Articles | Volume 17, issue 6
https://doi.org/10.5194/acp-17-3963-2017
© Author(s) 2017. 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-17-3963-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Review article
| 
24 Mar 2017
Review article |
| 24 Mar 2017
Constraining sector-specific CO2 and CH4 emissions in the US
Department of Global Ecology, Carnegie Institution for Science, Stanford, CA, USA
Anna M. Michalak
Department of Global Ecology, Carnegie Institution for Science, Stanford, CA, USA
Related authors
Malena Sabaté Landman, Julianne Chung, Jiahua Jiang, Scot Miller, and Arvind Saibaba
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-90, https://doi.org/10.5194/gmd-2024-90, 2024
Revised manuscript under review for GMD
Short summary
Short summary
Making an informed decision about what prior information to incorporate or discard in an inverse model is important yet very challenging, as it is often not straightforward to distinguish between informative and non-informative variables. In this study, we develop a new approach for incorporating prior information in an inverse model using predictor variables, while simultaneously selecting the relevant predictor variables for the estimation of the unknown quantity of interest.
Brendan Byrne, David F. Baker, Sourish Basu, Michael Bertolacci, Kevin W. Bowman, Dustin Carroll, Abhishek Chatterjee, Frédéric Chevallier, Philippe Ciais, Noel Cressie, David Crisp, Sean Crowell, Feng Deng, Zhu Deng, Nicholas M. Deutscher, Manvendra K. Dubey, Sha Feng, Omaira E. García, David W. T. Griffith, Benedikt Herkommer, Lei Hu, Andrew R. Jacobson, Rajesh Janardanan, Sujong Jeong, Matthew S. Johnson, Dylan B. A. Jones, Rigel Kivi, Junjie Liu, Zhiqiang Liu, Shamil Maksyutov, John B. Miller, Scot M. Miller, Isamu Morino, Justus Notholt, Tomohiro Oda, Christopher W. O'Dell, Young-Suk Oh, Hirofumi Ohyama, Prabir K. Patra, Hélène Peiro, Christof Petri, Sajeev Philip, David F. Pollard, Benjamin Poulter, Marine Remaud, Andrew Schuh, Mahesh K. Sha, Kei Shiomi, Kimberly Strong, Colm Sweeney, Yao Té, Hanqin Tian, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, John R. Worden, Debra Wunch, Yuanzhi Yao, Jeongmin Yun, Andrew Zammit-Mangion, and Ning Zeng
Earth Syst. Sci. Data, 15, 963–1004, https://doi.org/10.5194/essd-15-963-2023, https://doi.org/10.5194/essd-15-963-2023, 2023
Short summary
Short summary
Changes in the carbon stocks of terrestrial ecosystems result in emissions and removals of CO2. These can be driven by anthropogenic activities (e.g., deforestation), natural processes (e.g., fires) or in response to rising CO2 (e.g., CO2 fertilization). This paper describes a dataset of CO2 emissions and removals derived from atmospheric CO2 observations. This pilot dataset informs current capabilities and future developments towards top-down monitoring and verification systems.
Taewon Cho, Julianne Chung, Scot M. Miller, and Arvind K. Saibaba
Geosci. Model Dev., 15, 5547–5565, https://doi.org/10.5194/gmd-15-5547-2022, https://doi.org/10.5194/gmd-15-5547-2022, 2022
Short summary
Short summary
Atmospheric inverse modeling describes the process of estimating greenhouse gas fluxes or air pollution emissions at the Earth's surface using observations of these gases collected in the atmosphere. The launch of new satellites, the expansion of surface observation networks, and a desire for more detailed maps of surface fluxes have yielded numerous computational and statistical challenges. This article describes computationally efficient methods for large-scale atmospheric inverse modeling.
Xiaoling Liu, August L. Weinbren, He Chang, Jovan M. Tadić, Marikate E. Mountain, Michael E. Trudeau, Arlyn E. Andrews, Zichong Chen, and Scot M. Miller
Geosci. Model Dev., 14, 4683–4696, https://doi.org/10.5194/gmd-14-4683-2021, https://doi.org/10.5194/gmd-14-4683-2021, 2021
Short summary
Short summary
Observations of greenhouse gases have become far more numerous in recent years due to new satellite observations. The sheer size of these datasets makes it challenging to incorporate these data into statistical models and use these data to estimate greenhouse gas sources and sinks. In this paper, we develop an approach to reduce the size of these datasets while preserving the most information possible. We subsequently test this approach using satellite observations of carbon dioxide.
