Articles | Volume 14, issue 11
https://doi.org/10.5194/acp-14-5513-2014
© 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-14-5513-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
04 Jun 2014
Research article |
| 04 Jun 2014
Contrasting the direct radiative effect and direct radiative forcing of aerosols
C. L. Heald
Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA, USA
D. A. Ridley
Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
J. H. Kroll
Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA
S. R. H. Barrett
Department of Aeronautics and Astronautics, Massachusetts Institute of Technology, Cambridge, MA, USA
K. E. Cady-Pereira
Atmospheric and Environmental Research (AER), Lexington, MA, USA
M. J. Alvarado
Atmospheric and Environmental Research (AER), Lexington, MA, USA
C. D. Holmes
Department of Earth System Science, University of California, Irvine, CA, USA
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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
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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
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Sam J. Silva, Colette L. Heald, Jeffrey A. Geddes, Kemen G. Austin, Prasad S. Kasibhatla, and Miriam E. Marlier
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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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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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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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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
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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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. V. Spracklen and C. L. Heald
Atmos. Chem. Phys., 14, 9051–9059, https://doi.org/10.5194/acp-14-9051-2014, https://doi.org/10.5194/acp-14-9051-2014, 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
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
Sebastian D. Eastham, Guillaume P. Chossière, Raymond L. Speth, Daniel J. Jacob, and Steven R. H. Barrett
Atmos. Chem. Phys., 24, 2687–2703, https://doi.org/10.5194/acp-24-2687-2024, https://doi.org/10.5194/acp-24-2687-2024, 2024
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Emissions from aircraft are known to cause air quality impacts worldwide, but the scale and mechanisms of this impact are not well understood. This work uses high-resolution computational modeling of the atmosphere to show that air pollution changes from aviation are mostly the result of emissions during cruise (high-altitude) operations, that these impacts are related to how much non-aviation pollution is present, and that prior regional assessments have underestimated these impacts.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Irene Constantina Dedoussi, Daven K. Henze, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-233, https://doi.org/10.5194/gmd-2023-233, 2024
Revised manuscript under review for GMD
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Atmospheric model gradients provide a meaningful tool for better understanding the underlying atmospheric processes. Adjoint modeling enables computationally efficient gradient calculations. We present the adjoint of the GEOS-Chem unified chemistry extension (UCX). With this development, the GEOS-Chem adjoint model can capture stratospheric ozone and other processes jointly with tropospheric processes. We apply it to characterize the Antarctic ozone depletion potential of active halogen species.
Karen E. Cady-Pereira, Xuehui Guo, Rui Wang, April B. Leytem, Chase Calkins, Elizabeth Berry, Kang Sun, Markus Müller, Armin Wisthaler, Vivienne H. Payne, Mark W. Shephard, Mark A. Zondlo, and Valentin Kantchev
Atmos. Meas. Tech., 17, 15–36, https://doi.org/10.5194/amt-17-15-2024, https://doi.org/10.5194/amt-17-15-2024, 2024
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Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
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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.
Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Haipeng Lin, Elizabeth W. Lundgren, Steve Goldhaber, Steven R. H. Barrett, and Daniel J. Jacob
Geosci. Model Dev., 15, 8669–8704, https://doi.org/10.5194/gmd-15-8669-2022, https://doi.org/10.5194/gmd-15-8669-2022, 2022
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We bring the state-of-the-science chemistry module GEOS-Chem into the Community Earth System Model (CESM). We show that some known differences between results from GEOS-Chem and CESM's CAM-chem chemistry module may be due to the configuration of model meteorology rather than inherent differences in the model chemistry. This is a significant step towards a truly modular Earth system model and allows two strong but currently separate research communities to benefit from each other's advances.
Nicole A. June, Anna L. Hodshire, Elizabeth B. Wiggins, Edward L. Winstead, Claire E. Robinson, K. Lee Thornhill, Kevin J. Sanchez, Richard H. Moore, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Matthew M. Coggon, Jonathan M. Dean-Day, T. Paul Bui, Jeff Peischl, Robert J. Yokelson, Matthew J. Alvarado, Sonia M. Kreidenweis, Shantanu H. Jathar, and Jeffrey R. Pierce
Atmos. Chem. Phys., 22, 12803–12825, https://doi.org/10.5194/acp-22-12803-2022, https://doi.org/10.5194/acp-22-12803-2022, 2022
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The evolution of organic aerosol composition and size is uncertain due to variability within and between smoke plumes. We examine the impact of plume concentration on smoke evolution from smoke plumes sampled by the NASA DC-8 during FIREX-AQ. We find that observed organic aerosol and size distribution changes are correlated to plume aerosol mass concentrations. Additionally, coagulation explains the majority of the observed growth.
Helen M. Worden, Gene L. Francis, Susan S. Kulawik, Kevin W. Bowman, Karen Cady-Pereira, Dejian Fu, Jennifer D. Hegarty, Valentin Kantchev, Ming Luo, Vivienne H. Payne, John R. Worden, Róisín Commane, and Kathryn McKain
Atmos. Meas. Tech., 15, 5383–5398, https://doi.org/10.5194/amt-15-5383-2022, https://doi.org/10.5194/amt-15-5383-2022, 2022
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Satellite observations of global carbon monoxide (CO) are essential for understanding atmospheric chemistry and pollution sources. This paper describes a new data product using radiance measurements from the Cross-track Infrared Sounder (CrIS) instrument on the Suomi National Polar-orbiting Partnership (SNPP) satellite that provides vertical profiles of CO from single-field-of-view observations. We show how these satellite CO profiles compare to aircraft observations and evaluate their biases.
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.
Michael Sitwell, Mark W. Shephard, Yves Rochon, Karen Cady-Pereira, and Enrico Dammers
Atmos. Chem. Phys., 22, 6595–6624, https://doi.org/10.5194/acp-22-6595-2022, https://doi.org/10.5194/acp-22-6595-2022, 2022
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Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
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.
Jennifer D. Hegarty, Karen E. Cady-Pereira, Vivienne H. Payne, Susan S. Kulawik, John R. Worden, Valentin Kantchev, Helen M. Worden, Kathryn McKain, Jasna V. Pittman, Róisín Commane, Bruce C. Daube Jr., and Eric A. Kort
Atmos. Meas. Tech., 15, 205–223, https://doi.org/10.5194/amt-15-205-2022, https://doi.org/10.5194/amt-15-205-2022, 2022
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Carbon monoxide (CO) is produced by combustion of substances such as fossil fuels and plays an important role in atmospheric pollution and climate. We evaluated estimates of atmospheric CO derived from outgoing radiation measurements of the Atmospheric Infrared Sounder (AIRS) on a satellite orbiting the Earth against CO measurements from aircraft to show that these satellite measurements are reliable for continuous global monitoring of atmospheric CO concentrations.
Anna L. Hodshire, Emily Ramnarine, Ali Akherati, Matthew L. Alvarado, Delphine K. Farmer, Shantanu H. Jathar, Sonia M. Kreidenweis, Chantelle R. Lonsdale, Timothy B. Onasch, Stephen R. Springston, Jian Wang, Yang Wang, Lawrence I. Kleinman, Arthur J. Sedlacek III, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 6839–6855, https://doi.org/10.5194/acp-21-6839-2021, https://doi.org/10.5194/acp-21-6839-2021, 2021
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Biomass burning emits particles and vapors that can impact both health and climate. Here, we investigate the role of dilution in the evolution of aerosol size and composition in observed US wildfire smoke plumes. Centers of plumes dilute more slowly than edges. We see differences in concentrations and composition between the centers and edges both in the first measurement and in subsequent measurements. Our findings support the hypothesis that plume dilution influences smoke aging.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Nikolaos Evangeliou, Yves Balkanski, Sabine Eckhardt, Anne Cozic, Martin Van Damme, Pierre-François Coheur, Lieven Clarisse, Mark W. Shephard, Karen E. Cady-Pereira, and Didier Hauglustaine
Atmos. Chem. Phys., 21, 4431–4451, https://doi.org/10.5194/acp-21-4431-2021, https://doi.org/10.5194/acp-21-4431-2021, 2021
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Ammonia, a substance that has played a key role in sustaining life, has been increasing in the atmosphere, affecting climate and humans. Understanding the reasons for this increase is important for the beneficial use of ammonia. The evolution of satellite products gives us the opportunity to calculate ammonia emissions easier. We calculated global ammonia emissions over the last 10 years, incorporated them into a chemistry model and recorded notable improvement in reproducing observations.
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.
Inés Sanz-Morère, Sebastian D. Eastham, Florian Allroggen, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 21, 1649–1681, https://doi.org/10.5194/acp-21-1649-2021, https://doi.org/10.5194/acp-21-1649-2021, 2021
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Contrails cause ~50 % of aviation climate impacts, but this is highly uncertain. This is partly due to the effect of overlap between contrails and other cloud layers. We developed a model to quantify this effect, finding that overlap with natural clouds increased contrails' radiative forcing in 2015. This suggests that cloud avoidance may help in reducing aviation's climate impacts. We also find that contrail–contrail overlap reduces impacts by ~3 %, increasing non-linearly with optical depth.
Susan S. Kulawik, John R. Worden, Vivienne H. Payne, Dejian Fu, Steven C. Wofsy, Kathryn McKain, Colm Sweeney, Bruce C. Daube Jr., Alan Lipton, Igor Polonsky, Yuguang He, Karen E. Cady-Pereira, Edward J. Dlugokencky, Daniel J. Jacob, and Yi Yin
Atmos. Meas. Tech., 14, 335–354, https://doi.org/10.5194/amt-14-335-2021, https://doi.org/10.5194/amt-14-335-2021, 2021
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This paper shows comparisons of a new single-footprint methane product from the AIRS satellite to aircraft-based observations. We show that this AIRS methane product provides useful information to study seasonal and global methane trends of this important greenhouse gas.
