Articles | Volume 23, issue 2
https://doi.org/10.5194/acp-23-843-2023
© 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/acp-23-843-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
18 Jan 2023
Research article |
| 18 Jan 2023
| 18 Jan 2023
Observed changes in stratospheric circulation: decreasing lifetime of N2O, 2005–2021
Earth System Science Department, University of California Irvine,
Irvine, CA 92697-3100, USA
Lucien Froidevaux
Jet Propulsion Laboratory, California Institute of Technology,
Pasadena, CA 91011, USA
Nathaniel J. Livesey
Jet Propulsion Laboratory, California Institute of Technology,
Pasadena, CA 91011, USA
Related authors
Srinath Krishnan, Ragnhild Bieltvedt Skeie, Øivind Hodnebrog, Gunnar Myhre, Maria Sand, Marit Sandstad, Hannah Bryant, Didier A. Hauglustaine, Fabien Paulot, Michael Prather, and David Stevenson
EGUsphere, https://doi.org/10.5194/egusphere-2025-4898, https://doi.org/10.5194/egusphere-2025-4898, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Hydrogen (H2) is an indirect greenhouse gas that can affect climate through chemical reactions in the atmosphere. To better understand this impact, it is important to constrain the sources and sinks of hydrogen. Using a suite of three-dimensional and one-dimensional models, we find that atmospheric production of hydrogen is 37–60 Tg/yr and that the geological source of H2 is much smaller than suggested. More field and isotopic measurements are needed to improve these estimates.
Maryam Ramezani Ziarani, Miriam Sinnhuber, Thomas Reddmann, Bernd Funke, Stefan Bender, and Michael Prather
Geosci. Model Dev., 18, 7891–7905, https://doi.org/10.5194/gmd-18-7891-2025, https://doi.org/10.5194/gmd-18-7891-2025, 2025
Short summary
Short summary
Our study aims to present a new method for incorporating top-down solar forcing into stratospheric ozone relying on linearized ozone scheme. The addition of geomagnetic forcing led to significant ozone losses in the polar upper stratosphere of both hemispheres due to the catalytic cycles involving NOy. In addition to the particle precipitation effect, accounting for solar UV variability in the ICON-ART model leads to the changes in ozone in the tropical stratosphere.
Gunnar Myhre, Øivind Hodnebrog, Srinath Krishnan, Maria Sand, Marit Sandstad, Ragnhild B. Skeie, Lieven Clarisse, Bruno Franco, Dylan B. Millet, Kelley C. Wells, Alexander Archibald, Hannah N. Bryant, Alex T. Chaudhri, David S. Stevenson, Didier Hauglustaine, Michael Prather, J. Christopher Kaiser, Dirk J. L. Olivie, Michael Schulz, Oliver Wild, Ye Wang, Thérèse Salameh, Jason E. Williams, Philippe Le Sager, Fabien Paulot, Kostas Tsigaridis, and Haley E. Plaas
EGUsphere, https://doi.org/10.5194/egusphere-2025-3057, https://doi.org/10.5194/egusphere-2025-3057, 2025
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
Short summary
Short summary
Volatile organic compounds (VOCs) affect air quality and climate, but their behavior in the atmosphere is still uncertain. We launched a global research effort to compare how different models represent these compounds and to improve their accuracy. By analyzing model results alongside observations and satellite data, we aim to better understand the atmospheric composition of these compounds.
Jinbo Xie, Qi Tang, Michael Prather, Jadwiga Richter, and Shixuan Zhang
Atmos. Chem. Phys., 25, 9315–9333, https://doi.org/10.5194/acp-25-9315-2025, https://doi.org/10.5194/acp-25-9315-2025, 2025
Short summary
Short summary
Analysis of the interaction between the climate and ozone in the stratosphere is complicated by the inability of climate models to simulate the quasi-biennial oscillation (QBO) – an important climate mode in the stratosphere. We use a set of model simulations that realistically simulate QBO and a novel ozone diagnostic tool to separate temperature- and circulation-driven QBO impacts. These are important for diagnosing model–model differences in QBO–ozone responses for climate projections.
Paul T. Griffiths, Laura J. Wilcox, Robert J. Allen, Vaishali Naik, Fiona M. O'Connor, Michael Prather, Alex Archibald, Florence Brown, Makoto Deushi, William Collins, Stephanie Fiedler, Naga Oshima, Lee T. Murray, Bjørn H. Samset, Chris Smith, Steven Turnock, Duncan Watson-Parris, and Paul J. Young
Atmos. Chem. Phys., 25, 8289–8328, https://doi.org/10.5194/acp-25-8289-2025, https://doi.org/10.5194/acp-25-8289-2025, 2025
Short summary
Short summary
The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) aimed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. We review its contribution to AR6 (Sixth Assessment Report of the Intergovernmental Panel on Climate Change) and the wider understanding of the role of these species in climate and climate change. We identify challenges and provide recommendations to improve the utility and uptake of climate model data, detailed summary tables of CMIP6 models, experiments, and emergent diagnostics.
