Articles | Volume 14, issue 17
https://doi.org/10.5194/acp-14-9051-2014
© Author(s) 2014. 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-14-9051-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
The contribution of fungal spores and bacteria to regional and global aerosol number and ice nucleation immersion freezing rates
D. V. Spracklen
School of Earth and Environment, University of Leeds, Leeds, UK
C. L. Heald
Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
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S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
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Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
D. V. Spracklen and R. Righelato
Biogeosciences, 11, 2741–2754, https://doi.org/10.5194/bg-11-2741-2014, https://doi.org/10.5194/bg-11-2741-2014, 2014
Kevin John Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose-Luis Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-857, https://doi.org/10.5194/acp-2022-857, 2023
Revised manuscript under review for ACP
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the Western US into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations, and will also directly inform atmospheric and climate models.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
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.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Ruud H. H. Janssen, Colette L. Heald, Allison L. Steiner, Anne E. Perring, J. Alex Huffman, Ellis S. Robinson, Cynthia H. Twohy, and Luke D. Ziemba
Atmos. Chem. Phys., 21, 4381–4401, https://doi.org/10.5194/acp-21-4381-2021, https://doi.org/10.5194/acp-21-4381-2021, 2021
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Bioaerosols are ubiquitous in the atmosphere and have the potential to affect cloud formation, as well as human and ecosystem health. However, their emissions are not well quantified, which hinders the assessment of their role in atmospheric processes. Here, we develop two new emission schemes for fungal spores based on multi-annual datasets of spore counts. We find that our modeled global emissions and burden are an order of magnitude lower than previous estimates.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Sam J. Silva, Colette L. Heald, and Alex B. Guenther
Geosci. Model Dev., 13, 2569–2585, https://doi.org/10.5194/gmd-13-2569-2020, https://doi.org/10.5194/gmd-13-2569-2020, 2020
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Simulating the influence of the biosphere on atmospheric chemistry has traditionally been computationally intensive. We describe a surrogate canopy physics model parameterized using a statistical learning technique and specifically designed for use in large-scale chemical transport models. Our surrogate model reproduces a more detailed model to within 10 % without a large computational demand, improving the process representation of biosphere–atmosphere exchange.
Sidhant J. Pai, Colette L. Heald, Jeffrey R. Pierce, Salvatore C. Farina, Eloise A. Marais, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Ann M. Middlebrook, Hugh Coe, John E. Shilling, Roya Bahreini, Justin H. Dingle, and Kennedy Vu
Atmos. Chem. Phys., 20, 2637–2665, https://doi.org/10.5194/acp-20-2637-2020, https://doi.org/10.5194/acp-20-2637-2020, 2020
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Aerosols in the atmosphere have significant health and climate impacts. Organic aerosol (OA) accounts for a large fraction of the total aerosol burden, but models have historically struggled to accurately simulate it. This study compares two very different OA model schemes and evaluates them against a suite of globally distributed airborne measurements with the goal of providing insight into the strengths and weaknesses of each approach across different environments.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
Maria A. Zawadowicz, Karl D. Froyd, Anne E. Perring, Daniel M. Murphy, Dominick V. Spracklen, Colette L. Heald, Peter R. Buseck, and Daniel J. Cziczo
Atmos. Chem. Phys., 19, 13859–13870, https://doi.org/10.5194/acp-19-13859-2019, https://doi.org/10.5194/acp-19-13859-2019, 2019
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We report measurements of small particles of biological origin (for example, fragments of bacteria, pollen, or fungal spores) in the atmosphere over the continental United States. We use a recently developed identification technique based on airborne mass spectrometry in conjunction with an extensive aircraft dataset. We show that biological particles are present at altitudes up to 10 km and we quantify typical concentrations.
William C. Porter and Colette L. Heald
Atmos. Chem. Phys., 19, 13367–13381, https://doi.org/10.5194/acp-19-13367-2019, https://doi.org/10.5194/acp-19-13367-2019, 2019
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In this paper we explore the connection between changes in surface temperature and changes in ozone pollution. While explanations for this connection have been proposed in the past, we attempt to better quantify them using models and statistics. We find that some of the most commonly cited mechanisms, including biogenic emissions and temperature-dependent chemical processes, can explain less than half of the O3–T correlation. Meteorology is identified as the most likely driver for the remainder.
Shan S. Zhou, Amos P. K. Tai, Shihan Sun, Mehliyar Sadiq, Colette L. Heald, and Jeffrey A. Geddes
Atmos. Chem. Phys., 18, 14133–14148, https://doi.org/10.5194/acp-18-14133-2018, https://doi.org/10.5194/acp-18-14133-2018, 2018
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Surface ozone pollution harms vegetation. As plants play key roles shaping air quality, the plant damage may further worsen air pollution. We use various computer models to examine such feedback effects, and find that ozone-induced decline in leaf density can lead to much higher ozone levels in forested regions, mostly due to the reduced ability of leaves to absorb pollutants. This study highlights the importance of considering the two-way interactions between plants and air pollution.
Harri Kokkola, Thomas Kühn, Anton Laakso, Tommi Bergman, Kari E. J. Lehtinen, Tero Mielonen, Antti Arola, Scarlet Stadtler, Hannele Korhonen, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Ina Tegen, Colombe Siegenthaler-Le Drian, Martin G. Schultz, Isabelle Bey, Philip Stier, Nikos Daskalakis, Colette L. Heald, and Sami Romakkaniemi
Geosci. Model Dev., 11, 3833–3863, https://doi.org/10.5194/gmd-11-3833-2018, https://doi.org/10.5194/gmd-11-3833-2018, 2018
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In this paper we present a global aerosol–chemistry–climate model with the focus on its representation for atmospheric aerosol particles. In the model, aerosols are simulated using the aerosol module SALSA2.0, which in this paper is compared to satellite, ground, and aircraft-based observations of the properties of atmospheric aerosol. Based on this study, the model simulated aerosol properties compare well with the observations.
Luke D. Schiferl, Colette L. Heald, and David Kelly
Biogeosciences, 15, 4301–4315, https://doi.org/10.5194/bg-15-4301-2018, https://doi.org/10.5194/bg-15-4301-2018, 2018
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To understand future food security, it is critical to develop realistic crop models with reliable sensitivity to environmental factors. We find that particulate matter (PM) causes a significant, but smaller, enhancement for global wheat and rice production than estimated without nutrient and physiological limitations imposed by a crop model. In contrast, maize grows near its physiological maximum, with little enhancement from PM. Nitrogen deposition leads to a small increase in crop production.
