses). Accordingly, we are able to explain the strong seasonality of the molecular composition by aged wood smoke and biogenic SOA during winter and summer. Our results could also explain the predominance of non-fossil organic carbon at European locations throughout the year.
Eoghan Darbyshire, William T. Morgan, James D. Allan, Dantong Liu, Michael J. Flynn, James R. Dorsey, Sebastian J. O'Shea, Douglas Lowe, Kate Szpek, Franco Marenco, Ben T. Johnson, Stephane Bauguitte, Jim M. Haywood, Joel F. Brito, Paulo Artaxo, Karla M. Longo, and Hugh Coe
Atmos. Chem. Phys., 19, 5771–5790, https://doi.org/10.5194/acp-19-5771-2019, https://doi.org/10.5194/acp-19-5771-2019, 2019
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A novel analysis of aerosol and gas-phase vertical profiles shows a marked regional pollution contrast: composition is driven by the fire regime and vertical distribution is driven by thermodynamics. These drivers ought to be well represented in simulations to ensure realistic prediction of climate and air quality impacts. The BC : CO ratio in haze and plumes increases with altitude – long-range transport or fire stage coupled to plume dynamics may be responsible. Further enquiry is advocated.
James Brooks, James D. Allan, Paul I. Williams, Dantong Liu, Cathryn Fox, Jim Haywood, Justin M. Langridge, Ellie J. Highwood, Sobhan K. Kompalli, Debbie O'Sullivan, Suresh S. Babu, Sreedharan K. Satheesh, Andrew G. Turner, and Hugh Coe
Atmos. Chem. Phys., 19, 5615–5634, https://doi.org/10.5194/acp-19-5615-2019, https://doi.org/10.5194/acp-19-5615-2019, 2019
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Our study, for the first time, presents measurements of aerosol chemical composition and physical characteristics across northern India in the pre-monsoon and monsoon seasons of 2016 using the FAAM BAe-146 UK research aircraft. Across northern India, an elevated aerosol layer dominated by sulfate aerosol exists that diminishes with monsoon arrival. The Indo-Gangetic Plain (IGP) boundary layer is dominated by organics, whereas outside the IGP sulfate dominates with increased scattering aerosol.
Xiaoli Shen, Harald Saathoff, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, and Thomas Leisner
Atmos. Meas. Tech., 12, 2219–2240, https://doi.org/10.5194/amt-12-2219-2019, https://doi.org/10.5194/amt-12-2219-2019, 2019
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Based on single-particle mass spectra from field measurements in the upper Rhine valley, we identified characteristic particle classes and estimated their mass contributions without the need of a reference instrument in the field. Our study provides a good example for quantitative interpretation of single-particle data. Together with the complimentary results from bulk measurements, we have shown how a better understanding of the mixing state of ambient aerosol particles can be achieved.
Conner Daube, Stephen Conley, Ian C. Faloona, Claudia Arndt, Tara I. Yacovitch, Joseph R. Roscioli, and Scott C. Herndon
Atmos. Meas. Tech., 12, 2085–2095, https://doi.org/10.5194/amt-12-2085-2019, https://doi.org/10.5194/amt-12-2085-2019, 2019
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This study describes aircraft measurements of methane from dairy farms in central California. A small deliberate release of a tracer gas is done on the ground and measured from the air and the ratio of methane to tracer used to quantify emissions. Farm-scale methane emissions are determined as well as the fraction of those emissions coming from animal activity versus liquid manure management. These findings were within the uncertainty of two established methods.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
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We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Ghislain Motos, Julia Schmale, Joel C. Corbin, Rob. L. Modini, Nadine Karlen, Michele Bertò, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 19, 3833–3855, https://doi.org/10.5194/acp-19-3833-2019, https://doi.org/10.5194/acp-19-3833-2019, 2019
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Atmospheric black carbon (BC) particles are strong light absorbers that contribute to global warming. In situ cloud measurements performed at a high-altitude site showed that cloud supersaturation mainly drives the activation of BC to cloud droplets. It was further shown how BC particle size and mixing state modulate this nucleation scavenging in agreement with simplified theoretical predictions. These findings can inform model simulations towards a better representation of the BC life cycle.
Jianhui Jiang, Sebnem Aksoyoglu, Giancarlo Ciarelli, Emmanouil Oikonomakis, Imad El-Haddad, Francesco Canonaco, Colin O'Dowd, Jurgita Ovadnevaite, María Cruz Minguillón, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 3747–3768, https://doi.org/10.5194/acp-19-3747-2019, https://doi.org/10.5194/acp-19-3747-2019, 2019
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Biogenic volatile organic compound (BVOC) emissions from vegetation are essential inputs for air quality models but their uncertainties are very high. In this study we show the importance of BVOC emissions for modelled ozone and aerosol concentrations in Europe. Using different biogenic emissions from MEGAN and PSI models significantly affected organic aerosols (smaller effect on ozone), indicating the importance of harmonising the BVOC emissions in the model inter-comparison studies.
Daniel C. Anderson, Jessica Pavelec, Conner Daube, Scott C. Herndon, Walter B. Knighton, Brian M. Lerner, J. Robert Roscioli, Tara I. Yacovitch, and Ezra C. Wood
Atmos. Chem. Phys., 19, 2845–2860, https://doi.org/10.5194/acp-19-2845-2019, https://doi.org/10.5194/acp-19-2845-2019, 2019
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San Antonio is one of the largest cities in the United States and is in non-attainment of the 8 h ozone standard. Using the Aerodyne Mobile Laboratory, we made observations of ozone and its precursors at three sites in the San Antonio region to determine the main drivers of its production. We found that compounds produced by plants were the dominant organic compound for ozone production and that to limit ozone production at the study site, emissions of nitrogen oxides should be reduced.
Nicholas A. Marsden, Romy Ullrich, Ottmar Möhler, Stine Eriksen Hammer, Konrad Kandler, Zhiqiang Cui, Paul I. Williams, Michael J. Flynn, Dantong Liu, James D. Allan, and Hugh Coe
Atmos. Chem. Phys., 19, 2259–2281, https://doi.org/10.5194/acp-19-2259-2019, https://doi.org/10.5194/acp-19-2259-2019, 2019
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The composition of airborne dust influences climate and ecosystems but its measurements presents a huge analytical challenge. Using online single-particle mass spectrometry, we demonstrate differences in mineralogy and mixing state can be detected in real time in both laboratory studies and ambient measurements. The results provide insights into the temporal and spatial evolution of dust properties that will be useful for aerosol–cloud interaction studies and dust cycle modelling.
Ghislain Motos, Julia Schmale, Joel C. Corbin, Marco Zanatta, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Chem. Phys., 19, 2183–2207, https://doi.org/10.5194/acp-19-2183-2019, https://doi.org/10.5194/acp-19-2183-2019, 2019
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Clouds form by condensation of water vapour on aerosol particles. We showed that black carbon, a subset of particles responsible for a climate warming due to their strong light absorption and known to be insoluble in water, were able to form droplets when the humidity of the air is very slightly over 100 %. This is made possible by their acquisition of a
coatingmade of hydrophilic material during atmospheric aging. The predictability of this process using theory was successfully tested.
