Articles | Volume 21, issue 22
https://doi.org/10.5194/acp-21-17115-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-17115-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
25 Nov 2021
Research article |
| 25 Nov 2021
| 25 Nov 2021
Changes in PM2.5 concentrations and their sources in the US from 1990 to 2010
Ksakousti Skyllakou
Institute of Chemical Engineering Sciences (FORTH/ICE-HT), 26504,
Patras, Greece
Pablo Garcia Rivera
Department of Chemical Engineering, Carnegie Mellon University,
Pittsburgh, PA 15213, USA
Brian Dinkelacker
Department of Chemical Engineering, Carnegie Mellon University,
Pittsburgh, PA 15213, USA
Eleni Karnezi
Department of Chemical Engineering, Carnegie Mellon University,
Pittsburgh, PA 15213, USA
Earth Sciences, Barcelona Supercomputing Center, 08034, Barcelona, Spain
Ioannis Kioutsioukis
Department of Physics, University of Patras, 26500, Patras, Greece
Carlos Hernandez
Department of Civil and Environmental Engineering, Carnegie Mellon
University, Pittsburgh, PA 15213, USA
Peter J. Adams
Department of Civil and Environmental Engineering, Carnegie Mellon
University, Pittsburgh, PA 15213, USA
Spyros N. Pandis
CORRESPONDING AUTHOR
Institute of Chemical Engineering Sciences (FORTH/ICE-HT), 26504,
Patras, Greece
Department of Chemical Engineering, University of Patras, 26500,
Patras, Greece
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Brian T. Dinkelacker, Pablo Garcia Rivera, Ksakousti Skyllakou, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-648, https://doi.org/10.5194/acp-2022-648, 2022
Revised manuscript not accepted
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A number of factors have influenced the biogenic secondary organic aerosol (SOA) levels in the southeastern US from 2001 to 2010. The increases in temperature have led to an increase of the emissions of biogenic volatile organic compounds by trees and a corresponding increase of the SOA. However, this increase has been balanced by the reductions in the anthropogenic emissions of organic gases and particulate matter as well as of the oxides of nitrogen keeping the biogenic SOA roughly constant.
Anna Maria Neroladaki, Maria Tsagkaraki, Kyriaki Papoutsidaki, Kalliopi Tavernaraki, Filothei Boufidou, Pavlos Zarmpas, Irini Tsiodra, Eleni Liakakou, Aikaterini Bougiatioti, Giorgos Kouvarakis, Nikos Kalivitis, Christos Kaltsonoudis, Athanasios Karagioras, Dimitrios Balis, Konstantinos Mihailidis, Konstantinos Kourtidis, Stelios Myriokefalitakis, Nikos Hatzianastassiou, Spyros N. Pandis, Athanasios Nenes, Nikolaos Mihalopoulos, and Maria Kanakidou
EGUsphere, https://doi.org/10.5194/egusphere-2025-3223, https://doi.org/10.5194/egusphere-2025-3223, 2025
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Aerosol acidity affects aerosol composition and properties, and therefore climate, human health and ecosystems. We use summer and winter fine aerosol observations at 6 sites across Greece, and a thermodynamic model to calculate the spatial and seasonal variability of aerosol acidity. Aerosols were acidic to moderately acidic and more acidic during summer than winter. The importance of organics for aerosol acidity was small. Depending on location different factors controlled aerosol acidity.
Susanne M. C. Scholz, Vlassis A. Karydis, Georgios I. Gkatzelis, Hendrik Fuchs, Spyros N. Pandis, and Alexandra P. Tsimpidi
EGUsphere, https://doi.org/10.5194/egusphere-2025-2510, https://doi.org/10.5194/egusphere-2025-2510, 2025
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We studied how pollution from cars and trucks contributes to tiny airborne particles that affect air quality and climate. These particles, called secondary organic aerosols, were often underestimated in global models. By improving how certain overlooked emissions from fuel use are represented in our model, we found that their impact is much larger than previously thought. Our results suggest that road traffic plays a far greater role in global air pollution than earlier estimates showed.
Maria P. Georgopoulou, Kalliopi Florou, Angeliki Matrali, Georgia Starida, Christos Kaltsonoudis, Athanasios Nenes, and Spyros N. Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2025-2728, https://doi.org/10.5194/egusphere-2025-2728, 2025
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Residential biomass burning is an important wintertime source of aerosols. This study examined the complex diurnal aging cycles on biomass burning aerosol composition and oxidative potential, a key toxicity metric. Additional organic aerosol (OA) mass was produced after the two (day/night and night/day) cycles, varying from 35 to 90 % of the initial OA. The aging of the emissions led to a final oxidative potential increase of 60 % for both cycles.