Luke D. Schiferl and Colette L. Heald
Atmos. Chem. Phys., 18, 5953–5966, https://doi.org/10.5194/acp-18-5953-2018, https://doi.org/10.5194/acp-18-5953-2018, 2018
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Global population growth and industrialization have contributed to poor air quality worldwide, and increasing population will put pressure on global food production. We therefore assess how air pollution may impact crop growth. Ozone has previously been shown to damage crops. We demonstrate that the impact of particles associated with enhanced light scattering promotes growth, offsetting much, if not all, ozone damage. This has implications for air quality management and global food security.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
David H. Hagan, Gabriel Isaacman-VanWertz, Jonathan P. Franklin, Lisa M. M. Wallace, Benjamin D. Kocar, Colette L. Heald, and Jesse H. Kroll
Atmos. Meas. Tech., 11, 315–328, https://doi.org/10.5194/amt-11-315-2018, https://doi.org/10.5194/amt-11-315-2018, 2018
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The use of low-cost sensors for air pollution research has outpaced our understanding of their capabilities and limitations under real-world conditions. Here we describe the deployment, calibration and evaluation of electrochemical sensors on the Island of Hawai‘i. We obtain excellent performance (RMSE < 7 ppb, r2 = 0.997) across a wide dynamic range (1 ppb–2 ppm). We introduce a hybrid regression algorithm which works across a large dynamic range and shows little decay in sensitivity over time.
Molly B. Smith, Natalie M. Mahowald, Samuel Albani, Aaron Perry, Remi Losno, Zihan Qu, Beatrice Marticorena, David A. Ridley, and Colette L. Heald
Atmos. Chem. Phys., 17, 3253–3278, https://doi.org/10.5194/acp-17-3253-2017, https://doi.org/10.5194/acp-17-3253-2017, 2017
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Using different meteorology reanalyses to drive dust in climate modeling can produce dissimilar global dust distributions, especially in the Southern Hemisphere (SH). It may therefore not be advisable for SH dust studies to base results on simulations driven by one reanalysis. Northern Hemisphere dust varies mostly on seasonal timescales, while SH dust varies on interannual timescales. Dust is an important part of climate modeling, and we hope this contributes to understanding these simulations.
David A. Ridley, Colette L. Heald, Jasper F. Kok, and Chun Zhao
Atmos. Chem. Phys., 16, 15097–15117, https://doi.org/10.5194/acp-16-15097-2016, https://doi.org/10.5194/acp-16-15097-2016, 2016
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Mineral dust aerosol affects climate through interaction with radiation and clouds, human health through contribution to particulate matter, and ecosystem health through nutrient transport and deposition. In this study, we use satellite and in situ retrievals to derive an observational estimate of the global dust AOD with which evaluate modeled dust AOD. Differences in the seasonality and regional distribution of dust AOD between observations and models are highlighted.
Colette L. Heald and Jeffrey A. Geddes
Atmos. Chem. Phys., 16, 14997–15010, https://doi.org/10.5194/acp-16-14997-2016, https://doi.org/10.5194/acp-16-14997-2016, 2016
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Humans have altered the surface of the Earth since preindustrial times. These changes (largely expansion of croplands and pasturelands) have modified biosphere–atmosphere fluxes. In this study we use a global model to assess the impact of these changes on the formation of secondary particulate matter and troposphere ozone. We find that there are significant air quality and climate impacts associated with these changes.
Xuan Wang, Colette L. Heald, Arthur J. Sedlacek, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Thomas B. Watson, Allison C. Aiken, Stephen R. Springston, and Paulo Artaxo
Atmos. Chem. Phys., 16, 12733–12752, https://doi.org/10.5194/acp-16-12733-2016, https://doi.org/10.5194/acp-16-12733-2016, 2016
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We describe a new approach to estimate the absorption of brown carbon (BrC) from multiple-wavelength absorption measurements. By applying this method to column and surface observations globally, we find that BrC contributes up to 40 % of the absorption measured at 440 nm. The analysis of two surface sites also suggests that BrC absorptivity decreases with photochemical aging in biomass burning plumes, but not in typical urban conditions.
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-16-12305-2016, https://doi.org/10.5194/acp-16-12305-2016, 2016
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This study combines new observations and a simulation to assess the interannual variability of atmospheric ammonia concentrations over the United States. The model generally underrepresents the observed variability. Nearly two-thirds of the simulated variability is caused by meteorology, twice that caused by regulations on fossil fuel combustion emissions. Adding ammonia emissions variability does not substantially improve the simulation and has little impact on summer particle concentrations.
Sam J. Silva, Colette L. Heald, Jeffrey A. Geddes, Kemen G. Austin, Prasad S. Kasibhatla, and Miriam E. Marlier
Atmos. Chem. Phys., 16, 10621–10635, https://doi.org/10.5194/acp-16-10621-2016, https://doi.org/10.5194/acp-16-10621-2016, 2016
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We investigate the impacts of current (2010) and future (2020) oil palm plantations across Southeast Asia on surface–atmosphere exchange and air quality using satellite data, land maps, and a chemical transport model. These changes lead to increases in surface ozone and particulate matter. Oil palm plantations are likely to continue to degrade regional air quality in the coming decade and hinder efforts to achieve air quality regulations in major urban areas such as Kuala Lumpur and Singapore.
Matthew J. Alvarado, Chantelle R. Lonsdale, Helen L. Macintyre, Huisheng Bian, Mian Chin, David A. Ridley, Colette L. Heald, Kenneth L. Thornhill, Bruce E. Anderson, Michael J. Cubison, Jose L. Jimenez, Yutaka Kondo, Lokesh K. Sahu, Jack E. Dibb, and Chien Wang
Atmos. Chem. Phys., 16, 9435–9455, https://doi.org/10.5194/acp-16-9435-2016, https://doi.org/10.5194/acp-16-9435-2016, 2016
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Understanding the scattering and absorption of light by aerosols is necessary for understanding air quality and climate change. We used data from the 2008 ARCTAS campaign to evaluate aerosol optical property models using a closure methodology that separates errors in these models from other errors in aerosol emissions, chemistry, or transport. We find that the models on average perform reasonably well, and make suggestions for how remaining biases could be reduced.