Zichong Chen, Junjie Liu, Daven K. Henze, Deborah N. Huntzinger, Kelley C. Wells, Stephen Sitch, Pierre Friedlingstein, Emilie Joetzjer, Vladislav Bastrikov, Daniel S. Goll, Vanessa Haverd, Atul K. Jain, Etsushi Kato, Sebastian Lienert, Danica L. Lombardozzi, Patrick C. McGuire, Joe R. Melton, Julia E. M. S. Nabel, Benjamin Poulter, Hanqin Tian, Andrew J. Wiltshire, Sönke Zaehle, and Scot M. Miller
Atmos. Chem. Phys., 21, 6663–6680, https://doi.org/10.5194/acp-21-6663-2021, https://doi.org/10.5194/acp-21-6663-2021, 2021
Short summary
Short summary
NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes atmospheric CO2 globally. We use a multiple regression and inverse model to quantify the relationships between OCO-2 and environmental drivers within individual years for 2015–2018 and within seven global biomes. Our results point to limitations of current space-based observations for inferring environmental relationships but also indicate the potential to inform key relationships that are very uncertain in process-based models.
Scot M. Miller, Arvind K. Saibaba, Michael E. Trudeau, Marikate E. Mountain, and Arlyn E. Andrews
Geosci. Model Dev., 13, 1771–1785, https://doi.org/10.5194/gmd-13-1771-2020, https://doi.org/10.5194/gmd-13-1771-2020, 2020
Short summary
Short summary
New observations of greenhouse gases from satellites and aircraft provide an unprecedented window into global carbon sources and sinks. However, these new datasets also present enormous computational challenges due to the sheer number of observations. In this article, we discuss the challenges of estimating greenhouse gas source and sinks using very large atmospheric datasets and evaluate several strategies for overcoming these challenges.
Scot M. Miller and Anna M. Michalak
Atmos. Chem. Phys., 20, 323–331, https://doi.org/10.5194/acp-20-323-2020, https://doi.org/10.5194/acp-20-323-2020, 2020
Short summary
Short summary
NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes CO2 in the atmosphere. The satellite measures radiation, and these measurements are then converted to an estimate of atmospheric CO2. This conversion or retrieval algorithm has improved markedly since the satellite launch. We find that these improvements in the CO2 retrieval are having a potentially transformative effect on satellite-based estimates of the global biospheric carbon balance.
Scot M. Miller, Anna M. Michalak, Vineet Yadav, and Jovan M. Tadić
Atmos. Chem. Phys., 18, 6785–6799, https://doi.org/10.5194/acp-18-6785-2018, https://doi.org/10.5194/acp-18-6785-2018, 2018
Short summary
Short summary
NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes CO2 in the atmosphere globally. We evaluate the extent to which current OCO-2 observations can inform scientific understanding of the biospheric carbon balance. We find that current observations are best-equipped to constrain the biospheric carbon balance across continental or hemispheric regions and provide limited information on smaller regions.
Nils Hase, Scot M. Miller, Peter Maaß, Justus Notholt, Mathias Palm, and Thorsten Warneke
Geosci. Model Dev., 10, 3695–3713, https://doi.org/10.5194/gmd-10-3695-2017, https://doi.org/10.5194/gmd-10-3695-2017, 2017
Short summary
Short summary
Inverse modeling uses atmospheric measurements to estimate emissions of greenhouse gases, which are key to understand the climate system. However, the measurement information alone is typically insufficient to provide reasonable emission estimates. Additional information is required. This article applies modern mathematical inversion techniques to formulate such additional knowledge. It is a prime example of how such tools can improve the quality of estimates compared to commonly used methods.
Jovan M. Tadić, Xuemei Qiu, Scot Miller, and Anna M. Michalak
Geosci. Model Dev., 10, 709–720, https://doi.org/10.5194/gmd-10-709-2017, https://doi.org/10.5194/gmd-10-709-2017, 2017
Short summary
Short summary
We developed a new method to create contiguous maps from sparse and/or noisy satellite observations. This approach could be used to produce retroactive or real-time estimates of environmental data observed by satellites which exhibit spatio-temporal autocorrelations. The method could be applied in a standalone mode or as part of a broader satellite data processing package. Maps produced in this way could then be incorporated into physical and biogeochemical models of the Earth system.