Georgia A. Argyropoulou, Kalliopi Florou, and Spyros N. Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2025-1147, https://doi.org/10.5194/egusphere-2025-1147, 2025
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Ultrafine particles (diameter less than 100 nm) are suspected to cause significant health effects. Accurately measuring their chemical composition and physical properties in real-time is challenging due to their low mass and interference from larger particles. This study proposes a method for the continuous, automated measurement of their composition, tested in a pilot field study to explore their chemical characteristics, physical properties, and sources.
Ioannis Kioutsioukis, Christian Hogrefe, Paul A. Makar, Ummugulsun Alyuz, Jessy O. Bash, Roberto Bellasio, Roberto Bianconi, Tim Buttler, Olivia E. Clifton, Philippe Cheung, Alma Hodzic, Richard Kranenburg, Aurelia Lupascu, Kester Momoh, Juan Luis Perez-Camaño, John Pleim, Young-Hee Ryu, Robero San Jose, Donna Schwede, Ranjeet Sokhi, and Stefano Galmarini
EGUsphere, https://doi.org/10.5194/egusphere-2025-1091, https://doi.org/10.5194/egusphere-2025-1091, 2025
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Deposition is a key in air quality modelling. An evaluation of the AQMEII4 models is performed prior to analysing the different deposition schemes in relation to the LULC used. Such analysis is unprecedented. Among the results, LULC masks have to be harmonised and up-to-date information used in place of outdated and too course masks. Alternatively LULC masks should be evaluated and intercom pared when multiple model results are analysed.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark W. Shephard, Ranjeet S. Sokhi, and Stefano Galmarini
Atmos. Chem. Phys., 25, 3049–3107, https://doi.org/10.5194/acp-25-3049-2025, https://doi.org/10.5194/acp-25-3049-2025, 2025
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The large range of sulfur and nitrogen deposition estimates from air quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulfur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by hydrometeors, aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, gas deposition via plant cuticles and soil, and land use data.
David Patoulias, Kalliopi Florou, and Spyros N. Pandis
Geosci. Model Dev., 18, 1103–1118, https://doi.org/10.5194/gmd-18-1103-2025, https://doi.org/10.5194/gmd-18-1103-2025, 2025
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The effect of the assumed atmospheric nucleation mechanism on particle number concentrations and size distribution was investigated. Two quite different mechanisms involving sulfuric acid and ammonia or a biogenic organic vapor gave quite similar results which were consistent with measurements at 26 measurement stations across Europe. The number of larger particles that serve as cloud condensation nuclei showed little sensitivity to the assumed nucleation mechanism.
Christian Hogrefe, Stefano Galmarini, Paul A. Makar, Ioannis Kioutsioukis, Olivia E. Clifton, Ummugulsum Alyuz, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Tim Butler, Philip Cheung, Alma Hodzic, Richard Kranenburg, Aurelia Lupascu, Kester Momoh, Juan Luis Perez-Camanyo, Jonathan E. Pleim, Young-Hee Ryu, Roberto San Jose, Martijn Schaap, Donna B. Schwede, and Ranjeet Sokhi
EGUsphere, https://doi.org/10.5194/egusphere-2025-225, https://doi.org/10.5194/egusphere-2025-225, 2025
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Performed under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in regional-scale models. The results also strongly suggest that improvement and harmonization of the representation of land use in these models would serve the community in their future development efforts.
Andreas Aktypis, Dontavious J. Sippial, Christina N. Vasilakopoulou, Angeliki Matrali, Christos Kaltsonoudis, Andrea Simonati, Marco Paglione, Matteo Rinaldi, Stefano Decesari, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 13769–13791, https://doi.org/10.5194/acp-24-13769-2024, https://doi.org/10.5194/acp-24-13769-2024, 2024
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A dual-chamber system was deployed in two different environments (Po Valley, Italy, and Pertouli forest, Greece) to study the potential of ambient air directly injected into the chambers, to form secondary organic aerosol (SOA). In the Po Valley, the system reacts rapidly, forming large amounts of SOA, while in Pertouli the SOA formation chemistry appears to have been practically terminated before the beginning of most experiments, so there is little additional SOA formation potential left.
