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https://doi.org/10.5194/egusphere-2023-1966
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/egusphere-2023-1966
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
12 Sep 2023
| 12 Sep 2023
Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations
Abstract. The sulfur cycle plays a key role in atmospheric air quality, climate, and ecosystems. In this study, we compare the spatial and temporal distribution of four sulfur-containing species, dimethyl sulfide (DMS), sulfur dioxide (SO2), particulate methanesulfonate (MSA), and particulate sulfate (SO4), that were measured during the airborne NASA Atmospheric Tomography (ATom) mission and simulated by five AeroCom-III models to analyze the budget of sulfur cycle from the models. This study focuses on remote regions over the Pacific, Atlantic, and Southern Oceans from near the ocean surface to ~12-km altitude range, and covers all four seasons. These regions provide us with highly heterogeneous natural and anthropogenic source environments, which is not usually the case for traditional continental studies. We examine the vertical and seasonal variations of these sulfur species over tropical, mid-, and high-latitude regions in both hemispheres. We identify their origins from land versus ocean and from anthropogenic versus natural sources with sensitivity studies by applying tagged tracers linking to emission types and regions. In general, the differences among model results can be greater than one-order of magnitude. Comparing with observations, simulated SO2 is generally low while SO4 is high, and the model-observation agreement is much better in ATom-4 (April–May, 2018). There are much larger DMS concentrations simulated close to the sea surface than observed, indicating that the DMS emissions may be too high from all models. Anthropogenic emissions are the dominant source (40–60 % of the total amount) for atmospheric sulfate simulated at locations and times along the ATom flight tracks at almost every altitude, followed by volcanic emissions (18–32 %) and oceanic sources (16–32 %). Similar source contributions can also be derived at broad ocean basin and monthly scales, indicating that any reductions of anthropogenic sulfur emissions would have global impacts in modern times.
How to cite. Bian, H., Chin, M., Colarco, P. R., Apel, E. C., Blake, D. R., Froyd, K., Hornbrook, R. S., Jimenez, J., Jost, P. C., Lawler, M., Liu, M., Lund, M. T., Matsui, H., Nault, B. A., Penner, J. E., Rollins, A. W., Schill, G., Skeie, R. B., Wang, H., Xu, L., Zhang, K., and Zhu, J.: Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations, EGUsphere [preprint], https://doi.org/10.5194/egusphere-2023-1966, 2023.
Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this preprint. The responsibility to include appropriate place names lies with the authors.
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Journal article(s) based on this preprint
07 Feb 2024
Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations
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
Short summary
Short summary
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.
Interactive discussion
Status: closed
Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor
| : Report abuse
-
RC1: 'Comment on egusphere-2023-1966', Anonymous Referee #1, 12 Oct 2023
Review of: Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulationsÂThis paper analyzes the sulfur cycle in the marine atmosphere using measurements from the NASA ATom mission and simulations from the AeroCom models. The study compares sulfur species measurements (DMS, SO2, MSA, and SO4) between observations and model simulations, discusses the discrepancies and the possible causes, and analyses the sources and transport of these sulfur species in the atmosphere. The results showed the dominance of anthropogenic emissions in atmospheric sulfate, especially in the upper levels of the atmosphere, and the importance of ocean emissions to the local areas near the surface. By analyzing the discrepancies between model and observation, as well as between models, the authors emphasize the need for further investigation into emissions and the chemical/dynamical processes to improve the model performance.ÂThe paper maintains a coherent structure and meticulously examines extensive data sets from multiple dimensions. The ocean not only covers most of the Earth but also acts as an important source of sulfur.  