Scot M. Miller, Roisin Commane, Joe R. Melton, Arlyn E. Andrews, Joshua Benmergui, Edward J. Dlugokencky, Greet Janssens-Maenhout, Anna M. Michalak, Colm Sweeney, and Doug E. J. Worthy
Biogeosciences, 13, 1329–1339, https://doi.org/10.5194/bg-13-1329-2016, https://doi.org/10.5194/bg-13-1329-2016, 2016
Short summary
Short summary
We use atmospheric data from the US and Canada to examine seven wetland methane flux estimates. Relative to existing estimates, we find a methane source that is smaller in magnitude with a broader seasonal cycle. Furthermore, we estimate the largest fluxes over the Hudson Bay Lowlands, a spatial distribution that differs from commonly used remote sensing estimates of wetland location.
S. M. Miller, M. N. Hayek, A. E. Andrews, I. Fung, and J. Liu
Atmos. Chem. Phys., 15, 2903–2914, https://doi.org/10.5194/acp-15-2903-2015, https://doi.org/10.5194/acp-15-2903-2015, 2015
S. M. Miller, A. M. Michalak, and P. J. Levi
Geosci. Model Dev., 7, 303–315, https://doi.org/10.5194/gmd-7-303-2014, https://doi.org/10.5194/gmd-7-303-2014, 2014
Malena Sabaté Landman, Julianne Chung, Jiahua Jiang, Scot Miller, and Arvind Saibaba
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-90, https://doi.org/10.5194/gmd-2024-90, 2024
Revised manuscript under review for GMD
Short summary
Short summary
Making an informed decision about what prior information to incorporate or discard in an inverse model is important yet very challenging, as it is often not straightforward to distinguish between informative and non-informative variables. In this study, we develop a new approach for incorporating prior information in an inverse model using predictor variables, while simultaneously selecting the relevant predictor variables for the estimation of the unknown quantity of interest.
Kelsey T. Foster, Wu Sun, Yoichi P. Shiga, Jiafu Mao, and Anna M. Michalak
Biogeosciences, 21, 869–891, https://doi.org/10.5194/bg-21-869-2024, https://doi.org/10.5194/bg-21-869-2024, 2024
Short summary
Short summary
Assessing agreement between bottom-up and top-down methods across spatial scales can provide insights into the relationship between ensemble spread (difference across models) and model accuracy (difference between model estimates and reality). We find that ensemble spread is unlikely to be a good indicator of actual uncertainty in the North American carbon balance. However, models that are consistent with atmospheric constraints show stronger agreement between top-down and bottom-up estimates.
Brendan Byrne, David F. Baker, Sourish Basu, Michael Bertolacci, Kevin W. Bowman, Dustin Carroll, Abhishek Chatterjee, Frédéric Chevallier, Philippe Ciais, Noel Cressie, David Crisp, Sean Crowell, Feng Deng, Zhu Deng, Nicholas M. Deutscher, Manvendra K. Dubey, Sha Feng, Omaira E. García, David W. T. Griffith, Benedikt Herkommer, Lei Hu, Andrew R. Jacobson, Rajesh Janardanan, Sujong Jeong, Matthew S. Johnson, Dylan B. A. Jones, Rigel Kivi, Junjie Liu, Zhiqiang Liu, Shamil Maksyutov, John B. Miller, Scot M. Miller, Isamu Morino, Justus Notholt, Tomohiro Oda, Christopher W. O'Dell, Young-Suk Oh, Hirofumi Ohyama, Prabir K. Patra, Hélène Peiro, Christof Petri, Sajeev Philip, David F. Pollard, Benjamin Poulter, Marine Remaud, Andrew Schuh, Mahesh K. Sha, Kei Shiomi, Kimberly Strong, Colm Sweeney, Yao Té, Hanqin Tian, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, John R. Worden, Debra Wunch, Yuanzhi Yao, Jeongmin Yun, Andrew Zammit-Mangion, and Ning Zeng
Earth Syst. Sci. Data, 15, 963–1004, https://doi.org/10.5194/essd-15-963-2023, https://doi.org/10.5194/essd-15-963-2023, 2023
Short summary
Short summary
Changes in the carbon stocks of terrestrial ecosystems result in emissions and removals of CO2. These can be driven by anthropogenic activities (e.g., deforestation), natural processes (e.g., fires) or in response to rising CO2 (e.g., CO2 fertilization). This paper describes a dataset of CO2 emissions and removals derived from atmospheric CO2 observations. This pilot dataset informs current capabilities and future developments towards top-down monitoring and verification systems.