Konstantinos Mataras, Evangelia Siouti, David Patoulias, and Spyros Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2024-3357, https://doi.org/10.5194/egusphere-2024-3357, 2024
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Predicted levels of ultrafine particle mass (PM0.1) vary substantially over Europe with higher values in the summer than in the winter. In summer, PM0.1 was mostly comprised of sulfate (38 %) and secondary organics (32 %). During winter the sulfate fraction increased to 47 % and primary organics contributed 23 %. Correlations between PM0.1 and the regulated PM2.5 were low. This suggests that there are significant differences between the dominant sources and processes of PM0.1 and PM2.5.
Romanos Foskinis, Ghislain Motos, Maria I. Gini, Olga Zografou, Kunfeng Gao, Stergios Vratolis, Konstantinos Granakis, Ville Vakkari, Kalliopi Violaki, Andreas Aktypis, Christos Kaltsonoudis, Zongbo Shi, Mika Komppula, Spyros N. Pandis, Konstantinos Eleftheriadis, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9827–9842, https://doi.org/10.5194/acp-24-9827-2024, https://doi.org/10.5194/acp-24-9827-2024, 2024
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Analysis of modeling, in situ, and remote sensing measurements reveals the microphysical state of orographic clouds and their response to aerosol from the boundary layer and free troposphere. We show that cloud response to aerosol is robust, as predicted supersaturation and cloud droplet number levels agree with those determined from in-cloud measurements. The ability to determine if clouds are velocity- or aerosol-limited allows for novel model constraints and remote sensing products.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Olga Zografou, Christos Kaltsonoudis, Maria Gini, Angeliki Matrali, Elias Panagiotopoulos, Alexandros Lekkas, Dimitris Papanastasiou, Spyros N. Pandis, and Konstantinos Eleftheriadis
EGUsphere, https://doi.org/10.5194/egusphere-2024-2126, https://doi.org/10.5194/egusphere-2024-2126, 2024
Preprint archived
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A novel charge transfer ionization orthogonal Time-of-Flight Mass Spectrometer (oToF-MS) was field evaluated for the first time during a field campaign at the suburban DEM station in Athens, Greece from May to August 2023 focusing on key ambient Volatile Organic Compounds (VOCs). The results demonstrate the strengths of the new instrument in performing online, real time measurements of ambient VOCs.
Alexandros Milousis, Alexandra P. Tsimpidi, Holger Tost, Spyros N. Pandis, Athanasios Nenes, Astrid Kiendler-Scharr, and Vlassis A. Karydis
Geosci. Model Dev., 17, 1111–1131, https://doi.org/10.5194/gmd-17-1111-2024, https://doi.org/10.5194/gmd-17-1111-2024, 2024
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This study aims to evaluate the newly developed ISORROPIA-lite aerosol thermodynamic module within the EMAC model and explore discrepancies in global atmospheric simulations of aerosol composition and acidity by utilizing different aerosol phase states. Even though local differences were found in regions where the RH ranged from 20 % to 60 %, on a global scale the results are similar. Therefore, ISORROPIA-lite can be a reliable and computationally effective alternative to ISORROPIA II in EMAC.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Andreas Aktypis, Christos Kaltsonoudis, David Patoulias, Panayiotis Kalkavouras, Angeliki Matrali, Christina N. Vasilakopoulou, Evangelia Kostenidou, Kalliopi Florou, Nikos Kalivitis, Aikaterini Bougiatioti, Konstantinos Eleftheriadis, Stergios Vratolis, Maria I. Gini, Athanasios Kouras, Constantini Samara, Mihalis Lazaridis, Sofia-Eirini Chatoutsidou, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 65–84, https://doi.org/10.5194/acp-24-65-2024, https://doi.org/10.5194/acp-24-65-2024, 2024
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Extensive continuous particle number size distribution measurements took place during two summers (2020 and 2021) at 11 sites in Greece for the investigation of the frequency and the spatial extent of new particle formation. The frequency during summer varied from close to zero in southwestern Greece to more than 60 % in the northern, central, and eastern regions. The spatial variability can be explained by the proximity of the sites to coal-fired power plants and agricultural areas.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Petro Uruci, Dontavious Sippial, Anthoula Drosatou, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 3155–3172, https://doi.org/10.5194/amt-16-3155-2023, https://doi.org/10.5194/amt-16-3155-2023, 2023
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In this work we develop an algorithm for the synthesis of the measurements performed in atmospheric simulation chambers regarding the formation of secondary organic aerosol (SOA). Novel features of the algorithm are its ability to use measurements of SOA yields, thermodenuders, and isothermal dilution; its estimation of parameters that can be used directly in atmospheric chemical transport models; and finally its estimates of the uncertainty in SOA formation yields.