Junfeng Wang, Dantong Liu, Xinlei Ge, Yangzhou Wu, Fuzhen Shen, Mindong Chen, Jian Zhao, Conghui Xie, Qingqing Wang, Weiqi Xu, Jie Zhang, Jianlin Hu, James Allan, Rutambhara Joshi, Pingqing Fu, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 447–458, https://doi.org/10.5194/acp-19-447-2019, https://doi.org/10.5194/acp-19-447-2019, 2019
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This work is part of the UK-China APHH campaign. We used a laser-only Aerodyne soot particle aerosol mass spectrometer, for the first time, to investigate the concentrations, size distributions and chemical compositions for those ambient submicron aerosol particles only with black carbon as cores. Our findings are valuable to understand the BC properties and processes in the densely populated megacities.
Conghui Xie, Weiqi Xu, Junfeng Wang, Qingqing Wang, Dantong Liu, Guiqian Tang, Ping Chen, Wei Du, Jian Zhao, Yingjie Zhang, Wei Zhou, Tingting Han, Qingyun Bian, Jie Li, Pingqing Fu, Zifa Wang, Xinlei Ge, James Allan, Hugh Coe, and Yele Sun
Atmos. Chem. Phys., 19, 165–179, https://doi.org/10.5194/acp-19-165-2019, https://doi.org/10.5194/acp-19-165-2019, 2019
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We present the first simultaneous real-time online measurements of aerosol optical properties at ground level and at 260 m on a meteorological tower in urban Beijing in winter. The vertical similarities and differences in scattering and absorption coefficients were characterized. The increases in MAC of BC were mainly associated with the coating materials on rBC. Coal combustion was the dominant source contribution of brown carbon followed by biomass burning and SOA in winter in Beijing.
Krystal T. Vasquez, Hannah M. Allen, John D. Crounse, Eric Praske, Lu Xu, Anke C. Noelscher, and Paul O. Wennberg
Atmos. Meas. Tech., 11, 6815–6832, https://doi.org/10.5194/amt-11-6815-2018, https://doi.org/10.5194/amt-11-6815-2018, 2018
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Oxygenated volatile organic compounds (OVOCs) are difficult to measure in the atmosphere due to their high reactivity and low concentrations. This hinders our understanding of their impact on air quality and climate. Therefore, we have developed a field-deployable instrument capable of providing isomer-resolved measurements of OVOCs in the ambient air. Its performance is assessed through data collected both in the laboratory and during two field studies.
Nivedita K. Kumar, Joel C. Corbin, Emily A. Bruns, Dario Massabó, Jay G. Slowik, Luka Drinovec, Griša Močnik, Paolo Prati, Athanasia Vlachou, Urs Baltensperger, Martin Gysel, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 17843–17861, https://doi.org/10.5194/acp-18-17843-2018, https://doi.org/10.5194/acp-18-17843-2018, 2018
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It is clear that considerable uncertainties still exist in understanding the magnitude of aerosol absorption on a global scale and its contribution to global warming. This manuscript provides a comprehensive assessment of the optical absorption by organic aerosols (brown carbon) from residential wood combustion as a function of atmospheric aging.
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.
Tuomo Nieminen, Veli-Matti Kerminen, Tuukka Petäjä, Pasi P. Aalto, Mikhail Arshinov, Eija Asmi, Urs Baltensperger, David C. S. Beddows, Johan Paul Beukes, Don Collins, Aijun Ding, Roy M. Harrison, Bas Henzing, Rakesh Hooda, Min Hu, Urmas Hõrrak, Niku Kivekäs, Kaupo Komsaare, Radovan Krejci, Adam Kristensson, Lauri Laakso, Ari Laaksonen, W. Richard Leaitch, Heikki Lihavainen, Nikolaos Mihalopoulos, Zoltán Németh, Wei Nie, Colin O'Dowd, Imre Salma, Karine Sellegri, Birgitta Svenningsson, Erik Swietlicki, Peter Tunved, Vidmantas Ulevicius, Ville Vakkari, Marko Vana, Alfred Wiedensohler, Zhijun Wu, Annele Virtanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 14737–14756, https://doi.org/10.5194/acp-18-14737-2018, https://doi.org/10.5194/acp-18-14737-2018, 2018
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Atmospheric aerosols have diverse effects on air quality, human health, and global climate. One important source of aerosols is their formation via nucleation and growth in the atmosphere. We have analyzed long-term observations of regional new particle formation events around the globe and provide a comprehensive view on the characteristics of this phenomenon in diverse environments. The results are useful in developing more realistic representation of atmospheric aerosols in global models.
Marco Zanatta, Paolo Laj, Martin Gysel, Urs Baltensperger, Stergios Vratolis, Konstantinos Eleftheriadis, Yutaka Kondo, Philippe Dubuisson, Victor Winiarek, Stelios Kazadzis, Peter Tunved, and Hans-Werner Jacobi
Atmos. Chem. Phys., 18, 14037–14057, https://doi.org/10.5194/acp-18-14037-2018, https://doi.org/10.5194/acp-18-14037-2018, 2018
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The research community aims to quantify the actual contribution of soot particles to the recent Arctic warming. We discovered that mixing of soot with other components might enhance its light absorption power by 50 %. The neglection of such amplification might lead to the underestimation of radiative forcing by 0.12 W m−2. Thus a better understanding of the optical properties of soot is a crucial step for an accurate quantification of the radiative impact of soot in the Arctic atmosphere.
Michael Priestley, Michael le Breton, Thomas J. Bannan, Stephen D. Worrall, Asan Bacak, Andrew R. D. Smedley, Ernesto Reyes-Villegas, Archit Mehra, James Allan, Ann R. Webb, Dudley E. Shallcross, Hugh Coe, and Carl J. Percival
Atmos. Chem. Phys., 18, 13481–13493, https://doi.org/10.5194/acp-18-13481-2018, https://doi.org/10.5194/acp-18-13481-2018, 2018
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.
Elena Spinei, Andrew Whitehill, Alan Fried, Martin Tiefengraber, Travis N. Knepp, Scott Herndon, Jay R. Herman, Moritz Müller, Nader Abuhassan, Alexander Cede, Dirk Richter, James Walega, James Crawford, James Szykman, Lukas Valin, David J. Williams, Russell Long, Robert J. Swap, Youngjae Lee, Nabil Nowak, and Brett Poche
Atmos. Meas. Tech., 11, 4943–4961, https://doi.org/10.5194/amt-11-4943-2018, https://doi.org/10.5194/amt-11-4943-2018, 2018
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Formaldehyde is toxic to humans and is formed in the atmosphere in the presence of air pollution, but the measurements are sparse. Pandonia Global Network instruments measure total formaldehyde column from the surface to the top of troposphere and will be widely available. This study compared formaldehyde Pandora columns with the surface and aircraft-integrated columns near Seoul, South Korea. Relatively good agreement was observed between the three datasets with some overestimation by Pandora.