By analyzing and comparing observations and simulations, the authors point out potential directions that modelers should be working towards to improve the module performance on the sulfur cycle. However, the substantial volume of data presented is overwhelming, potentially obfuscating the main points for the readers. Thus, my principal suggestion is to simplify certain sections of the paper. Also, instead of summarizing the paper, the authors should address the implications of their new findings in the conclusion section.ÂI recommend minor revisions before accepting the paper.            ÂScientific Comments:Â1. Relevance and novelty of this study:It would be helpful if the authors could state the reasons for focusing on sulfur species in a more straightforward way in the introduction section. While the introduction highlights the environmental impacts of sulfur species, other pollutants not discussed in this paper also affect the environment. Why should we focus on sulfur species? Is the bias of aerosol climate models predominantly due to sulfur?ÂI would appreciate it if the authors could highlight the novelty of their work. Has any other research analyzed the ATOM data specifically for sulfur species? Is this the first study that utilizes ATOM measurements in comparison with AeroCom models? If there have been studies on sulfur variability and sources over the ocean, what novel findings does this paper present?  The authors should make some comparison with other studies in a new section or talk about it in an existing section of the paper.ÂFurthermore, if we improve sulfur simulation, what advantages can we expect? It would be helpful if the authors could briefly discuss the implications of the new findings in the conclusion section.ÂÂ2. Information Overload and Simplification:Some parts of the paper contain overwhelming information that may be simplified or moved to supplements. For instance, Section 3.1 allocates 28 lines (L212-L239) to discuss three different sampling intervals, which may not be key information the readers need to know. This information (corresponding to Fig 2 (a)(d)(g)(i)) only builds up one-third content in Figure 2, which makes the main point of Figure 2 very hard to catch.ÂÂAnother example starts from L317 where the authors spent time explaining how the flag ‘-888’ is replaced by ‘0’ to represent the low values, which, although crucial for validating results, may not be necessary for most readers.ÂAdditionally, the division of 5 models into 3 groups from L340-L354 seems superfluous and is never referenced throughout the paper. I would recommend a description without grouping the models.Â3. Layout and Readability of Figures:Due to the huge load of information that is shown, optimizing the layout of figures is crucial to enhance readability. For example, I would recommend relocating the legends in Figures 5-8 and putting this information on the top/bottom or right side of the charts.ÂÂSince you ‘use 10-s merged data where observations above DL throughout the main text unless otherwise stated’ (L241), could you just show the results of 10-s data only on Figure 2 and move the other to the supplement?ÂAdditionally, as Atom-1/2/3/4 are not following the order of the four seasons, I recommend adding notes on the seasons at a proper place in Figures 9,10,11, and 13 to guide the readers when reading through the section about seasonal changes in the paper.Â4. Conclusion:The conclusion section is mostly a summary of the content. As mentioned earlier, the implication of the new findings can be stated in this section.ÂÂTechnical comments:Â1. Please standardize the color and font of the indices of panels in Figure 2.Â2. Please refine Figure 12 to maintain the consistent style of other figures.ÂÂ3. In the caption of Figure 9, AMS should be orange instead of ‘red’.ÂÂ4. Please replace the vertical bar in Figure 13 with a straight line as the shape and color is misleading.ÂÂ5. In L467, please add a period after ‘4’.ÂCitation: https://doi.org/
10.5194/egusphere-2023-1966-RC1 -
RC2: 'Comment on egusphere-2023-1966 tagging method', Anonymous Referee #2, 13 Oct 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-1966/egusphere-2023-1966-RC2-supplement.pdf
-
RC3: 'Comment on egusphere-2023-1966', Anonymous Referee #3, 23 Oct 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-1966/egusphere-2023-1966-RC3-supplement.pdf
-
AC1: 'Reply to Comment on egusphere-2023-1966', Huisheng Bian, 05 Dec 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-1966/egusphere-2023-1966-AC1-supplement.pdf
Interactive discussion
Status: closed
Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor
| : Report abuse
-
RC1: 'Comment on egusphere-2023-1966', Anonymous Referee #1, 12 Oct 2023