Taewon Cho, Julianne Chung, Scot M. Miller, and Arvind K. Saibaba
Geosci. Model Dev., 15, 5547–5565, https://doi.org/10.5194/gmd-15-5547-2022, https://doi.org/10.5194/gmd-15-5547-2022, 2022
Short summary
Short summary
Atmospheric inverse modeling describes the process of estimating greenhouse gas fluxes or air pollution emissions at the Earth's surface using observations of these gases collected in the atmosphere. The launch of new satellites, the expansion of surface observation networks, and a desire for more detailed maps of surface fluxes have yielded numerous computational and statistical challenges. This article describes computationally efficient methods for large-scale atmospheric inverse modeling.
Xiaoling Liu, August L. Weinbren, He Chang, Jovan M. Tadić, Marikate E. Mountain, Michael E. Trudeau, Arlyn E. Andrews, Zichong Chen, and Scot M. Miller
Geosci. Model Dev., 14, 4683–4696, https://doi.org/10.5194/gmd-14-4683-2021, https://doi.org/10.5194/gmd-14-4683-2021, 2021
Short summary
Short summary
Observations of greenhouse gases have become far more numerous in recent years due to new satellite observations. The sheer size of these datasets makes it challenging to incorporate these data into statistical models and use these data to estimate greenhouse gas sources and sinks. In this paper, we develop an approach to reduce the size of these datasets while preserving the most information possible. We subsequently test this approach using satellite observations of carbon dioxide.
Zichong Chen, Junjie Liu, Daven K. Henze, Deborah N. Huntzinger, Kelley C. Wells, Stephen Sitch, Pierre Friedlingstein, Emilie Joetzjer, Vladislav Bastrikov, Daniel S. Goll, Vanessa Haverd, Atul K. Jain, Etsushi Kato, Sebastian Lienert, Danica L. Lombardozzi, Patrick C. McGuire, Joe R. Melton, Julia E. M. S. Nabel, Benjamin Poulter, Hanqin Tian, Andrew J. Wiltshire, Sönke Zaehle, and Scot M. Miller
Atmos. Chem. Phys., 21, 6663–6680, https://doi.org/10.5194/acp-21-6663-2021, https://doi.org/10.5194/acp-21-6663-2021, 2021
Short summary
Short summary
NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes atmospheric CO2 globally. We use a multiple regression and inverse model to quantify the relationships between OCO-2 and environmental drivers within individual years for 2015–2018 and within seven global biomes. Our results point to limitations of current space-based observations for inferring environmental relationships but also indicate the potential to inform key relationships that are very uncertain in process-based models.
Scot M. Miller, Arvind K. Saibaba, Michael E. Trudeau, Marikate E. Mountain, and Arlyn E. Andrews
Geosci. Model Dev., 13, 1771–1785, https://doi.org/10.5194/gmd-13-1771-2020, https://doi.org/10.5194/gmd-13-1771-2020, 2020
Short summary
Short summary
New observations of greenhouse gases from satellites and aircraft provide an unprecedented window into global carbon sources and sinks. However, these new datasets also present enormous computational challenges due to the sheer number of observations. In this article, we discuss the challenges of estimating greenhouse gas source and sinks using very large atmospheric datasets and evaluate several strategies for overcoming these challenges.
Scot M. Miller and Anna M. Michalak
Atmos. Chem. Phys., 20, 323–331, https://doi.org/10.5194/acp-20-323-2020, https://doi.org/10.5194/acp-20-323-2020, 2020
Short summary
Short summary
NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes CO2 in the atmosphere. The satellite measures radiation, and these measurements are then converted to an estimate of atmospheric CO2. This conversion or retrieval algorithm has improved markedly since the satellite launch. We find that these improvements in the CO2 retrieval are having a potentially transformative effect on satellite-based estimates of the global biospheric carbon balance.
Peter J. Rayner, Anna M. Michalak, and Frédéric Chevallier
Atmos. Chem. Phys., 19, 13911–13932, https://doi.org/10.5194/acp-19-13911-2019, https://doi.org/10.5194/acp-19-13911-2019, 2019
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This paper describes the methods for combining models and data to understand how nutrients and pollutants move through natural systems. The methods are analogous to the process of weather forecasting in which previous information is combined with new observations and a model to improve our knowledge of the internal state of the physical system. The methods appear highly diverse but the paper shows that they are all examples of a single underlying formalism.