Martine Collaud Coen, Elisabeth Andrews, Diego Aliaga, Marcos Andrade, Hristo Angelov, Nicolas Bukowiecki, Marina Ealo, Paulo Fialho, Harald Flentje, A. Gannet Hallar, Rakesh Hooda, Ivo Kalapov, Radovan Krejci, Neng-Huei Lin, Angela Marinoni, Jing Ming, Nhat Anh Nguyen, Marco Pandolfi, Véronique Pont, Ludwig Ries, Sergio Rodríguez, Gerhard Schauer, Karine Sellegri, Sangeeta Sharma, Junying Sun, Peter Tunved, Patricio Velasquez, and Dominique Ruffieux
Atmos. Chem. Phys., 18, 12289–12313, https://doi.org/10.5194/acp-18-12289-2018, https://doi.org/10.5194/acp-18-12289-2018, 2018
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High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer. An ABL-TopoIndex is defined from a topography analysis around the stations. This new index allows ranking stations as a function of the ABL influence due to topography or help to choose a new site to sample FT. The ABL-TopoIndex is validated by aerosol optical properties and number concentration measured at 29 high altitude stations of five continents.
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.
Kelly L. Pereira, Rachel Dunmore, James Whitehead, M. Rami Alfarra, James D. Allan, Mohammed S. Alam, Roy M. Harrison, Gordon McFiggans, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 18, 11073–11096, https://doi.org/10.5194/acp-18-11073-2018, https://doi.org/10.5194/acp-18-11073-2018, 2018
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Exhaust emissions from a light-duty diesel engine were introduced into an atmospheric simulation chamber which was used as a holding-cell for sampling, allowing instruments capable of providing detailed chemical speciation of exhaust gas emissions to be used. The effect of different engine conditions on the exhaust gas composition was investigated. The exhaust composition changed considerably due to two influencing factors, engine combustion and diesel oxidative catalyst efficiency.
Amelie Bertrand, Giulia Stefenelli, Simone M. Pieber, Emily A. Bruns, Brice Temime-Roussel, Jay G. Slowik, Henri Wortham, André S. H. Prévôt, Imad El Haddad, and Nicolas Marchand
Atmos. Chem. Phys., 18, 10915–10930, https://doi.org/10.5194/acp-18-10915-2018, https://doi.org/10.5194/acp-18-10915-2018, 2018
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We model the evolution of several BBOA markers including levoglucosan during aging experiments conducted in an atmospheric Teflon chamber, in order to evaluate the influence of vapor wall loss on the determination of the rate constants of the compounds with hydroxyl radicals (OH).
Ramakrishna Ramisetty, Ahmed Abdelmonem, Xiaoli Shen, Harald Saathoff, Thomas Leisner, and Claudia Mohr
Atmos. Meas. Tech., 11, 4345–4360, https://doi.org/10.5194/amt-11-4345-2018, https://doi.org/10.5194/amt-11-4345-2018, 2018
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In this study we coupled a laser ablation aerosol time-of-flight (LAAPTOF) single-particle mass spectrometer, originally equipped with an excimer laser, to a femtosecond laser. The objective was to assess the influence of the higher laser power density of the femtosecond laser on ablation–ionization of atmospheric particles, ion signal, and ultimately quantitative abilities of the single-particle mass spectrometer.
Simone M. Pieber, Nivedita K. Kumar, Felix Klein, Pierre Comte, Deepika Bhattu, Josef Dommen, Emily A. Bruns, Doǧuşhan Kılıç, Imad El Haddad, Alejandro Keller, Jan Czerwinski, Norbert Heeb, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 9929–9954, https://doi.org/10.5194/acp-18-9929-2018, https://doi.org/10.5194/acp-18-9929-2018, 2018
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We studied primary emissions and secondary organic aerosol (SOA) from gasoline direct injection (GDI) vehicles including GDIs retrofitted with gasoline particle filters (GPF). GPF retrofitting significantly decreased the primary particulate matter, particularly through removal of refractory black carbon and, to a lesser extent, of non-refractory organic particulates. SOA experiments were conducted in a batch and flow reactor. GPF retrofitting did not significantly affect precursors or yields.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Martin Wild, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 9741–9765, https://doi.org/10.5194/acp-18-9741-2018, https://doi.org/10.5194/acp-18-9741-2018, 2018
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We report a model sensitivity study on the impact of aerosol–radiation interaction (ARI) changes in Europe between 1990 and 2010 on summer surface ozone via effects on photolysis rates and biogenic emissions. The overall impact of ARI changes on ozone was relatively small when compared to the total ozone concentrations, but it was more important when compared to the order of magnitude of ozone trends, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.
Anja H. Tremper, Anna Font, Max Priestman, Samera H. Hamad, Tsai-Chia Chung, Ari Pribadi, Richard J. C. Brown, Sharon L. Goddard, Nathalie Grassineau, Krag Petterson, Frank J. Kelly, and David C. Green
Atmos. Meas. Tech., 11, 3541–3557, https://doi.org/10.5194/amt-11-3541-2018, https://doi.org/10.5194/amt-11-3541-2018, 2018
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Measuring the chemical composition of airborne particulates can provide valuable information on the concentration of regulated toxic metals and their sources and assist in the identification and validation of abatement techniques. Undertaking these measurements at a high time resolution enables computer modelling techniques to be more robustly linked to emission processes. This study describes a comprehensive laboratory and field evaluation of a high time resolution metal monitoring instrument.
Marco Pandolfi, Lucas Alados-Arboledas, Andrés Alastuey, Marcos Andrade, Christo Angelov, Begoña Artiñano, John Backman, Urs Baltensperger, Paolo Bonasoni, Nicolas Bukowiecki, Martine Collaud Coen, Sébastien Conil, Esther Coz, Vincent Crenn, Vadimas Dudoitis, Marina Ealo, Kostas Eleftheriadis, Olivier Favez, Prodromos Fetfatzis, Markus Fiebig, Harald Flentje, Patrick Ginot, Martin Gysel, Bas Henzing, Andras Hoffer, Adela Holubova Smejkalova, Ivo Kalapov, Nikos Kalivitis, Giorgos Kouvarakis, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Chris Lunder, Krista Luoma, Hassan Lyamani, Angela Marinoni, Nikos Mihalopoulos, Marcel Moerman, José Nicolas, Colin O'Dowd, Tuukka Petäjä, Jean-Eudes Petit, Jean Marc Pichon, Nina Prokopciuk, Jean-Philippe Putaud, Sergio Rodríguez, Jean Sciare, Karine Sellegri, Erik Swietlicki, Gloria Titos, Thomas Tuch, Peter Tunved, Vidmantas Ulevicius, Aditya Vaishya, Milan Vana, Aki Virkkula, Stergios Vratolis, Ernest Weingartner, Alfred Wiedensohler, and Paolo Laj
Atmos. Chem. Phys., 18, 7877–7911, https://doi.org/10.5194/acp-18-7877-2018, https://doi.org/10.5194/acp-18-7877-2018, 2018
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This investigation presents the variability in near-surface in situ aerosol particle light-scattering measurements obtained over the past decade at 28 measuring atmospheric observatories which are part of the ACTRIS Research Infrastructure, and most of them belong to the GAW network. This paper provides a comprehensive picture of the spatial and temporal variability of aerosol particles optical properties in Europe.
Amelie Bertrand, Giulia Stefenelli, Coty N. Jen, Simone M. Pieber, Emily A. Bruns, Haiyan Ni, Brice Temime-Roussel, Jay G. Slowik, Allen H. Goldstein, Imad El Haddad, Urs Baltensperger, André S. H. Prévôt, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, https://doi.org/10.5194/acp-18-7607-2018, 2018
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A thermal desorption aerosol gas chromatograph coupled to an aerosol mass spectrometer (TAG–AMS) is connected to an atmospheric chamber. The setup serves the quantitative study of the impact of combustion conditions and atmospheric aging on the chemical fingerprint at the molecular level of biomass burning organic aerosol.
