Articles | Volume 24, issue 14
https://doi.org/10.5194/acp-24-8263-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-8263-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Measurement report
| 
22 Jul 2024
Measurement report |
| 22 Jul 2024
| 22 Jul 2024
Measurement report: Vanadium-containing ship exhaust particles detected in and above the marine boundary layer in the remote atmosphere
Maya Abou-Ghanem
CORRESPONDING AUTHOR
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, 80305, USA
Daniel M. Murphy
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, 80305, USA
Gregory P. Schill
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, 80305, USA
Michael J. Lawler
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, 80309, USA
Karl D. Froyd
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, Boulder, 80305, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, 80309, USA
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Allison R. Moon, Leyang Liu, Xuan Wang, Yuk-Chun Chan, Alyson Fritzmann, Ryan Pound, Amy Lees, Lewis Marden, Mat Evans, Lucy J. Carpenter, Jochen Stutz, Joel A. Thornton, Gordon Novak, Andrew Rollins, Gregory P. Schill, Xu-cheng He, Henning Finkenzeller, Margarita Reza, Rainer Volkamer, Kelvin H. Bates, Alfonso Saiz-Lopez, Anoop S. Mahajan, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2025-4725, https://doi.org/10.5194/egusphere-2025-4725, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Global chemical transport models previously treated aerosols as a sink for reactive iodine (Iy); however, aerosol iodide is also a source of Iy via heterogeneous reactions involving hypohalous acids and halogen nitrates. We implemented this chemistry into GEOS-Chem, in addition to explicitly representing three aerosol iodine types: soluble organic iodine (SOI), iodide, and iodate. We found that aerosol recycling of iodide to form Iy is more than twice as fast as the other Iy sources combined.
Larissa Lacher, A. Gannet Hallar, Ian B. McCubbin, Joey Bail, Karl D. Froyd, Justin Jacquot, Xiaoli Shen, Christopher Rapp, Ottmar Möhler, and Daniel Cziczo
EGUsphere, https://doi.org/10.5194/egusphere-2025-4492, https://doi.org/10.5194/egusphere-2025-4492, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We observe a trend of increasing ice-nucleating particle (INP) concentration in spring in the Rocky Mountains, related to regional dust emissions that may intensify with climate change. Additionally, super-micrometer particles were found as the most important contributors to the INP population. This finding was partly enabled by a novel setup of the Portable Ice Nucleation Experiment (PINE), coupled with a pumped-counterflow virtual impactor allowing for direct analysis of INP properties.
Kane Stone, Susan Solomon, Pengfei Yu, Daniel M. Murphy, Douglas Kinnison, and Jian Guan
Atmos. Chem. Phys., 25, 7683–7697, https://doi.org/10.5194/acp-25-7683-2025, https://doi.org/10.5194/acp-25-7683-2025, 2025
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The Australian 2019–2020 wildfires injected a substantial amount of smoke into the upper atmosphere, causing unusual chemical reactions that altered the chemical makeup of the upper atmosphere. This led to ozone depletion in the Southern Hemisphere midlatitudes that likely did not fully recover until 2 years after the initial event due to the persistent chemical effects of the smoke.
Paul J. DeMott, Jessica A. Mirrielees, Sarah Suda Petters, Daniel J. Cziczo, Markus D. Petters, Heinz G. Bingemer, Thomas C. J. Hill, Karl Froyd, Sarvesh Garimella, A. Gannet Hallar, Ezra J. T. Levin, Ian B. McCubbin, Anne E. Perring, Christopher N. Rapp, Thea Schiebel, Jann Schrod, Kaitlyn J. Suski, Daniel Weber, Martin J. Wolf, Maria Zawadowicz, Jake Zenker, Ottmar Möhler, and Sarah D. Brooks
Atmos. Meas. Tech., 18, 639–672, https://doi.org/10.5194/amt-18-639-2025, https://doi.org/10.5194/amt-18-639-2025, 2025
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The Fifth International Ice Nucleation Workshop Phase 3 (FIN-03) compared the ambient atmospheric performance of ice-nucleating particle (INP) measuring systems and explored general methods for discerning atmospheric INP compositions. Mirroring laboratory results, INP concentrations agreed within 5–10 factors. Measurements of total aerosol properties and investigations of INP compositions supported a dominant role of soil and plant organic aerosol elements as INPs during the study.
Kasper Juurikkala, Christina J. Williamson, Karl D. Froyd, Jonathan Dean-Day, and Ari Laaksonen
EGUsphere, https://doi.org/10.5194/egusphere-2025-163, https://doi.org/10.5194/egusphere-2025-163, 2025
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This study uses UCLALES-SALSA simulations to investigate synoptic cirrus clouds from NASA’s MACPEX campaign. Results show that prior heterogeneous ice nucleation depletes ice nuclei, creating conditions for subsequent homogeneous freezing. The findings highlight limitations of ice residual analysis in capturing cirrus evolution and provide insights into aerosol-cloud interactions critical to atmospheric and climate processes.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
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.