Ju-Mee Ryoo, Laura T. Iraci, Tomoaki Tanaka, Josette E. Marrero, Emma L. Yates, Inez Fung, Anna M. Michalak, Jovan Tadić, Warren Gore, T. Paul Bui, Jonathan M. Dean-Day, and Cecilia S. Chang
Atmos. Meas. Tech., 12, 2949–2966, https://doi.org/10.5194/amt-12-2949-2019, https://doi.org/10.5194/amt-12-2949-2019, 2019
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We designed cylindrical flights and computed the emission fluxes using a kriging method and Gauss's theorem over Sacramento, California. Differences in wind treatment and background affect the emission estimates by a factor of 1.5 to 7. The effects of the vertical layer average and the vertical mass transfer on the emission estimates are found to be small, esp. local scale. The result also suggests a closed-shape flight profile can better contain total emissions than a one-sided curtain flight.
Scot M. Miller, Anna M. Michalak, Vineet Yadav, and Jovan M. Tadić
Atmos. Chem. Phys., 18, 6785–6799, https://doi.org/10.5194/acp-18-6785-2018, https://doi.org/10.5194/acp-18-6785-2018, 2018
Short summary
Short summary
NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes CO2 in the atmosphere globally. We evaluate the extent to which current OCO-2 observations can inform scientific understanding of the biospheric carbon balance. We find that current observations are best-equipped to constrain the biospheric carbon balance across continental or hemispheric regions and provide limited information on smaller regions.
Nils Hase, Scot M. Miller, Peter Maaß, Justus Notholt, Mathias Palm, and Thorsten Warneke
Geosci. Model Dev., 10, 3695–3713, https://doi.org/10.5194/gmd-10-3695-2017, https://doi.org/10.5194/gmd-10-3695-2017, 2017
Short summary
Short summary
Inverse modeling uses atmospheric measurements to estimate emissions of greenhouse gases, which are key to understand the climate system. However, the measurement information alone is typically insufficient to provide reasonable emission estimates. Additional information is required. This article applies modern mathematical inversion techniques to formulate such additional knowledge. It is a prime example of how such tools can improve the quality of estimates compared to commonly used methods.
Anna M. Michalak, Nina A. Randazzo, and Frédéric Chevallier
Atmos. Chem. Phys., 17, 7405–7421, https://doi.org/10.5194/acp-17-7405-2017, https://doi.org/10.5194/acp-17-7405-2017, 2017
Short summary
Short summary
The use of inverse modeling for quantifying emissions of greenhouse gases is increasing. Estimates are very difficult to evaluate objectively, however, due to limited atmospheric observations and the lack of direct emissions measurements at compatible scales. Diagnostic tools have been proposed to partially circumvent these limitations. This paper presents the first systematic review of the scope and applicability of these tools for atmospheric inversions of long-lived greenhouse gases.
Jovan M. Tadić, Xuemei Qiu, Scot Miller, and Anna M. Michalak
Geosci. Model Dev., 10, 709–720, https://doi.org/10.5194/gmd-10-709-2017, https://doi.org/10.5194/gmd-10-709-2017, 2017
Short summary
Short summary
We developed a new method to create contiguous maps from sparse and/or noisy satellite observations. This approach could be used to produce retroactive or real-time estimates of environmental data observed by satellites which exhibit spatio-temporal autocorrelations. The method could be applied in a standalone mode or as part of a broader satellite data processing package. Maps produced in this way could then be incorporated into physical and biogeochemical models of the Earth system.
Sander Houweling, Peter Bergamaschi, Frederic Chevallier, Martin Heimann, Thomas Kaminski, Maarten Krol, Anna M. Michalak, and Prabir Patra
Atmos. Chem. Phys., 17, 235–256, https://doi.org/10.5194/acp-17-235-2017, https://doi.org/10.5194/acp-17-235-2017, 2017
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The aim of this paper is to present an overview of inverse modeling methods, developed over the years, for estimating the global sources and sinks of the greenhouse gas methane from atmospheric measurements. It provides insight into how techniques and estimates have evolved over time, what the remaining shortcomings are, new developments, and promising future directions.