Doğuşhan Kılıç, Imad El Haddad, Benjamin T. Brem, Emily Bruns, Carlo Bozetti, Joel Corbin, Lukas Durdina, Ru-Jin Huang, Jianhui Jiang, Felix Klein, Avi Lavi, Simone M. Pieber, Theo Rindlisbacher, Yinon Rudich, Jay G. Slowik, Jing Wang, Urs Baltensperger, and Andre S. H. Prévôt
Atmos. Chem. Phys., 18, 7379–7391, https://doi.org/10.5194/acp-18-7379-2018, https://doi.org/10.5194/acp-18-7379-2018, 2018
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We study primary emissions and secondary aerosol (SA) from an aircraft turbofan. By monitoring the chemical composition of both gaseous and particulate emissions at different engine loads, we explained SA formed in an oxidation flow reactor (PAM) by the oxidation of gaseous species. At idle, more than 90 % of the secondary particle mass was organic and could be explained by the oxidation of gaseous aromatic species, while at an approximated cruise load sulfates comprised 85 % of the total SA.
Jun Zhou, Peter Zotter, Emily A. Bruns, Giulia Stefenelli, Deepika Bhattu, Samuel Brown, Amelie Bertrand, Nicolas Marchand, Houssni Lamkaddam, Jay G. Slowik, André S. H. Prévôt, Urs Baltensperger, Thomas Nussbaumer, Imad El-Haddad, and Josef Dommen
Atmos. Chem. Phys., 18, 6985–7000, https://doi.org/10.5194/acp-18-6985-2018, https://doi.org/10.5194/acp-18-6985-2018, 2018
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We thoroughly studied the reactive oxygen species (ROS) generation potential of particulate wood combustion emissions, from different combustion technologies, fuel types, operation methods, combustion regimes and phases. ROS from automatically operated combustion devices under optimal conditions were much lower than those from manually operated appliances. We examined the impact of atmospheric aging on ROS content in SOA and determined the controlling parameters, by using an online ROS analyzer.
Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Benjamin Chazeau, Gary A. Salazar, Soenke Szidat, Jean-Luc Jaffrezo, Christoph Hueglin, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 6187–6206, https://doi.org/10.5194/acp-18-6187-2018, https://doi.org/10.5194/acp-18-6187-2018, 2018
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Carbonaceous aerosols are related to adverse human health effects, which depend on the aerosol chemical composition and size. Here, we combine aerosol mass spectrometry and radiocarbon measurements of size-resolved samples collected over a long term to identify the origins of primary and secondary carbonaceous aerosols in the fine and coarse modes.
Miguel Zavala, Luisa T. Molina, Pablo Maiz, Israel Monsivais, Judith C. Chow, John G. Watson, Jose Luis Munguia, Beatriz Cardenas, Edward C. Fortner, Scott C. Herndon, Joseph R. Roscioli, Charles E. Kolb, and Walter B. Knighton
Atmos. Chem. Phys., 18, 6023–6037, https://doi.org/10.5194/acp-18-6023-2018, https://doi.org/10.5194/acp-18-6023-2018, 2018
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Black carbon, organic carbon, and co-pollutant emissions and energy efficiency from two traditional brick kilns and one MK2 kiln in Mexico were quantified using tracer ratio and sampling probe techniques. Both techniques captured similar temporal profiles of the kiln emissions and produced comparable emission factors; the MK2 generated lower emissions and higher energy efficiency. This study contributes to the limited database of brick production emissions useful for assessing their impact.
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.
Amy K. Hodgson, William T. Morgan, Sebastian O'Shea, Stéphane Bauguitte, James D. Allan, Eoghan Darbyshire, Michael J. Flynn, Dantong Liu, James Lee, Ben Johnson, Jim M. Haywood, Karla M. Longo, Paulo E. Artaxo, and Hugh Coe
Atmos. Chem. Phys., 18, 5619–5638, https://doi.org/10.5194/acp-18-5619-2018, https://doi.org/10.5194/acp-18-5619-2018, 2018
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We flew a large atmospheric research aircraft across a number of different biomass burning environments in the Amazon Basin in September and October 2012. In this paper, we focus on smoke sampled very close to fresh fires (only 600–900 m above the fires and smoke that was 4–6 min old) to examine the chemical components that make up the smoke and their abundance. We found substantial differences in the emitted smoke that are due to the fuel type and combustion processes driving the fires.
Xiaoli Shen, Ramakrishna Ramisetty, Claudia Mohr, Wei Huang, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 11, 2325–2343, https://doi.org/10.5194/amt-11-2325-2018, https://doi.org/10.5194/amt-11-2325-2018, 2018
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This paper presents performance data and reference spectra from the commercially available single-particle mass spectrometer LAAPTOF. The main characteristics of the instrument, like its detection efficiency, are given for a wide particle size range. Furthermore, reference mass spectra for 32 well-defined different particle types relevant for atmospheric aerosol compounds are presented. It is shown that these reference mass spectra are very useful in analysis of atmospheric aerosol particles.
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.
Ernesto Reyes-Villegas, Michael Priestley, Yu-Chieh Ting, Sophie Haslett, Thomas Bannan, Michael Le Breton, Paul I. Williams, Asan Bacak, Michael J. Flynn, Hugh Coe, Carl Percival, and James D. Allan
Atmos. Chem. Phys., 18, 4093–4111, https://doi.org/10.5194/acp-18-4093-2018, https://doi.org/10.5194/acp-18-4093-2018, 2018
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This work presents the analysis of a special event with high biomass burning emissions, named Bonfire Night. Nitrogen chemistry was observed and it was possible to study the night time chemistry. It was possible to quantify particulate organic oxides of nitrogen (PON) concentrations of 2.8 µg m−3 using 46 : 30 ratios from aerosol mass spectrometry measurements. The use of the receptor model positive matrix factorization (PMF) allowed to separate organic aerosols into different sources.
Yan-Lin Zhang, Imad El-Haddad, Ru-Jin Huang, Kin-Fai Ho, Jun-Ji Cao, Yongming Han, Peter Zotter, Carlo Bozzetti, Kaspar R. Daellenbach, Jay G. Slowik, Gary Salazar, André S. H. Prévôt, and Sönke Szidat
Atmos. Chem. Phys., 18, 4005–4017, https://doi.org/10.5194/acp-18-4005-2018, https://doi.org/10.5194/acp-18-4005-2018, 2018
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Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time of flight aerosol mass spectrometer measurements. We demonstrate a dominant contribution of non-fossil emissions to WSOC aerosols in the Northern Hemisphere. However, the fossil fraction is substantially larger in aerosols from East Asia and the east Asian pollution outflow, especially during winter, due to increasing coal combustion.
