Articles | Volume 25, issue 23
https://doi.org/10.5194/acp-25-17553-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-25-17553-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
04 Dec 2025
Research article |
| 04 Dec 2025
| 04 Dec 2025
Evaluation of and updates to the oxidized reactive nitrogen gaseous dry-deposition parameterization from the GEOS-Chem model, including a pathway for ground surface NO2 hydrolysis
Brian L. Boys
CORRESPONDING AUTHOR
Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada
Randall V. Martin
Department of Energy, Environmental, and Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA
Trevor C. VandenBoer
Department of Chemistry, York University, Toronto, ON, Canada
Related authors
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Moxy Shah, Kifle Aregahegn, Danial Nodeh-Farahani, Leigh Crilley, Tasnia Hasan, Yashar Ebrahimi-Iranpour, Fahim Sarker, Nick Nickerson, Chance Creelman, Sarah Ellis, Alexander Moravek, and Trevor VandenBoer
EGUsphere, https://doi.org/10.5194/egusphere-2025-4662, https://doi.org/10.5194/egusphere-2025-4662, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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A commercial dynamic chamber system is modified to measure reactive nitrogen and greenhouse gas fluxes of interest for climate and air quality. The system is optimized for high performance so that fluxes of surface-active gases like ammonia, or reactive gases like nitrogen dioxide, can be made robustly. Lab and field measurements demonstrate consistent fluxes with those from other in-situ agricultural soil reports, as these are expected hot spots of reactive nitrogen gas exchange.
Dandan Zhang, Randall V. Martin, Xuan Liu, Aaron van Donkelaar, Christopher R. Oxford, Yanshun Li, Jun Meng, Danny M. Leung, Jasper F. Kok, Longlei Li, Haihui Zhu, Jay R. Turner, Yu Yan, Michael Brauer, Yinon Rudich, and Eli Windwer
Geosci. Model Dev., 18, 6767–6803, https://doi.org/10.5194/gmd-18-6767-2025, https://doi.org/10.5194/gmd-18-6767-2025, 2025
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This study develops the fine mineral dust simulation in GEOS-Chem by: 1) implementing a new dust emission scheme with further refinements; 2) revisiting the size distribution of emitted dust; 3) explicitly tracking fine dust for emission, transport and deposition in 4 size bins; 4) updating the parametrization for below-cloud scavenging. All revisions significantly reduce the overestimation of surface fine dust from 94 % to 35 % while retaining comparable skill in representing columnar abundance.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, P. Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankararaman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Johann Engelbrecht, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbigniew Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gómez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal L. Weagle, and Xi Zhao
Atmos. Chem. Phys., 25, 4665–4702, https://doi.org/10.5194/acp-25-4665-2025, https://doi.org/10.5194/acp-25-4665-2025, 2025
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Aerosol particles are an important part of the Earth system, but their concentrations are spatially and temporally heterogeneous, as well as being variable in size and composition. Here, we present a new compilation of PM2.5 and PM10 aerosol observations, focusing on the spatial variability across different observational stations, including composition, and demonstrate a method for comparing the data sets to model output.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Haihui Zhu, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Chi Li, Jun Meng, Christopher R. Oxford, Xuan Liu, Yanshun Li, Dandan Zhang, Inderjeet Singh, and Alexei Lyapustin
Atmos. Chem. Phys., 24, 11565–11584, https://doi.org/10.5194/acp-24-11565-2024, https://doi.org/10.5194/acp-24-11565-2024, 2024
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Ambient fine particulate matter (PM2.5) contributes to 4 million deaths globally each year. Satellite remote sensing of aerosol optical depth (AOD), coupled with a simulated PM2.5–AOD relationship (η), can provide global PM2.5 estimations. This study aims to understand the spatial patterns and driving factors of η to guide future measurement and modeling efforts. We quantified η globally and regionally and found that its spatial variation is strongly influenced by aerosol composition.
