the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Enhancing Long-Term Trend Simulation of Global Tropospheric OH and Its Drivers from 2005–2019: A Synergistic Integration of Model Simulations and Satellite Observations
Abstract. The tropospheric hydroxyl radical (TOH) is a key player in regulating oxidation of various compounds in Earth’s atmosphere. Despite its pivotal role, the spatiotemporal distributions of OH are poorly constrained. Past modeling studies suggest that the main drivers of OH, including NO2, tropospheric ozone (TO3), and H2O(v), have increased TOH globally. However, these findings often offer a global average and may not include more recent changes in diverse compounds emitted on various spatiotemporal scales. Here, we aim to deepen our understanding of global TOH trends for more recent years (2005–2019) at 1×1 degrees. To achieve this, we use satellite observations of HCHO and NO2 to constrain simulated TOH using a technique based on a Bayesian data fusion method, alongside an interpretable machine learning module named ECCOH, which is integrated into NASA’s GEOS global model. This innovative module helps efficiently predict the convoluted response of TOH to its drivers/proxies. Aura Ozone Monitoring Instrument (OMI) NO2 observations suggest that the simulation has high biases over biomass burning activities in Africa and Eastern Europe, resulting in overestimation of up to 20 % in TOH, regionally. OMI HCHO primarily impacts oceans where TOH linearly correlates with this proxy. Five key parameters including TO3, H2O(v), NO2, HCHO, and stratospheric ozone can collectively explain 65 % of variance in TOH trends. The overall trend of TOH influenced by NO2 remains positive, but it varies greatly because of the differences in the signs of anthropogenic emissions. Over oceans, TOH trends are primarily positive in the northern hemisphere, resulting from the upward trends in HCHO, TO3, and H2O(v). Using the present framework, we can tap the power of satellites to quickly gain a deeper understanding of simulated TOH trends and biases.
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Notice on discussion status
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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Preprint
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Supplement
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(9254 KB) - Metadata XML
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Supplement
(5163 KB) - BibTeX
- EndNote
- Final revised paper
Journal article(s) based on this preprint
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2024-410', Anonymous Referee #1, 08 Apr 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-410/egusphere-2024-410-RC1-supplement.pdf
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AC1: 'Reply on RC1', Amir Souri, 13 May 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-410/egusphere-2024-410-AC1-supplement.pdf
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AC1: 'Reply on RC1', Amir Souri, 13 May 2024
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RC2: 'Comment on egusphere-2024-410', Anonymous Referee #2, 27 May 2024
Hydroxyl radical (OH) is the most important oxidant in the troposphere that governs the oxidation power, while its spatial-temporal patterns are yet to be clear at present. The authors of this study developed an integrated data- and model-driven approach to predict the convoluted response of TOH to its five proxies, which include NO2, HCHO, H2O, Trop O3, and Strat O3. They investigated the trends and drivers of global, hemispheric, and regional OH from 2005 to 2019. Overall, this study has provided interesting results, which will help deepen our understanding of the changes in global tropospheric OH over the past decades. I have several concerns about the method that could impact the robustness of the results.
1) Is there any method to evaluate the response of OH to different input parametrizations that were calculated by Eq. (5)? These semi-normalized sensitivities laid the foundation for understanding the impacts from different proxies/drivers on tropospheric OH. I would like to see some aspects of “evaluation” or at least a comparison with previous other studies.
2) The input parameters were perturbed by the scaling factors of 1.1 and 0.9 in the ECCOH offline framework. What about the impacts of these assumed scaling factors? NOx and VOCs emissions might change by over 10% between 2005 and 2019, in both developed countries with advanced air pollution control and developing countries with rapid economic growth.
3) I feel that the trends in OH present in this study are substantially impacted by the trends of NO2 and HCHO, which were constrained by OMI. What about the impacts of uncertainties in the trends of OMI observations on the OH estimates? Especially for HCHO, I have seen some papers showing that there were systematic errors in the global and latitudinal trends.