Bonne Ford and Colette L. Heald
Atmos. Chem. Phys., 16, 3499–3523, https://doi.org/10.5194/acp-16-3499-2016, https://doi.org/10.5194/acp-16-3499-2016, 2016
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As motivation for air quality research, many studies cite the fact that exposure to particulate matter is associated with premature mortality. Recently, more studies have also tried to quantify this burden; however, there are many data sets that can be used and many different methodological choices to be made. In this paper, we seek to explain the different sources of uncertainty in health impact assessments through the example of using model and satellite-based PM2.5 concentrations.
Jeffrey A. Geddes, Colette L. Heald, Sam J. Silva, and Randall V. Martin
Atmos. Chem. Phys., 16, 2323–2340, https://doi.org/10.5194/acp-16-2323-2016, https://doi.org/10.5194/acp-16-2323-2016, 2016
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Land use and land cover changes driven by anthropogenic activities or natural causes (e.g., forestry management, agriculture, wildfires) can impact climate and air quality in many complex ways. Using a state-of-the-art chemistry model, we investigate how tree mortality in the US due to insect infestation and disease outbreak may impact atmospheric composition. We find that the surface concentrations of ozone and aerosol can be altered due to changing background emissions and loss processes.
W. C. Porter, C. L. Heald, D. Cooley, and B. Russell
Atmos. Chem. Phys., 15, 10349–10366, https://doi.org/10.5194/acp-15-10349-2015, https://doi.org/10.5194/acp-15-10349-2015, 2015
S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
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Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
M. Val Martin, C. L. Heald, J.-F. Lamarque, S. Tilmes, L. K. Emmons, and B. A. Schichtel
Atmos. Chem. Phys., 15, 2805–2823, https://doi.org/10.5194/acp-15-2805-2015, https://doi.org/10.5194/acp-15-2805-2015, 2015
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We present for the first time the relative effect of climate, emissions, and land use change on ozone and PM25 over the United States, focusing on the national parks. Air quality in 2050 will likely be dominated by emission patterns, but climate and land use changes alone can lead to a substantial increase in air pollution over most of the US, with important implications for O3 air quality, visibility and ecosystem health degradation in the national parks.
X. Wang, C. L. Heald, D. A. Ridley, J. P. Schwarz, J. R. Spackman, A. E. Perring, H. Coe, D. Liu, and A. D. Clarke
Atmos. Chem. Phys., 14, 10989–11010, https://doi.org/10.5194/acp-14-10989-2014, https://doi.org/10.5194/acp-14-10989-2014, 2014
D. A. Ridley, C. L. Heald, and J. M. Prospero
Atmos. Chem. Phys., 14, 5735–5747, https://doi.org/10.5194/acp-14-5735-2014, https://doi.org/10.5194/acp-14-5735-2014, 2014
C. L. Heald, D. A. Ridley, J. H. Kroll, S. R. H. Barrett, K. E. Cady-Pereira, M. J. Alvarado, and C. D. Holmes
Atmos. Chem. Phys., 14, 5513–5527, https://doi.org/10.5194/acp-14-5513-2014, https://doi.org/10.5194/acp-14-5513-2014, 2014
D. V. Spracklen and R. Righelato
Biogeosciences, 11, 2741–2754, https://doi.org/10.5194/bg-11-2741-2014, https://doi.org/10.5194/bg-11-2741-2014, 2014
M. Van Damme, L. Clarisse, C. L. Heald, D. Hurtmans, Y. Ngadi, C. Clerbaux, A. J. Dolman, J. W. Erisman, and P. F. Coheur
Atmos. Chem. Phys., 14, 2905–2922, https://doi.org/10.5194/acp-14-2905-2014, https://doi.org/10.5194/acp-14-2905-2014, 2014
B. Ford and C. L. Heald
Atmos. Chem. Phys., 13, 9269–9283, https://doi.org/10.5194/acp-13-9269-2013, https://doi.org/10.5194/acp-13-9269-2013, 2013
M. Val Martin, C. L. Heald, B. Ford, A. J. Prenni, and C. Wiedinmyer
Atmos. Chem. Phys., 13, 7429–7439, https://doi.org/10.5194/acp-13-7429-2013, https://doi.org/10.5194/acp-13-7429-2013, 2013
A. R. Berg, C. L. Heald, K. E. Huff Hartz, A. G. Hallar, A. J. H. Meddens, J. A. Hicke, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 13, 3149–3161, https://doi.org/10.5194/acp-13-3149-2013, https://doi.org/10.5194/acp-13-3149-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Opinion: Coordinated development of emission inventories for climate forcers and air pollutants
Differences between recent emission inventories strongly affect anthropogenic aerosol evolution from 1990 to 2019
Seasonal modeling analysis of nitrate formation pathways in Yangtze River Delta region, China
Global Nitrogen and Sulfur Budgets Using a Measurement-Model Fusion Approach
Modeling radiative and climatic effects of brown carbon aerosols with the ARPEGE-Climat global climate model
Numerical simulation of the impact of COVID-19 lockdown on tropospheric composition and aerosol radiative forcing in Europe
Evaluation of the WRF and CHIMERE models for the simulation of PM2.5 in large East African urban conurbations
Impact of urban heat island on inorganic aerosol in the lower free troposphere: a case study in Hangzhou, China
Statistical and machine learning methods for evaluating trends in air quality under changing meteorological conditions
Simulating the radiative forcing of oceanic dimethylsulfide (DMS) in Asia based on machine learning estimates
Quantifying the effects of mixing state on aerosol optical properties
Secondary organic aerosol formation via multiphase reaction of hydrocarbons in urban atmospheres using CAMx integrated with the UNIPAR model
Contrasting source contributions of Arctic black carbon to atmospheric concentrations, deposition flux, and atmospheric and snow radiative effects
Effect of dust on rainfall over the Red Sea coast based on WRF-Chem model simulations
A new assessment of global and regional budgets, fluxes, and lifetimes of atmospheric reactive N and S gases and aerosols
Limitations in representation of physical processes prevent successful simulation of PM2.5 during KORUS-AQ
Eurodelta multi-model simulated and observed particulate matter trends in Europe in the period of 1990–2010
Elucidating the critical oligomeric steps in secondary organic aerosol and brown carbon formation
Fast climate responses to emission reductions in aerosol and ozone precursors in China during 2013–2017
Secondary PM2.5 decreases significantly less than NO2 emission reductions during COVID lockdown in Germany