Fangxuan Ren, Jintai Lin, Chenghao Xu, Jamiu A. Adeniran, Jingxu Wang, Randall V. Martin, Aaron van Donkelaar, Melanie S. Hammer, Larry W. Horowitz, Steven T. Turnock, Naga Oshima, Jie Zhang, Susanne Bauer, Kostas Tsigaridis, Øyvind Seland, Pierre Nabat, David Neubauer, Gary Strand, Twan van Noije, Philippe Le Sager, and Toshihiko Takemura
Geosci. Model Dev., 17, 4821–4836, https://doi.org/10.5194/gmd-17-4821-2024, https://doi.org/10.5194/gmd-17-4821-2024, 2024
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We evaluate the performance of 14 CMIP6 ESMs in simulating total PM2.5 and its 5 components over China during 2000–2014. PM2.5 and its components are underestimated in almost all models, except that black carbon (BC) and sulfate are overestimated in two models, respectively. The underestimation is the largest for organic carbon (OC) and the smallest for BC. Models reproduce the observed spatial pattern for OC, sulfate, nitrate and ammonium well, yet the agreement is poorer for BC.
Alessia A. Colussi, Daniel Persaud, Melodie Lao, Bryan K. Place, Rachel F. Hems, Susan E. Ziegler, Kate A. Edwards, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 17, 3697–3718, https://doi.org/10.5194/amt-17-3697-2024, https://doi.org/10.5194/amt-17-3697-2024, 2024
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A new modular and affordable instrument was developed to automatically collect wet deposition continuously with an off-grid solar top-up power package. Monthly collections were performed across the Newfoundland and Labrador Boreal Ecosystem Latitudinal Transect of experimental forest sites from 2015 to 2016. The proof-of-concept systems were validated with baseline measurements of pH and conductivity and then applied to dissolved organic carbon as an analyte of emerging biogeochemical interest.
Natalie M. Mahowald, Longlei Li, Julius Vira, Marje Prank, Douglas S. Hamilton, Hitoshi Matsui, Ron L. Miller, Louis Lu, Ezgi Akyuz, Daphne Meidan, Peter Hess, Heikki Lihavainen, Christine Wiedinmyer, Jenny Hand, Maria Grazia Alaimo, Célia Alves, Andres Alastuey, Paulo Artaxo, Africa Barreto, Francisco Barraza, Silvia Becagli, Giulia Calzolai, Shankarararman Chellam, Ying Chen, Patrick Chuang, David D. Cohen, Cristina Colombi, Evangelia Diapouli, Gaetano Dongarra, Konstantinos Eleftheriadis, Corinne Galy-Lacaux, Cassandra Gaston, Dario Gomez, Yenny González Ramos, Hannele Hakola, Roy M. Harrison, Chris Heyes, Barak Herut, Philip Hopke, Christoph Hüglin, Maria Kanakidou, Zsofia Kertesz, Zbiginiw Klimont, Katriina Kyllönen, Fabrice Lambert, Xiaohong Liu, Remi Losno, Franco Lucarelli, Willy Maenhaut, Beatrice Marticorena, Randall V. Martin, Nikolaos Mihalopoulos, Yasser Morera-Gomez, Adina Paytan, Joseph Prospero, Sergio Rodríguez, Patricia Smichowski, Daniela Varrica, Brenna Walsh, Crystal Weagle, and Xi Zhao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2024-1, https://doi.org/10.5194/essd-2024-1, 2024
Preprint withdrawn
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Aerosol particles can interact with incoming solar radiation and outgoing long wave radiation, change cloud properties, affect photochemistry, impact surface air quality, and when deposited impact surface albedo of snow and ice, and modulate carbon dioxide uptake by the land and ocean. Here we present a new compilation of aerosol observations including composition, a methodology for comparing the datasets to model output, and show the implications of these results using one model.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
Atmos. Chem. Phys., 23, 12525–12543, https://doi.org/10.5194/acp-23-12525-2023, https://doi.org/10.5194/acp-23-12525-2023, 2023
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We developed and evaluated processes affecting within-day (diel) variability in PM2.5 concentrations in a chemical transport model over the contiguous US. Diel variability in PM2.5 for the contiguous US is driven by early-morning accumulation into a shallow mixed layer, decreases from mid-morning through afternoon with mixed-layer growth, increases from mid-afternoon through evening as the mixed-layer collapses, and decreases overnight as emissions decrease.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Chi Li, Randall V. Martin, Ronald C. Cohen, Liam Bindle, Dandan Zhang, Deepangsu Chatterjee, Hongjian Weng, and Jintai Lin
Atmos. Chem. Phys., 23, 3031–3049, https://doi.org/10.5194/acp-23-3031-2023, https://doi.org/10.5194/acp-23-3031-2023, 2023
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Models are essential to diagnose the significant effects of nitrogen oxides (NOx) on air pollution. We use an air quality model to illustrate the variability of NOx resolution-dependent simulation biases; how these biases depend on specific chemical environments, driving mechanisms, and vertical variabilities; and how these biases affect the interpretation of satellite observations. High-resolution simulations are thus critical to accurately interpret NOx and its relevance to air quality.