Vineet Yadav and Anna M. Michalak
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2016-204, https://doi.org/10.5194/gmd-2016-204, 2016
Revised manuscript has not been submitted
Short summary
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Multiplication of two matrices that consists of few non-zero entries is a fundamental operation in problems that involve estimation of greenhouse gas fluxes from atmospheric measurements. To increase computational efficiency of estimating these quantities, modification of the standard matrix multiplication algorithm for multiplying these matrices is proposed in this research.
Bjorn-Gustaf J. Brooks, Ankur R. Desai, Britton B. Stephens, Anna M. Michalak, and Jakob Zscheischler
Biogeosciences Discuss., https://doi.org/10.5194/bg-2016-223, https://doi.org/10.5194/bg-2016-223, 2016
Manuscript not accepted for further review
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CO2 is the primary greenhouse gas, and its abundance in the atmosphere tends to increase during disturbances like drought. This paper demonstrates how CO2 measurements are combined with models to determine not only how strongly different locations influence CO2 measurement stations, but also the capacity of those measurement stations to detect drought effects. Understanding detection sensitivity will help assess what kinds of changes and turnings points can be monitored using atmospheric CO2.
Scot M. Miller, Roisin Commane, Joe R. Melton, Arlyn E. Andrews, Joshua Benmergui, Edward J. Dlugokencky, Greet Janssens-Maenhout, Anna M. Michalak, Colm Sweeney, and Doug E. J. Worthy
Biogeosciences, 13, 1329–1339, https://doi.org/10.5194/bg-13-1329-2016, https://doi.org/10.5194/bg-13-1329-2016, 2016
Short summary
Short summary
We use atmospheric data from the US and Canada to examine seven wetland methane flux estimates. Relative to existing estimates, we find a methane source that is smaller in magnitude with a broader seasonal cycle. Furthermore, we estimate the largest fluxes over the Hudson Bay Lowlands, a spatial distribution that differs from commonly used remote sensing estimates of wetland location.
J. M. Tadić, X. Qiu, V. Yadav, and A. M. Michalak
Geosci. Model Dev., 8, 3311–3319, https://doi.org/10.5194/gmd-8-3311-2015, https://doi.org/10.5194/gmd-8-3311-2015, 2015
J. Ray, J. Lee, V. Yadav, S. Lefantzi, A. M. Michalak, and B. van Bloemen Waanders
Geosci. Model Dev., 8, 1259–1273, https://doi.org/10.5194/gmd-8-1259-2015, https://doi.org/10.5194/gmd-8-1259-2015, 2015
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The paper presents a statistical method (shrinkage) that can be used to estimate rough emission fields, e.g., fossil fuel CO2 emissions, from measurements of concentrations. This method is demonstrated in a test case where the emissions are modeled using wavelets. We find that the method can eliminate unnecessary complexity from the wavelet model, ensures non-negativity of the emissions, is computationally efficient and is, by construction, insensitive to prior guesses of the total emission.
S. M. Miller, M. N. Hayek, A. E. Andrews, I. Fung, and J. Liu
Atmos. Chem. Phys., 15, 2903–2914, https://doi.org/10.5194/acp-15-2903-2015, https://doi.org/10.5194/acp-15-2903-2015, 2015
Y. Wei, S. Liu, D. N. Huntzinger, A. M. Michalak, N. Viovy, W. M. Post, C. R. Schwalm, K. Schaefer, A. R. Jacobson, C. Lu, H. Tian, D. M. Ricciuto, R. B. Cook, J. Mao, and X. Shi
Geosci. Model Dev., 7, 2875–2893, https://doi.org/10.5194/gmd-7-2875-2014, https://doi.org/10.5194/gmd-7-2875-2014, 2014
J. Ray, V. Yadav, A. M. Michalak, B. van Bloemen Waanders, and S. A. McKenna
Geosci. Model Dev., 7, 1901–1918, https://doi.org/10.5194/gmd-7-1901-2014, https://doi.org/10.5194/gmd-7-1901-2014, 2014
S. M. Miller, A. M. Michalak, and P. J. Levi
Geosci. Model Dev., 7, 303–315, https://doi.org/10.5194/gmd-7-303-2014, https://doi.org/10.5194/gmd-7-303-2014, 2014
A. Chatterjee and A. M. Michalak
Atmos. Chem. Phys., 13, 11643–11660, https://doi.org/10.5194/acp-13-11643-2013, https://doi.org/10.5194/acp-13-11643-2013, 2013
V. Yadav and A. M. Michalak
Geosci. Model Dev., 6, 583–590, https://doi.org/10.5194/gmd-6-583-2013, https://doi.org/10.5194/gmd-6-583-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
The impact of gaseous degradation on the gas–particle partitioning of methylated polycyclic aromatic hydrocarbons
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry–climate model surface ozone fields
A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles
High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills
Summertime tropospheric ozone source apportionment study in the Madrid region (Spain)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
Ether and ester formation from peroxy radical recombination: A qualitative reaction channel analysis
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Tropospheric Ozone Precursors: Global and Regional Distributions, Trends and Variability
Contribution of expanded marine sulfur chemistry to the seasonal variability of dimethyl sulfide oxidation products and size-resolved sulfate aerosol
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
Spatial disparities of ozone pollution in the Sichuan Basin spurred by extreme, hot weather
Global impacts of aviation on air quality evaluated at high resolution
Bias correction of OMI HCHO columns based on FTIR and aircraft measurements and impact on top-down emission estimates
Investigation of the renewed methane growth post-2007 with high-resolution 3-D variational inverse modeling and isotopic constraints
Revisiting day-of-week ozone patterns in an era of evolving US air quality
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
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Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
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Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
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In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
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Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
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This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
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This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
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This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
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Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
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We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