Molecular-level nucleation mechanism of iodic acid and methanesulfonic acid
Estimation of secondary PM2.5 in China and the United States using a multi-tracer approach
Two-way coupled meteorology and air quality models in Asia: a systematic review and meta-analysis of impacts of aerosol feedbacks on meteorology and air quality
OCEANFILMS (Organic Compounds from Ecosystems to Aerosols: Natural Films and Interfaces via Langmuir Molecular Surfactants) sea spray organic aerosol emissions – implementation in a global climate model and impacts on clouds
The pathway of impacts of aerosol direct effects on secondary inorganic aerosol formation
The impact of molecular self-organisation on the atmospheric fate of a cooking aerosol proxy
The formation and mitigation of nitrate pollution: comparison between urban and suburban environments
Impacts of aerosol–photolysis interaction and aerosol–radiation feedback on surface-layer ozone in North China during multi-pollutant air pollution episodes
Reducing future air-pollution-related premature mortality over Europe by mitigating emissions from the energy sector: assessing an 80 % renewable energies scenario
The impact of chlorine chemistry combined with heterogeneous N2O5 reactions on air quality in China
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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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.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia M. Upchurch, Thomas Tuch, Alfred Wiedensohler, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
Atmos. Chem. Phys., 23, 5641–5678, https://doi.org/10.5194/acp-23-5641-2023, https://doi.org/10.5194/acp-23-5641-2023, 2023
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Remote and local anthropogenic emissions contribute to wintertime Arctic haze, with enhanced aerosol concentrations, but natural sources, which also contribute, are less well studied. Here, modelled wintertime sea-spray aerosols are improved in WRF-Chem over the wider Arctic by including updated wind speed and temperature-dependent treatments. As a result, anthropogenic nitrate aerosols are also improved. Open leads are confirmed to be the main source of sea-spray aerosols over northern Alaska.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
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.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys., 23, 4149–4163, https://doi.org/10.5194/acp-23-4149-2023, https://doi.org/10.5194/acp-23-4149-2023, 2023
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Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between foreign-transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys., 23, 4091–4104, https://doi.org/10.5194/acp-23-4091-2023, https://doi.org/10.5194/acp-23-4091-2023, 2023
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From 12 March to 6 April 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days, and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing and then conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
Arineh Cholakian, Matthias Beekmann, Guillaume Siour, Isabelle Coll, Manuela Cirtog, Elena Ormeño, Pierre-Marie Flaud, Emilie Perraudin, and Eric Villenave
Atmos. Chem. Phys., 23, 3679–3706, https://doi.org/10.5194/acp-23-3679-2023, https://doi.org/10.5194/acp-23-3679-2023, 2023
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This article revolves around the simulation of biogenic secondary organic aerosols in the Landes forest (southwestern France). Several sensitivity cases involving biogenic emission factors, land cover data, anthropogenic emissions, and physical or meteorological parameters were performed and each compared to measurements both in the forest canopy and around the forest. The chemistry behind the formation of these aerosols and their production and transport in the forest canopy is discussed.
Marina Liaskoni, Peter Huszar, Lukáš Bartík, Alvaro Patricio Prieto Perez, Jan Karlický, and Ondřej Vlček
Atmos. Chem. Phys., 23, 3629–3654, https://doi.org/10.5194/acp-23-3629-2023, https://doi.org/10.5194/acp-23-3629-2023, 2023
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Wind-blown dust (WBD) emissions emitted from European soils are estimated for the 2007–2016 period, and their impact on the total particulate matter (PM) concentration is calculated. We found a considerable increase in PM concentrations due to such emissions, especially on selected days (rather than on a seasonal average). We also found that WBD emissions are strongest over western Europe, and the highest impacts on PM are calculated for this region.
Yunyao Li, Daniel Tong, Siqi Ma, Saulo R. Freitas, Ravan Ahmadov, Mikhail Sofiev, Xiaoyang Zhang, Shobha Kondragunta, Ralph Kahn, Youhua Tang, Barry Baker, Patrick Campbell, Rick Saylor, Georg Grell, and Fangjun Li
Atmos. Chem. Phys., 23, 3083–3101, https://doi.org/10.5194/acp-23-3083-2023, https://doi.org/10.5194/acp-23-3083-2023, 2023
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Plume height is important in wildfire smoke dispersion and affects air quality and human health. We assess the impact of plume height on wildfire smoke dispersion and the exceedances of the National Ambient Air Quality Standards. A higher plume height predicts lower pollution near the source region, but higher pollution in downwind regions, due to the faster spread of the smoke once ejected, affects pollution exceedance forecasts and the early warning of extreme air pollution events.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Jingyu An, Cheng Huang, Dandan Huang, Momei Qin, Huan Liu, Rusha Yan, Liping Qiao, Min Zhou, Yingjie Li, Shuhui Zhu, Qian Wang, and Hongli Wang
Atmos. Chem. Phys., 23, 323–344, https://doi.org/10.5194/acp-23-323-2023, https://doi.org/10.5194/acp-23-323-2023, 2023
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This paper aims to build up an approach to establish a high-resolution emission inventory of intermediate-volatility and semi-volatile organic compounds in city-scale and detailed source categories and incorporate it into the CMAQ model. We believe this approach can be widely applied to improve the simulation of secondary organic aerosol and its source contributions.