David H. Hagan and Jesse H. Kroll
Atmos. Meas. Tech., 13, 6343–6355, https://doi.org/10.5194/amt-13-6343-2020, https://doi.org/10.5194/amt-13-6343-2020, 2020
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Assessing the error of low-cost particulate matter (PM) sensors has been difficult as each empirical study presents unique limitations. Here, we present a new, open-sourced, physics-based model (opcsim) and use it to understand how the properties of different particle sensors alter their accuracy. We offer a summary of likely sources of error for different sensor types, environmental conditions, and particle classes and offer recommendations for the choice of optimal calibrant.
Chantelle R. Lonsdale, Matthew J. Alvarado, Anna L. Hodshire, Emily Ramnarine, and Jeffrey R. Pierce
Geosci. Model Dev., 13, 4579–4593, https://doi.org/10.5194/gmd-13-4579-2020, https://doi.org/10.5194/gmd-13-4579-2020, 2020
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The System for Atmospheric Modelling (SAM) has been coupled with the detailed gas/aerosol chemistry model, the Aerosol Simulation Program (ASP), to capture cross-plume concentration gradients as fire plumes evolve downwind. SAM-ASP v1.0 will lead to the development of parameterizations of near-source biomass burning chemistry that can be used to more accurately simulate biomass burning chemical and physical transformations of trace gases and aerosols within coarser chemical transport models.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
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.
Thibaud M. Fritz, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 20, 5697–5727, https://doi.org/10.5194/acp-20-5697-2020, https://doi.org/10.5194/acp-20-5697-2020, 2020
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Aircraft exhaust drives formation of ozone and is a dominant anthropogenic influence in the upper troposphere. These impacts are mitigated by non-linear chemistry inside the aircraft plume, which cuts off part of the ozone production pathway and reduces the long-term impact of aircraft in a way which is not captured by current models. The ice clouds which form in aircraft exhaust ("contrails") also play a role, converting emitted nitrogen oxides into more stable forms such as nitric acid.
Robert L. Herman, John Worden, David Noone, Dean Henze, Kevin Bowman, Karen Cady-Pereira, Vivienne H. Payne, Susan S. Kulawik, and Dejian Fu
Atmos. Meas. Tech., 13, 1825–1834, https://doi.org/10.5194/amt-13-1825-2020, https://doi.org/10.5194/amt-13-1825-2020, 2020
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This study is the first assessment and validation of AIRS HDO / H2O retrieved by optimal estimation. Initial comparisons with in situ measurements from NASA ORACLES are promising: the small bias and consistent rms of AIRS suggest that AIRS has well-characterized HDO / H2O. This analysis opens the possibility of a new 17-year long-term data record of global tropospheric HDO / H2O measured from space.
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.
Mark W. Shephard, Enrico Dammers, Karen E. Cady-Pereira, Shailesh K. Kharol, Jesse Thompson, Yonatan Gainariu-Matz, Junhua Zhang, Chris A. McLinden, Andrew Kovachik, Michael Moran, Shabtai Bittman, Christopher E. Sioris, Debora Griffin, Matthew J. Alvarado, Chantelle Lonsdale, Verica Savic-Jovcic, and Qiong Zheng
Atmos. Chem. Phys., 20, 2277–2302, https://doi.org/10.5194/acp-20-2277-2020, https://doi.org/10.5194/acp-20-2277-2020, 2020
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Presented is a description and survey demonstrating the capabilities of the CrIS ammonia product for monitoring, air quality forecast model evaluation, dry deposition estimates, and emission estimates of an agricultural hotspot.
Crystal D. McClure, Christopher Y. Lim, David H. Hagan, Jesse H. Kroll, and Christopher D. Cappa
Atmos. Chem. Phys., 20, 1531–1547, https://doi.org/10.5194/acp-20-1531-2020, https://doi.org/10.5194/acp-20-1531-2020, 2020
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We characterized various optical, chemical, and physical properties of particles produced from combustion of a variety of different biomass fuels, many representative of those found in the western US. We find that many properties scale with the ratio between bulk average organic aerosol and black carbon mass concentrations, although there are some properties that do not.
Abigail R. Koss, Manjula R. Canagaratna, Alexander Zaytsev, Jordan E. Krechmer, Martin Breitenlechner, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joseph R. Roscioli, Frank N. Keutsch, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 1021–1041, https://doi.org/10.5194/acp-20-1021-2020, https://doi.org/10.5194/acp-20-1021-2020, 2020
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Oxidation chemistry of organic compounds in the atmosphere produces a diverse spectrum of products. This diversity is difficult to represent in air quality and climate models, and in laboratory experiments it results in large and complex datasets. This work evaluates several methods to simplify the chemistry of oxidation systems in environmental chambers, including positive matrix factorization, hierarchical clustering analysis, and gamma kinetics parameterization.
Camille Viatte, Tianze Wang, Martin Van Damme, Enrico Dammers, Frederik Meleux, Lieven Clarisse, Mark W. Shephard, Simon Whitburn, Pierre François Coheur, Karen E. Cady-Pereira, and Cathy Clerbaux
Atmos. Chem. Phys., 20, 577–596, https://doi.org/10.5194/acp-20-577-2020, https://doi.org/10.5194/acp-20-577-2020, 2020
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We study concentrations and spatiotemporal variabilities of atmospheric NH3 from the agricultural sector to gain insights on its effects on the Paris megacity air quality using satellite data from IASI and CrIS.
We evaluate the regional CHIMERE model capacity to reproduce NH3 and particulate matter (PM2.5) concentrations and variabilities in the domain of study.
We quantify the main meteorological parameters driving the optimal conditions involved in the PM2.5 formation from NH3 in Paris.
Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
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.
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Enrico Dammers, Chris A. McLinden, Debora Griffin, Mark W. Shephard, Shelley Van Der Graaf, Erik Lutsch, Martijn Schaap, Yonatan Gainairu-Matz, Vitali Fioletov, Martin Van Damme, Simon Whitburn, Lieven Clarisse, Karen Cady-Pereira, Cathy Clerbaux, Pierre Francois Coheur, and Jan Willem Erisman
Atmos. Chem. Phys., 19, 12261–12293, https://doi.org/10.5194/acp-19-12261-2019, https://doi.org/10.5194/acp-19-12261-2019, 2019
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Ammonia is an essential molecule in the environment, but at its current levels it is unsustainable. However, the emissions are highly uncertain. We explore the use of satellites to estimate the ammonia lifetime and emissions around point sources to help improve the budget. The same method applied to different satellite instruments shows consistent results. Comparison to the emission inventories shows that those are underestimating emissions of point sources by on average a factor of 2.5.
Emily Ramnarine, John K. Kodros, Anna L. Hodshire, Chantelle R. Lonsdale, Matthew J. Alvarado, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 6561–6577, https://doi.org/10.5194/acp-19-6561-2019, https://doi.org/10.5194/acp-19-6561-2019, 2019
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Biomass burning aerosols have important global radiative effects that depend on particle size. However, model estimates of these effects do not explicitly account for the coagulation of particles in biomass burning plumes. In this work, we present the first use of a sub-grid coagulation scheme in a global aerosol model to account for in-plume coagulation. We find that this in-plume coagulation leads to important changes in the biomass burning aerosol radiative effects.
John R. Worden, Susan S. Kulawik, Dejian Fu, Vivienne H. Payne, Alan E. Lipton, Igor Polonsky, Yuguang He, Karen Cady-Pereira, Jean-Luc Moncet, Robert L. Herman, Fredrick W. Irion, and Kevin W. Bowman
Atmos. Meas. Tech., 12, 2331–2339, https://doi.org/10.5194/amt-12-2331-2019, https://doi.org/10.5194/amt-12-2331-2019, 2019
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In this paper we take the first steps towards generating a multi-decadal record of the deuterium content of water vapor, useful for evaluating the moisture sources and processes affecting water vapor, by estimating the deuterium content from thermal IR radiances from the AIRS instrument. We find the AIRS-based measurements are sensitive to the deuterium content of water vapor in the middle and lower troposphere with a single measurement uncertainty of ~ 3 % and an accuracy of ~ 0.7 %.
Alexander Zaytsev, Martin Breitenlechner, Abigail R. Koss, Christopher Y. Lim, James C. Rowe, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 1861–1870, https://doi.org/10.5194/amt-12-1861-2019, https://doi.org/10.5194/amt-12-1861-2019, 2019
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We present the development of a chemical ionization mass spectrometer which can be operated with either ammonium (NH4+) or hydronium (H3O+) as the reagent ion. We describe a mass spectrometric voltage scanning procedure based on collision-induced dissociation that allows us to determine the stability of detected ammonium–organic ions and hence constrain the sensitivity of the instrument to a wide range of organic compounds that cannot be calibrated directly.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671, https://doi.org/10.5194/amt-12-1659-2019, https://doi.org/10.5194/amt-12-1659-2019, 2019
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Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
Cristen Adams, Chris A. McLinden, Mark W. Shephard, Nolan Dickson, Enrico Dammers, Jack Chen, Paul Makar, Karen E. Cady-Pereira, Naomi Tam, Shailesh K. Kharol, Lok N. Lamsal, and Nickolay A. Krotkov
Atmos. Chem. Phys., 19, 2577–2599, https://doi.org/10.5194/acp-19-2577-2019, https://doi.org/10.5194/acp-19-2577-2019, 2019
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We estimated how much carbon monoxide, ammonia, and nitrogen oxides were emitted in the smoke from the Fort McMurray Horse River wildfire using satellite data and air quality models. The fire emitted amounts of carbon monoxide that were similar to anthropogenic (human-caused) emissions for all of Alberta over a full year. We also estimated large amounts of ammonia and nitrogen oxides emitted from the fire. These results can be used to evaluate the performance of air quality forecasting models.
