Xuewei Hou,Ryan Hossaini,Oliver Wild,Andrea Mazzeo,Richard J. Pope,Ye Wang,Siyuan Wang,Yuanhong Zhao,James Lee,Bin Zhu,Tianliang Zhao,Alok K. Pandey
{"title":"Tropospheric OH and its trends: new insight into atmospheric processes and implications for methane lifetime","authors":"Xuewei Hou,Ryan Hossaini,Oliver Wild,Andrea Mazzeo,Richard J. Pope,Ye Wang,Siyuan Wang,Yuanhong Zhao,James Lee,Bin Zhu,Tianliang Zhao,Alok K. Pandey","doi":"10.5194/acp-26-13767-2026","DOIUrl":"https://doi.org/10.5194/acp-26-13767-2026","url":null,"abstract":"The hydroxyl radical (OH) is a critical determinant of global oxidative capacity and trace gas lifetimes, but its variation remains poorly constrained. This study investigates the sensitivity of modelled tropospheric OH concentration changes to new understanding of physical and chemical processes using the FRSGC/UCI chemistry transport model. We show that simulated tropospheric O 3 and NO 2 agree well with satellite observations, but that annual variations in CO do not, likely due to uncertainties in biomass burning emissions in the southern hemisphere and overestimated CO trends over Asia. This discrepancy, along with the background increase in CO, may lead to an underestimation of OH increase or overestimation of OH decrease from 2000 to 2017. Changes in tropospheric OH column show substantial spatial heterogeneity, with increases in OH in high-emission regions and decreases in the tropics. Global mean OH trends are dependent on the assumed trend in emissions: with time-varying emissions there is little change in OH, while under annually invariant emissions, OH increases in response to changes in meteorological conditions. Inclusion of water vapor UV absorption, heterogeneous reactions, and updates to the OH+NO 2 reaction rate have a smaller impact, but decrease OH levels by 3.6 %, 5.8 %, and 7.0 %, respectively, increasing CH 4 lifetimes by 4.2 %, 5.2 %, and 8.4 %. Incorporating oceanic CH 3 CHO emissions reduces global mean OH by up to 1.5 %, increasing the CH 4 lifetime by up to 1.6 %. These results provide a quantitative basis for understanding the drivers of tropospheric OH variability and their implications for global methane chemistry.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"36 1","pages":"13767-13793"},"PeriodicalIF":6.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149088325","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chlöe N. Schooling,Liang Feng,Ingrid Super,Paul I. Palmer
{"title":"Inferring European fossil fuel CO\u0000 2\u0000 emissions using TROPOMI NO\u0000 2\u0000 data and sector-based NO\u0000 \u0000 x\u0000 \u0000 : CO\u0000 2\u0000 emission ratios","authors":"Chlöe N. Schooling,Liang Feng,Ingrid Super,Paul I. Palmer","doi":"10.5194/acp-26-13743-2026","DOIUrl":"https://doi.org/10.5194/acp-26-13743-2026","url":null,"abstract":"Accurate monitoring of fossil fuel CO 2 (ffCO 2 ) emissions is essential for tracking climate mitigation, yet natural carbon-cycle fluxes often obscure human-induced signals in atmospheric observations. This study presents a proof-of-concept satellite-driven data assimilation framework that uses nitrogen oxides (NO x = NO + NO 2 ) – short-lived trace gases co-emitted with CO 2 –, to estimate ffCO 2 emissions. We estimate European NO x emissions for 2021 by assimilating TROPOMI NO 2 observations into an Ensemble Kalman Filter (EnKF) framework, optimised within the GEOS-Chem atmospheric transport model. We use a computationally efficient offline treatment of NO x chemistry, enabling large-ensemble inversions while retaining sensitivity to changes in photochemistry. Assimilating these data leads to a systematic reduction in the state vector uncertainty, with the mean uncertainty in total ffCO 2 emissions over Europe decreasing from 5.6 % in the prior to 3.3 % in the posterior. As well as overall improvement in model agreement with observations that corresponds to an annual correlation increase, Δ r =0.12, derived from the correlation of all daily model–observation pairs across all grid cells in the European domain. By leveraging sector-specific NO x : CO 2 emission ratios, we translate our posterior NO x flux estimates into corresponding ffCO 2 estimates that capture enhanced seasonal variability. Our inferred ffCO 2 emissions exhibit elevated values in autumn and winter, spatially concentrated over major source regions and consistent with surface temperature variability. The inferred posterior adjustments include substantial increases in national emissions in several regions (20 %–91 % in national annual combustion CO 2 ), highlighting both the sensitivity of the method and the need for further validation and multi-species observational constraints. Independent evaluation against in situ measurements confirms significant improvements in mean error statistics in some regions. And updated national posterior ffCO 2 emissions show improved agreement with EDGAR across five high emitting European countries. This study demonstrates the potential of ensemble data assimilation and reduced-complexity chemistry to provide a first-order constraint on European ffCO 2 estimates, establishing a vital foundation for future joint NO 2 –CO 2 inversion systems.","PeriodicalId":8611,"journal":{"name":"Atmospheric Chemistry and Physics","volume":"31 1","pages":"13743-13766"},"PeriodicalIF":6.3,"publicationDate":"2026-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149088083","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"地球科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}