Huibin Dai, Hong Liao, Ke Li, Xu Yue, Yang Yang, Jia Zhu, Jianbing Jin, Baojie Li, and Xingwen Jiang
Atmos. Chem. Phys., 23, 23–39, https://doi.org/10.5194/acp-23-23-2023, https://doi.org/10.5194/acp-23-23-2023, 2023
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We apply the 3-D global chemical transport model (GEOS-Chem) to simulate co-polluted days by O3 and PM2.5 (O3–PM2.5PDs) in Beijing–Tianjin–Hebei in 2013–2020 and investigate the chemical and physical characteristics of O3–PM2.5PDs by composited analyses of such days that are captured by both the observations and the model. We report for the first time the unique features in vertical distributions of aerosols during O3–PM2.5PDs and the physical and chemical characteristics of O3–PM2.5PDs.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-729, https://doi.org/10.5194/acp-2022-729, 2023
Revised manuscript accepted for ACP
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A multi-air pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measurement with NOx emission decresed by ~40 %. Emissions of other species were only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicates that the lockdown only has limited effects on the control of PM2.5 and O3 in China.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-748, https://doi.org/10.5194/acp-2022-748, 2023
Revised manuscript accepted for ACP
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New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics-multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been underdetected and modulating their abundance leads to significantly improved simulation-observation agreement.
Rachel A. Bergin, Monica Harkey, Alicia Hoffman, Richard H. Moore, Bruce Anderson, Andreas Beyersdorf, Luke Ziemba, Lee Thornhill, Edward Winstead, Tracey Holloway, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 15449–15468, https://doi.org/10.5194/acp-22-15449-2022, https://doi.org/10.5194/acp-22-15449-2022, 2022
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Correctly predicting aerosol surface area concentrations is important for determining the rate of heterogeneous reactions in chemical transport models. Here, we compare aircraft measurements of aerosol surface area with a regional model. In polluted air masses, we show that the model underpredicts aerosol surface area by a factor of 2. Despite this disagreement, the representation of heterogeneous chemistry still dominates the overall uncertainty in the loss rate of molecules such as N2O5.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 14529–14546, https://doi.org/10.5194/acp-22-14529-2022, https://doi.org/10.5194/acp-22-14529-2022, 2022
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Quantum chemical methods are applied to gain insight into the oligomerization reaction mechanisms and kinetics of distinct stabilized Criegee intermediate (SCI) reactions with hydroperoxide esters, where calculations show that SCI addition reactions with hydroperoxide esters proceed through the successive insertion of SCIs to form oligomers that involve SCIs as the repeating unit. The saturated vapor pressure of the formed oligomers decreases monotonically with the increasing number of SCIs.
Mathieu Lachatre, Sylvain Mailler, Laurent Menut, Arineh Cholakian, Pasquale Sellitto, Guillaume Siour, Henda Guermazi, Giuseppe Salerno, and Salvatore Giammanco
Atmos. Chem. Phys., 22, 13861–13879, https://doi.org/10.5194/acp-22-13861-2022, https://doi.org/10.5194/acp-22-13861-2022, 2022
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In this study, we have evaluated the predominance of various pathways of volcanic SO2 conversion to sulfates in the upper troposphere. We show that the main conversion pathway was gaseous oxidation by OH, although the liquid pathways were expected to be predominant. These results are interesting with respect to a better understanding of sulfate formation in the middle and upper troposphere and are an important component to help evaluate particulate matter radiative forcing.
Siying Lian, Luxi Zhou, Daniel M. Murphy, Karl D. Froyd, Owen B. Toon, and Pengfei Yu
Atmos. Chem. Phys., 22, 13659–13676, https://doi.org/10.5194/acp-22-13659-2022, https://doi.org/10.5194/acp-22-13659-2022, 2022
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Parameterizations of dust lifting and microphysical properties of dust in climate models are still subject to large uncertainty. Here we use a sectional aerosol climate model to investigate the global vertical distributions of the dust. Constrained by a suite of observations, the model suggests that, although North African dust dominates global dust mass loading at the surface, the relative contribution of Asian dust increases with altitude and becomes dominant in the upper troposphere.
Steven J. Smith, Erin E. McDuffie, and Molly Charles
Atmos. Chem. Phys., 22, 13201–13218, https://doi.org/10.5194/acp-22-13201-2022, https://doi.org/10.5194/acp-22-13201-2022, 2022
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Emissions into the atmosphere of greenhouse gases (GHGs) and air pollutants, quantified in emission inventories, impact human health, ecosystems, and the climate. We review how air pollutant and GHG inventory activities have historically been structured and their different uses and requirements. We discuss the benefits of increasing coordination between air pollutant and GHG inventory development efforts, but also caution that there are differences in appropriate methodologies and applications.
Marianne Tronstad Lund, Gunnar Myhre, Ragnhild Bieltvedt Skeie, Bjørn Hallvard Samset, and Zbigniew Klimont
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-639, https://doi.org/10.5194/acp-2022-639, 2022
Revised manuscript accepted for ACP
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Here we show that differences, in magnitude and trend, between recent global anthropogenic emission inventories have notable influence on simulated abundances of anthropogenic aerosol, and their radiative forcing (RF), over the 1990–2019 period. This, in turn, affect estimates of radiative forcing. Our findings form a basis for comparing existing and upcoming studies anthropogenic aerosols using different emission inventories.
Jinjin Sun, Momei Qin, Xiaodong Xie, Wenxing Fu, Yang Qin, Li Sheng, Lin Li, Jingyi Li, Ishaq Dimeji Sulaymon, Lei Jiang, Lin Huang, Xingna Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 12629–12646, https://doi.org/10.5194/acp-22-12629-2022, https://doi.org/10.5194/acp-22-12629-2022, 2022
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NO3- has become the dominant and the least reduced chemical component of fine particulate matter in China. NO3- formation is mostly in the NH3-rich regime in the Yangtze River Delta (YRD). OH + NO2 contributes 60 %–83 % of the TNO3 production rates, and the N2O5 heterogeneous pathway contributes 10 %–36 %. The N2O5 heterogeneous pathway becomes more important in cold seasons. Local emissions and regional transportation contribute 50 %–62 % and 38 %–50 % to YRD NO3- concentrations, respectively.
Hannah J. Rubin, Joshua S. Fu, Frank Dentener, Rui Li, Kan Huang, and Hongbo Fu
EGUsphere, https://doi.org/10.5194/egusphere-2022-873, https://doi.org/10.5194/egusphere-2022-873, 2022
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We update the 2010 global deposition budget for nitrogen and sulfur with new regional wet deposition measurements, improving the ensemble results of eleven global chemistry transport models from HTAP-II. Our study demonstrates that a global measurement-model fusion approach can substantially improve N and S deposition model estimates at a regional scale and represents a step forward toward the WMO’s goal of global fusion products for accurately mapping harmful air pollution.