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We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O. T. Pye
EGUsphere, https://doi.org/10.5194/egusphere-2024-1680, https://doi.org/10.5194/egusphere-2024-1680, 2024
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Here, we develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry representation, we then estimate the cancer risk in the contiguous US from exposure to ambient formaldehyde and estimate 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
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The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
EGUsphere, https://doi.org/10.5194/egusphere-2024-1715, https://doi.org/10.5194/egusphere-2024-1715, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation of this parameter for future modifications to models.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
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NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Willem Elias van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
EGUsphere, https://doi.org/10.5194/egusphere-2024-1422, https://doi.org/10.5194/egusphere-2024-1422, 2024
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Methane in the atmosphere contributes to the production of ozone gas, which is an air pollutant as well as a greenhouse gas. In this study, the impact of reducing methane emissions on surface ozone is investigated for the United Nations Economic Commission for Europe (UNECE) region excluding North America and Israel (the "EMEP region"), in particular in terms of its importance in reaching the ozone exposure guideline limits set by the World Health Organization.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
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A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
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A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
Atmos. Chem. Phys., 24, 6095–6103, https://doi.org/10.5194/acp-24-6095-2024, https://doi.org/10.5194/acp-24-6095-2024, 2024
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Gas–particle (G–P) partitioning is an important atmospheric behavior for semi-volatile organic compounds (SVOCs). Diurnal variation in G–P partitioning of methylated polycyclic aromatic hydrocarbons (Me-PAHs) demonstrates the possible influence of gaseous degradation; the enhancement of gaseous degradation (1.10–5.58 times) on G–P partitioning is verified by a steady-state G–P partitioning model. The effect of gaseous degradation on G–P partitioning of (especially light) SVOCs is important.
Christoph Staehle, Harald E. Rieder, Arlene M. Fiore, and Jordan L. Schnell
Atmos. Chem. Phys., 24, 5953–5969, https://doi.org/10.5194/acp-24-5953-2024, https://doi.org/10.5194/acp-24-5953-2024, 2024
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Chemistry–climate models show biases compared to surface ozone observations and thus require bias correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained from more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
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We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
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This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
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In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
EGUsphere, https://doi.org/10.5194/egusphere-2024-886, https://doi.org/10.5194/egusphere-2024-886, 2024
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We incoporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratios predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understading chemical transport models, with implications for better air quality mangement and environmental protection in the region.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
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We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyong Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2024-811, https://doi.org/10.5194/egusphere-2024-811, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show, that SF6 emissions are decreasing in the USA and Europe, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, Europe, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
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The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
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In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Lauri Johannes Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Christian Kurtén
EGUsphere, https://doi.org/10.5194/egusphere-2024-920, https://doi.org/10.5194/egusphere-2024-920, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions, and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we are qualitatively investigating a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discovering which of these reactions are most atmospherically important.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
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Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Yasin Elshorbany, Jerald Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca Buchholz, Benjamin Gaubert, Néstor Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-720, https://doi.org/10.5194/egusphere-2024-720, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the Tropospheric Column of Ozone and its precursors, nitrogen dioxide, formaldehyde, and total column of CO as well as ozonesonde data and model simulations.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Tia Scarpelli, Paul Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
EGUsphere, https://doi.org/10.5194/egusphere-2024-416, https://doi.org/10.5194/egusphere-2024-416, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Nan Wang, Yunsong Du, Dongyang Chen, Haiyan Meng, Xi Chen, Li Zhou, Guangming Shi, Yu Zhan, Miao Feng, Wei Li, Mulan Chen, Zhenliang Li, and Fumo Yang
Atmos. Chem. Phys., 24, 3029–3042, https://doi.org/10.5194/acp-24-3029-2024, https://doi.org/10.5194/acp-24-3029-2024, 2024
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In the scorching August 2022 heatwave, China's Sichuan Basin saw a stark contrast in ozone (O3) levels between Chengdu and Chongqing. The regional disparities were studied considering meteorology, precursors, photochemistry, and transportation. The study highlighted the importance of tailored pollution control measures and underlined the necessity for region-specific strategies to combat O3 pollution on a regional scale.