Wei Huang, Harald Saathoff, Aki Pajunoja, Xiaoli Shen, Karl-Heinz Naumann, Robert Wagner, Annele Virtanen, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, https://doi.org/10.5194/acp-18-2883-2018, 2018
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Qiao Zhu, Xiao-Feng Huang, Li-Ming Cao, Lin-Tong Wei, Bin Zhang, Ling-Yan He, Miriam Elser, Francesco Canonaco, Jay G. Slowik, Carlo Bozzetti, Imad El-Haddad, and André S. H. Prévôt
Atmos. Meas. Tech., 11, 1049–1060, https://doi.org/10.5194/amt-11-1049-2018, https://doi.org/10.5194/amt-11-1049-2018, 2018
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Organic aerosol constitutes one of the major components of atmospheric particulate matter globally and is emitted from various sources. Therefore, identifying and quantifying the sources of organic aerosol accurately is a key task in the field. In this study, we applied a rather novel procedure for an improved source apportionment method (ME-2) to resolve the
less meaningful or mixed factorsproblems for organic aerosol using the traditional method (PMF).
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.
Lisa K. Whalley, Daniel Stone, Rachel Dunmore, Jacqueline Hamilton, James R. Hopkins, James D. Lee, Alastair C. Lewis, Paul Williams, Jörg Kleffmann, Sebastian Laufs, Robert Woodward-Massey, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 2547–2571, https://doi.org/10.5194/acp-18-2547-2018, https://doi.org/10.5194/acp-18-2547-2018, 2018
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This paper presents the first radical observations made in London and subsequent model comparisons. This work highlights that there are uncertainties in the degradation mechanism of complex biogenic and diesel-related VOC species under low-NOx conditions and under high-NOx conditions there is a missing source of RO2 radicals. The impact of these model uncertainties on in situ ozone production as a function of NOx is discussed.
Kaspar R. Daellenbach, Imad El-Haddad, Lassi Karvonen, Athanasia Vlachou, Joel C. Corbin, Jay G. Slowik, Maarten F. Heringa, Emily A. Bruns, Samuel M. Luedin, Jean-Luc Jaffrezo, Sönke Szidat, Andrea Piazzalunga, Raquel Gonzalez, Paola Fermo, Valentin Pflueger, Guido Vogel, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 2155–2174, https://doi.org/10.5194/acp-18-2155-2018, https://doi.org/10.5194/acp-18-2155-2018, 2018
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A novel offline LDI-MS method was developed to analyse particulate matter (PM) collected at multiple sites in central Europe during the entire year of 2013. PM sources were identified by positive matrix factorization. Wood burning emissions were separated according to the burning conditions; inefficient burns had a larger impact on air quality in southern Alpine valleys than in northern Switzerland. Moreover, primary tailpipe exhaust was distinguished from aged/secondary traffic emissions.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 2175–2198, https://doi.org/10.5194/acp-18-2175-2018, https://doi.org/10.5194/acp-18-2175-2018, 2018
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We report a modeling study investigating the uncertainties in ozone production in Europe. Using various methods for different emission and meteorological scenarios, we searched for the possible reasons for underestimation of high ozone levels in Europe by models. Our results suggest that emissions, especially NOx, might be too low in the European inventories. Improvement of the modeled ozone production will contribute to more consistent and effective ozone mitigation strategies for the future.
Ugo Molteni, Federico Bianchi, Felix Klein, Imad El Haddad, Carla Frege, Michel J. Rossi, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 1909–1921, https://doi.org/10.5194/acp-18-1909-2018, https://doi.org/10.5194/acp-18-1909-2018, 2018
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Anthropogenic volatile organic compounds often dominate the urban atmosphere and consist to a large degree of aromatics. These compounds are already known as important precursors for the formation of secondary organic aerosol. This study shows how the oxidation of aromatics with an OH radical leads to subsequent autoxidation chain reactions forming highly oxygenated molecules. We hypothesize that these may contribute substantially to new particle formation events detected in urban areas.
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.
Sophie L. Haslett, J. Chris Thomas, William T. Morgan, Rory Hadden, Dantong Liu, James D. Allan, Paul I. Williams, Sekou Keita, Cathy Liousse, and Hugh Coe
Atmos. Chem. Phys., 18, 385–403, https://doi.org/10.5194/acp-18-385-2018, https://doi.org/10.5194/acp-18-385-2018, 2018
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Wood burning is chaotic, so the particles emitted can be difficult to study in a repeatable way. Here, we addressed this problem by carefully controlling small wood fires in the lab. We saw three burning phases, which could be told apart chemically; we also saw evidence of these in measurements of wood burning in London in 2012. Controlled experiments like this help us to understand why emissions are so variable and to recognise burning conditions just from the particles seen in the atmosphere.
Nicholas A. Marsden, Michael J. Flynn, James D. Allan, and Hugh Coe
Atmos. Meas. Tech., 11, 195–213, https://doi.org/10.5194/amt-11-195-2018, https://doi.org/10.5194/amt-11-195-2018, 2018
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Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is lost. We introduce a novel technique that enables the online differentiation of mineral phase in silicate particles by single-particle mass spectrometry.
Jun Zhou, Emily A. Bruns, Peter Zotter, Giulia Stefenelli, André S. H. Prévôt, Urs Baltensperger, Imad El-Haddad, and Josef Dommen
Atmos. Meas. Tech., 11, 65–80, https://doi.org/10.5194/amt-11-65-2018, https://doi.org/10.5194/amt-11-65-2018, 2018
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Reactive oxygen species (ROS) in the particle phase may induce oxidative stress in the human lungs upon inhalation. Here we present and thoroughly characterize a modified online and offline ROS analyzer. Selected model organic compounds were tested and potential interferences from gas-phase and matrix effects of particulate constituents were evaluated. ROS measurements of filter samples revealed the rapid decay of a substantial ROS fraction, supporting the application of online measurements.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
Larissa Lacher, Ulrike Lohmann, Yvonne Boose, Assaf Zipori, Erik Herrmann, Nicolas Bukowiecki, Martin Steinbacher, and Zamin A. Kanji
Atmos. Chem. Phys., 17, 15199–15224, https://doi.org/10.5194/acp-17-15199-2017, https://doi.org/10.5194/acp-17-15199-2017, 2017
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We characterize the new Horizontal Ice Nucleation Chamber HINC to measure ambient ice nucleating particle concentrations at mixed‐phase cloud conditions. Results from winter measurements at the High Altitude Research Station Jungfraujoch compare well to previous measurements. We find increased ice nucleating particle concentrations during the influence of Saharan dust events and marine events, which highlights the importance of these species on ice nucleation in the free troposphere.
Miguel Zavala, Luisa T. Molina, Tara I. Yacovitch, Edward C. Fortner, Joseph R. Roscioli, Cody Floerchinger, Scott C. Herndon, Charles E. Kolb, Walter B. Knighton, Victor Hugo Paramo, Sergio Zirath, José Antonio Mejía, and Aron Jazcilevich
Atmos. Chem. Phys., 17, 15293–15305, https://doi.org/10.5194/acp-17-15293-2017, https://doi.org/10.5194/acp-17-15293-2017, 2017
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Emission factors of black carbon and other chemically speciated particulate matter and gaseous pollutants were measured in real-world driving conditions for 20 diesel vehicles with multiple emission technologies in Mexico City using a mobile laboratory and a remote sensing technique. The results demonstrated the need to use locally obtained emissions data for diesel vehicles, especially in the developing world, to reduce uncertainty and improve the effectiveness of mitigation measures.