Thomas Drugé, Pierre Nabat, Marc Mallet, Martine Michou, Samuel Rémy, and Oleg Dubovik
Atmos. Chem. Phys., 22, 12167–12205, https://doi.org/10.5194/acp-22-12167-2022, https://doi.org/10.5194/acp-22-12167-2022, 2022
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This study presents the implementation of brown carbon in the atmospheric component of the CNRM global climate model and particularly in its aerosol scheme TACTIC. Several simulations were carried out with this climate model, over the period 2000–2014, to evaluate the model by comparison with different reference datasets (PARASOL-GRASP, OMI-OMAERUVd, MACv2, FMI_SAT, AERONET) and to analyze the brown carbon radiative and climatic effects.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Andrea Mazzeo, Michael Burrow, Andrew Quinn, Eloise A. Marais, Ajit Singh, David Ng'ang'a, Michael J. Gatari, and Francis D. Pope
Atmos. Chem. Phys., 22, 10677–10701, https://doi.org/10.5194/acp-22-10677-2022, https://doi.org/10.5194/acp-22-10677-2022, 2022
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A modelling system for meteorology and chemistry transport processes, WRF–CHIMERE, has been tested and validated for three East African conurbations using the most up-to-date anthropogenic emissions available. Results show that the model is able to reproduce hourly and daily temporal variabilities in aerosol concentrations that are close to observations in both urban and rural environments, encouraging the adoption of numerical modelling as a tool for air quality management in East Africa.
Hanqing Kang, Bin Zhu, Gerrit de Leeuw, Bu Yu, Ronald J. van der A, and Wen Lu
Atmos. Chem. Phys., 22, 10623–10634, https://doi.org/10.5194/acp-22-10623-2022, https://doi.org/10.5194/acp-22-10623-2022, 2022
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This study quantified the contribution of each urban-induced meteorological effect (temperature, humidity, and circulation) to aerosol concentration. We found that the urban heat island (UHI) circulation dominates the UHI effects on aerosol. The UHI circulation transports aerosol and its precursor gases from the warmer lower boundary layer to the colder lower free troposphere and promotes the secondary formation of ammonium nitrate aerosol in the cold atmosphere.
Minghao Qiu, Corwin Zigler, and Noelle E. Selin
Atmos. Chem. Phys., 22, 10551–10566, https://doi.org/10.5194/acp-22-10551-2022, https://doi.org/10.5194/acp-22-10551-2022, 2022
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Evaluating impacts of emission changes on air quality requires accounting for meteorological variability. Many studies use simple regression methods to correct for meteorology, but little is known about their performance. Using cases in the US and China, we show that widely used regression models do not perform well and can lead to biased estimates of emission-driven trends. We propose a novel machine learning method with lower bias and provide recommendations to policymakers and researchers.
Junri Zhao, Weichun Ma, Kelsey R. Bilsback, Jeffrey R. Pierce, Shengqian Zhou, Ying Chen, Guipeng Yang, and Yan Zhang
Atmos. Chem. Phys., 22, 9583–9600, https://doi.org/10.5194/acp-22-9583-2022, https://doi.org/10.5194/acp-22-9583-2022, 2022
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Marine dimethylsulfide (DMS) emissions play important roles in atmospheric sulfur cycle and climate effects. In this study, DMS emissions were estimated by using the machine learning method and drove the global 3D chemical transport model to simulate their climate effects. To our knowledge, this is the first study in the Asian region that quantifies the combined impacts of DMS on sulfate, particle number concentration, and radiative forcings.
Yu Yao, Jeffrey H. Curtis, Joseph Ching, Zhonghua Zheng, and Nicole Riemer
Atmos. Chem. Phys., 22, 9265–9282, https://doi.org/10.5194/acp-22-9265-2022, https://doi.org/10.5194/acp-22-9265-2022, 2022
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Investigating the impacts of aerosol mixing state on aerosol optical properties has a long history from both the modeling and experimental perspective. In this study, we used particle-resolved simulations as a benchmark to determine the error in optical properties when using simplified aerosol representations. We found that errors in single scattering albedo due to the internal mixture assumptions can have substantial effects on calculating aerosol direct radiative forcing.
Zechen Yu, Myoseon Jang, Soontae Kim, Kyuwon Son, Sanghee Han, Azad Madhu, and Jinsoo Park
Atmos. Chem. Phys., 22, 9083–9098, https://doi.org/10.5194/acp-22-9083-2022, https://doi.org/10.5194/acp-22-9083-2022, 2022
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The UNIPAR model was incorporated into CAMx to predict the ambient concentration of organic matter in urban atmospheres during the KORUS-AQ campaign. CAMx–UNIPAR significantly improved the simulation of SOA formation under the wet aerosol condition through the consideration of aqueous reactions of reactive organic species and gas–aqueous partitioning into the wet inorganic aerosol.
Hitoshi Matsui, Tatsuhiro Mori, Sho Ohata, Nobuhiro Moteki, Naga Oshima, Kumiko Goto-Azuma, Makoto Koike, and Yutaka Kondo
Atmos. Chem. Phys., 22, 8989–9009, https://doi.org/10.5194/acp-22-8989-2022, https://doi.org/10.5194/acp-22-8989-2022, 2022
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Using a global aerosol model, we find that the source contributions to radiative effects of black carbon (BC) in the Arctic are quite different from those to mass concentrations and deposition flux of BC in the Arctic. This is because microphysical properties (e.g., mixing state), altitudes, and seasonal variations of BC in the atmosphere differ among emissions sources. These differences need to be considered for accurate simulations of Arctic BC and its source contributions and climate impacts.