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.
Jean-François Müller, Trissevgeni Stavrakou, Glenn-Michael Oomen, Beata Opacka, Isabelle De Smedt, Alex Guenther, Corinne Vigouroux, Bavo Langerock, Carlos Augusto Bauer Aquino, Michel Grutter, James Hannigan, Frank Hase, Rigel Kivi, Erik Lutsch, Emmanuel Mahieu, Maria Makarova, Jean-Marc Metzger, Isamu Morino, Isao Murata, Tomoo Nagahama, Justus Notholt, Ivan Ortega, Mathias Palm, Amelie Röhling, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, and Alan Fried
Atmos. Chem. Phys., 24, 2207–2237, https://doi.org/10.5194/acp-24-2207-2024, https://doi.org/10.5194/acp-24-2207-2024, 2024
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Formaldehyde observations from satellites can be used to constrain the emissions of volatile organic compounds, but those observations have biases. Using an atmospheric model, aircraft and ground-based remote sensing data, we quantify these biases, propose a correction to the data, and assess the consequence of this correction for the evaluation of emissions.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, and Philippe Bousquet
Atmos. Chem. Phys., 24, 2129–2167, https://doi.org/10.5194/acp-24-2129-2024, https://doi.org/10.5194/acp-24-2129-2024, 2024
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We investigate the causes of the renewed growth of atmospheric methane (CH4) after 2007 using inverse modeling. We use the additional information provided by observations of CH4 isotopic compositions to better differentiate between the emission categories. Accounting for the large uncertainties in source signatures, our results suggest that the post-2007 increase in atmospheric CH4 was caused by similar increases in emissions from (1) fossil fuels and (2) agriculture and waste.
Heather Simon, Christian Hogrefe, Andrew Whitehill, Kristen M. Foley, Jennifer Liljegren, Norm Possiel, Benjamin Wells, Barron H. Henderson, Lukas C. Valin, Gail Tonnesen, K. Wyat Appel, and Shannon Koplitz
Atmos. Chem. Phys., 24, 1855–1871, https://doi.org/10.5194/acp-24-1855-2024, https://doi.org/10.5194/acp-24-1855-2024, 2024
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We assess observed and modeled ozone weekend–weekday differences in the USA from 2002–2019. A subset of urban areas that were NOx-saturated at the beginning of the period transitioned to NOx-limited conditions. Multiple rural areas of California were NOx-limited for the entire period but become less influenced by local day-of-week emission patterns in more recent years. The model produces more NOx-saturated conditions than the observations but captures trends in weekend–weekday ozone patterns.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
EGUsphere, https://doi.org/10.5194/egusphere-2024-324, https://doi.org/10.5194/egusphere-2024-324, 2024
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We quantified the contributions of land transport, shipping and aviation emissions to tropospheric ozone and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highllight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long life-time.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
EGUsphere, https://doi.org/10.5194/egusphere-2023-2937, https://doi.org/10.5194/egusphere-2023-2937, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to assess ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the behaviour of ozone in the tropics, except in Southeast Asia. Results demonstrate that UKESM1 can be used for health assessments and highlights areas that would benefit from further observations.
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Short summary
We reviewed recent efforts to estimate state- and national-scale carbon dioxide and methane emissions from individual anthropogenic source sectors in the United States. State and federal greenhouse gas regulations almost always target reductions from specific source sectors, and reliable emission estimates are important to support and evaluate these policies. We also describe a number of forward-looking opportunities that would improve sector-specific estimates.
We reviewed recent efforts to estimate state- and national-scale carbon dioxide and methane...
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