Christina N. Vasilakopoulou, Kalliopi Florou, Christos Kaltsonoudis, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 2837–2850, https://doi.org/10.5194/amt-16-2837-2023, https://doi.org/10.5194/amt-16-2837-2023, 2023
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The offline aerosol mass spectrometry technique is a useful tool for the source apportionment of organic aerosol in areas and periods during which an aerosol mass spectrometer is not available. In this work, an improved offline technique was developed and evaluated in an effort to capture most of the partially soluble and insoluble organic aerosol material, reducing the uncertainty of the corresponding source apportionment significantly.
Iason Markantonis, Diamando Vlachogiannis, Athanasios Sfetsos, Ioannis Kioutsioukis, and Nadia Politi
Adv. Sci. Res., 19, 145–158, https://doi.org/10.5194/asr-19-145-2023, https://doi.org/10.5194/asr-19-145-2023, 2023
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This paper examines the simulataneous exceedance of daily accumulated precipitation (RR) and minimum (TN) temperature thresholds in Greece for the period 1980–2004 and for each month in the period November to April. Available data from observations and projection simulations are used to calculate the probabilities of extreme wet-cold compound events at the past. Models are validated by the observational data.
Spiro D. Jorga, Kalliopi Florou, David Patoulias, and Spyros N. Pandis
Atmos. Chem. Phys., 23, 85–97, https://doi.org/10.5194/acp-23-85-2023, https://doi.org/10.5194/acp-23-85-2023, 2023
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We take advantage of this unexpected low, new particle formation frequency in Greece and use a dual atmospheric simulation chamber system with starting point ambient air in an effort to gain insight about the chemical species that is limiting nucleation in this area. A potential nucleation precursor, ammonia, was added in one of the chambers while the other one was used as a reference. The addition of ammonia assisted new particle formation in almost 50 % of the experiments conducted.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Geosci. Model Dev., 15, 8899–8912, https://doi.org/10.5194/gmd-15-8899-2022, https://doi.org/10.5194/gmd-15-8899-2022, 2022
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The performance of a chemical transport model in reproducing PM2.5 concentrations and composition was evaluated at the finest scale using measurements from regulatory sites as well as a network of low-cost monitors. Total PM2.5 mass is reproduced well by the model during the winter when compared to regulatory measurements, but in the summer PM2.5 is underpredicted, mainly due to difficulties in reproducing regional secondary organic aerosol levels.
Christina Vasilakopoulou, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 15, 6419–6431, https://doi.org/10.5194/amt-15-6419-2022, https://doi.org/10.5194/amt-15-6419-2022, 2022
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Offline aerosol mass spectrometer (AMS) measurements can provide valuable information about ambient organic aerosols when online AMS measurements are not available. In this study, we examine whether and how the low time resolution (usually 24 h) of the offline technique affects source apportionment results. We concluded that use of the daily averages resulted in estimated average contributions that were within 8 % of the total OA compared with the high-resolution analysis.
Iason Markantonis, Diamando Vlachogiannis, Athanasios Sfetsos, and Ioannis Kioutsioukis
Earth Syst. Dynam., 13, 1491–1504, https://doi.org/10.5194/esd-13-1491-2022, https://doi.org/10.5194/esd-13-1491-2022, 2022
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This work focuses on the study of daily wet–cold compound events in Greece in the period November–April. We firstly study the historic period 1980–2004 in which we validate projection models with observations. Then we compare the model results with future period 2025–2049 RCP4.5 and RCP8.5 scenarios. The aim of the study is to calculate the probability of the events and to locate the areas where those are higher and how the probabilities will change at the future.