Clara Orbe, Alison Ming, Gabriel Chiodo, Michael Prather, Mohamadou Diallo, Qi Tang, Andreas Chrysanthou, Hiroaki Naoe, Xin Zhou, Irina Thaler, Dillon Elsbury, Ewa Bednarz, Jonathon S. Wright, Aaron Match, Shingo Watanabe, James Anstey, Tobias Kerzenmacher, Stefan Versick, Marion Marchand, Feng Li, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2025-2761, https://doi.org/10.5194/egusphere-2025-2761, 2025
Short summary
Short summary
The quasi-biennial oscillation (QBO) is the main source of wind fluctuations in the tropical stratosphere, which can couple to surface climate. However, models do a poor job of simulating the QBO in the lower stratosphere, for reasons that remain unclear. One possibility is that models do not completely represent how ozone influences the QBO-associated wind variations. Here we propose a multi-model framework for assessing how ozone influences the QBO in recent past and future climates.
Calum P. Wilson and Michael J. Prather
Atmos. Meas. Tech., 18, 1757–1769, https://doi.org/10.5194/amt-18-1757-2025, https://doi.org/10.5194/amt-18-1757-2025, 2025
Short summary
Short summary
We evaluated how well we can infer air pollutant levels (ozone, carbon monoxide, and nitrogen oxides) between air quality stations throughout South Korea, finding good representation in most densely measured cities in spite of intense small-scale emission hotspots. Comparing observed air quality with gridded model output is desirable, and so we created gridded datasets over South Korea using air quality station measurements, which agreed with airborne measurements around Seoul.
Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
Earth Syst. Sci. Data, 16, 2543–2604, https://doi.org/10.5194/essd-16-2543-2024, https://doi.org/10.5194/essd-16-2543-2024, 2024
Short summary
Short summary
Atmospheric concentrations of nitrous oxide (N2O), a greenhouse gas 273 times more potent than carbon dioxide, have increased by 25 % since the preindustrial period, with the highest observed growth rate in 2020 and 2021. This rapid growth rate has primarily been due to a 40 % increase in anthropogenic emissions since 1980. Observed atmospheric N2O concentrations in recent years have exceeded the worst-case climate scenario, underscoring the importance of reducing anthropogenic N2O emissions.
Hsiang-He Lee, Qi Tang, and Michael Prather
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-203, https://doi.org/10.5194/gmd-2023-203, 2024
Revised manuscript not accepted
Short summary
Short summary
The E3SM Chemistry diagnostics package (ChemDyg) is a software tool, which is designed for the global climate model (E3SM) chemistry development. ChemDyg generates several diagnostic plots and tables for model-to-model and model-to-observation comparison, including 2-dimentional contour mapping plots, diurnal and annual cycle, time-series plots, and comprehensive processing tables. This paper is to introduce the details of each diagnostics set and its required input data formats in ChemDyg.
Michael J. Prather, Hao Guo, and Xin Zhu
Earth Syst. Sci. Data, 15, 3299–3349, https://doi.org/10.5194/essd-15-3299-2023, https://doi.org/10.5194/essd-15-3299-2023, 2023
Short summary
Short summary
The Atmospheric Tomography Mission (ATom) measured the chemical composition in air parcels from 0–12 km altitude on 2 km horizontal by 80 m vertical scales for four seasons, resolving most scales of chemical heterogeneity. ATom is one of the first missions designed to calculate the chemical evolution of each parcel, providing semi-global diurnal budgets for ozone and methane. Observations covered the remote troposphere: Pacific and Atlantic Ocean basins, Southern Ocean, Arctic basin, Antarctica.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
Short summary
Short summary
We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Michael J. Prather
Earth Syst. Dynam., 13, 703–709, https://doi.org/10.5194/esd-13-703-2022, https://doi.org/10.5194/esd-13-703-2022, 2022
Short summary
Short summary
Atmospheric CO2 fluctuations point to changes in fossil fuel emissions plus natural and perturbed variations in the natural carbon cycle. One unstudied source of variability is the stratosphere, where the influx of aged CO2-depleted air can cause surface fluctuations. Using modeling and, separately, scaling the observed N2O variability, I find that stratosphere-driven surface variability in CO2 is not a significant uncertainty (at most 10 % of the observed interannual variability).
Daniel J. Ruiz and Michael J. Prather
Atmos. Chem. Phys., 22, 2079–2093, https://doi.org/10.5194/acp-22-2079-2022, https://doi.org/10.5194/acp-22-2079-2022, 2022
Short summary
Short summary
The stratosphere is an important source of tropospheric ozone, which affects climate, chemistry, and air quality, but is extremely difficult to quantify given the large production and loss terms in the troposphere. Here, we use other gases that are well observed and quantified as a reference to test our simulations of ozone transport in the atmosphere. This allows us to better constrain the stratospheric source of ozone and also offers guidance to improve future simulations of ozone transport.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
Short summary
Short summary
The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Qi Tang, Michael J. Prather, Juno Hsu, Daniel J. Ruiz, Philip J. Cameron-Smith, Shaocheng Xie, and Jean-Christophe Golaz
Geosci. Model Dev., 14, 1219–1236, https://doi.org/10.5194/gmd-14-1219-2021, https://doi.org/10.5194/gmd-14-1219-2021, 2021
Srinath Krishnan, Ragnhild Bieltvedt Skeie, Øivind Hodnebrog, Gunnar Myhre, Maria Sand, Marit Sandstad, Hannah Bryant, Didier A. Hauglustaine, Fabien Paulot, Michael Prather, and David Stevenson
EGUsphere, https://doi.org/10.5194/egusphere-2025-4898, https://doi.org/10.5194/egusphere-2025-4898, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
Hydrogen (H2) is an indirect greenhouse gas that can affect climate through chemical reactions in the atmosphere. To better understand this impact, it is important to constrain the sources and sinks of hydrogen. Using a suite of three-dimensional and one-dimensional models, we find that atmospheric production of hydrogen is 37–60 Tg/yr and that the geological source of H2 is much smaller than suggested. More field and isotopic measurements are needed to improve these estimates.