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
Gouri Prabhakar, Caroline L. Parworth, Xiaolu Zhang, Hwajin Kim, Dominique E. Young, Andreas J. Beyersdorf, Luke D. Ziemba, John B. Nowak, Timothy H. Bertram, Ian C. Faloona, Qi Zhang, and Christopher D. Cappa
Atmos. Chem. Phys., 17, 14747–14770, https://doi.org/10.5194/acp-17-14747-2017, https://doi.org/10.5194/acp-17-14747-2017, 2017
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This work assesses the processes that control the ambient concentrations of particulate nitrate in the the wintertime San Joaquin Valley of California through a combination of aircraft and surface measurements made during the DISCOVER-AQ study. We provide an observational demonstration of how nocturnal production and advection in aloft layers combines with daytime production and loss from entrainment and deposition to give rise to a distinct diurnal profile in surface nitrate concentrations.
Marc D. Mallet, Maximilien J. Desservettaz, Branka Miljevic, Andelija Milic, Zoran D. Ristovski, Joel Alroe, Luke T. Cravigan, E. Rohan Jayaratne, Clare Paton-Walsh, David W. T. Griffith, Stephen R. Wilson, Graham Kettlewell, Marcel V. van der Schoot, Paul Selleck, Fabienne Reisen, Sarah J. Lawson, Jason Ward, James Harnwell, Min Cheng, Rob W. Gillett, Suzie B. Molloy, Dean Howard, Peter F. Nelson, Anthony L. Morrison, Grant C. Edwards, Alastair G. Williams, Scott D. Chambers, Sylvester Werczynski, Leah R. Williams, V. Holly L. Winton, Brad Atkinson, Xianyu Wang, and Melita D. Keywood
Atmos. Chem. Phys., 17, 13681–13697, https://doi.org/10.5194/acp-17-13681-2017, https://doi.org/10.5194/acp-17-13681-2017, 2017
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Fires play an important role within atmosphere. Gaseous and aerosol emissions influence Earth's temperature but these emissions can vary drastically across region and season. The SAFIRED (Savannah Fires in the Early Dry Season) campaign was undertaken at the Australian Tropical Research Station in north Australia during the 2014 early dry season. This paper presents an overview of the fires in this region, the measurements of their emissions and the implications of these fires on the atmosphere.
Kaspar R. Daellenbach, Giulia Stefenelli, Carlo Bozzetti, Athanasia Vlachou, Paola Fermo, Raquel Gonzalez, Andrea Piazzalunga, Cristina Colombi, Francesco Canonaco, Christoph Hueglin, Anne Kasper-Giebl, Jean-Luc Jaffrezo, Federico Bianchi, Jay G. Slowik, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 13265–13282, https://doi.org/10.5194/acp-17-13265-2017, https://doi.org/10.5194/acp-17-13265-2017, 2017
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We present offline AMS analyses for the organic aerosol (OA) in PM10 at nine sites in central Europe for 2013. Primary OA is separated into traffic, cooking, and wood-burning components. A factor explaining sulfur-containing ions, with an event-driven time series, is also separated. We observe enhanced production of secondary OA (SOA) in summer, following biogenic emissions with temperature. In winter a SOA component is dominant, which correlates with anthropogenic inorganic species.
Sebastian J. O'Shea, Thomas W. Choularton, Michael Flynn, Keith N. Bower, Martin Gallagher, Jonathan Crosier, Paul Williams, Ian Crawford, Zoë L. Fleming, Constantino Listowski, Amélie Kirchgaessner, Russell S. Ladkin, and Thomas Lachlan-Cope
Atmos. Chem. Phys., 17, 13049–13070, https://doi.org/10.5194/acp-17-13049-2017, https://doi.org/10.5194/acp-17-13049-2017, 2017
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Few direct measurements have been made of Antarctic cloud and aerosol properties. As part of the 2015 Microphysics of Antarctic Clouds (MAC) field campaign, detailed airborne and ground-based measurements were made over the Weddell Sea and Antarctic coastal continent. This paper presents the first results from this campaign and discusses the cloud properties and processes important in this region.
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.
Eben S. Cross, Leah R. Williams, David K. Lewis, Gregory R. Magoon, Timothy B. Onasch, Michael L. Kaminsky, Douglas R. Worsnop, and John T. Jayne
Atmos. Meas. Tech., 10, 3575–3588, https://doi.org/10.5194/amt-10-3575-2017, https://doi.org/10.5194/amt-10-3575-2017, 2017
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Low-cost air quality sensor technologies offer new opportunities for fast and distributed measurements of air pollution, but a persistent characterization gap remains when it comes to evaluating sensor performance under realistic environmental sampling conditions. We present results from a newly developed integrated AQ-sensor system (ARISense) and demonstrate the utility of using high-dimensional model representation to improve the conversion of raw sensor signal to ambient concentration.
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.
Stephen Conley, Ian Faloona, Shobhit Mehrotra, Maxime Suard, Donald H. Lenschow, Colm Sweeney, Scott Herndon, Stefan Schwietzke, Gabrielle Pétron, Justin Pifer, Eric A. Kort, and Russell Schnell
Atmos. Meas. Tech., 10, 3345–3358, https://doi.org/10.5194/amt-10-3345-2017, https://doi.org/10.5194/amt-10-3345-2017, 2017
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This paper describes a new method of quantifying surface trace gas emissions (e.g. methane) from small aircraft (e.g. Mooney, Cessna) in about 30 min. This technique greatly enhances our ability to rapidly respond in the event of catastrophic failures such as Aliso Canyon and Deep Water Horizon.
Jakob Lindaas, Delphine K. Farmer, Ilana B. Pollack, Andrew Abeleira, Frank Flocke, Rob Roscioli, Scott Herndon, and Emily V. Fischer
Atmos. Chem. Phys., 17, 10691–10707, https://doi.org/10.5194/acp-17-10691-2017, https://doi.org/10.5194/acp-17-10691-2017, 2017
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Wildfire smoke is becoming increasingly important for air quality in the US. We used measurements taken during the summer 2015 near Denver, CO, to provide a case study of how wildfire smoke can impact air quality, specifically ozone, which is harmful to humans. Wildfire smoke during this time period was associated with about 15 % more ozone than we would expect under normal conditions. This smoke came from fires in the Pacific Northwest and likely impacted much of the central and western US.
Georgios Tsagkogeorgas, Pontus Roldin, Jonathan Duplissy, Linda Rondo, Jasmin Tröstl, Jay G. Slowik, Sebastian Ehrhart, Alessandro Franchin, Andreas Kürten, Antonio Amorim, Federico Bianchi, Jasper Kirkby, Tuukka Petäjä, Urs Baltensperger, Michael Boy, Joachim Curtius, Richard C. Flagan, Markku Kulmala, Neil M. Donahue, and Frank Stratmann
Atmos. Chem. Phys., 17, 8923–8938, https://doi.org/10.5194/acp-17-8923-2017, https://doi.org/10.5194/acp-17-8923-2017, 2017
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The H2SO4 vapour pressure plays key role in Earth's and Venus' atmospheres. In regions where RH is low and stabilising bases are scarce, H2SO4 can evaporate from particles; however the H2SO4 vapour pressure at low RH is uncertain. To address this, we measured H2SO4 evaporation versus T and RH in the CLOUD chamber and constrained the equilibrium constants for dissociation and dehydration of H2SO4. This study is important for nucleation, particle growth and H2SO4 formation occurring in atmosphere.