Kang Sun, Lei Zhu, Karen Cady-Pereira, Christopher Chan Miller, Kelly Chance, Lieven Clarisse, Pierre-François Coheur, Gonzalo González Abad, Guanyu Huang, Xiong Liu, Martin Van Damme, Kai Yang, and Mark Zondlo
Atmos. Meas. Tech., 11, 6679–6701, https://doi.org/10.5194/amt-11-6679-2018, https://doi.org/10.5194/amt-11-6679-2018, 2018
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An agile, physics-based approach is developed to oversample irregular satellite observations to a high-resolution common grid. Instead of assuming each sounding as a point or a polygon as in previous methods, the proposed physical oversampling represents soundings as distributions of sensitivity on the ground. This sensitivity distribution can be determined by the spatial response function of each satellite sensor, parameterized as generalized 2-D super Gaussian functions.
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.
Anna L. Hodshire, Brett B. Palm, M. Lizabeth Alexander, Qijing Bian, Pedro Campuzano-Jost, Eben S. Cross, Douglas A. Day, Suzane S. de Sá, Alex B. Guenther, Armin Hansel, James F. Hunter, Werner Jud, Thomas Karl, Saewung Kim, Jesse H. Kroll, Jeong-Hoo Park, Zhe Peng, Roger Seco, James N. Smith, Jose L. Jimenez, and Jeffrey R. Pierce
Atmos. Chem. Phys., 18, 12433–12460, https://doi.org/10.5194/acp-18-12433-2018, https://doi.org/10.5194/acp-18-12433-2018, 2018
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We investigate the nucleation and growth processes that shape the aerosol size distribution inside oxidation flow reactors (OFRs) that sampled ambient air from Colorado and the Amazon rainforest. Results indicate that organics are important for both nucleation and growth, vapor uptake was limited to accumulation-mode particles, fragmentation reactions were important to limit particle growth at higher OH exposures, and an H2SO4-organics nucleation mechanism captured new particle formation well.
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.
Emily V. Fischer, Liye Zhu, Vivienne H. Payne, John R. Worden, Zhe Jiang, Susan S. Kulawik, Steven Brey, Arsineh Hecobian, Daniel Gombos, Karen Cady-Pereira, and Frank Flocke
Atmos. Chem. Phys., 18, 5639–5653, https://doi.org/10.5194/acp-18-5639-2018, https://doi.org/10.5194/acp-18-5639-2018, 2018
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PAN is an atmospheric reservoir for nitrogen oxide radicals, and it plays a lead role in their redistribution in the troposphere. We analyze new Tropospheric Emission Spectrometer (TES) PAN observations over North America during July 2006 to 2009. We identify smoke-impacted TES PAN retrievals by co-location with NOAA Hazard Mapping System (HMS) smoke plumes. Depending on the year, 15–32 % of cases where elevated PAN is identified in TES observations overlap with smoke plumes.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Cynthia H. Whaley, Paul A. Makar, Mark W. Shephard, Leiming Zhang, Junhua Zhang, Qiong Zheng, Ayodeji Akingunola, Gregory R. Wentworth, Jennifer G. Murphy, Shailesh K. Kharol, and Karen E. Cady-Pereira
Atmos. Chem. Phys., 18, 2011–2034, https://doi.org/10.5194/acp-18-2011-2018, https://doi.org/10.5194/acp-18-2011-2018, 2018
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Using a modified air quality forecasting model, we have found that a significant fraction (> 50 %) of ambient ammonia comes from re-emission from plants and soils in the broader Athabasca Oil Sands region and much of Alberta and Saskatchewan. We also found that about 20 % of ambient ammonia in Alberta and Saskatchewan came from forest fires in the summer of 2013. The addition of these two processes improved modelled ammonia, which was a motivating factor in undertaking this research.
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.
Karen E. Cady-Pereira, Vivienne H. Payne, Jessica L. Neu, Kevin W. Bowman, Kazuyuki Miyazaki, Eloise A. Marais, Susan Kulawik, Zitely A. Tzompa-Sosa, and Jennifer D. Hegarty
Atmos. Chem. Phys., 17, 9379–9398, https://doi.org/10.5194/acp-17-9379-2017, https://doi.org/10.5194/acp-17-9379-2017, 2017
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Air quality is a major issue for megacities. Our paper looks at satellite measurements over Mexico City and Lagos of several trace gases gases related to air quality to determine the temporal and spatial variability of these gases, and it relates this variability to local conditions, such as topography, winds and biomass burning events. We find that, while Mexico City is known for severe pollution events, the levels of of pollution in Lagos are much higher and more persistent.
Enrico Dammers, Mark W. Shephard, Mathias Palm, Karen Cady-Pereira, Shannon Capps, Erik Lutsch, Kim Strong, James W. Hannigan, Ivan Ortega, Geoffrey C. Toon, Wolfgang Stremme, Michel Grutter, Nicholas Jones, Dan Smale, Jacob Siemons, Kevin Hrpcek, Denis Tremblay, Martijn Schaap, Justus Notholt, and Jan Willem Erisman
Atmos. Meas. Tech., 10, 2645–2667, https://doi.org/10.5194/amt-10-2645-2017, https://doi.org/10.5194/amt-10-2645-2017, 2017
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Presented here is the validation of the CrIS fast physical retrieval (CFPR) NH3 column and profile measurements using ground-based Fourier transform infrared (FTIR) observations. The overall FTIR and CrIS total columns have a positive correlation of r = 0.77 (N = 218) with very little bias (a slope of 1.02). Furthermore, we find that CrIS and FTIR profile comparison differences are mostly within the range of the estimated retrieval uncertainties, with differences in the range of ~ 20 to 40 %.
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.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
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.
Carly L. Reddington, Dominick V. Spracklen, Paulo Artaxo, David A. Ridley, Luciana V. Rizzo, and Andrea Arana
Atmos. Chem. Phys., 16, 11083–11106, https://doi.org/10.5194/acp-16-11083-2016, https://doi.org/10.5194/acp-16-11083-2016, 2016
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We use a global aerosol model evaluated against long-term observations of surface aerosol and aerosol optical depth (AOD) to better understand the impacts of biomass burning on tropical aerosol. We use three satellite-derived fire emission datasets in the model, identifying regions where these datasets capture observations and where emissions are likely to be underestimated. For coincident observations of surface aerosol and AOD, model underestimation of AOD is greater than of surface aerosol.
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.
John K. Kodros, Rachel Cucinotta, David A. Ridley, Christine Wiedinmyer, and Jeffrey R. Pierce
Atmos. Chem. Phys., 16, 6771–6784, https://doi.org/10.5194/acp-16-6771-2016, https://doi.org/10.5194/acp-16-6771-2016, 2016
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We provide a first estimate of the aerosol radiative effects from open, uncontrolled combustion of domestic waste. We find the direct and cloud-albedo indirect radiative effects are predominantly negative (cooling tendency) with regional forcings exceeding −0.4 W m−2; however, the magnitude of these effects depends on the assumed emitted aerosol size, mass, and optical properties.
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.
Brett B. Palm, Pedro Campuzano-Jost, Amber M. Ortega, Douglas A. Day, Lisa Kaser, Werner Jud, Thomas Karl, Armin Hansel, James F. Hunter, Eben S. Cross, Jesse H. Kroll, Zhe Peng, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 2943–2970, https://doi.org/10.5194/acp-16-2943-2016, https://doi.org/10.5194/acp-16-2943-2016, 2016
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Ambient pine forest air was oxidized by OH radicals in a PAM oxidation flow reactor during the BEACHON-RoMBAS campaign to study secondary organic aerosol formation. Approximately 4.4 times more secondary organic aerosol was formed in the reactor than could be explained by the volatile organic gases (VOCs) measured in ambient air. The organic aerosol formation can be explained by including an SOA yield from typically unmeasured semivolatile and intermediate-volatility organic gases (S/IVOCs).
Melanie S. Hammer, Randall V. Martin, Aaron van Donkelaar, Virginie Buchard, Omar Torres, David A. Ridley, and Robert J. D. Spurr
Atmos. Chem. Phys., 16, 2507–2523, https://doi.org/10.5194/acp-16-2507-2016, https://doi.org/10.5194/acp-16-2507-2016, 2016
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We interpret satellite observations to infer the global absorption properties of brown carbon (BrC) aerosols. We incorporate these BrC absorption properties into a chemical transport model to estimate global direct radiative effects and changes in hydroxyl radical (OH) concentrations. To our knowledge, this is the first time the effect of BrC absorption on atmospheric photochemistry has been considered in a global chemical transport model.
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.
M. W. Shephard, C. A. McLinden, K. E. Cady-Pereira, M. Luo, S. G. Moussa, A. Leithead, J. Liggio, R. M. Staebler, A. Akingunola, P. Makar, P. Lehr, J. Zhang, D. K. Henze, D. B. Millet, J. O. Bash, L. Zhu, K. C. Wells, S. L. Capps, S. Chaliyakunnel, M. Gordon, K. Hayden, J. R. Brook, M. Wolde, and S.-M. Li
Atmos. Meas. Tech., 8, 5189–5211, https://doi.org/10.5194/amt-8-5189-2015, https://doi.org/10.5194/amt-8-5189-2015, 2015
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This study provides direct validations of Tropospheric Emission Spectrometer (TES) satellite retrieved profiles against coincident aircraft profiles of carbon monoxide, ammonia, methanol, and formic acid, all of which are of interest for air quality. The comparisons are performed over the Canadian oil sands region during an intensive field campaign in support of the Joint Canada-Alberta Implementation Plan for the Oil Sands Monitoring (JOSM). Initial model evaluations are also provided.
L. Zhu, D. Henze, J. Bash, G.-R. Jeong, K. Cady-Pereira, M. Shephard, M. Luo, F. Paulot, and S. Capps
Atmos. Chem. Phys., 15, 12823–12843, https://doi.org/10.5194/acp-15-12823-2015, https://doi.org/10.5194/acp-15-12823-2015, 2015
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We implement new diurnal variation scheme for ammonia livestock emissions and bidirectional exchange scheme and its adjoint in the GEOS-Chem global chemical transport model. Updated diurnal variability improves modeled-to-hourly in situ measurements comparison. The ammonium soil pool in the bidirectional exchange model largely extends the ammonia lifetime in the atmosphere. Large model biases remain as livestock emissions are still underestimated.