Maryam Ramezani Ziarani, Miriam Sinnhuber, Thomas Reddmann, Bernd Funke, Stefan Bender, and Michael Prather
Geosci. Model Dev., 18, 7891–7905, https://doi.org/10.5194/gmd-18-7891-2025, https://doi.org/10.5194/gmd-18-7891-2025, 2025
Short summary
Short summary
Our study aims to present a new method for incorporating top-down solar forcing into stratospheric ozone relying on linearized ozone scheme. The addition of geomagnetic forcing led to significant ozone losses in the polar upper stratosphere of both hemispheres due to the catalytic cycles involving NOy. In addition to the particle precipitation effect, accounting for solar UV variability in the ICON-ART model leads to the changes in ozone in the tropical stratosphere.
Viktoria F. Sofieva, Alexandra Laeng, Thomas von Clarmann, Gabriele Stiller, Michael Kiefer, Johanna Tamminen, Alexey Rozanov, Carlo Arosio, Nathaniel Livesey, Robert Damadeo, Patrick Sheese, Kaley A. Walker, Doug Degenstein, Daniel Zawada, Natalya A. Kramarova, and Arno Keppens
EGUsphere, https://doi.org/10.5194/egusphere-2025-2830, https://doi.org/10.5194/egusphere-2025-2830, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
For satellite measurements of atmospheric composition, the random uncertainty estimates provided by retrieval algorithms might be imperfect due to various approximations used in the retrievals or presence of unknown error sources. This paper presents an overview of the methods used for validation of random uncertainty estimates. All methods discussed in this study are categorized, and assumptions and limitations of each method are discussed.
Gunnar Myhre, Øivind Hodnebrog, Srinath Krishnan, Maria Sand, Marit Sandstad, Ragnhild B. Skeie, Lieven Clarisse, Bruno Franco, Dylan B. Millet, Kelley C. Wells, Alexander Archibald, Hannah N. Bryant, Alex T. Chaudhri, David S. Stevenson, Didier Hauglustaine, Michael Prather, J. Christopher Kaiser, Dirk J. L. Olivie, Michael Schulz, Oliver Wild, Ye Wang, Thérèse Salameh, Jason E. Williams, Philippe Le Sager, Fabien Paulot, Kostas Tsigaridis, and Haley E. Plaas
EGUsphere, https://doi.org/10.5194/egusphere-2025-3057, https://doi.org/10.5194/egusphere-2025-3057, 2025
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
Short summary
Short summary
Volatile organic compounds (VOCs) affect air quality and climate, but their behavior in the atmosphere is still uncertain. We launched a global research effort to compare how different models represent these compounds and to improve their accuracy. By analyzing model results alongside observations and satellite data, we aim to better understand the atmospheric composition of these compounds.
Jinbo Xie, Qi Tang, Michael Prather, Jadwiga Richter, and Shixuan Zhang
Atmos. Chem. Phys., 25, 9315–9333, https://doi.org/10.5194/acp-25-9315-2025, https://doi.org/10.5194/acp-25-9315-2025, 2025
Short summary
Short summary
Analysis of the interaction between the climate and ozone in the stratosphere is complicated by the inability of climate models to simulate the quasi-biennial oscillation (QBO) – an important climate mode in the stratosphere. We use a set of model simulations that realistically simulate QBO and a novel ozone diagnostic tool to separate temperature- and circulation-driven QBO impacts. These are important for diagnosing model–model differences in QBO–ozone responses for climate projections.
Paul T. Griffiths, Laura J. Wilcox, Robert J. Allen, Vaishali Naik, Fiona M. O'Connor, Michael Prather, Alex Archibald, Florence Brown, Makoto Deushi, William Collins, Stephanie Fiedler, Naga Oshima, Lee T. Murray, Bjørn H. Samset, Chris Smith, Steven Turnock, Duncan Watson-Parris, and Paul J. Young
Atmos. Chem. Phys., 25, 8289–8328, https://doi.org/10.5194/acp-25-8289-2025, https://doi.org/10.5194/acp-25-8289-2025, 2025
Short summary
Short summary
The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) aimed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. We review its contribution to AR6 (Sixth Assessment Report of the Intergovernmental Panel on Climate Change) and the wider understanding of the role of these species in climate and climate change. We identify challenges and provide recommendations to improve the utility and uptake of climate model data, detailed summary tables of CMIP6 models, experiments, and emergent diagnostics.
Clara Orbe, Alison Ming, Gabriel Chiodo, Michael Prather, Mohamadou Diallo, Qi Tang, Andreas Chrysanthou, Hiroaki Naoe, Xin Zhou, Irina Thaler, Dillon Elsbury, Ewa Bednarz, Jonathon S. Wright, Aaron Match, Shingo Watanabe, James Anstey, Tobias Kerzenmacher, Stefan Versick, Marion Marchand, Feng Li, and James Keeble
EGUsphere, https://doi.org/10.5194/egusphere-2025-2761, https://doi.org/10.5194/egusphere-2025-2761, 2025
Short summary
Short summary
The quasi-biennial oscillation (QBO) is the main source of wind fluctuations in the tropical stratosphere, which can couple to surface climate. However, models do a poor job of simulating the QBO in the lower stratosphere, for reasons that remain unclear. One possibility is that models do not completely represent how ozone influences the QBO-associated wind variations. Here we propose a multi-model framework for assessing how ozone influences the QBO in recent past and future climates.