Stella E. I. Manavi and Spyros N. Pandis
Geosci. Model Dev., 15, 7731–7749, https://doi.org/10.5194/gmd-15-7731-2022, https://doi.org/10.5194/gmd-15-7731-2022, 2022
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The paper describes the first step towards the development of a simulation framework for the chemistry and secondary organic aerosol production of intermediate-volatility organic compounds (IVOCs). These compounds can be a significant source of organic particulate matter. Our approach treats IVOCs as lumped compounds that retain their chemical characteristics. Estimated IVOC emissions from road transport were a factor of 8 higher than emissions used in previous applications.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ksakousti Skyllakou, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-648, https://doi.org/10.5194/acp-2022-648, 2022
Revised manuscript not accepted
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A number of factors have influenced the biogenic secondary organic aerosol (SOA) levels in the southeastern US from 2001 to 2010. The increases in temperature have led to an increase of the emissions of biogenic volatile organic compounds by trees and a corresponding increase of the SOA. However, this increase has been balanced by the reductions in the anthropogenic emissions of organic gases and particulate matter as well as of the oxides of nitrogen keeping the biogenic SOA roughly constant.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
David Patoulias and Spyros N. Pandis
Atmos. Chem. Phys., 22, 1689–1706, https://doi.org/10.5194/acp-22-1689-2022, https://doi.org/10.5194/acp-22-1689-2022, 2022
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Our simulations indicate that the recently identified production and subsequent condensation effect of extremely low-volatility organic compounds have a smaller-than-expected effect on the total concentration of atmospheric particles. On the other hand, the oxidation of intermediate-volatility organic compounds leads to decreases in the ultrafine-particle concentrations. These results improve our understanding of the links between secondary organic aerosol formation and ultrafine particles.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 1131–1148, https://doi.org/10.5194/acp-22-1131-2022, https://doi.org/10.5194/acp-22-1131-2022, 2022
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An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory, and regional modeling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm particles.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Georgia N. Theodoritsi, Giancarlo Ciarelli, and Spyros N. Pandis
Geosci. Model Dev., 14, 2041–2055, https://doi.org/10.5194/gmd-14-2041-2021, https://doi.org/10.5194/gmd-14-2041-2021, 2021
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Two schemes based on the volatility basis set were used for the simulation of biomass burning organic aerosol (bbOA) in the continental US. The first is the default scheme of the PMCAMx-SR model, and the second is a recently developed scheme based on laboratory experiments. The alternative bbOA scheme predicts much higher concentrations. The default scheme performed better during summer and fall, while the alternative scheme was a little better during spring.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Dana L. McGuffin, Yuanlong Huang, Richard C. Flagan, Tuukka Petäjä, B. Erik Ydstie, and Peter J. Adams
Geosci. Model Dev., 14, 1821–1839, https://doi.org/10.5194/gmd-14-1821-2021, https://doi.org/10.5194/gmd-14-1821-2021, 2021
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Atmospheric particle formation, emissions, and growth process rates are significant sources of uncertainty in predicting climate change. We aim to reduce that uncertainty by using measurements from several ground-based sites across Europe. We developed an estimation technique to adapt the governing process rates so model–measurement bias decays. The estimation framework developed has potential to improve model predictions while providing insight into the underlying atmospheric particle physics.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Antonios Tasoglou, Evangelos Louvaris, Kalliopi Florou, Aikaterini Liangou, Eleni Karnezi, Christos Kaltsonoudis, Ningxin Wang, and Spyros N. Pandis
Atmos. Chem. Phys., 20, 11625–11637, https://doi.org/10.5194/acp-20-11625-2020, https://doi.org/10.5194/acp-20-11625-2020, 2020
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A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption. The measured light absorption was two or more times higher than that of fresh black carbon. The absorption enhancement due to the coating of black carbon cores by other aerosol components could explain only part of this absorption enhancement. The rest was due to brown carbon, mostly in the form of extremely low volatility organic compounds.
Cited articles
Beckerman, B. S., Jerrett, M., Serre, M., Martin, R. V., Lee, S.-J., van
Donkelaar, A., Ross, Z., Su, J., and Burnett, R. T.: A hybrid approach to
estimating national scale spatiotemporal variability of PM2.5 in the
contiguous United States, Environ. Sci. Technol., 47, 7233–7241, 2013.
Donahue, N. M., Robinson, A. L., Stanier, C. O., and Pandis, S. N.: Coupled
partitioning, dilution, and chemical aging of semivolatile organics,
Environ. Sci. Technol., 40, 2635–2643, 2006.
Eeftens, M., Beelen, R., de Hoogh, K., Bellander, T., Cesaroni, G., Cirach,
M., Declercq, C., Delele, A., Dons, E., and de Nazelle, A.: Development of land
use regression models for PM2.5 absorbance, PM10 and PMCoarse
in 20 European study areas, results of the ESCAPE Project, Environ. Sci.