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
F. D. Lopez-Hilfiker, C. Mohr, M. Ehn, F. Rubach, E. Kleist, J. Wildt, Th. F. Mentel, A. J. Carrasquillo, K. E. Daumit, J. F. Hunter, J. H. Kroll, D. R. Worsnop, and J. A. Thornton
Atmos. Chem. Phys., 15, 7765–7776, https://doi.org/10.5194/acp-15-7765-2015, https://doi.org/10.5194/acp-15-7765-2015, 2015
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We measured a large suite organic compounds using a recently developed Filter Inlet for Gases and AEROsols (FIGAERO) coupled to a (HR-ToF-CIMS). The instrument was deployed on environmental simulation chambers to study monoterpene oxidation as a secondary organic aerosol (SOA) source. We find that approximately 50% of the detected particle phase mass is associated with compounds having effective vapor pressures 4, or more, orders of magnitude lower than commonly measured products.
M. J. Alvarado, C. R. Lonsdale, R. J. Yokelson, S. K. Akagi, H. Coe, J. S. Craven, E. V. Fischer, G. R. McMeeking, J. H. Seinfeld, T. Soni, J. W. Taylor, D. R. Weise, and C. E. Wold
Atmos. Chem. Phys., 15, 6667–6688, https://doi.org/10.5194/acp-15-6667-2015, https://doi.org/10.5194/acp-15-6667-2015, 2015
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Being able to understand and simulate the chemical evolution of biomass burning smoke plumes under a wide variety of conditions is a critical part of forecasting the impact of these fires on air quality, atmospheric composition, and climate. Here we use an improved model of this chemistry to simulate the evolution of ozone and secondary organic aerosol within a young biomass burning smoke plume from the Williams prescribed burn in chaparral, which was sampled over California in November 2009.
S. R. Arnold, L. K. Emmons, S. A. Monks, K. S. Law, D. A. Ridley, S. Turquety, S. Tilmes, J. L. Thomas, I. Bouarar, J. Flemming, V. Huijnen, J. Mao, B. N. Duncan, S. Steenrod, Y. Yoshida, J. Langner, and Y. Long
Atmos. Chem. Phys., 15, 6047–6068, https://doi.org/10.5194/acp-15-6047-2015, https://doi.org/10.5194/acp-15-6047-2015, 2015
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The extent to which forest fires produce the air pollutant and greenhouse gas ozone (O3) in the atmosphere at high latitudes in not well understood. We have compared how fire emissions produce O3 and its precursors in several models of atmospheric chemistry. We find enhancements in O3 in air dominated by fires in all models, which increase on average as fire emissions age. We also find that in situ O3 production in the Arctic is sensitive to details of organic chemistry and vertical lifting.
M. W. Shephard and K. E. Cady-Pereira
Atmos. Meas. Tech., 8, 1323–1336, https://doi.org/10.5194/amt-8-1323-2015, https://doi.org/10.5194/amt-8-1323-2015, 2015
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Presented is a robust retrieval algorithm that demonstrates the capabilities of utilizing Cross-track Infrared Sounder (CrIS) satellite observations to globally retrieval ammonia (NH3) concentrations. Initial NH3 retrieval results show that CrIS is (i) sensitive to NH3 in the boundary layer, with peak vertical sensitivity typically around 850–750hPa (~2km), (ii) has a minimum detection limit of ~1ppbv (peak profile value typically at the surface), and (iii) typically has up to ~1 DOFS.
A. T. Lambe, P. S. Chhabra, T. B. Onasch, W. H. Brune, J. F. Hunter, J. H. Kroll, M. J. Cummings, J. F. Brogan, Y. Parmar, D. R. Worsnop, C. E. Kolb, and P. Davidovits
Atmos. Chem. Phys., 15, 3063–3075, https://doi.org/10.5194/acp-15-3063-2015, https://doi.org/10.5194/acp-15-3063-2015, 2015
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We compared the chemistry and yields of SOA generated from OH oxidation of gas-phase precursors in a flow reactor (high OH, short residence time) and environmental chambers (low OH, long residence time). We find that chemical composition of SOA produced in the flow reactor and in chambers is similar. SOA yields measured in the flow reactor are lower than in chambers. Seed particles increase the yield of SOA produced in the flow reactor and may account in part for higher SOA yields in chambers.
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.
M. J. Alvarado, V. H. Payne, K. E. Cady-Pereira, J. D. Hegarty, S. S. Kulawik, K. J. Wecht, J. R. Worden, J. V. Pittman, and S. C. Wofsy
Atmos. Meas. Tech., 8, 965–985, https://doi.org/10.5194/amt-8-965-2015, https://doi.org/10.5194/amt-8-965-2015, 2015
M. R. Canagaratna, J. L. Jimenez, J. H. Kroll, Q. Chen, S. H. Kessler, P. Massoli, L. Hildebrandt Ruiz, E. Fortner, L. R. Williams, K. R. Wilson, J. D. Surratt, N. M. Donahue, J. T. Jayne, and D. R. Worsnop
Atmos. Chem. Phys., 15, 253–272, https://doi.org/10.5194/acp-15-253-2015, https://doi.org/10.5194/acp-15-253-2015, 2015
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Atomic oxygen-to-carbon (O:C), hydrogen-to-carbon (H:C), and organic mass-to-organic carbon (OM:OC) ratios of ambient organic aerosol (OA) species provide key constraints for understanding their sources and impacts. Here an improved method for obtaining accurate O:C, H:C, and OM:OC with a widely used aerosol mass spectrometer is developed. These results imply that OA is more oxidized than previously estimated and indicate the need for new chemical mechanisms that simulate ambient oxidation.
V. H. Payne, M. J. Alvarado, K. E. Cady-Pereira, J. R. Worden, S. S. Kulawik, and E. V. Fischer
Atmos. Meas. Tech., 7, 3737–3749, https://doi.org/10.5194/amt-7-3737-2014, https://doi.org/10.5194/amt-7-3737-2014, 2014
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Peroxyacetyl nitrate (PAN) plays an important role in the distribution of lower-atmospheric ozone. PAN can be transported far from the original pollution source, leading to ozone formation and degraded air quality in remote areas. Satellite observations from the Tropospheric Emission Spectrometer (TES) are sensitive to PAN at lower altitude than previous global data sets. We describe characteristics of the data and show elevated PAN associated with boreal fires and outflow of Asian pollution.
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
K. E. Daumit, A. J. Carrasquillo, J. F. Hunter, and J. H. Kroll
Atmos. Chem. Phys., 14, 10773–10784, https://doi.org/10.5194/acp-14-10773-2014, https://doi.org/10.5194/acp-14-10773-2014, 2014
D. V. Spracklen and C. L. Heald
Atmos. Chem. Phys., 14, 9051–9059, https://doi.org/10.5194/acp-14-9051-2014, https://doi.org/10.5194/acp-14-9051-2014, 2014
J. L. Schnell, C. D. Holmes, A. Jangam, and M. J. Prather
Atmos. Chem. Phys., 14, 7721–7739, https://doi.org/10.5194/acp-14-7721-2014, https://doi.org/10.5194/acp-14-7721-2014, 2014
K. E. Cady-Pereira, S. Chaliyakunnel, M. W. Shephard, D. B. Millet, M. Luo, and K. C. Wells
Atmos. Meas. Tech., 7, 2297–2311, https://doi.org/10.5194/amt-7-2297-2014, https://doi.org/10.5194/amt-7-2297-2014, 2014
C. D. Holmes, M. J. Prather, and G. C. M. Vinken
Atmos. Chem. Phys., 14, 6801–6812, https://doi.org/10.5194/acp-14-6801-2014, https://doi.org/10.5194/acp-14-6801-2014, 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
G. W. Mann, K. S. Carslaw, C. L. Reddington, K. J. Pringle, M. Schulz, A. Asmi, D. V. Spracklen, D. A. Ridley, M. T. Woodhouse, L. A. Lee, K. Zhang, S. J. Ghan, R. C. Easter, X. Liu, P. Stier, Y. H. Lee, P. J. Adams, H. Tost, J. Lelieveld, S. E. Bauer, K. Tsigaridis, T. P. C. van Noije, A. Strunk, E. Vignati, N. Bellouin, M. Dalvi, C. E. Johnson, T. Bergman, H. Kokkola, K. von Salzen, F. Yu, G. Luo, A. Petzold, J. Heintzenberg, A. Clarke, J. A. Ogren, J. Gras, U. Baltensperger, U. Kaminski, S. G. Jennings, C. D. O'Dowd, R. M. Harrison, D. C. S. Beddows, M. Kulmala, Y. Viisanen, V. Ulevicius, N. Mihalopoulos, V. Zdimal, M. Fiebig, H.-C. Hansson, E. Swietlicki, and J. S. Henzing
Atmos. Chem. Phys., 14, 4679–4713, https://doi.org/10.5194/acp-14-4679-2014, https://doi.org/10.5194/acp-14-4679-2014, 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
K. C. Wells, D. B. Millet, K. E. Cady-Pereira, M. W. Shephard, D. K. Henze, N. Bousserez, E. C. Apel, J. de Gouw, C. Warneke, and H. B. Singh
Atmos. Chem. Phys., 14, 2555–2570, https://doi.org/10.5194/acp-14-2555-2014, https://doi.org/10.5194/acp-14-2555-2014, 2014
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
E. S. Cross, J. F. Hunter, A. J. Carrasquillo, J. P. Franklin, S. C. Herndon, J. T. Jayne, D. R. Worsnop, R. C. Miake-Lye, and J. H. Kroll
Atmos. Chem. Phys., 13, 7845–7858, https://doi.org/10.5194/acp-13-7845-2013, https://doi.org/10.5194/acp-13-7845-2013, 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
M. J. Alvarado, V. H. Payne, E. J. Mlawer, G. Uymin, M. W. Shephard, K. E. Cady-Pereira, J. S. Delamere, and J.-L. Moncet
Atmos. Chem. Phys., 13, 6687–6711, https://doi.org/10.5194/acp-13-6687-2013, https://doi.org/10.5194/acp-13-6687-2013, 2013
J. Worden, K. Wecht, C. Frankenberg, M. Alvarado, K. Bowman, E. Kort, S. Kulawik, M. Lee, V. Payne, and H. Worden
Atmos. Chem. Phys., 13, 3679–3692, https://doi.org/10.5194/acp-13-3679-2013, https://doi.org/10.5194/acp-13-3679-2013, 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: Physics (physical properties and processes)
Improved simulations of biomass burning aerosol optical properties and lifetimes in the NASA GEOS Model during the ORACLES-I campaign
Sharp increase in Saharan dust intrusions over the western Euro-Mediterranean in February–March 2020–2022 and associated atmospheric circulation
Temporal and spatial variations in dust activity in Australia based on remote sensing and reanalysis datasets
Sensitivity of global direct aerosol shortwave radiative forcing to uncertainties in aerosol optical properties
Molecular-level study on the role of methanesulfonic acid in iodine oxoacid nucleation
Regional to global distributions, trends, and drivers of biogenic volatile organic compound emission from 2001 to 2020