Calum P. Wilson and Michael J. Prather
Atmos. Meas. Tech., 18, 1757–1769, https://doi.org/10.5194/amt-18-1757-2025, https://doi.org/10.5194/amt-18-1757-2025, 2025
Short summary
Short summary
We evaluated how well we can infer air pollutant levels (ozone, carbon monoxide, and nitrogen oxides) between air quality stations throughout South Korea, finding good representation in most densely measured cities in spite of intense small-scale emission hotspots. Comparing observed air quality with gridded model output is desirable, and so we created gridded datasets over South Korea using air quality station measurements, which agreed with airborne measurements around Seoul.
Lucien Froidevaux, Douglas E. Kinnison, Benjamin Gaubert, Michael J. Schwartz, Nathaniel J. Livesey, William G. Read, Charles G. Bardeen, Jerry R. Ziemke, and Ryan A. Fuller
Atmos. Chem. Phys., 25, 597–624, https://doi.org/10.5194/acp-25-597-2025, https://doi.org/10.5194/acp-25-597-2025, 2025
Short summary
Short summary
We compare observed changes in ozone (O3) and carbon monoxide (CO) in the tropical upper troposphere (10–15 km altitude) for 2005–2020 to predictions from model simulations that track the evolution of natural and industrial emissions transported to this region. An increasing trend in measured upper-tropospheric O3 is well matched by model trends. We find that changes in modeled industrial CO surface emissions lead to better model agreement with observed slight decreases in upper-tropospheric CO.
Kimberlee Dubé, Susann Tegtmeier, Adam Bourassa, Daniel Zawada, Douglas Degenstein, William Randel, Sean Davis, Michael Schwartz, Nathaniel Livesey, and Anne Smith
Atmos. Chem. Phys., 24, 12925–12941, https://doi.org/10.5194/acp-24-12925-2024, https://doi.org/10.5194/acp-24-12925-2024, 2024
Short summary
Short summary
Greenhouse gas emissions that warm the troposphere also result in stratospheric cooling. The cooling rate is difficult to quantify above 35 km due to a deficit of long-term observational data with high vertical resolution in this region. We use satellite observations from several instruments, including a new temperature product from OSIRIS, to show that the upper stratosphere, from 35–60 km, cooled by 0.5 to 1 K per decade over 2005–2021 and by 0.6 K per decade over 1979–2021.
Hanqin Tian, Naiqing Pan, Rona L. Thompson, Josep G. Canadell, Parvadha Suntharalingam, Pierre Regnier, Eric A. Davidson, Michael Prather, Philippe Ciais, Marilena Muntean, Shufen Pan, Wilfried Winiwarter, Sönke Zaehle, Feng Zhou, Robert B. Jackson, Hermann W. Bange, Sarah Berthet, Zihao Bian, Daniele Bianchi, Alexander F. Bouwman, Erik T. Buitenhuis, Geoffrey Dutton, Minpeng Hu, Akihiko Ito, Atul K. Jain, Aurich Jeltsch-Thömmes, Fortunat Joos, Sian Kou-Giesbrecht, Paul B. Krummel, Xin Lan, Angela Landolfi, Ronny Lauerwald, Ya Li, Chaoqun Lu, Taylor Maavara, Manfredi Manizza, Dylan B. Millet, Jens Mühle, Prabir K. Patra, Glen P. Peters, Xiaoyu Qin, Peter Raymond, Laure Resplandy, Judith A. Rosentreter, Hao Shi, Qing Sun, Daniele Tonina, Francesco N. Tubiello, Guido R. van der Werf, Nicolas Vuichard, Junjie Wang, Kelley C. Wells, Luke M. Western, Chris Wilson, Jia Yang, Yuanzhi Yao, Yongfa You, and Qing Zhu
Earth Syst. Sci. Data, 16, 2543–2604, https://doi.org/10.5194/essd-16-2543-2024, https://doi.org/10.5194/essd-16-2543-2024, 2024
Short summary
Short summary
Atmospheric concentrations of nitrous oxide (N2O), a greenhouse gas 273 times more potent than carbon dioxide, have increased by 25 % since the preindustrial period, with the highest observed growth rate in 2020 and 2021. This rapid growth rate has primarily been due to a 40 % increase in anthropogenic emissions since 1980. Observed atmospheric N2O concentrations in recent years have exceeded the worst-case climate scenario, underscoring the importance of reducing anthropogenic N2O emissions.
Hsiang-He Lee, Qi Tang, and Michael Prather
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-203, https://doi.org/10.5194/gmd-2023-203, 2024
Revised manuscript not accepted
Short summary
Short summary
The E3SM Chemistry diagnostics package (ChemDyg) is a software tool, which is designed for the global climate model (E3SM) chemistry development. ChemDyg generates several diagnostic plots and tables for model-to-model and model-to-observation comparison, including 2-dimentional contour mapping plots, diurnal and annual cycle, time-series plots, and comprehensive processing tables. This paper is to introduce the details of each diagnostics set and its required input data formats in ChemDyg.