Christopher E. Lawrence, Paul Casson, Richard Brandt, James J. Schwab, James E. Dukett, Phil Snyder, Elizabeth Yerger, Daniel Kelting, Trevor C. VandenBoer, and Sara Lance
Atmos. Chem. Phys., 23, 1619–1639, https://doi.org/10.5194/acp-23-1619-2023, https://doi.org/10.5194/acp-23-1619-2023, 2023
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Atmospheric aqueous chemistry can have profound effects on our environment, as illustrated by historical data from Whiteface Mountain (WFM) that were critical for uncovering the process of acid rain. The current study updates the long-term trends in cloud water composition at WFM for the period 1994 to 2021. We highlight the emergence of a new chemical regime at WFM dominated by organics and ammonium, quite different from the highly acidic regime observed in the past but not necessarily
clean.
Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 15, 8731–8748, https://doi.org/10.5194/gmd-15-8731-2022, https://doi.org/10.5194/gmd-15-8731-2022, 2022
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as standalone models. The widely used GEOS-Chem model operates both online and offline, but the classic offline version is not suitable for massively parallel simulations. We describe a new generation of the offline high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores, including on the cloud, with improved access, performance, and accuracy.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Teles C. Furlani, Patrick R. Veres, Kathryn E. R. Dawe, J. Andrew Neuman, Steven S. Brown, Trevor C. VandenBoer, and Cora J. Young
Atmos. Meas. Tech., 14, 5859–5871, https://doi.org/10.5194/amt-14-5859-2021, https://doi.org/10.5194/amt-14-5859-2021, 2021
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This study characterized and validated a commercial spectroscopic instrument for the measurement of hydrogen chloride (HCl) in the atmosphere. Near the Earth’s surface, HCl acts as the dominant reservoir for other chlorine-containing reactive chemicals that play an important role in atmospheric chemistry. The properties of HCl make it challenging to measure. This instrument can overcome many of these challenges, enabling reliable HCl measurements.
Jun Meng, Randall V. Martin, Paul Ginoux, Melanie Hammer, Melissa P. Sulprizio, David A. Ridley, and Aaron van Donkelaar
Geosci. Model Dev., 14, 4249–4260, https://doi.org/10.5194/gmd-14-4249-2021, https://doi.org/10.5194/gmd-14-4249-2021, 2021
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Dust emissions in models, for example, GEOS-Chem, have a strong nonlinear dependence on meteorology, which means dust emission strengths calculated from different resolution meteorological fields are different. Offline high-resolution dust emissions with an optimized global dust strength, presented in this work, can be implemented into GEOS-Chem as offline emission inventory so that it could promote model development by harmonizing dust emissions across simulations of different resolutions.
Erin E. McDuffie, Steven J. Smith, Patrick O'Rourke, Kushal Tibrewal, Chandra Venkataraman, Eloise A. Marais, Bo Zheng, Monica Crippa, Michael Brauer, and Randall V. Martin
Earth Syst. Sci. Data, 12, 3413–3442, https://doi.org/10.5194/essd-12-3413-2020, https://doi.org/10.5194/essd-12-3413-2020, 2020
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Global emission inventories are vital to understanding the impacts of air pollution on the environment, human health, and society. We update the open-source Community Emissions Data System (CEDS) to provide global gridded emissions of seven key air pollutants from 1970–2017 for 11 source sectors and multiple fuel types, including coal, solid biofuel, and liquid oil and natural gas. This dataset includes both monthly global gridded emissions and annual national totals.
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Short summary
A widely used dry-deposition parameterization for NO2 has been updated to include a well-known heterogeneous hydrolysis reaction on deposition surfaces. This update addresses a large low bias of -80 % in simulated NO2 nocturnal deposition velocities evaluated against long-term eddy covariance flux observations over Harvard Forest. We highlight the importance of canopy surface area effects as well as soil NO emissions in formulating and evaluating NO2 dry-deposition parameterizations.
A widely used dry-deposition parameterization for NO2 has been updated to include a well-known...
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