Impacts of ice-nucleating particles on cirrus clouds and radiation derived from global model simulations with MADE3 in EMAC
Seasonal characteristics of emission, distribution, and radiative effect of marine organic aerosols over the western Pacific Ocean: an investigation with a coupled regional climate aerosol model
Fire–precipitation interactions amplify the quasi-biennial variability in fires over southern Mexico and Central America
Improved estimates of smoke exposure during Australia fire seasons: importance of quantifying plume injection heights
New particle formation induced by anthropogenic–biogenic interactions on the southeastern Tibetan Plateau
Investigation of observed dust trends over the Middle East region in NASA Goddard Earth Observing System (GEOS) model simulations
A new process-based and scale-aware desert dust emission scheme for global climate models – Part II: Evaluation in the Community Earth System Model version 2 (CESM2)
Aerosols in the central Arctic cryosphere: Satellite and model integrated insights during Arctic spring and summer
How well do Earth system models reproduce the observed aerosol response to rapid emission reductions? A COVID-19 case study
Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations
Impact of acidity and surface-modulated acid dissociation on cloud response to organic aerosol
The contribution of residential wood combustion to the PM2.5 concentrations in the Helsinki metropolitan area
Analysis of atmospheric particle growth based on vapor concentrations measured at the high-altitude GAW station Chacaltaya in the Bolivian Andes
Expanding the simulation of East Asian super dust storms: physical transport mechanisms impacting the western Pacific
Improving 3-day deterministic air pollution forecasts using machine learning algorithms
Opinion: The importance of historical and paleoclimate aerosol radiative effects
Assessing the assimilation of Himawari-8 observations on aerosol forecasts and radiative effects during pollution transport from South Asia to the Tibetan Plateau
Aerosol–meteorology feedback diminishes the transboundary transport of black carbon into the Tibetan Plateau
Associations of interannual variation in summer tropospheric ozone with the Western Pacific Subtropical High in China from 1999 to 2017
Climate intervention using marine cloud brightening (MCB) compared with stratospheric aerosol injection (SAI) in the UKESM1 climate model
Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 2: Strong surfactants
Increased importance of aerosol–cloud interactions for surface PM2.5 pollution relative to aerosol–radiation interactions in China with the anthropogenic emission reductions
The role of temporal scales in extracting dominant meteorological drivers of major airborne pollutants
Biomass-burning smoke's properties and its interactions with marine stratocumulus clouds in WRF-CAM5 and southeastern Atlantic field campaigns
Air pollution trapping in the Dresden Basin from gray-zone scale urban modeling
The effect of atmospherically relevant aminium salts on water uptake
Droplet collection efficiencies estimated from satellite retrievals constrain effective radiative forcing of aerosol-cloud interactions
Intercomparison of Aerosol Optical Depths from four reanalyses and their multi-reanalysis-consensus
The impact of aerosols on stratiform clouds over southern West Africa: a large-eddy-simulation study
Numerical simulation and evaluation of global ultrafine particle concentrations at the Earth's surface
Rapid Iodine Oxoacids Nucleation Enhanced by Dimethylamine in Broad Marine Regions
Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
Global aviation contrail climate effects from 2019 to 2021
Global aerosol typing classification using a new hybrid algorithm utilizing Aerosol Robotic Network data
Diagnosing uncertainties in global biomass burning emission inventories and their impact on modeled air pollutants
The underappreciated role of transboundary pollution in future air quality and health improvements in China
The export of African mineral dust across the Atlantic and its impact over the Amazon Basin
Assimilation of POLDER observations to estimate aerosol emissions
Role of atmospheric aerosols in severe winter fog over Indo Gangetic Plains of India: a case study
Effect of radiation interaction and aerosol processes on ventilation and aerosol concentrations in a real urban neighbourhood in Helsinki
Numerical evidence that the impact of CCN and INP concentrations on mixed-phase clouds is observable with cloud radars
Atlantic Multidecadal Oscillation modulates the relationship between El Niño–Southern Oscillation and fire weather in Australia
Phase state and viscosity of secondary organic aerosols over China simulated by WRF-Chem
Identifying climate model structural inconsistencies allows for tight constraint of aerosol radiative forcing
Sampa Das, Peter R. Colarco, Huisheng Bian, and Santiago Gassó
Atmos. Chem. Phys., 24, 4421–4449, https://doi.org/10.5194/acp-24-4421-2024, https://doi.org/10.5194/acp-24-4421-2024, 2024
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The smoke aerosols emitted from vegetation burning can alter the regional energy budget via multiple pathways. We utilized detailed observations from the NASA ORACLES airborne campaign based in Namibia during September 2016 to improve the representation of smoke aerosol properties and lifetimes in our GEOS Earth system model. The improved model simulations are for the first time able to capture the observed changes in the smoke absorption during long-range plume transport.
Emilio Cuevas-Agulló, David Barriopedro, Rosa Delia García, Silvia Alonso-Pérez, Juan Jesús González-Alemán, Ernest Werner, David Suárez, Juan José Bustos, Gerardo García-Castrillo, Omaira García, África Barreto, and Sara Basart
Atmos. Chem. Phys., 24, 4083–4104, https://doi.org/10.5194/acp-24-4083-2024, https://doi.org/10.5194/acp-24-4083-2024, 2024
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During February–March (FM) 2020–2022, unusually intense dust storms from northern Africa hit the western Euro-Mediterranean (WEM). Using dust products from satellites and atmospheric reanalysis for 2003–2022, results show that cut-off lows and European blocking are key drivers of FM dust intrusions over the WEM. A higher frequency of cut-off lows associated with subtropical ridges is observed in the late 2020–2022 period.
Yahui Che, Bofu Yu, and Katherine Bracco
Atmos. Chem. Phys., 24, 4105–4128, https://doi.org/10.5194/acp-24-4105-2024, https://doi.org/10.5194/acp-24-4105-2024, 2024
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Dust events occur more frequently during the Austral spring and summer in dust regions, including central Australia, the southwest of Western Australia, and the northern and southern regions of eastern Australia using remote sensing and reanalysis datasets. High-concentration dust is distributed around central Australia and in the downwind northern and southern Australia. Typically, around 50 % of the dust lifted settles on Australian land, with the remaining half being deposited in the ocean.
Jonathan Elsey, Nicolas Bellouin, and Claire Ryder
Atmos. Chem. Phys., 24, 4065–4081, https://doi.org/10.5194/acp-24-4065-2024, https://doi.org/10.5194/acp-24-4065-2024, 2024
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Aerosols influence the Earth's energy balance. The uncertainty in this radiative forcing is large depending partly on uncertainty in measurements of aerosol optical properties. We have developed a freely available new framework of millions of radiative transfer simulations spanning aerosol uncertainty and assess the impact on radiative forcing uncertainty. We find that reducing these uncertainties would reduce radiative forcing uncertainty, but non-aerosol uncertainties must also be considered.
Jing Li, Nan Wu, Biwu Chu, An Ning, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 3989–4000, https://doi.org/10.5194/acp-24-3989-2024, https://doi.org/10.5194/acp-24-3989-2024, 2024
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Iodic acid (HIO3) nucleates with iodous acid (HIO2) efficiently in marine areas; however, whether methanesulfonic acid (MSA) can synergistically participate in the HIO3–HIO2-based nucleation is unclear. We provide molecular-level evidence that MSA can efficiently promote the formation of HIO3–HIO2-based clusters using a theoretical approach. The proposed MSA-enhanced iodine nucleation mechanism may help us to deeply understand marine new particle formation events with bursts of iodine particles.
Hao Wang, Xiaohong Liu, Chenglai Wu, and Guangxing Lin
Atmos. Chem. Phys., 24, 3309–3328, https://doi.org/10.5194/acp-24-3309-2024, https://doi.org/10.5194/acp-24-3309-2024, 2024
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We quantified different global- and regional-scale drivers of biogenic volatile organic compound (BVOC) emission trends over the past 20 years. The results show that global greening trends significantly boost BVOC emissions and deforestation reduces BVOC emissions in South America and Southeast Asia. Elevated temperature in Europe and increased soil moisture in East and South Asia enhance BVOC emissions. The results deepen our understanding of long-term BVOC emission trends in hotspots.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 24, 3217–3240, https://doi.org/10.5194/acp-24-3217-2024, https://doi.org/10.5194/acp-24-3217-2024, 2024
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Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, the understanding of their global impacts is still uncertain. We perform numerical simulations with a global aerosol–climate model to analyse INP-induced cirrus changes and the resulting climate impacts. We evaluate various sources of uncertainties, e.g. the ice-nucleating ability of INPs and the role of model dynamics, and provide a new estimate for the global INP–cirrus effect.