Michael J. Prather, Hao Guo, and Xin Zhu
Earth Syst. Sci. Data, 15, 3299–3349, https://doi.org/10.5194/essd-15-3299-2023, https://doi.org/10.5194/essd-15-3299-2023, 2023
Short summary
Short summary
The Atmospheric Tomography Mission (ATom) measured the chemical composition in air parcels from 0–12 km altitude on 2 km horizontal by 80 m vertical scales for four seasons, resolving most scales of chemical heterogeneity. ATom is one of the first missions designed to calculate the chemical evolution of each parcel, providing semi-global diurnal budgets for ozone and methane. Observations covered the remote troposphere: Pacific and Atlantic Ocean basins, Southern Ocean, Arctic basin, Antarctica.
Frank Werner, Nathaniel J. Livesey, Luis F. Millán, William G. Read, Michael J. Schwartz, Paul A. Wagner, William H. Daffer, Alyn Lambert, Sasha N. Tolstoff, and Michelle L. Santee
Atmos. Meas. Tech., 16, 2733–2751, https://doi.org/10.5194/amt-16-2733-2023, https://doi.org/10.5194/amt-16-2733-2023, 2023
Short summary
Short summary
The algorithm that produces the near-real-time data products of the Aura Microwave Limb Sounder has been updated. The new algorithm is based on machine learning techniques and yields data products with much improved accuracy. It is shown that the new algorithm outperforms the previous versions, even when it is trained on only a few years of satellite observations. This confirms the potential of applying machine learning to the near-real-time efforts of other current and future mission concepts.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
Short summary
Short summary
We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Eliane Maillard Barras, Alexander Haefele, René Stübi, Achille Jouberton, Herbert Schill, Irina Petropavlovskikh, Koji Miyagawa, Martin Stanek, and Lucien Froidevaux
Atmos. Chem. Phys., 22, 14283–14302, https://doi.org/10.5194/acp-22-14283-2022, https://doi.org/10.5194/acp-22-14283-2022, 2022
Short summary
Short summary
Intercomparisons of three Dobson and three Brewer spectrophotometers at Arosa/Davos, Switzerland, are used for the homogenization of the longest Umkehr ozone profiles time series worldwide. Dynamic linear modeling (DLM) reveals a significant positive trend after 2004 in the upper stratosphere, a persistent negative trend between 25 and 30 km in the middle stratosphere, and a negative trend at 20 km in the lower stratosphere, with different levels of significance depending on the dataset.
Sophie Godin-Beekmann, Niramson Azouz, Viktoria F. Sofieva, Daan Hubert, Irina Petropavlovskikh, Peter Effertz, Gérard Ancellet, Doug A. Degenstein, Daniel Zawada, Lucien Froidevaux, Stacey Frith, Jeannette Wild, Sean Davis, Wolfgang Steinbrecht, Thierry Leblanc, Richard Querel, Kleareti Tourpali, Robert Damadeo, Eliane Maillard Barras, René Stübi, Corinne Vigouroux, Carlo Arosio, Gerald Nedoluha, Ian Boyd, Roeland Van Malderen, Emmanuel Mahieu, Dan Smale, and Ralf Sussmann
Atmos. Chem. Phys., 22, 11657–11673, https://doi.org/10.5194/acp-22-11657-2022, https://doi.org/10.5194/acp-22-11657-2022, 2022
Short summary
Short summary
An updated evaluation up to 2020 of stratospheric ozone profile long-term trends at extrapolar latitudes based on satellite and ground-based records is presented. Ozone increase in the upper stratosphere is confirmed, with significant trends at most latitudes. In this altitude region, a very good agreement is found with trends derived from chemistry–climate model simulations. Observed and modelled trends diverge in the lower stratosphere, but the differences are non-significant.
Lucien Froidevaux, Douglas E. Kinnison, Michelle L. Santee, Luis F. Millán, Nathaniel J. Livesey, William G. Read, Charles G. Bardeen, John J. Orlando, and Ryan A. Fuller
Atmos. Chem. Phys., 22, 4779–4799, https://doi.org/10.5194/acp-22-4779-2022, https://doi.org/10.5194/acp-22-4779-2022, 2022
Short summary
Short summary
We analyze satellite-derived distributions of chlorine monoxide (ClO) and hypochlorous acid (HOCl) in the upper atmosphere. For 2005–2020, from 50°S to 50°N and over ~30 to 45 km, ClO and HOCl decreased by −0.7 % and −0.4 % per year, respectively. A detailed model of chemistry and dynamics agrees with the results. These decreases confirm the effectiveness of the 1987 Montreal Protocol, which limited emissions of chlorine- and bromine-containing source gases, in order to protect the ozone layer.
Michael J. Prather
Earth Syst. Dynam., 13, 703–709, https://doi.org/10.5194/esd-13-703-2022, https://doi.org/10.5194/esd-13-703-2022, 2022
Short summary
Short summary
Atmospheric CO2 fluctuations point to changes in fossil fuel emissions plus natural and perturbed variations in the natural carbon cycle. One unstudied source of variability is the stratosphere, where the influx of aged CO2-depleted air can cause surface fluctuations. Using modeling and, separately, scaling the observed N2O variability, I find that stratosphere-driven surface variability in CO2 is not a significant uncertainty (at most 10 % of the observed interannual variability).