Carlo Bozzetti, Imad El Haddad, Dalia Salameh, Kaspar Rudolf Daellenbach, Paola Fermo, Raquel Gonzalez, María Cruz Minguillón, Yoshiteru Iinuma, Laurent Poulain, Miriam Elser, Emanuel Müller, Jay Gates Slowik, Jean-Luc Jaffrezo, Urs Baltensperger, Nicolas Marchand, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 17, 8247–8268, https://doi.org/10.5194/acp-17-8247-2017, https://doi.org/10.5194/acp-17-8247-2017, 2017
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We present the first long-term organic aerosol source apportionment in an environment influenced by anthropogenic emissions including biomass burning and industrial processes and an active photochemistry. Online and offline aerosol mass spectrometry were used to characterize these emissions and their transformation. Measurements of organic markers provided insights into the origin of biomass smoke in this area, with different seasonal contributions from domestic heating and agricultural burning.
Sebnem Aksoyoglu, Giancarlo Ciarelli, Imad El-Haddad, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 7757–7773, https://doi.org/10.5194/acp-17-7757-2017, https://doi.org/10.5194/acp-17-7757-2017, 2017
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Sources of inorganic aerosols in Europe were investigated using a regional air quality model. Results of this study suggested that biogenic volatile organic coumpounds emitted from vegetation had a significant effect on inorganic aerosols, especially on ammonium nitrate concentrations. Sensitivity analyses showed that it is mainly terpene reactions with nitrate radical at night that lead to a decrease in ammonium nitrate.
David O. Topping, James Allan, M. Rami Alfarra, and Bernard Aumont
Geosci. Model Dev., 10, 2365–2377, https://doi.org/10.5194/gmd-10-2365-2017, https://doi.org/10.5194/gmd-10-2365-2017, 2017
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Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA) formation is thought to be hampered by the complexity of the system. In this proof of concept study, the ability to train supervised methods to predict electron impact ionisation (EI) mass spectra for the AMS is evaluated to facilitate improved model evaluation. The study demonstrates the use of a methodology that would be improved with more training data and data from simple mixed systems.
Giancarlo Ciarelli, Imad El Haddad, Emily Bruns, Sebnem Aksoyoglu, Ottmar Möhler, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 10, 2303–2320, https://doi.org/10.5194/gmd-10-2303-2017, https://doi.org/10.5194/gmd-10-2303-2017, 2017
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In Europe, residential wood-burning emissions constitute one of the main anthropogenic sources of air pollution. Novel wood-burning experiments performed in a state-of-the-art smog chamber provide valuable information on the chemical properties of wood-burning emissions and the transformation in the atmosphere. In this study, these new data were used in a box model to constrain a parameterization suitable for predicting the contribution of wood burning to air pollution with large-scale models.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Imad El Haddad, Emily A. Bruns, Monica Crippa, Laurent Poulain, Mikko Äijälä, Samara Carbone, Evelyn Freney, Colin O'Dowd, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 7653–7669, https://doi.org/10.5194/acp-17-7653-2017, https://doi.org/10.5194/acp-17-7653-2017, 2017
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Organic aerosol (OA) comprises the main fraction of fine particulate matter (PM1). Using a new VBS parameterization, we performed model-based source apportionment studies to assess the importance of different emission sources to the total OA loads in Europe during winter periods. Our results indicate that residential wood burning emissions represent the major source of OA, followed by non-residential emission sources (i.e. traffic and industries).
Markus Furger, María Cruz Minguillón, Varun Yadav, Jay G. Slowik, Christoph Hüglin, Roman Fröhlich, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Meas. Tech., 10, 2061–2076, https://doi.org/10.5194/amt-10-2061-2017, https://doi.org/10.5194/amt-10-2061-2017, 2017
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An Xact 625 Ambient Metals Monitor was tested during a 3-week summer field campaign at a rural, traffic-influenced site in Switzerland. The objective was to characterize the operation of the instrument, evaluate the data quality by intercomparison with other independent measurements, and test its applicability for aerosol source quantification. The results demonstrate significant advantages compared to traditional elemental analysis methods, with some desirable improvements.
Lisa Stirnweis, Claudia Marcolli, Josef Dommen, Peter Barmet, Carla Frege, Stephen M. Platt, Emily A. Bruns, Manuel Krapf, Jay G. Slowik, Robert Wolf, Andre S. H. Prévôt, Urs Baltensperger, and Imad El-Haddad
Atmos. Chem. Phys., 17, 5035–5061, https://doi.org/10.5194/acp-17-5035-2017, https://doi.org/10.5194/acp-17-5035-2017, 2017
Peter Zotter, Hanna Herich, Martin Gysel, Imad El-Haddad, Yanlin Zhang, Griša Močnik, Christoph Hüglin, Urs Baltensperger, Sönke Szidat, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 4229–4249, https://doi.org/10.5194/acp-17-4229-2017, https://doi.org/10.5194/acp-17-4229-2017, 2017
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Most studies use a single Ångström exponent for wood burning (αWB) and traffic (αTR) emissions in the Aethalometer model, used for source apportionment of black carbon, derived from previous work. However, accurate determination of the α values is currently lacking. Comparing radiocarbon measurements (14C) with the Aehtalometer model, good agreement was found, indicating that the Aethalometer model reproduces reasonably well the 14C results using our best estimate of a single αWB and αTR.
Andelija Milic, Marc D. Mallet, Luke T. Cravigan, Joel Alroe, Zoran D. Ristovski, Paul Selleck, Sarah J. Lawson, Jason Ward, Maximilien J. Desservettaz, Clare Paton-Walsh, Leah R. Williams, Melita D. Keywood, and Branka Miljevic
Atmos. Chem. Phys., 17, 3945–3961, https://doi.org/10.5194/acp-17-3945-2017, https://doi.org/10.5194/acp-17-3945-2017, 2017
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This study reports chemical characterization of fresh and processed aerosols sampled over a month-long field campaign, during the intense fire period in Australian tropical savannah region. The study illustrates diversity in fire emissions and importance of processed fire emissions and formation of secondary species, including biogenic secondary species, in northern Australia.
Luka Drinovec, Asta Gregorič, Peter Zotter, Robert Wolf, Emily Anne Bruns, André S. H. Prévôt, Jean-Eudes Petit, Olivier Favez, Jean Sciare, Ian J. Arnold, Rajan K. Chakrabarty, Hans Moosmüller, Agnes Filep, and Griša Močnik
Atmos. Meas. Tech., 10, 1043–1059, https://doi.org/10.5194/amt-10-1043-2017, https://doi.org/10.5194/amt-10-1043-2017, 2017
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Black carbon measurements are usually conducted with absorption filter photometers, which are prone to the filter-loading effect – a saturation of the instrumental response due to the accumulation of the sample in the filter matrix. In this paper, we conducted several field campaigns to investigate the hypothesis that this filter-loading effect depends on the optical properties of particles present in the filter matrix, especially on the coating of black carbon particles.