4) Lines 498-500, the authors said “The correction factors, however, worsen the trends over the southeast US and Canada. This is essentially due to the use of the fractional errors in the a priori making the OMI corrections more impactful (i.e., higher Kalman gain) in summertime than in wintertime.” I did not understand what these sentences meant. Why did more impactful OMI corrections worsen the trends over the southeast US and Canada?
Citation: https://doi.org/10.5194/egusphere-2024-410-RC2 -
AC2: 'Reply on RC2', Amir Souri, 31 May 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-410/egusphere-2024-410-AC2-supplement.pdf
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AC2: 'Reply on RC2', Amir Souri, 31 May 2024
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2024-410', Anonymous Referee #1, 08 Apr 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-410/egusphere-2024-410-RC1-supplement.pdf
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AC1: 'Reply on RC1', Amir Souri, 13 May 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-410/egusphere-2024-410-AC1-supplement.pdf
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AC1: 'Reply on RC1', Amir Souri, 13 May 2024
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RC2: 'Comment on egusphere-2024-410', Anonymous Referee #2, 27 May 2024
Hydroxyl radical (OH) is the most important oxidant in the troposphere that governs the oxidation power, while its spatial-temporal patterns are yet to be clear at present. The authors of this study developed an integrated data- and model-driven approach to predict the convoluted response of TOH to its five proxies, which include NO2, HCHO, H2O, Trop O3, and Strat O3. They investigated the trends and drivers of global, hemispheric, and regional OH from 2005 to 2019. Overall, this study has provided interesting results, which will help deepen our understanding of the changes in global tropospheric OH over the past decades. I have several concerns about the method that could impact the robustness of the results.
1) Is there any method to evaluate the response of OH to different input parametrizations that were calculated by Eq. (5)? These semi-normalized sensitivities laid the foundation for understanding the impacts from different proxies/drivers on tropospheric OH. I would like to see some aspects of “evaluation” or at least a comparison with previous other studies.
2) The input parameters were perturbed by the scaling factors of 1.1 and 0.9 in the ECCOH offline framework. What about the impacts of these assumed scaling factors? NOx and VOCs emissions might change by over 10% between 2005 and 2019, in both developed countries with advanced air pollution control and developing countries with rapid economic growth.
3) I feel that the trends in OH present in this study are substantially impacted by the trends of NO2 and HCHO, which were constrained by OMI. What about the impacts of uncertainties in the trends of OMI observations on the OH estimates? Especially for HCHO, I have seen some papers showing that there were systematic errors in the global and latitudinal trends.
4) Lines 498-500, the authors said “The correction factors, however, worsen the trends over the southeast US and Canada. This is essentially due to the use of the fractional errors in the a priori making the OMI corrections more impactful (i.e., higher Kalman gain) in summertime than in wintertime.” I did not understand what these sentences meant. Why did more impactful OMI corrections worsen the trends over the southeast US and Canada?
Citation: https://doi.org/10.5194/egusphere-2024-410-RC2 -
AC2: 'Reply on RC2', Amir Souri, 31 May 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-410/egusphere-2024-410-AC2-supplement.pdf
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AC2: 'Reply on RC2', Amir Souri, 31 May 2024
Peer review completion
Journal article(s) based on this preprint
Model code and software
OI-SAT-GMI Amir H. Souri https://doi.org/10.5281/zenodo.10520136
Offline ECCOH Amir H. Souri https://doi.org/10.5281/zenodo.10685100
GEOS model NASA GSFC https://github.com/GEOS-ESM/GEOSgcm.git
GEOS-Quickchem Michael Manyin https://github.com/GEOS-ESM/QuickChem.git
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Amir H. Souri
Bryan N. Duncan
Sarah A. Strode
Daniel C. Anderson
Michael E. Manyin
Junhua Liu
Luke D. Oman
Zhen Zhang
Brad Weir
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(9254 KB) - Metadata XML
-
Supplement
(5163 KB) - BibTeX
- EndNote
- Final revised paper