Siying Lian, Luxi Zhou, Daniel M. Murphy, Karl D. Froyd, Owen B. Toon, and Pengfei Yu
Atmos. Chem. Phys., 22, 13659–13676, https://doi.org/10.5194/acp-22-13659-2022, https://doi.org/10.5194/acp-22-13659-2022, 2022
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Parameterizations of dust lifting and microphysical properties of dust in climate models are still subject to large uncertainty. Here we use a sectional aerosol climate model to investigate the global vertical distributions of the dust. Constrained by a suite of observations, the model suggests that, although North African dust dominates global dust mass loading at the surface, the relative contribution of Asian dust increases with altitude and becomes dominant in the upper troposphere.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
Adam T. Ahern, Frank Erdesz, Nicholas L. Wagner, Charles A. Brock, Ming Lyu, Kyra Slovacek, Richard H. Moore, Elizabeth B. Wiggins, and Daniel M. Murphy
Atmos. Meas. Tech., 15, 1093–1105, https://doi.org/10.5194/amt-15-1093-2022, https://doi.org/10.5194/amt-15-1093-2022, 2022
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Particles in the atmosphere play a significant role in climate change by scattering light back into space, reducing the amount of energy available to be absorbed by greenhouse gases. We built a new instrument to measure what direction light is scattered by particles, e.g., wildfire smoke. This is important because, depending on the angle of the sun, some particles scatter light into space (cooling the planet), but some light is also scattered towards the Earth (not cooling the planet).
Li Zhang, Georg A. Grell, Stuart A. McKeen, Ravan Ahmadov, Karl D. Froyd, and Daniel Murphy
Geosci. Model Dev., 15, 467–491, https://doi.org/10.5194/gmd-15-467-2022, https://doi.org/10.5194/gmd-15-467-2022, 2022
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Applying the chemistry package from WRF-Chem into the Flow-following finite-volume Icosahedra Model, we essentially make it possible to explore the importance of different levels of complexity in gas and aerosol chemistry, as well as in physics parameterizations, for the interaction processes in global modeling systems. The model performance validated by the Atmospheric Tomography Mission aircraft measurements in summer 2016 shows good performance in capturing the aerosol and gas-phase tracers.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Michael J. Lawler, Savannah L. Lewis, Lynn M. Russell, Patricia K. Quinn, Timothy S. Bates, Derek J. Coffman, Lucia M. Upchurch, and Eric S. Saltzman
Atmos. Chem. Phys., 20, 16007–16022, https://doi.org/10.5194/acp-20-16007-2020, https://doi.org/10.5194/acp-20-16007-2020, 2020
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This work describes new measurements of aerosol (particles) composition over the North Atlantic Ocean. It provides concentrations of polysaccharide material likely made from organisms in the surface ocean and improves our understanding of the relative importance of such fresh biogenic material compared to more recalcitrant organic carbon in forming marine organic aerosol. We aim ultimately to understand the role that ocean biology plays in cloud formation in marine regions.
Agnieszka Kupc, Christina J. Williamson, Anna L. Hodshire, Jan Kazil, Eric Ray, T. Paul Bui, Maximilian Dollner, Karl D. Froyd, Kathryn McKain, Andrew Rollins, Gregory P. Schill, Alexander Thames, Bernadett B. Weinzierl, Jeffrey R. Pierce, and Charles A. Brock
Atmos. Chem. Phys., 20, 15037–15060, https://doi.org/10.5194/acp-20-15037-2020, https://doi.org/10.5194/acp-20-15037-2020, 2020
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Tropical upper troposphere over the Atlantic and Pacific oceans is a major source region of new particles. These particles are associated with the outflow from deep convection. We investigate the processes that govern the formation of these particles and their initial growth and show that none of the formation schemes commonly used in global models are consistent with observations. Using newer schemes indicates that organic compounds are likely important as nucleating and initial growth agents.
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Short summary
Using particle analysis by laser mass spectrometry, we examine vanadium-containing ship exhaust particles measured on NASA's DC-8 during the Atmospheric Tomography Mission (ATom). Our results reveal ship exhaust particles are sufficiently widespread in the marine atmosphere and experience atmospheric aging. Finally, we use laboratory calibrations to determine the vanadium, sulfate, and organic single-particle mass fractions of vanadium-containing ship exhaust particles.
Using particle analysis by laser mass spectrometry, we examine vanadium-containing ship exhaust...
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