Jiawei Li, Zhiwei Han, Pingqing Fu, Xiaohong Yao, and Mingjie Liang
Atmos. Chem. Phys., 24, 3129–3161, https://doi.org/10.5194/acp-24-3129-2024, https://doi.org/10.5194/acp-24-3129-2024, 2024
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Organic aerosols of marine origin are important for aerosol climatic effects but are poorly understood. For the first time, an online coupled regional chemistry–climate model is applied to explore the characteristics of emission, distribution, and direct and indirect radiative effects of marine organic aerosols over the western Pacific, which reveals an important role of marine organic aerosols in perturbing cloud and radiation and promotes understanding of global aerosol climatic impact.
Yawen Liu, Yun Qian, Philip J. Rasch, Kai Zhang, Lai-yung Ruby Leung, Yuhang Wang, Minghuai Wang, Hailong Wang, Xin Huang, and Xiu-Qun Yang
Atmos. Chem. Phys., 24, 3115–3128, https://doi.org/10.5194/acp-24-3115-2024, https://doi.org/10.5194/acp-24-3115-2024, 2024
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Fire management has long been a challenge. Here we report that spring-peak fire activity over southern Mexico and Central America (SMCA) has a distinct quasi-biennial signal by measuring multiple fire metrics. This signal is initially driven by quasi-biennial variability in precipitation and is further amplified by positive feedback of fire–precipitation interaction at short timescales. This work highlights the importance of fire–climate interactions in shaping fires on an interannual scale.
Xu Feng, Loretta J. Mickley, Michelle L. Bell, Tianjia Liu, Jenny A. Fisher, and Maria Val Martin
Atmos. Chem. Phys., 24, 2985–3007, https://doi.org/10.5194/acp-24-2985-2024, https://doi.org/10.5194/acp-24-2985-2024, 2024
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During severe wildfire seasons, smoke can have a significant impact on air quality in Australia. Our study demonstrates that characterization of the smoke plume injection fractions greatly affects estimates of surface smoke PM2.5. Using the plume behavior predicted by the machine learning method leads to the best model agreement with observed surface PM2.5 in key cities across Australia, with smoke PM2.5 accounting for 5 %–52 % of total PM2.5 on average during fire seasons from 2009 to 2020.
Shiyi Lai, Ximeng Qi, Xin Huang, Sijia Lou, Xuguang Chi, Liangduo Chen, Chong Liu, Yuliang Liu, Chao Yan, Mengmeng Li, Tengyu Liu, Wei Nie, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Aijun Ding
Atmos. Chem. Phys., 24, 2535–2553, https://doi.org/10.5194/acp-24-2535-2024, https://doi.org/10.5194/acp-24-2535-2024, 2024
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By combining in situ measurements and chemical transport modeling, this study investigates new particle formation (NPF) on the southeastern Tibetan Plateau. We found that the NPF was driven by the presence of biogenic gases and the transport of anthropogenic precursors. The NPF was vertically heterogeneous and shaped by the vertical mixing. This study highlights the importance of anthropogenic–biogenic interactions and meteorological dynamics in NPF in this climate-sensitive region.
Adriana Rocha-Lima, Peter R. Colarco, Anton S. Darmenov, Edward P. Nowottnick, Arlindo M. da Silva, and Luke D. Oman
Atmos. Chem. Phys., 24, 2443–2464, https://doi.org/10.5194/acp-24-2443-2024, https://doi.org/10.5194/acp-24-2443-2024, 2024
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Observations show an increasing aerosol optical depth trend in the Middle East between 2003–2012. We evaluate the NASA Goddard Earth Observing System (GEOS) model's ability to capture these trends and examine the meteorological and surface parameters driving dust emissions. Our results highlight the importance of data assimilation for long-term trends of atmospheric aerosols and support the hypothesis that vegetation cover loss may have contributed to increasing dust emissions in the period.
Danny M. Leung, Jasper F. Kok, Longlei Li, Natalie M. Mahowald, David M. Lawrence, Simone Tilmes, Erik Kluzek, Martina Klose, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 2287–2318, https://doi.org/10.5194/acp-24-2287-2024, https://doi.org/10.5194/acp-24-2287-2024, 2024
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This study uses a premier Earth system model to evaluate a new desert dust emission scheme proposed in our companion paper. We show that our scheme accounts for more dust emission physics, hence matching better against observations than other existing dust emission schemes do. Our scheme's dust emissions also couple tightly with meteorology, hence likely improving the modeled dust sensitivity to climate change. We believe this work is vital for improving dust representation in climate models.
Basudev Swain, Marco Vountas, Aishwarya Singh, Nidhi L. Anchan, Adrien Deroubaix, Luca Lelli, Yanick Ziegler, Sachin S. Gunthe, Hartmut Bösch, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-440, https://doi.org/10.5194/egusphere-2024-440, 2024
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Arctic amplification (AA) accelerates the warming of the central Arctic cryosphere and affects aerosol dynamics. Limited observations hinder a comprehensive analysis. This study uses AEROSNOW AOD data and GEOS-Chem simulations to assess AOD variability. Discrepancies highlight the need for improved observational integration into models to refine understanding of aerosol effects on cloud microphysics, ice nucleation and radiative forcing under evolving AA.
Ruth A. R. Digby, Nathan P. Gillett, Adam H. Monahan, Knut von Salzen, Antonis Gkikas, Qianqian Song, and Zhibo Zhang
Atmos. Chem. Phys., 24, 2077–2097, https://doi.org/10.5194/acp-24-2077-2024, https://doi.org/10.5194/acp-24-2077-2024, 2024
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The COVID-19 lockdowns reduced aerosol emissions. We ask whether these reductions affected regional aerosol optical depth (AOD) and compare the observed changes to predictions from Earth system models. Only India has an observed AOD reduction outside of typical variability. Models overestimate the response in some regions, but when key biases have been addressed, the agreement is improved. Our results suggest that current models can realistically predict the effects of future emission changes.
Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
Atmos. Chem. Phys., 24, 1717–1741, https://doi.org/10.5194/acp-24-1717-2024, https://doi.org/10.5194/acp-24-1717-2024, 2024
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This work studies sulfur in the remote troposphere at global and seasonal scales using aircraft measurements and multi-model simulations. The goal is to understand the sulfur cycle over remote oceans, spread of model simulations, and observation–model discrepancies. Such an understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulations and improve understanding of the sulfur cycle in atmospheric air quality, climate, and ecosystems.
Gargi Sengupta, Minjie Zheng, and Nønne L. Prisle
Atmos. Chem. Phys., 24, 1467–1487, https://doi.org/10.5194/acp-24-1467-2024, https://doi.org/10.5194/acp-24-1467-2024, 2024
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The effect of organic acid aerosol on sulfur chemistry and cloud properties was investigated in an atmospheric model. Organic acid dissociation was considered using both bulk and surface-related properties. We found that organic acid dissociation leads to increased hydrogen ion concentrations and sulfate aerosol mass in aqueous aerosols, increasing cloud formation. This could be important in large-scale climate models as many organic aerosol components are both acidic and surface-active.
Leena Kangas, Jaakko Kukkonen, Mari Kauhaniemi, Kari Riikonen, Mikhail Sofiev, Anu Kousa, Jarkko V. Niemi, and Ari Karppinen
Atmos. Chem. Phys., 24, 1489–1507, https://doi.org/10.5194/acp-24-1489-2024, https://doi.org/10.5194/acp-24-1489-2024, 2024
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Residential wood combustion is a major source of fine particulate matter. This study has evaluated the contribution of residential wood combustion to fine particle concentrations and its year-to-year and seasonal variation in te Helsinki metropolitan area. The average concentrations attributed to wood combustion in winter were up to 10- or 15-fold compared to summer. Wood combustion caused 12 % to 14 % of annual fine particle concentrations. In winter, the contribution ranged from 16 % to 21 %.
Arto Heitto, Cheng Wu, Diego Aliaga, Luis Blacutt, Xuemeng Chen, Yvette Gramlich, Liine Heikkinen, Wei Huang, Radovan Krejci, Paolo Laj, Isabel Moreno, Karine Sellegri, Fernando Velarde, Kay Weinhold, Alfred Wiedensohler, Qiaozhi Zha, Federico Bianchi, Marcos Andrade, Kari E. J. Lehtinen, Claudia Mohr, and Taina Yli-Juuti
Atmos. Chem. Phys., 24, 1315–1328, https://doi.org/10.5194/acp-24-1315-2024, https://doi.org/10.5194/acp-24-1315-2024, 2024
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Particle growth at the Chacaltaya station in Bolivia was simulated based on measured vapor concentrations and ambient conditions. Major contributors to the simulated growth were low-volatility organic compounds (LVOCs). Also, sulfuric acid had major role when volcanic activity was occurring in the area. This study provides insight on nanoparticle growth at this high-altitude Southern Hemispheric site and hence contributes to building knowledge of early growth of atmospheric particles.
Steven Soon-Kai Kong, Saginela Ravindra Babu, Sheng-Hsiang Wang, Stephen M. Griffith, Jackson Hian-Wui Chang, Ming-Tung Chuang, Guey-Rong Sheu, and Neng-Huei Lin
Atmos. Chem. Phys., 24, 1041–1058, https://doi.org/10.5194/acp-24-1041-2024, https://doi.org/10.5194/acp-24-1041-2024, 2024
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In this study, we combined ground observations from 7-SEAS Dongsha Experiment, MERRA-2 reanalysis, and MODIS satellite images for evaluation and improvement of the CMAQ dust model for cases of East Asian Dust reaching the Taiwan region, including Dongsha in the western Pacific. We proposed a better CMAQ dust treatment over East Asia and for the first time revealed the impact of typhoons on dust transport.