Daniel J. Ruiz and Michael J. Prather
Atmos. Chem. Phys., 22, 2079–2093, https://doi.org/10.5194/acp-22-2079-2022, https://doi.org/10.5194/acp-22-2079-2022, 2022
Short summary
Short summary
The stratosphere is an important source of tropospheric ozone, which affects climate, chemistry, and air quality, but is extremely difficult to quantify given the large production and loss terms in the troposphere. Here, we use other gases that are well observed and quantified as a reference to test our simulations of ozone transport in the atmosphere. This allows us to better constrain the stratospheric source of ozone and also offers guidance to improve future simulations of ozone transport.
Frank Werner, Nathaniel J. Livesey, Michael J. Schwartz, William G. Read, Michelle L. Santee, and Galina Wind
Atmos. Meas. Tech., 14, 7749–7773, https://doi.org/10.5194/amt-14-7749-2021, https://doi.org/10.5194/amt-14-7749-2021, 2021
Short summary
Short summary
In this study we present an improved cloud detection scheme for the Microwave Limb Sounder, which is based on a feedforward artificial neural network. This new algorithm is shown not only to reliably detect high and mid-level convection containing even small amounts of cloud water but also to distinguish between high-reaching and mid-level to low convection.
Hugh C. Pumphrey, Michael J. Schwartz, Michelle L. Santee, George P. Kablick III, Michael D. Fromm, and Nathaniel J. Livesey
Atmos. Chem. Phys., 21, 16645–16659, https://doi.org/10.5194/acp-21-16645-2021, https://doi.org/10.5194/acp-21-16645-2021, 2021
Short summary
Short summary
Forest fires in British Columbia in August 2017 caused an unusual phenomonon: smoke and gases from the fires rose quickly to a height of 10 km. From there, the pollution continued to rise more slowly for many weeks, travelling around the world as it did so. In this paper, we describe how we used data from a satellite instrument to observe this polluted volume of air. The satellite has now been working for 16 years but has observed only three events of this type.
Nathaniel J. Livesey, William G. Read, Lucien Froidevaux, Alyn Lambert, Michelle L. Santee, Michael J. Schwartz, Luis F. Millán, Robert F. Jarnot, Paul A. Wagner, Dale F. Hurst, Kaley A. Walker, Patrick E. Sheese, and Gerald E. Nedoluha
Atmos. Chem. Phys., 21, 15409–15430, https://doi.org/10.5194/acp-21-15409-2021, https://doi.org/10.5194/acp-21-15409-2021, 2021
Short summary
Short summary
The Microwave Limb Sounder (MLS), an instrument on NASA's Aura mission launched in 2004, measures vertical profiles of the temperature and composition of Earth's "middle atmosphere" (the region from ~12 to ~100 km altitude). We describe how, among the 16 trace gases measured by MLS, the measurements of water vapor (H2O) and nitrous oxide (N2O) have started to drift since ~2010. The paper also discusses the origins of this drift and work to ameliorate it in a new version of the MLS dataset.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
Short summary
Short summary
The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Viktoria F. Sofieva, Monika Szeląg, Johanna Tamminen, Erkki Kyrölä, Doug Degenstein, Chris Roth, Daniel Zawada, Alexei Rozanov, Carlo Arosio, John P. Burrows, Mark Weber, Alexandra Laeng, Gabriele P. Stiller, Thomas von Clarmann, Lucien Froidevaux, Nathaniel Livesey, Michel van Roozendael, and Christian Retscher
Atmos. Chem. Phys., 21, 6707–6720, https://doi.org/10.5194/acp-21-6707-2021, https://doi.org/10.5194/acp-21-6707-2021, 2021
Short summary
Short summary
The MErged GRIdded Dataset of Ozone Profiles is a long-term (2001–2018) stratospheric ozone profile climate data record with resolved longitudinal structure that combines the data from six limb satellite instruments. The dataset can be used for various analyses, some of which are discussed in the paper. In particular, regionally and vertically resolved ozone trends are evaluated, including trends in the polar regions.
Qi Tang, Michael J. Prather, Juno Hsu, Daniel J. Ruiz, Philip J. Cameron-Smith, Shaocheng Xie, and Jean-Christophe Golaz
Geosci. Model Dev., 14, 1219–1236, https://doi.org/10.5194/gmd-14-1219-2021, https://doi.org/10.5194/gmd-14-1219-2021, 2021
Seidai Nara, Tomohiro O. Sato, Takayoshi Yamada, Tamaki Fujinawa, Kota Kuribayashi, Takeshi Manabe, Lucien Froidevaux, Nathaniel J. Livesey, Kaley A. Walker, Jian Xu, Franz Schreier, Yvan J. Orsolini, Varavut Limpasuvan, Nario Kuno, and Yasuko Kasai
Atmos. Meas. Tech., 13, 6837–6852, https://doi.org/10.5194/amt-13-6837-2020, https://doi.org/10.5194/amt-13-6837-2020, 2020
Short summary
Short summary
In the atmosphere, more than 80 % of chlorine compounds are anthropogenic. Hydrogen chloride (HCl), the main stratospheric chlorine reservoir, is useful to estimate the total budget of the atmospheric chlorine compounds. We report, for the first time, the HCl vertical distribution from the middle troposphere to the lower thermosphere using a high-sensitivity SMILES measurement; the data quality is quantified by comparisons with other measurements and via theoretical error analysis.