Sagar P. Parajuli, Georgiy L. Stenchikov, Alexander Ukhov, Suleiman Mostamandi, Paul A. Kucera, Duncan Axisa, William I. Gustafson Jr., and Yannian Zhu
Atmos. Chem. Phys., 22, 8659–8682, https://doi.org/10.5194/acp-22-8659-2022, https://doi.org/10.5194/acp-22-8659-2022, 2022
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Rainfall affects the distribution of surface- and groundwater resources, which are constantly declining over the Middle East and North Africa (MENA) due to overexploitation. Here, we explored the effects of dust on rainfall using WRF-Chem model simulations. Although dust is considered a nuisance from an air quality perspective, our results highlight the positive fundamental role of dust particles in modulating rainfall formation and distribution, which has implications for cloud seeding.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 22, 8343–8368, https://doi.org/10.5194/acp-22-8343-2022, https://doi.org/10.5194/acp-22-8343-2022, 2022
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Reactive N and S gases and aerosols are critical determinants of air quality. We report a comprehensive analysis of the concentrations, wet and dry deposition, fluxes, and lifetimes of these species globally as well as for 10 world regions. We used the EMEP MSC-W model coupled with WRF meteorology and 2015 global emissions. Our work demonstrates the substantial regional variation in these quantities and the need for modelling to simulate atmospheric responses to precursor emissions.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257, https://doi.org/10.5194/acp-22-7207-2022, https://doi.org/10.5194/acp-22-7207-2022, 2022
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Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Yuemeng Ji, Qiuju Shi, Xiaohui Ma, Lei Gao, Jiaxin Wang, Yixin Li, Yanpeng Gao, Guiying Li, Renyi Zhang, and Taicheng An
Atmos. Chem. Phys., 22, 7259–7271, https://doi.org/10.5194/acp-22-7259-2022, https://doi.org/10.5194/acp-22-7259-2022, 2022
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The formation mechanisms of secondary organic aerosol and brown carbon from small α-carbonyls are still unclear. Thus, the mechanisms and kinetics of aqueous-phase reactions of glyoxal were investigated using quantum chemical and kinetic rate calculations. Several essential isomeric processes were identified, including protonation to yield diol/tetrol and carbenium ions as well as nucleophilic addition of carbenium ions to diol/tetrol and free methylamine/ammonia.
Jiyuan Gao, Yang Yang, Hailong Wang, Pinya Wang, Huimin Li, Mengyun Li, Lili Ren, Xu Yue, and Hong Liao
Atmos. Chem. Phys., 22, 7131–7142, https://doi.org/10.5194/acp-22-7131-2022, https://doi.org/10.5194/acp-22-7131-2022, 2022
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China has been implementing a sequence of policies for clean air since the year 2013. The aerosol decline produced a 0.09 ± 0.10°C warming during 2013–2017 estimated in this study, and the increase in ozone in the lower troposphere during this time period accelerated the warming, leading to a total 0.16 ± 0.15°C temperature increase in eastern China. Residential emission reductions led to a cooling effect because of a substantial decrease in light-absorbing aerosols.
Vigneshkumar Balamurugan, Jia Chen, Zhen Qu, Xiao Bi, and Frank N. Keutsch
Atmos. Chem. Phys., 22, 7105–7129, https://doi.org/10.5194/acp-22-7105-2022, https://doi.org/10.5194/acp-22-7105-2022, 2022
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In this study, we investigated the response of secondary pollutants to changes in precursor emissions, focusing on the formation of secondary PM, during the COVID-19 lockdown period. We show that, due to the decrease in primary NOx emissions, atmospheric oxidizing capacity is increased. The nighttime increase in ozone, caused by less NO titration, results in higher NO3 radicals, which contribute significantly to the formation of PM nitrates. O3 should be limited in order to control PM pollution.
An Ning, Ling Liu, Lin Ji, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 6103–6114, https://doi.org/10.5194/acp-22-6103-2022, https://doi.org/10.5194/acp-22-6103-2022, 2022
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Iodic acid (IA) and methanesulfonic acid (MSA) were previously proved to be significant nucleation precursors in marine areas. However, the nucleation process involved in IA and MSA remains unclear. We show the enhancement of MSA on IA cluster formation and reveal the IAM-SA nucleating mechanism using a theoretical approach. This study helps to understand the clustering process in which marine sulfur- and iodine-containing species are jointly involved and its impact on new particle formation.
Haoran Zhang, Nan Li, Keqin Tang, Hong Liao, Chong Shi, Cheng Huang, Hongli Wang, Song Guo, Min Hu, Xinlei Ge, Mindong Chen, Zhenxin Liu, Huan Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 5495–5514, https://doi.org/10.5194/acp-22-5495-2022, https://doi.org/10.5194/acp-22-5495-2022, 2022
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We developed a new algorithm with low economic/technique costs to identify primary and secondary components of PM2.5. Our model was shown to be reliable by comparison with different observation datasets. We systematically explored the patterns and changes in the secondary PM2.5 pollution in China at large spatial and time scales. We believe that this method is a promising tool for efficiently estimating primary and secondary PM2.5, and has huge potential for future PM mitigation.
Chao Gao, Aijun Xiu, Xuelei Zhang, Qingqing Tong, Hongmei Zhao, Shichun Zhang, Guangyi Yang, and Mengduo Zhang
Atmos. Chem. Phys., 22, 5265–5329, https://doi.org/10.5194/acp-22-5265-2022, https://doi.org/10.5194/acp-22-5265-2022, 2022
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With ever-growing applications of two-way coupled meteorology and air quality models in Asia over the past decade, this paper summarizes the current status and research focuses, as well as how aerosol effects impact model performance, meteorology, and air quality. These models enable investigations of ARI and ACI effects induced by natural and anthropogenic aerosols in Asia, which has serious air pollution problems. The current gaps and perspectives are also presented and discussed.
Susannah M. Burrows, Richard C. Easter, Xiaohong Liu, Po-Lun Ma, Hailong Wang, Scott M. Elliott, Balwinder Singh, Kai Zhang, and Philip J. Rasch
Atmos. Chem. Phys., 22, 5223–5251, https://doi.org/10.5194/acp-22-5223-2022, https://doi.org/10.5194/acp-22-5223-2022, 2022
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Sea spray particles are composed of a mixture of salts and organic substances from oceanic microorganisms. In prior work, our team developed an approach connecting sea spray chemistry to ocean biology, called OCEANFILMS. Here we describe its implementation within an Earth system model, E3SM. We show that simulated sea spray chemistry is consistent with observed seasonal cycles and that sunlight reflected by simulated Southern Ocean clouds increases, consistent with analysis of satellite data.