Technol., 46, 11195–11205, 2012.
Emery, C., Liu, Z., Russell, A. G., Odman, M. T., Yarwood, G., and Kumar,
N.: Recommendations on statistics and benchmarks to assess photochemical
model performance, J. Air Waste Manage., 67, 582–598, 2017.
Environ: Comprehensive Air Quality Model with Extensions Version 4.40, Users
Guide, ENVIRON Int. Corp., Novato, CA, available at: http://www.camx.com (last access: November 2020), 2006.
Fountoukis, C., Racherla, P. N., Denier van der Gon, H. A. C., Polymeneas, P., Charalampidis, P. E., Pilinis, C., Wiedensohler, A., Dall'Osto, M., O'Dowd, C., and Pandis, S. N.: Evaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign, Atmos. Chem. Phys., 11, 10331–10347, https://doi.org/10.5194/acp-11-10331-2011, 2011.
Gan, C.-M., Hogrefe, C., Mathur, R., Pleim, J., Xing, J., Wong, D., Gilliam,
R., Pouliot, G., and Wei, C.: Assessment of the effects of horizontal grid
resolution on long-term air quality trends using coupled WRF-CMAQ
simulations, Atmos. Environ., 132, 207–216, 2016.
Gilliam, R. C. and Pleim, J. E.: Performance assessment of new land surface and
planetary boundary layer physics in the WRF-ARW, J. Appl.
Meteorol. Clim., 49, 760–774, 2010.
Hogrefe, C., Pouliot, G., Wong, D., Torian, A., Roselle, S., Pleim, J.,
Mathur, R.: Annual application and evaluation of the online coupled WRF-CMAQ
system over North America under AQMEII phase 2, Atmos. Environ., 115,
683–694, 2015.
Iacono, M. J., Delamere, J. S., Mlawer, E. J., Shephard, M. W., Clough, S. A., and
Collins, W. D.: Radiative forcing by long-lived greenhouse gases:
Calculations with the AER radiative transfer models, J. Geophys. Res., 113,
2–9, 2008.
IMPROVE: IMPROVE Data Guide. Univ. of California, Davis, available at:
https://vista.cira.colostate.edu/improve/Publications/OtherDocs/IMPROVEDataGuide/IMPROVEDataGuide.htm (last access: September 2020),
1995.
Jiang, X., Guenther, A., Potosnak, M., Geron, C., Seco, R., Karl, T., Kim,
S., Gu, L., and Pallardy, S.: Isoprene emission response to drought and the
impact on global atmospheric chemistry, Atmos. Environ., 183, 69–83, 2018.
Jin, X., Fiore A. M., Civerolo, K., Bi, J., Liu, Y., Donkelaar, A., Martin,
R. V., Al-Hamdan, M., Zhang, Y., Insaf, T. Z., Kioumourtzoglou, M., He, M.
Z., and Kinney, P. L.: Comparison of multiple PM2.5 exposure products
for estimating health benefits of emission controls over New York State,
USA, Environ. Res. Lett., 14, 084023, https://doi.org/10.1088/1748-9326/ab2dcb, 2019.
Kain, J. S.: The Kain–Fritsch convective parameterization: An update, J.
Appl. Meteorol., 43, 170–181, 2004.
Karamchandani, P., Vijayaraghavan, K., and Yarwood, G.: Sub-grid scale plume
modeling, Atmosphere, 2, 389–406, 2011.
Karydis, V. A., Tsimpidi, A. P., and Pandis, S. N.: Evaluation of a
three-dimensional chemical transport model (PMCAMx) in the eastern United
States for all four seasons, J. Geophys. Res., 112, D14211,
https://doi.org/10.1029/2006JD007890, 2007.
Karydis, V. A., Tsimpidi, A. P., Fountoukis, C., Nenes, A., Zavala, M., Lei,
W., Molina, L. T., and Pandis, S. N.: Simulating the fine and coarse inorganic
particulate matter concentrations in a polluted megacity, Atmos. Environ.,
44, 608–620, 2010.
Lane, T. E., Donahue, N. M., and Pandis, S. N.: Effect of NOx on secondary
organic aerosol concentrations, Environ. Sci. Technol., 42, 6022–6027,
2008.
Li, L., Wu, A. H., Cheng, I., Chen, J.-C., and Wu, J.: Spatiotemporal estimation
of historical PM2.5 concentrations using PM10 meteorological
variables, and spatial effect, Atmos. Environ., 166, 182–191, 2017a.