Cited articles
Abalos, M., Calvo, N., Benito-Barca, S., Garny, H., Hardiman, S. C., Lin, P., Andrews, M. B., Butchart, N., Garcia, R., Orbe, C., Saint-Martin, D., Watanabe, S., and Yoshida, K.: The Brewer–Dobson circulation in CMIP6, Atmos. Chem. Phys., 21, 13571–13591, https://doi.org/10.5194/acp-21-13571-2021, 2021.
Bernath P. F., Steffen J., Crouse J., and Boone C. D.: Sixteen-year trends
in atmospheric trace gases from orbit, J. Quant. Spectrosc. Ra., 253, 107178,
https://doi.org/10.1016/j.jqsrt.2020.107178, 2020.
Butchart, N.: The Brewer-Dobson circulation, Rev. Geophys., 52,
157–184, https://doi.org/10.1002/2013RG000448, 2014.
Butchart, N. and Scaife, A.: Removal of chlorofluorocarbons by increased mass
exchange between the stratosphere and troposphere in a changing climate,
Nature, 410, 799–802, https://doi.org/10.1038/35071047, 2001.
Chipperfield, M. P., Liang, Q., Strahan, S. E., Morgenstern, O., Dhomse, S. S.,
Abraham, N. L., Archibald, A. T., Bekki, S., Braesicke, P., Di Genova, G.,
Fleming, E. L., Hardiman, S. C., Iachetti, D., Jackman, C. H., Kinnison, D. E.,
Marchand, M., Pitari, G., Pyle, J. A., Rozanov, E., Stenke, A., and Tummon, F.:
Multi-model estimates of atmospheric lifetimes of long-lived Ozone-Depleting
Substances: Present and future, J. Geophys. Res., 119, 2555–2573,
https://doi.org/10.1002/2013JD021097, 2014.
Davidson, E. A.: Representative concentration pathways and mitigation
scenarios for nitrous oxide, Environ. Res. Lett., 7, 024005,
https://doi.org/10.1088/1748-9326/7/2/024005, 2012.
Dlugokencky, E.: Data from the NOAA web site, NOAA [data set],
https://gml.noaa.gov/webdata/ccgg/trends/n2o/n2o_mm_gl.txt (last access: 26 July 2023), 2022.
Forster, P., Storelvmo, T., Armour, K., Collins, W., Dufresne, J.-L., Frame, D.,
Lunt, D. J., Mauritsen, T., Palmer, M. D., Watanabe, M., Wild, M., and Zhang, H.: The Earth's Energy Budget, Climate Feedbacks, and Climate Sensitivity,
in: Climate Change 2021: The Physical Science Basis, Contribution of Working
Group I to the Sixth Assessment Report of the Intergovernmental Panel on
Climate Change, edited by: Masson-Delmotte, V., Zhai, P., Pirani, A., Connors, S. L., Péan, C., Berger, S., Caud, N., Chen, Y., Goldfarb, L., Gomis, M. I., Huang, M., Leitzell, K., Lonnoy, E., Matthews, J. B. R., Maycock, T. K., Waterfield, T., Yelekçi, O., Yu, R., and Zhou, B.,
Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA,
pp. 923–1054, https://www.ipcc.ch/report/ar6/wg1/ (last access: 13 January 2023), 2021.
Fritsch, F., Garny, H., Engel, A., Bönisch, H., and Eichinger, R.: Sensitivity of age of air trends to the derivation method for non-linear increasing inert SF6, Atmos. Chem. Phys., 20, 8709–8725, https://doi.org/10.5194/acp-20-8709-2020, 2020.
Froidevaux, L., Kinnison, D. E., Santee, M. L., Millán, L. F., Livesey, N. J., Read, W. G., Bardeen, C. G., Orlando, J. J., and Fuller, R. A.: Upper stratospheric ClO and HOCl trends (2005–2020): Aura Microwave Limb Sounder and model results, Atmos. Chem. Phys., 22, 4779–4799, https://doi.org/10.5194/acp-22-4779-2022, 2022.
Karpechko, A., Maycock, A., Abalos, M., Arblaster, J.,
Akiyoshi, H., Garfinkel, C., Rosenlof, K., and Sigmond, M.: Scientific Assessment of
Ozone Depletion: 2018, World Meteorological Organisation Global Ozone
Research and Monitoring Project-Report No. 58, WMO/UNEP Scientific
Assessment of Ozone Depletion: 2018. Chapter 5: Stratospheric Ozone Changes
and Climate, World Meteorological Organization, Geneva, Switzerland, 2018.
Lambert, A., Livesey, N., Read, W., and Fuller, R.: MLS/Aura Level 3 Monthly
Binned Nitrous Oxide (N2O) Mixing Ratio on Assorted Grids V005, Greenbelt,
MD, USA, Goddard Earth Sciences Data and Information Services Center (GES
DISC) [data set], https://disc.gsfc.nasa.gov/datasets/ML3MBN2O_005/summary (last access: 13 January 2023), 2021.