Jiandong Wang, Jia Xing, Shuxiao Wang, Rohit Mathur, Jiaping Wang, Yuqiang Zhang, Chao Liu, Jonathan Pleim, Dian Ding, Xing Chang, Jingkun Jiang, Peng Zhao, Shovan Kumar Sahu, Yuzhi Jin, David C. Wong, and Jiming Hao
Atmos. Chem. Phys., 22, 5147–5156, https://doi.org/10.5194/acp-22-5147-2022, https://doi.org/10.5194/acp-22-5147-2022, 2022
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Aerosols reduce surface solar radiation and change the photolysis rate and planetary boundary layer stability. In this study, the online coupled meteorological and chemistry model was used to explore the detailed pathway of how aerosol direct effects affect secondary inorganic aerosol. The effects through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter.
Adam Milsom, Adam M. Squires, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 22, 4895–4907, https://doi.org/10.5194/acp-22-4895-2022, https://doi.org/10.5194/acp-22-4895-2022, 2022
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Cooking emissions can self-organise into nanostructured lamellar bilayers, and this can influence reaction kinetics. We developed a kinetic multi-layer model-based description of decay data we obtained from laboratory experiments of the ozonolysis of coated films of such a self-organised system, demonstrating a decreased diffusivity for both oleic acid and ozone. Nanostructure formation can thus increase the reactive half-life of oleic acid by days under typical indoor and outdoor conditions.
Suxia Yang, Bin Yuan, Yuwen Peng, Shan Huang, Wei Chen, Weiwei Hu, Chenglei Pei, Jun Zhou, David D. Parrish, Wenjie Wang, Xianjun He, Chunlei Cheng, Xiao-Bing Li, Xiaoyun Yang, Yu Song, Haichao Wang, Jipeng Qi, Baolin Wang, Chen Wang, Chaomin Wang, Zelong Wang, Tiange Li, E Zheng, Sihang Wang, Caihong Wu, Mingfu Cai, Chenshuo Ye, Wei Song, Peng Cheng, Duohong Chen, Xinming Wang, Zhanyi Zhang, Xuemei Wang, Junyu Zheng, and Min Shao
Atmos. Chem. Phys., 22, 4539–4556, https://doi.org/10.5194/acp-22-4539-2022, https://doi.org/10.5194/acp-22-4539-2022, 2022
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We use a model constrained using observations to study the formation of nitrate aerosol in and downwind of a representative megacity. We found different contributions of various chemical reactions to ground-level nitrate concentrations between urban and suburban regions. We also show that controlling VOC emissions are effective for decreasing nitrate formation in both urban and regional environments, although VOCs are not direct precursors of nitrate aerosol.
Hao Yang, Lei Chen, Hong Liao, Jia Zhu, Wenjie Wang, and Xin Li
Atmos. Chem. Phys., 22, 4101–4116, https://doi.org/10.5194/acp-22-4101-2022, https://doi.org/10.5194/acp-22-4101-2022, 2022
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Aerosols can influence O3 through aerosol–radiation interactions, including aerosol–photolysis interaction (API) and aerosol–radiation feedback (ARF). The weakened photolysis rates and changed meteorological conditions reduce surface-layer O3 concentrations by up to 9.3–11.4 ppb, with API and ARF contributing 74.6 %–90.0 % and 10.0 %–25.4 % of the O3 decrease in three episodes, respectively, which indicates that API is the dominant way for O3 reduction related to aerosol–radiation interactions.
Patricia Tarín-Carrasco, Ulas Im, Camilla Geels, Laura Palacios-Peña, and Pedro Jiménez-Guerrero
Atmos. Chem. Phys., 22, 3945–3965, https://doi.org/10.5194/acp-22-3945-2022, https://doi.org/10.5194/acp-22-3945-2022, 2022
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The evidence of the effects of atmospheric pollution (and particularly fine particulate matter, PM2.5) on human mortality is now unquestionable. Here, 895 000 annual premature deaths (PD) are estimated for the present (1991–2010), which increases to 1 540 000 in the year 2050 due to the ageing of the European population. The implementation of a mitigation scenario (80 % of the energy production in Europe from renewable sources) could lead to a decrease of over 60 000 annual PD for the year 2050.
Xiajie Yang, Qiaoqiao Wang, Nan Ma, Weiwei Hu, Yang Gao, Zhijiong Huang, Junyu Zheng, Bin Yuan, Ning Yang, Jiangchuan Tao, Juan Hong, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3743–3762, https://doi.org/10.5194/acp-22-3743-2022, https://doi.org/10.5194/acp-22-3743-2022, 2022
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We use the GEOS-Chem model with additional anthropogenic and biomass burning chlorine emissions combined with updated parameterizations for N2O5 + Cl chemistry to investigate the impacts of chlorine chemistry on air quality in China. Our study not only significantly improves the model's performance but also demonstrates the importance of non-sea-salt chlorine sources as well as an appropriate parameterization for N2O5 + Cl chemistry to the impact of chlorine chemistry in China.
Cited articles
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Huffman, J. A., Prenni, A. J., DeMott, P. J., Pöhlker, C., Mason, R. H., Robinson, N. H., Fröhlich-Nowoisky, J., Tobo, Y., Després, V. R., Garcia, E., Gochis, D. J., Harris, E., Müller-Germann, I., Ruzene, C., Schmer, B., Sinha, B., Day, D. A., Andreae, M. O., Jimenez, J. L., Gallagher, M., Kreidenweis, S. M., Bertram, A. K., and Pöschl, U.: High concentrations of biological aerosol particles and ice nuclei during and after rain, Atmos. Chem. Phys., 13, 6151–6164, https://doi.org/10.5194/acp-13-6151-2013, 2013.
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Manktelow, P. T., Carslaw, K. S., Mann, G. W., and Spracklen, D. V.: The impact of dust on sulfate aerosol, CN and CCN during an East Asian dust storm, Atmos. Chem. Phys., 10, 365–382, https://doi.org/10.5194/acp-10-365-2010, 2010.
Mann, G. W., Carslaw, K. S., Spracklen, D. V., Ridley, D. A., Manktelow, P. T., Chipperfield, M. P., Pickering, S. J., and Johnson, C. E.: Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model, Geosci. Model Dev., 3, 519–551, https://doi.org/10.5194/gmd-3-519-2010, 2010.
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