Zhiguo Zhang, Christer Johansson, Magnuz Engardt, Massimo Stafoggia, and Xiaoliang Ma
Atmos. Chem. Phys., 24, 807–851, https://doi.org/10.5194/acp-24-807-2024, https://doi.org/10.5194/acp-24-807-2024, 2024
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Up-to-date information on present and near-future air quality help people avoid exposure to high levels of air pollution. We apply different machine learning models to significantly improve traditional forecasts of PM10, NOx, and O3 in Stockholm, Sweden. It is shown that forecasts of all air pollutants are improved by the input of lagged measurements and taking calendar information into account. The final modelled errors are substantially smaller than uncertainties in the measurements.
Natalie M. Mahowald, Longlei Li, Samuel Albani, Douglas S. Hamilton, and Jasper F. Kok
Atmos. Chem. Phys., 24, 533–551, https://doi.org/10.5194/acp-24-533-2024, https://doi.org/10.5194/acp-24-533-2024, 2024
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Estimating past aerosol radiative effects and their uncertainties is an important topic in climate science. Aerosol radiative effects propagate into large uncertainties in estimates of how present and future climate evolves with changing greenhouse gas emissions. A deeper understanding of how aerosols interacted with the atmospheric energy budget under past climates is hindered in part by a lack of relevant paleo-observations and in part because less attention has been paid to the problem.
Min Zhao, Tie Dai, Daisuke Goto, Hao Wang, and Guangyu Shi
Atmos. Chem. Phys., 24, 235–258, https://doi.org/10.5194/acp-24-235-2024, https://doi.org/10.5194/acp-24-235-2024, 2024
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During a springtime pollution input from South Asia to the Tibetan Plateau, we combined atmospheric chemistry modeling and data assimilation methods to assimilate and forecast aerosols from South Asia and the Tibetan Plateau. Assimilation of observations over a whole time window leads to a more reasonable distribution of daily variations in the aerosol forecast field. We also find that aerosol assimilation can improve the surface solar energy forecast in the Tibetan Plateau region.
Yuling Hu, Haipeng Yu, Shichang Kang, Junhua Yang, Mukesh Rai, Xiufeng Yin, Xintong Chen, and Pengfei Chen
Atmos. Chem. Phys., 24, 85–107, https://doi.org/10.5194/acp-24-85-2024, https://doi.org/10.5194/acp-24-85-2024, 2024
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The Tibetan Plateau (TP) saw a record-breaking aerosol pollution event from April 20 to May 10, 2016. We studied the impact of aerosol–meteorology feedback on the transboundary transport flux of black carbon (BC) during this severe pollution event. It was found that the aerosol–meteorology feedback decreases the transboundary transport flux of BC from the central and western Himalayas towards the TP. This study is of great significance for the protection of the ecological environment of the TP.
Xiaodong Zhang, Ruiyu Zhugu, Xiaohu Jian, Xinrui Liu, Kaijie Chen, Shu Tao, Junfeng Liu, Hong Gao, Tao Huang, and Jianmin Ma
Atmos. Chem. Phys., 23, 15629–15642, https://doi.org/10.5194/acp-23-15629-2023, https://doi.org/10.5194/acp-23-15629-2023, 2023
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WRF-Chem modeling was conducted to assess impacts of Western Pacific Subtropical High Pressure (WPSH) on interannual fluctuations of O3 pollution in China. We find that, while precursor emissions dominated the long-term trend and magnitude of O3 from 1999 to 2017, WPSH determined interannual variation of summer O3. The response of O3 pollution to WPSH in major urban clusters depended on the proximity of these urban areas to WPSH. The results could help long-term O3 pollution mitigation planning.
Jim M. Haywood, Andy Jones, Anthony C. Jones, Paul Halloran, and Philip J. Rasch
Atmos. Chem. Phys., 23, 15305–15324, https://doi.org/10.5194/acp-23-15305-2023, https://doi.org/10.5194/acp-23-15305-2023, 2023
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The difficulties in ameliorating global warming and the associated climate change via conventional mitigation are well documented, with all climate model scenarios exceeding 1.5 °C above the preindustrial level in the near future. There is therefore a growing interest in geoengineering to reflect a greater proportion of sunlight back to space and offset some of the global warming. We use a state-of-the-art Earth-system model to investigate two of the most prominent geoengineering strategies.
Sampo Vepsäläinen, Silvia M. Calderón, and Nønne L. Prisle
Atmos. Chem. Phys., 23, 15149–15164, https://doi.org/10.5194/acp-23-15149-2023, https://doi.org/10.5194/acp-23-15149-2023, 2023
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Atmospheric aerosols act as seeds for cloud formation. Many aerosols contain surface active material that accumulates at the surface of growing droplets. This can affect cloud droplet activation, but the broad significance of the effect and the best way to model it are still debated. We compare predictions of six models to surface activity of strongly surface active aerosol and find significant differences between the models, especially with large fractions of surfactant in the dry particles.
Da Gao, Bin Zhao, Shuxiao Wang, Yuan Wang, Brian Gaudet, Yun Zhu, Xiaochun Wang, Jiewen Shen, Shengyue Li, Yicong He, Dejia Yin, and Zhaoxin Dong
Atmos. Chem. Phys., 23, 14359–14373, https://doi.org/10.5194/acp-23-14359-2023, https://doi.org/10.5194/acp-23-14359-2023, 2023
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Surface PM2.5 concentrations can be enhanced by aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). In this study, we found PM2.5 enhancement induced by ACIs shows a significantly smaller decrease ratio than that induced by ARIs in China with anthropogenic emission reduction from 2013 to 2021, making ACIs more important for enhancing PM2.5 concentrations. ACI-induced PM2.5 enhancement needs to be emphatically considered to meet the national PM2.5 air quality standard.
Miaoqing Xu, Jing Yang, Manchun Li, Xiao Chen, Qiancheng Lv, Qi Yao, Bingbo Gao, and Ziyue Chen
Atmos. Chem. Phys., 23, 14065–14076, https://doi.org/10.5194/acp-23-14065-2023, https://doi.org/10.5194/acp-23-14065-2023, 2023
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Although the temporal-scale effects on PM2.5–meteorology associations have been discussed, no quantitative evidence has proved this before. Based on rare 3 h meteorology data, we revealed that the dominant meteorological factor for PM2.5 concentrations across China extracted at the 3 h and 24 h scales presented large variations. This research suggests that data sources of different temporal scales should be comprehensively considered for better attribution and prevention of airborne pollution.
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023, https://doi.org/10.5194/acp-23-13911-2023, 2023
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To better understand smoke properties and its interactions with clouds, we compare the WRF-CAM5 model with observations from ORACLES, CLARIFY, and LASIC field campaigns in the southeastern Atlantic in August 2017. The model transports and mixes smoke well but does not fully capture some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, sulfate particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.
Michael Weger and Bernd Heinold
Atmos. Chem. Phys., 23, 13769–13790, https://doi.org/10.5194/acp-23-13769-2023, https://doi.org/10.5194/acp-23-13769-2023, 2023
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This study investigates the effects of complex terrain on air pollution trapping using a numerical model which simulates the dispersion of emissions under real meteorological conditions. The additionally simulated aerosol age allows us to distinguish areas that accumulate aerosol over time from areas that are more influenced by fresh emissions. The Dresden Basin, a widened section of the Elbe Valley in eastern Germany, is selected as the target area in a case study to demonstrate the concept.
Noora Hyttinen
Atmos. Chem. Phys., 23, 13809–13817, https://doi.org/10.5194/acp-23-13809-2023, https://doi.org/10.5194/acp-23-13809-2023, 2023
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Water activity in aerosol particles describes how particles respond to variations in relative humidity. Here, water activities were calculated for a set of 80 salts that may be present in aerosol particles using a state-of-the-art quantum-chemistry-based method. The effect of the dissociated salt on water activity varies with both the cation and anion. Most of the studied salts increase water uptake compared to pure water-soluble organic particles.
Charlotte M. Beall, Po-Lun Ma, Matthew W. Christensen, Johannes Mülmenstädt, Adam Varble, Kentaroh Suzuki, and Takuro Michibata
EGUsphere, https://doi.org/10.5194/egusphere-2023-2161, https://doi.org/10.5194/egusphere-2023-2161, 2023
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Single-layer warm liquid clouds cover nearly one-third of the earth's surface, and uncertainties regarding the impact of aerosols on their radiative properties pose a significant challenge to climate prediction. Here, we demonstrate how satellite observations can be used to constrain Earth Systems Model estimates of the radiative forcing due to the interactions of aerosols with clouds due to warm rain processes.
Peng Xian, Jeffrey S. Reid, Melanie Ades, Angela Benedettie, Peter R. Colarco, Arlindo da Silva, Tom F. Eck, Johannes Flemming, Edward J. Hyer, Zak Kipling, Samuel Rémy, Tsuyoshi Thomas Sekiyama, Taichu Tanaka, Keiya Yumimoto, and Jianglong Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2354, https://doi.org/10.5194/egusphere-2023-2354, 2023
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The study compares and evaluates the monthly aerosol optical depth of four reanalyses (RA) and their consensus. The basic verification characteristics of these RA versus both AERONET and MODIS retrievals are presented. The study discusses the strength of each RA and identifies regions where diversity and challenges are prominent. The RA consensus usually performs very well on a global scale in terms of how well it matches the observational data, making it a good choice for various applications.
Lambert Delbeke, Chien Wang, Pierre Tulet, Cyrielle Denjean, Maurin Zouzoua, Nicolas Maury, and Adrien Deroubaix
Atmos. Chem. Phys., 23, 13329–13354, https://doi.org/10.5194/acp-23-13329-2023, https://doi.org/10.5194/acp-23-13329-2023, 2023
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Low-level stratiform clouds (LLSCs) appear frequently over southern West Africa during the West African monsoon. Local and remote aerosol sources (biomass burning aerosols from central Africa) play a significant role in the LLSC life cycle. Based on measurements by the DACCIWA campaign, large-eddy simulation (LES) was conducted using different aerosol scenarios. The results show that both indirect and semi-direct effects can act individually or jointly to influence the life cycles of LLSCs.