Livesey, N. J., Read, W. G., Froidevaux, L., Lambert, A., Santee, M. L., Schwartz, M. J., Millán, L. F., Jarnot, R. F., Wagner, P. A., Hurst, D. F., Walker, K. A., Sheese, P. E., and Nedoluha, G. E.: Investigation and amelioration of long-term instrumental drifts in water vapor and nitrous oxide measurements from the Aura Microwave Limb Sounder (MLS) and their implications for studies of variability and trends, Atmos. Chem. Phys., 21, 15409–15430, https://doi.org/10.5194/acp-21-15409-2021, 2021.
Maycock, A. C., Randel, W. J., Steiner, A. K., Karpechko, A. Y., Christy,
J., Saunders, R., Thompson, D. W. J., Zou, C.-Z., Chrysanthou, A., Abraham, N. L., Akiyoshi, H., Archibald, A. T., Butchart, N., Chipperfield, M., Dameris, M., Deushi, M., Dhomse, S., Di Genova, G., Jöckel, P., Kinnison, D. E., Kirner, O., Ladstaedter, F., Michou, M., Morgenstern, O., O'Connor, F., Oman, L., Pitari, G., Plummer, D. A., Revell, L. E., Rozanov, E., Stenke, A., Visioni, D., Yamashita, Y., and Zeng, G.: Revisiting the mystery of recent stratospheric
temperature trends, Geophys. Res. Lett., 45, 9919–9933,
https://doi.org/10.1029/2018GL078035, 2018.
Neu, J. L. and Plumb, R. A.: Age of air in a “leaky pipe” model of
stratospheric transport, J. Geophys. Res., 104, 19243–19255,
https://doi.org/10.1029/1999JD900251, 1999.
Nevison, C. D., Keim, E. R., Solomon, S., Fahey, D. W., Elkins, J. W.,
Lowenstein, M., and Podolske, J. R.: Constraints on N2O sinks inferred from
observed tracer correlations in the lower stratosphere, Global
Biogeochem. Cy., 13, 737–742, 1999.
Plumb, R. A. and Mahlman, J. D.: The zonally-averaged transport
characteristics of the GFDL general circulation/tracer model, J. Atmos.
Sci., 44, 298–327, https://doi.org/10.1175/1520-0469(1987)044<0298:TZATCO>2.0.CO;2, 1987.
Prather, M. J.: Time scales in atmospheric chemistry: coupled perturbations
to N2O, NOy, and O3, Science, 279, 1339–1341, 1998.
Prather, M. J., Holmes, C. D., and Hsu, J.: Reactive greenhouse gas scenarios:
Systematic exploration of uncertainties and the role of atmospheric
chemistry, Geophys. Res. Lett., 39, L09803, https://doi.org/10.1029/2012GL051440,
2012.
Prather, M. J., Hsu, J., DeLuca, N. M., Jackman, C. H., Oman, L. D., Douglass, A. R.,
Fleming, E. L., Strahan, S. E., Steenrod, S. D., Søvde, O. A.,
Isaksen, I. S. A., Froidevaux, L., and Funke, B.: Measuring and modeling the lifetime of
nitrous oxide including its variability, J. Geophys. Res.-Atmos., 120,
5693–5705, https://doi.org/10.1002/2015JD023267, 2015.
Ruiz, D. J., Prather, M. J., Strahan, S. E., Thompson, R. L.,
Froidevaux, L., and Steenrod, S. D.: How atmospheric chemistry and
transport drive surface variability of N2O and CFC-11, J. Geophys. Res.-Atmos., 126, e2020JD033979, https://doi.org/10.1029/2020JD033979, 2021.
Schwartz, M., Livesey, N., Read, W., and Fuller, R.: MLS/Aura Level 3
Monthly Binned Temperature on Assorted Grids V005, Greenbelt, MD, USA,
Goddard Earth Sciences Data and Information Services Center (GES DISC) [data set],
https://disc.gsfc.nasa.gov/datasets/ML3MBT_005/summary (last access: 13 January 2023),
2021a.
Schwartz, M., Froidevaux, L., Livesey, N., Read, W., and Fuller, R.:
MLS/Aura Level 3 Monthly Binned Ozone (O3) Mixing Ratio on Assorted Grids
V005, Greenbelt, MD, USA, Goddard Earth Sciences Data and Information
Services Center (GES DISC) [data set], https://disc.gsfc.nasa.gov/datasets/ML3MBO3_005/summary (last access: 13 January 2023), 2021b.
Strahan, S. E., Coy, L., Douglass, A. R., and Damon, M. R.: Faster tropical
upper stratospheric upwelling drives changes in ozone chemistry, Geophys.
Res. Lett., 49, e2022GL101075, https://doi.org/10.1029/2022GL101075, 2022.
World Meteorological Organization (WMO): Executive Summary, Scientific Assessment of Ozone Depletion: 2022, GAW Report No. 278, 56 pp., WMO: Geneva, ISBN 978-9914-733-99-0, 2022.
Short summary
From satellite data for nitrous oxide (N2O), ozone and temperature, we calculate the monthly loss of N2O and find it is increasing faster than expected, resulting in a shorter lifetime, which reduces the impact of anthropogenic emissions. We identify the cause as enhanced vertical lofting of high-N2O air into the tropical middle stratosphere, where it is destroyed photochemically. Because global warming is due in part to N2O, this finding presents a new negative climate-chemistry feedback.
From satellite data for nitrous oxide (N2O), ozone and temperature, we calculate the monthly...
Altmetrics
Final-revised paper
Preprint