Review of: Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulationsÂThis paper analyzes the sulfur cycle in the marine atmosphere using measurements from the NASA ATom mission and simulations from the AeroCom models. The study compares sulfur species measurements (DMS, SO2, MSA, and SO4) between observations and model simulations, discusses the discrepancies and the possible causes, and analyses the sources and transport of these sulfur species in the atmosphere. The results showed the dominance of anthropogenic emissions in atmospheric sulfate, especially in the upper levels of the atmosphere, and the importance of ocean emissions to the local areas near the surface. By analyzing the discrepancies between model and observation, as well as between models, the authors emphasize the need for further investigation into emissions and the chemical/dynamical processes to improve the model performance.ÂThe paper maintains a coherent structure and meticulously examines extensive data sets from multiple dimensions. The ocean not only covers most of the Earth but also acts as an important source of sulfur.  By analyzing and comparing observations and simulations, the authors point out potential directions that modelers should be working towards to improve the module performance on the sulfur cycle. However, the substantial volume of data presented is overwhelming, potentially obfuscating the main points for the readers. Thus, my principal suggestion is to simplify certain sections of the paper. Also, instead of summarizing the paper, the authors should address the implications of their new findings in the conclusion section.ÂI recommend minor revisions before accepting the paper.            ÂScientific Comments:Â1. Relevance and novelty of this study:It would be helpful if the authors could state the reasons for focusing on sulfur species in a more straightforward way in the introduction section. While the introduction highlights the environmental impacts of sulfur species, other pollutants not discussed in this paper also affect the environment. Why should we focus on sulfur species? Is the bias of aerosol climate models predominantly due to sulfur?ÂI would appreciate it if the authors could highlight the novelty of their work. Has any other research analyzed the ATOM data specifically for sulfur species? Is this the first study that utilizes ATOM measurements in comparison with AeroCom models? If there have been studies on sulfur variability and sources over the ocean, what novel findings does this paper present?  The authors should make some comparison with other studies in a new section or talk about it in an existing section of the paper.ÂFurthermore, if we improve sulfur simulation, what advantages can we expect? It would be helpful if the authors could briefly discuss the implications of the new findings in the conclusion section.ÂÂ2. Information Overload and Simplification:Some parts of the paper contain overwhelming information that may be simplified or moved to supplements. For instance, Section 3.1 allocates 28 lines (L212-L239) to discuss three different sampling intervals, which may not be key information the readers need to know. This information (corresponding to Fig 2 (a)(d)(g)(i)) only builds up one-third content in Figure 2, which makes the main point of Figure 2 very hard to catch.ÂÂAnother example starts from L317 where the authors spent time explaining how the flag ‘-888’ is replaced by ‘0’ to represent the low values, which, although crucial for validating results, may not be necessary for most readers.ÂAdditionally, the division of 5 models into 3 groups from L340-L354 seems superfluous and is never referenced throughout the paper. I would recommend a description without grouping the models.Â3. Layout and Readability of Figures:Due to the huge load of information that is shown, optimizing the layout of figures is crucial to enhance readability. For example, I would recommend relocating the legends in Figures 5-8 and putting this information on the top/bottom or right side of the charts.ÂÂSince you ‘use 10-s merged data where observations above DL throughout the main text unless otherwise stated’ (L241), could you just show the results of 10-s data only on Figure 2 and move the other to the supplement?ÂAdditionally, as Atom-1/2/3/4 are not following the order of the four seasons, I recommend adding notes on the seasons at a proper place in Figures 9,10,11, and 13 to guide the readers when reading through the section about seasonal changes in the paper.Â4. Conclusion:The conclusion section is mostly a summary of the content. As mentioned earlier, the implication of the new findings can be stated in this section.ÂÂTechnical comments:Â1. Please standardize the color and font of the indices of panels in Figure 2.Â2. Please refine Figure 12 to maintain the consistent style of other figures.ÂÂ3. In the caption of Figure 9, AMS should be orange instead of ‘red’.ÂÂ4. Please replace the vertical bar in Figure 13 with a straight line as the shape and color is misleading.ÂÂ5. In L467, please add a period after ‘4’.ÂCitation: https://doi.org/