Li, C., Martin, R. V., van Donkelaar, A., Boys, B. L., Hammer, M. S., Xu,
J.-W., Marais, E. A., Reff, A., Strum, M., Ridley, D. A., Crippa, M.,
Brauer, M., and Zhang, Q.: Trends in chemical composition of global and regional
population-weighted fine particulate matter estimated for 25 years, Environ.
Sci. Technol., 51, 11185–11195, 2017b.
Ma, Z., Hu, X., Sayer, A. M., Levy, R., Zhang, Q., Xue, Y., Tong, S., Bi,
J., Huang, L., and Liu, Y.: Satellite-based spatiotemporal trends in PM2.5 concentrations: China, 2004–2013, Environ. Health Persp., 124,
184–192, 2016.
Meng, J., Li, C., Martin, R. V., van Donkelaar, A., Hystad, P., and Brauer,
M.: Estimated long-term (1981–2016) concentrations of ambient fine
particulate matter across North America from chemical transport modeling,
satellite remote sensing and ground-based measurements, Environ. Sci.
Technol., 53, 5071–5079, 2019.
Milando, C., Huang, L., and Batterman, S.: Trends in PM2.5 emissions,
concentrations and apportionments in Detroit and Chicago, Atmos. Environ.,
129, 197–209, 2016.
Morris, R. E., McNally, D. E., Tesche, T. W., Tonnesen, G., Boylan, J. W.,
and Brewer, P.: Preliminary Evaluation of the Community Multiscale Air
Quality Model for 2002 over the Southeastern United States, J. Air Waste
Manage., 55, 1694–1708, 2005.
Morrison, H., Thompson, G., and Tatarskii, V.: Impact of cloud microphysics on
the development of trailing stratiform precipitation in a simulated squall
line: Comparison of one- and two-moment schemes, Mon. Weather Rev.,
137, 991–1007, 2008.
Murphy, B. N. and Pandis, S. N.: Simulating the formation of semivolatile
primary and secondary organic aerosol in a regional chemical transport
model, Environ. Sci. Technol., 43, 4722–4728, 2009.
Murphy, B. N. and Pandis, S. N.: Exploring summertime organic aerosol formation
in the Eastern United States using a regional-scale budget approach and
ambient measurements, J. Geophys. Res., 115, D24216,
https://doi.org/10.1029/2010JD014418, 2010.
Murphy, S. L., Xu, J., and Kochanek, K. D.: Deaths: Final Data for 2010, Division of Vital Statistics National Vital Statistics Reports, 61, 4, 2013.
Nenes, A., Pandis, S. N., and Pilinis, C.: ISORROPIA: a new thermodynamic
equilibrium model for multiphase multicomponent inorganic aerosols, Aq.
Geochem., 4, 123–152, 1998.
Nopmongcol, U., Alvarez, Y., Jung, J., Grant, J., Kumar, N., and Yarwood,
G.: Source contributions to United States ozone and particulate matter over
five decades from 1970 to 2020, Atmos. Environ., 167, 116–128, 2017.
Pandis, S. N., Wexler, A. S., and Seinfeld, J. H.: Secondary organic aerosol
formation and transport – II. Predicting the ambient secondary organic
aerosol size distribution, Atmos. Environ., 27, 2403–2416, 1993.
Pleim, J. E.: A Combined local and nonlocal closure model for the
atmospheric boundary layer. Part I: Model description and testing, J. Appl. Meteorol. Clim., 46, 1383–1395, 2007a.
Pleim, J. E.: A combined local and nonlocal closure model for the
atmospheric boundary layer. Part II: Application and evaluation in a
mesoscale meteorological model, J. Appl. Meteorol. Clim.,
46, 1396–1409, 2007b.
Posner, L. N., Theodoritsi, G., Robinson, A., Yarwood, G., Koo, B., Morris,
R., Mavko, M., Moore, T., and Pandis, S. N.: Simulation of fresh and
chemically-aged biomass burning organic aerosol, Atmos. Environ., 196,
27–37, 2019.
Rogers, R. E., Deng, A., Stauffer, D. R., Gaudet, B. J., Jia, Y., Soong, S.
T., and Tanrikulu, S.: Application of the weather research and forecasting model
for air quality modeling in the San Francisco bay area, J. Appl.