Marc D. Mallet, Luke T. Cravigan, Andelija Milic, Joel Alroe, Zoran D. Ristovski, Jason Ward, Melita Keywood, Leah R. Williams, Paul Selleck, and Branka Miljevic
Atmos. Chem. Phys., 17, 3605–3617, https://doi.org/10.5194/acp-17-3605-2017, https://doi.org/10.5194/acp-17-3605-2017, 2017
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This paper presents data on the size, composition and concentration of aerosol particles emitted from north Australian savannah fires and how these properties influence cloud condensation nuclei (CCN) concentrations. Both the size and composition of aerosol were found to be important in determining CCN. Despite large CCNc enhancements during periods of close biomass burning, the aerosol was very weakly hygroscopic which should be accounted for in climate models to avoid large CCNc overestimates.
Carla Frege, Federico Bianchi, Ugo Molteni, Jasmin Tröstl, Heikki Junninen, Stephan Henne, Mikko Sipilä, Erik Herrmann, Michel J. Rossi, Markku Kulmala, Christopher R. Hoyle, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 17, 2613–2629, https://doi.org/10.5194/acp-17-2613-2017, https://doi.org/10.5194/acp-17-2613-2017, 2017
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We present measurements of the chemical composition of atmospheric ions at high altitude (3450 m a.s.l.) during a 9-month campaign. We detected remarkably high correlation between methanesulfonic acid (MSA) and SO5−. Halogenated species were also detected frequently at this continental location. New-particle formation events occurred via the condensation of highly oxygenated molecules (HOMs) at very low sulfuric acid concentration or, less frequently, due to ammonia–sulfuric acid clusters.
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.
Emily A. Bruns, Jay G. Slowik, Imad El Haddad, Dogushan Kilic, Felix Klein, Josef Dommen, Brice Temime-Roussel, Nicolas Marchand, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 705–720, https://doi.org/10.5194/acp-17-705-2017, https://doi.org/10.5194/acp-17-705-2017, 2017
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We characterize primary and aged gaseous emissions from residential wood combustion using proton transfer reaction time-of-flight mass spectrometry. This approach allows for improved characterization, particularly of oxygenated gases, which are a considerable fraction of the total gaseous mass emitted during residential wood combustion. This study is the first thorough characterization of organic gases from this source and provides a benchmark for future studies.
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
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107, https://doi.org/10.5194/amt-10-83-2017, https://doi.org/10.5194/amt-10-83-2017, 2017
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The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
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.
Carlo Bozzetti, Yuliya Sosedova, Mao Xiao, Kaspar R. Daellenbach, Vidmantas Ulevicius, Vadimas Dudoitis, Genrik Mordas, Steigvilė Byčenkienė, Kristina Plauškaitė, Athanasia Vlachou, Benjamin Golly, Benjamin Chazeau, Jean-Luc Besombes, Urs Baltensperger, Jean-Luc Jaffrezo, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 117–141, https://doi.org/10.5194/acp-17-117-2017, https://doi.org/10.5194/acp-17-117-2017, 2017
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In this study we present the offline-AMS source apportionment of the submicron organic aerosol (OA) sources conducted over 1 year at three locations in the south east Baltic region, which has so far received small attention. Offline-AMS enabled broadening the AMS spatial and temporal coverage, and provided a full characterization of the OA sources. Source apportionment results revealed that biomass burning and biogenic secondary emissions were the major OA sources during winter and summer.
Ernesto Reyes-Villegas, David C. Green, Max Priestman, Francesco Canonaco, Hugh Coe, André S. H. Prévôt, and James D. Allan
Atmos. Chem. Phys., 16, 15545–15559, https://doi.org/10.5194/acp-16-15545-2016, https://doi.org/10.5194/acp-16-15545-2016, 2016
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For the first time in the UK, an Aerosol Chemical Speciation Monitor was used to measure aerosol concentrations in London in March–December 2013, with further organic aerosol (OA) source apportionment using the ME-2 factorization tool. Five OA sources were identified: biomass burning OA, hydrocarbon-like OA, cooking OA, semivolatile oxygenated OA and low-volatility oxygenated OA. This information can be used to take future action on the respective legislation in order to improve the air quality.
Nicholas Marsden, Michael J. Flynn, Jonathan W. Taylor, James D. Allan, and Hugh Coe
Atmos. Meas. Tech., 9, 6051–6068, https://doi.org/10.5194/amt-9-6051-2016, https://doi.org/10.5194/amt-9-6051-2016, 2016
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
Gillian Young, Hazel M. Jones, Thomas W. Choularton, Jonathan Crosier, Keith N. Bower, Martin W. Gallagher, Rhiannon S. Davies, Ian A. Renfrew, Andrew D. Elvidge, Eoghan Darbyshire, Franco Marenco, Philip R. A. Brown, Hugo M. A. Ricketts, Paul J. Connolly, Gary Lloyd, Paul I. Williams, James D. Allan, Jonathan W. Taylor, Dantong Liu, and Michael J. Flynn
Atmos. Chem. Phys., 16, 13945–13967, https://doi.org/10.5194/acp-16-13945-2016, https://doi.org/10.5194/acp-16-13945-2016, 2016
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Clouds are intricately coupled to the Arctic sea ice. Our inability to accurately model cloud fractions causes large uncertainties in predicted radiative interactions in this region, therefore, affecting sea ice forecasts. Here, we present measurements of cloud microphysics, aerosol properties, and thermodynamic structure over the transition from sea ice to ocean to improve our understanding of the relationship between the Arctic atmosphere and clouds which develop in this region.
Riinu Ots, Massimo Vieno, James D. Allan, Stefan Reis, Eiko Nemitz, Dominique E. Young, Hugh Coe, Chiara Di Marco, Anais Detournay, Ian A. Mackenzie, David C. Green, and Mathew R. Heal
Atmos. Chem. Phys., 16, 13773–13789, https://doi.org/10.5194/acp-16-13773-2016, https://doi.org/10.5194/acp-16-13773-2016, 2016
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Emissions of cooking organic aerosol (COA; from charbroiling, frying, etc.) are currently absent in European emissions inventories yet measurements have pointed to significant COA concentrations. In this study, emissions of COA were developed for the UK by model iteration against year-long measurements at two sites in London. Modelled COA dropped rapidly outside of major urban areas, suggesting that although a notable component in UK urban air, COA does not have a significant effect on rural PM.
Francis P. H. Wragg, Stephen J. Fuller, Ray Freshwater, David C. Green, Frank J. Kelly, and Markus Kalberer
Atmos. Meas. Tech., 9, 4891–4900, https://doi.org/10.5194/amt-9-4891-2016, https://doi.org/10.5194/amt-9-4891-2016, 2016
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A new portable, online instrument was designed, built and characterised to quantify reactive oxygen species (ROS) in atmospheric aerosols for laboratory and field deployment. ROS are potentially major contributors to the toxicity of particles. Our new instrument allows automated quantification of ROS over days with a detection limit of about 4 nmol [H2O2] equivalents per cubic metre of air, allowing for continuous atmospheric measurements of this important aerosol toxicity parameter.
Luke D. Schiferl, Colette L. Heald, Martin Van Damme, Lieven Clarisse, Cathy Clerbaux, Pierre-François Coheur, John B. Nowak, J. Andrew Neuman, Scott C. Herndon, Joseph R. Roscioli, and Scott J. Eilerman
Atmos. Chem. Phys., 16, 12305–12328, https://doi.org/10.5194/acp-