Matthias Kohl, Jos Lelieveld, Sourangsu Chowdhury, Sebastian Ehrhart, Disha Sharma, Yafang Cheng, Sachchida Nand Tripathi, Mathew Sebastian, Govindan Pandithurai, Hongli Wang, and Andrea Pozzer
Atmos. Chem. Phys., 23, 13191–13215, https://doi.org/10.5194/acp-23-13191-2023, https://doi.org/10.5194/acp-23-13191-2023, 2023
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Knowledge on atmospheric ultrafine particles (UFPs) with a diameter smaller than 100 nm is crucial for public health and the hydrological cycle. We present a new global dataset of UFP concentrations at the Earth's surface derived with a comprehensive chemistry–climate model and evaluated with ground-based observations. The evaluation results are combined with high-resolution primary emissions to downscale UFP concentrations to an unprecedented horizontal resolution of 0.1° × 0.1°.
Haotian Zu, Biwu Chu, Yiqun Lu, Ling Liu, and Xiuhui Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1774, https://doi.org/10.5194/egusphere-2023-1774, 2023
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The nucleation process of iodic acid (HIO3) and iodous acid (HIO2) was proved to be critical in marine areas. However, HIO3-HIO2 nucleation cannot effectively derive the observed rapid new particle formation in broad marine areas. We show the extensive participation of dimethylamine (DMA) in HIO3-HIO2 nucleation and find a significant enhancement of DMA on the HIO3-HIO2 nucleation, which establishes reasonable connections between the iodine oxoacids nucleation and the rapid marine new particles.
Alejandro Baró Pérez, Michael S. Diamond, Frida A.-M. Bender, Abhay Devasthale, Matthias Schwarz, Julien Savre, Juha Tonttila, Harri Kokkola, Hyunho Lee, David Painemal, and Annica M. L. Ekman
EGUsphere, https://doi.org/10.5194/egusphere-2023-2070, https://doi.org/10.5194/egusphere-2023-2070, 2023
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We use a numerical model to study interactions between humid light-absorbing aerosol plumes, clouds, and radiation over the Southeast Atlantic. We find that the warming produced by the aerosols reduces cloud cover, especially in highly polluted situations. Aerosol impacts on drizzle play a minor role. However, aerosol effects on cloud reflectivity and moisture-induced changes in cloud cover dominate the climatic response and lead to an overall cooling by the biomass-burning plumes.
Roger Teoh, Zebediah Engberg, Ulrich Schumann, Christiane Voigt, Marc Shapiro, Susanne Rohs, and Marc Stettler
EGUsphere, https://doi.org/10.5194/egusphere-2023-1859, https://doi.org/10.5194/egusphere-2023-1859, 2023
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The radiative forcing attributable to aviation contrails is estimated for 2019–21. We estimate a global contrail net RF that is approximately half the best estimate of a previous study. Contrail climate impacts have not scaled proportionally with air traffic growth due to higher growth in regions where contrails are less likely to form. There are significant opportunities to mitigate contrail impacts as only 2 % of all flights globally account for 80 % of the annual contrail energy forcing.
Xiaoli Wei, Qian Cui, Leiming Ma, Feng Zhang, Wenwen Li, and Peng Liu
EGUsphere, https://doi.org/10.5194/egusphere-2023-1754, https://doi.org/10.5194/egusphere-2023-1754, 2023
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A new aerosol-type classification algorithm was proposed. It includes an optical database building by Mie scattering and a complex refractive index working as a baseline to identify different aerosol types. The new algorithm shows high accuracy and efficiency. Hence, a global map of aerosol types was generated using the new algorithm to characterize aerosol types across the five continents. It will help improve the accuracy of aerosol inversion and determine the sources of aerosol pollution.
Wenxuan Hua, Sijia Lou, Xin Huang, Lian Xue, Ke Ding, Zilin Wang, and Aijun Ding
EGUsphere, https://doi.org/10.5194/egusphere-2023-1822, https://doi.org/10.5194/egusphere-2023-1822, 2023
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In this study, we diagnose uncertainties in CO and OC emissions from four inventories for seven majorwildfire-prone regions. Uncertainties in vegetation classification methods, fire detection products, and cloud obscuration effects lead to bias in these biomass burning (BB) emission inventories. By comparing simulations with measurements, we provide certain inventory recommendations. Our study has implications for reducing uncertainties in emissions in further studies.
Jun-Wei Xu, Jintai Lin, Dan Tong, and Lulu Chen
Atmos. Chem. Phys., 23, 10075–10089, https://doi.org/10.5194/acp-23-10075-2023, https://doi.org/10.5194/acp-23-10075-2023, 2023
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This study highlights the necessity of a low-carbon pathway in foreign countries for China to achieve air quality goals and to protect public health. We find that adopting the low-carbon instead of the fossil-fuel-intensive pathway in foreign countries would prevent 63 000–270 000 transboundary PM2.5-associated mortalities in China in 2060. Our study provides direct evidence of the necessity of inter-regional cooperation for air quality improvement.
Xurong Wang, Qiaoqiao Wang, Maria Prass, Christopher Pöhlker, Daniel Moran-Zuloaga, Paulo Artaxo, Jianwei Gu, Ning Yang, Xiajie Yang, Jiangchuan Tao, Juan Hong, Nan Ma, Yafang Cheng, Hang Su, and Meinrat O. Andreae
Atmos. Chem. Phys., 23, 9993–10014, https://doi.org/10.5194/acp-23-9993-2023, https://doi.org/10.5194/acp-23-9993-2023, 2023
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In this work, with an optimized particle mass size distribution, we captured observed aerosol optical depth (AOD) and coarse aerosol concentrations over source and/or receptor regions well, demonstrating good performance in simulating export of African dust toward the Amazon Basin. In addition to factors controlling the transatlantic transport of African dust, the study investigated the impact of African dust over the Amazon Basin, including the nutrient inputs associated with dust deposition.
Athanasios Tsikerdekis, Otto P. Hasekamp, Nick A. J. Schutgens, and Qirui Zhong
Atmos. Chem. Phys., 23, 9495–9524, https://doi.org/10.5194/acp-23-9495-2023, https://doi.org/10.5194/acp-23-9495-2023, 2023
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Aerosols are tiny particles of different substances (species) that can be emitted into the atmosphere by natural processes or by anthropogenic activities. However, the actual aerosol emission amount per species is highly uncertain. Thus in this work we correct the aerosol emissions used to drive a global aerosol–climate model using satellite observations through a process called data assimilation. These more accurate aerosol emissions can lead to a more accurate weather and climate prediction.
Chandrakala Bharali, Mary Barth, Rajesh Kumar, Sachin D. Ghude, Vinayak Sinha, and Baerbel Sinha
EGUsphere, https://doi.org/10.5194/egusphere-2023-1686, https://doi.org/10.5194/egusphere-2023-1686, 2023
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This study examines the role of atmospheric aerosols in winter fog over the Indo-Gangetic Plains of India using the WRF-Chem model. The increase in RH with aerosol-radiation feedback (ARF) is found to be important for fog formation as it promoted the growth of aerosol and increased aerosol activation in the polluted environment. ARF and aqueous phase chemistry affected the timing of fog formation by ~1–2 hours and the fog intensity by modulating the meteorology and aerosol concentration.
Jani Strömberg, Xiaoyu Li, Mona Kurppa, Heino Kuuluvainen, Liisa Pirjola, and Leena Järvi
Atmos. Chem. Phys., 23, 9347–9364, https://doi.org/10.5194/acp-23-9347-2023, https://doi.org/10.5194/acp-23-9347-2023, 2023
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We conclude that with low wind speeds, solar radiation has a larger decreasing effect (53 %) on pollutant concentrations than aerosol processes (18 %). Additionally, our results showed that with solar radiation included, pollutant concentrations were closer to observations (−13 %) than with only aerosol processes (+98 %). This has implications when planning simulations under calm conditions such as in our case and when deciding whether or not simulations need to include these processes.
Junghwa Lee, Patric Seifert, Tempei Hashino, Maximilian Maahn, Fabian Senf, and Oswald Knoth
EGUsphere, https://doi.org/10.5194/egusphere-2023-1887, https://doi.org/10.5194/egusphere-2023-1887, 2023
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Spectral-bin model simulations of an idealized supercooled stratiform cloud were performed with the AMPS model for variable CCN and INP concentrations. We performed radar forward simulations with PAMTRA to transfer the simulations into radar observational space. The derived radar reflectivity factors were compared to observational studies of stratiform mixed-phase clouds. These studies report a similar response of the radar reflectivity factor to aerosol perturbations as we found in our study.
Guanyu Liu, Jing Li, and Tong Ying
Atmos. Chem. Phys., 23, 9217–9228, https://doi.org/10.5194/acp-23-9217-2023, https://doi.org/10.5194/acp-23-9217-2023, 2023
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Fires in Australia are positively correlated with the El Niño–Southern Oscillation (ENSO). However, the correlation between ENSO and the Australian Fire Weather Index (FWI) increases from 0.17 to 0.70 when the Atlantic Multidecadal Oscillation (AMO) shifts from a negative to positive phase. This is explained by the teleconnection effect through which the warmer AMO generates Rossby wave trains and results in high pressures and a weather condition conducive to wildfires.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
EGUsphere, https://doi.org/10.5194/egusphere-2023-1444, https://doi.org/10.5194/egusphere-2023-1444, 2023
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Secondary organic aerosols (SOA) can exist in liquid, semi-solid or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in the northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David M. H. Sexton, Christopher Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John W. Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 8749–8768, https://doi.org/10.5194/acp-23-8749-2023, https://doi.org/10.5194/acp-23-8749-2023, 2023
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Aerosol forcing of Earth’s energy balance has persisted as a major cause of uncertainty in climate simulations over generations of climate model development. We show that structural deficiencies in a climate model are exposed by comprehensively exploring parametric uncertainty and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. This provides a future pathway towards building models with greater physical realism and lower uncertainty.
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