Meteorol. Clim., 52, 1953–1973, 2013.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, 3rd
Edn., John Wiley and Sons, New Jersey, USA, 2016.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Skyllakou, K., Murphy, B. N., Megaritis, A. G., Fountoukis, C., and Pandis, S. N.: Contributions of local and regional sources to fine PM in the megacity of Paris, Atmos. Chem. Phys., 14, 2343–2352, https://doi.org/10.5194/acp-14-2343-2014, 2014.
Skyllakou, K., Fountoukis, C., Charalampidis, P., and Pandis, S. N.:
Volatility-resolved source apportionment of primary and secondary organic
aerosol over Europe, Atmos. Environ., 167, 1–10, 2017.
Tessum, C. W., Apte, J. S., Goodkind, A. L., Muller, N. Z., Mullins, K.
A., Paolella, D. A., Polasky, S., Springer, N. P., Thakrar, S. K.,
Marshall, J. D., and Hill, J. D.: Inequity in consumption of goods and
services adds to racial–ethnic disparities in air pollution exposure, P.
Natl. Acad. Sci. USA, 116, 6001–6006, 2019.
Tsimpidi, A. P., Karydis, V. A., Pandis, S. N.: Response of Inorganic Fine
Particulate Matter to Emission Changes of Sulfur Dioxide and Ammonia: The
Eastern United States as a Case Study, J. Air Waste Manage., 57,
1489–1498, 2007.
Tsimpidi, A. P., Karydis, V. A., Zavala, M., Lei, W., Molina, L., Ulbrich, I. M., Jimenez, J. L., and Pandis, S. N.: Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area, Atmos. Chem. Phys., 10, 525–546, https://doi.org/10.5194/acp-10-525-2010, 2010.
US Census Bureau: Population Estimates, available at: https://www.census.gov, last access: November 2020.
US EPA (U.S. Environmental Protection Agency): User Guide: Air Quality System,
Report, Research Triangle Park, N. C., available at:
https://www.epa.gov/ttn/airs/airsaqs/ manuals/AQSUserGuide.pdf (last access:
September 2020), 2002.
US EPA (U.S. Environmental Protection Agency): Benefits and Costs of the Clean Air
Act 1990–2020, Report Documents and Graphics, available at:
https://www.epa.gov/sites/default/files/2015-07/documents/summaryreport.pdf (last access: August 2021), 2011.
Wagstrom, K. M., Pandis, S. N., Yarwood, G., Wilson, G. M., and Morris, R. E.:
Development and application of a computationally efficient particulate
matter apportionment algorithm in a three-dimensional chemical transport
model, Atmos. Environ., 42, 5650–5659, 2008.
Wagstrom, K. M. and Pandis, S. N.: Source receptor relationships for fine
particulate matter concentrations in the Eastern United States, Atmos.
Environ., 45, 347–356, 2011a.
Wagstrom, K. M. and Pandis, S. N.: Contribution of long-range transport to
local fine particulate matter concerns, Atmos. Environ., 45, 2730–2735,
2011b.
Walker, S. E., Slordal, L. H., Guerreiro, C., Gram, F., and Gronskei, K. E.: Air
pollution exposure monitoring and estimation part II. Model evaluation and
population exposure, J. Environ. Monitor., 1, 321–326, 1999.
WHO: Air Quality Guidelines for Particulate Matter, Ozone, Nitrogen Dioxide
and Sulfur Dioxide, GLOBAL Update 2005, Summary of Risk Assessment, World
Health Organization (WHO/SDE/PHE/OEH/06.02), 2006.
Xing, J., Pleim, J., Mathur, R., Pouliot, G., Hogrefe, C., Gan, C.-M., and Wei, C.: Historical gaseous and primary aerosol emissions in the United States from 1990 to 2010, Atmos. Chem. Phys., 13, 7531–7549, https://doi.org/10.5194/acp-13-7531-2013, 2013.
Xiu, A. and Pleim, J. E.: Development of a land surface model. Part I:
Application in a Mesoscale Meteorological Model, J. Appl. Meteorol.,
40, 192–209, 2002.
Yarwood, G., Rao, S., Yocke, M., and Whitten, G. Z.: Updates to The Carbon Bond
Chemical Mechanism, Research Triangle Park, 2005.
Zakoura, M. and Pandis, S. N: Improving fine aerosol nitrate predictions
using a Plume-in-Grid modeling approach, Atmos. Environ., 215, 116887, https://doi.org/10.1016/j.atmosenv.2019.116887, 2019.
Short summary
Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The...
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