Springtime transitions of NO2, CO, and O3 over North America: Model evaluation and analysis

• Published in: Journal of Geophysical Research
• Main Authors: Choi, Yunsoo, Wang, Yuhang, Zeng, Tao, Cunnold, Derek, Yang, Eun-Su, Martin, Randall, Chance, Kelly, Thouret, Valérie, Edgerton, Eric
• Other Authors: Chemistry Department, Shaanxi Key Laboratory of Physico-Inorganic Chemistry, Northwest University (Xi'an), Laboratoire d’Électrotechnique et d’Électronique de Puissance - ULR 2697 (L2EP), Centrale Lille-Université de Lille-Arts et Métiers Sciences et Technologies, HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-HESAM Université - Communauté d'universités et d'établissements Hautes écoles Sorbonne Arts et métiers université (HESAM)-JUNIA (JUNIA), Université catholique de Lille (UCL)-Université catholique de Lille (UCL), Methods and tools for gestural interactions (MINT), Laboratoire d'Informatique Fondamentale de Lille (LIFL), Université de Lille, Sciences et Technologies-Institut National de Recherche en Informatique et en Automatique (Inria)-Université de Lille, Sciences Humaines et Sociales-Centre National de la Recherche Scientifique (CNRS)-Université de Lille, Sciences et Technologies-Institut National de Recherche en Informatique et en Automatique (Inria)-Université de Lille, Sciences Humaines et Sociales-Centre National de la Recherche Scientifique (CNRS)-Inria Lille - Nord Europe, Institut National de Recherche en Informatique et en Automatique (Inria), School of Earth and Atmospheric Sciences Atlanta, Georgia Institute of Technology Atlanta, Department of Atmospheric Science Huntsville, University of Alabama in Huntsville (UAH), Department of Physics and Atmospheric Science Halifax, Dalhousie University Halifax, Harvard-Smithsonian Center for Astrophysics (CfA), Harvard University-Smithsonian Institution, Laboratoire d'aérologie (LAERO), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales Toulouse (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France-Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales Toulouse (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France-Centre National de la Recherche Scientifique (CNRS)
• Format: Article in Journal/Newspaper
• Language: English
• Published: HAL CCSD 2008
• Subjects: tropospheric ozone; spring transition; lightning; [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph]; North Atlantic
• Online Access: https://hal.science/hal-00622941; https://hal.science/hal-00622941/document; https://hal.science/hal-00622941/file/Journal%20of%20Geophysical%20Research%20Atmospheres%20-%202008%20-%20Choi%20-%20Springtime%20transitions%20of%20NO2%20CO%20and%20O3%20over%20North%20America%20.pdf; https://doi.org/10.1029/2007JD009632

International audience Surface observations from AIRNow and Southeastern Aerosol Research and Characterization Study networks, aircraft observations from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft program, ozonesondes, and remote sensing measurements from Global Ozone Mapping Experiment, Total Ozone Mapping Spectrometer (TOMS), and Stratospheric Aerosol and Gas Experiment (SAGE) II for February-May 2000 over North America are used to characterize the springtime transitions of O3 and its precursors. These measurements provide a comprehensive data set to evaluate the performance of the 3-D Regional Chemical Transport Model (REAM). The model is then applied to analyze the key factors affecting the springtime transitions of trace gas concentrations and export. The global GEOS-CHEM model is used to provide chemical initial and boundary conditions. Generally, the model results are in good agreement with the observations in the troposphere except for a low bias of upper tropospheric O3; the bias decreases toward the summer and lower latitudes. The rate of observed surface O3 increase in spring is simulated well by REAM. It is overestimated by GEOS-CHEM over the eastern United States. A key factor driving the model difference is daytime mixing depth. A shallow boundary layer in REAM leads to more efficient removal of radicals and hence slower activation of photochemistry in spring, when the primary radical source is relatively small. Comparison of top-down estimates of fossil fuel NOx emissions between REAM and GEOS-CHEM shows model dependence. The associated uncertainty is up to 20% on a monthly basis. Averaging over a season reduces this uncertainty. While tropospheric column NO2 decreases over the continent, it increases over the western North Atlantic due to lightning NOx production. Consequently, the REAM model simulates significant increases of tropospheric O3 over the region as indicated by column data derived from TOMS-SAGE II. Lightning impact is also evident in model-simulated NOx ...