10.5194/egusphere-2023-1966-RC1 -
RC2: 'Comment on egusphere-2023-1966 tagging method', Anonymous Referee #2, 13 Oct 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-1966/egusphere-2023-1966-RC2-supplement.pdf
-
RC3: 'Comment on egusphere-2023-1966', Anonymous Referee #3, 23 Oct 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-1966/egusphere-2023-1966-RC3-supplement.pdf
-
AC1: 'Reply to Comment on egusphere-2023-1966', Huisheng Bian, 05 Dec 2023
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-1966/egusphere-2023-1966-AC1-supplement.pdf
Peer review completion
AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload
AR by Huisheng Bian on behalf of the Authors (09 Dec 2023)
Author's response
Author's tracked changes
Manuscript
ED: Publish subject to minor revisions (review by editor) (18 Dec 2023) by Barbara Ervens
AR by Huisheng Bian on behalf of the Authors (20 Dec 2023)
Author's response
Author's tracked changes
Manuscript
ED: Publish as is (22 Dec 2023) by Barbara Ervens
AR by Huisheng Bian on behalf of the Authors (29 Dec 2023)
Journal article(s) based on this preprint
07 Feb 2024
Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations
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
Short summary
Short summary
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.
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Huisheng Bian
CORRESPONDING AUTHOR
Goddard Earth Sciences Technology and Research (GESTAR) II, University of Maryland at Baltimore County, Baltimore, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Mian Chin
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Peter R. Colarco
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Eric C. Apel
Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
Donald R. Blake
Department of Chemistry, University of California Irvine, CA, USA
Karl Froyd
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Rebecca S. Hornbrook
Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
Jose Jimenez
Department of Chemistry, University of Colorado, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Pedro Campuzano Jost
Department of Chemistry, University of Colorado, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Michael Lawler
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
NOAA Chemical Sciences Laboratory, Boulder, CO, USA
Mingxu Liu
Graduate School of Environmental Studies, Nagoya University, Nagoya, Japan
Marianne Tronstad Lund
CICERO Center for International Climate Research, Oslo, Norway
Hitoshi Matsui
Graduate School of Environmental Studies, Nagoya University, Nagoya, Japan
Benjamin A. Nault
Department of Chemistry, University of Colorado, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
now at: Department of Environmental Health and Engineering, Whiting School of Engineering, The Johns Hopkins, Baltimore, MD, USA
now at: Center for Aerosol and Cloud Chemistry, Aerodyne Research, Inc., Billerica, MA, USA
Joyce E. Penner
Dept. of Atmospheric, Oceanic and Space Sciences, University of Michigan, Ann Arbor, Michigan, USA
Andrew W. Rollins
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
NOAA Earth System Research Laboratory, Chemical Sciences Division, Boulder, CO, USA
Gregory Schill
NOAA Chemical Sciences Laboratory, Boulder, CO, USA
Ragnhild B. Skeie
CICERO Center for International Climate Research, Oslo, Norway
Hailong Wang
Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USA
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
now at: Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, Missouri, USA
Kai Zhang
Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USA
Jialei Zhu
Institute of Surface-Earth System Science, School of Earth System Science, Tianjin University, Tianjin, China
Download
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(6812 KB) - Metadata XML
-
Supplement
(5467 KB) - BibTeX
- EndNote
- Final revised paper
Short summary
This work studies sulfur in 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, the spread of model simulations, and the observation-model discrepancies. Such understanding and comparison with real observations are crucial to narrow down the uncertainties in model sulfur simulation and improve our understanding of sulfur cycle in atmospheric air quality, climate, and ecosystems.
This work studies sulfur in remote troposphere at global and seasonal scales using aircraft...