Articles | Volume 18, issue 3
https://doi.org/10.5194/acp-18-1507-2018
© Author(s) 2018. 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-18-1507-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Modelling the physical multiphase interactions of HNO3 between snow and air on the Antarctic Plateau (Dome C) and coast (Halley)
Hoi Ga Chan
British Antarctic Survey, Natural Environment Research Council, Cambridge, CB3 0ET, UK
Department of Earth Sciences, Royal Holloway University of London, Egham, Surrey, TW20 0EX, UK
British Antarctic Survey, Natural Environment Research Council, Cambridge, CB3 0ET, UK
Martin D. King
Department of Earth Sciences, Royal Holloway University of London, Egham, Surrey, TW20 0EX, UK
Related authors
H. G. Chan, M. D. King, and M. M. Frey
Atmos. Chem. Phys., 15, 7913–7927, https://doi.org/10.5194/acp-15-7913-2015, https://doi.org/10.5194/acp-15-7913-2015, 2015
Rosalie Shepherd, Martin King, Andrew Ward, Edward Stuckey, Rebecca Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
EGUsphere, https://doi.org/10.5194/egusphere-2024-2367, https://doi.org/10.5194/egusphere-2024-2367, 2024
Short summary
Short summary
Thin film formation at the air-water interface from material extracted from atmospheric aerosol was demonstrated, supporting core-shell morphology. The film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 hour. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top of the atmosphere albedo for urban films.
Benjamin Heutte, Nora Bergner, Hélène Angot, Jakob B. Pernov, Lubna Dada, Jessica A. Mirrielees, Ivo Beck, Andrea Baccarini, Matthew Boyer, Jessie M. Creamean, Kaspar R. Daellenbach, Imad El Haddad, Markus M. Frey, Silvia Henning, Tiaa Laurila, Vaios Moschos, Tuukka Petäjä, Kerri A. Pratt, Lauriane L. J. Quéléver, Matthew D. Shupe, Paul Zieger, Tuija Jokinen, and Julia Schmale
EGUsphere, https://doi.org/10.5194/egusphere-2024-1912, https://doi.org/10.5194/egusphere-2024-1912, 2024
Short summary
Short summary
Limited aerosol measurements in the central Arctic hinder our understanding of aerosol-climate interactions in the region. Our year-long observations of aerosol physicochemical properties during the MOSAiC expedition reveal strong seasonal variations in aerosol chemical composition, where the short-term variability is heavily affected by storms in the Arctic. Locally wind-generated particles are shown to be an important source of cloud seeds, especially in autumn.
V. Holly L. Winton, Robert Mulvaney, Joel Savarino, Kyle R. Clem, and Markus M. Frey
Clim. Past, 20, 1213–1232, https://doi.org/10.5194/cp-20-1213-2024, https://doi.org/10.5194/cp-20-1213-2024, 2024
Short summary
Short summary
In 2018, a new 120 m ice core was drilled in a region located under the Antarctic ozone hole. We present the first results including a 1300-year record of snow accumulation and aerosol chemistry. We investigate the aerosol and moisture source regions and atmospheric processes related to the ice core record and discuss what this means for developing a record of past ultraviolet radiation and ozone depletion using the stable isotopic composition of nitrate measured in the same ice core.
James Brean, David C. S. Beddows, Eija Asmi, Ari Virkkula, Lauriane L. J. Quéléver, Mikko Sipilä, Floortje Van Den Heuvel, Thomas Lachlan-Cope, Anna Jones, Markus Frey, Angelo Lupi, Jiyeon Park, Young Jun Yoon, Ralf Weller, Giselle L. Marincovich, Gabriela C. Mulena, Roy M. Harrison, and Manuel Dall´Osto
EGUsphere, https://doi.org/10.5194/egusphere-2024-987, https://doi.org/10.5194/egusphere-2024-987, 2024
Short summary
Short summary
Our results emphasize how understanding the geographical variation in surface types across the Antarctic is key to understanding secondary aerosol sources.
Amelia M. H. Bond, Markus M. Frey, Jan Kaiser, Jörg Kleffmann, Anna E. Jones, and Freya A. Squires
Atmos. Chem. Phys., 23, 5533–5550, https://doi.org/10.5194/acp-23-5533-2023, https://doi.org/10.5194/acp-23-5533-2023, 2023
Short summary
Short summary
Atmospheric nitrous acid (HONO) amount fractions measured at Halley Research Station, Antarctica, were found to be low. Vertical fluxes of HONO from the snow were also measured and agree with the estimated HONO production rate from photolysis of snow nitrate. In a simple box model of HONO sources and sinks, there was good agreement between the measured flux and amount fraction. HONO was found to be an important OH radical source at Halley.
Maxim L. Lamare, John D. Hedley, and Martin D. King
The Cryosphere, 17, 737–751, https://doi.org/10.5194/tc-17-737-2023, https://doi.org/10.5194/tc-17-737-2023, 2023
Short summary
Short summary
The reflectivity of sea ice is crucial for modern climate change and for monitoring sea ice from satellites. The reflectivity depends on the angle at which the ice is viewed and the angle illuminated. The directional reflectivity is calculated as a function of viewing angle, illuminating angle, thickness, wavelength and surface roughness. Roughness cannot be considered independent of thickness, illumination angle and the wavelength. Remote sensors will use the data to image sea ice from space.
Benjamin Heikki Redmond Roche and Martin D. King
The Cryosphere, 16, 3949–3970, https://doi.org/10.5194/tc-16-3949-2022, https://doi.org/10.5194/tc-16-3949-2022, 2022
Short summary
Short summary
Sea ice is bright, playing an important role in reflecting incoming solar radiation. The reflectivity of sea ice is affected by the presence of pollutants, such as crude oil, even at low concentrations. Modelling how the brightness of three types of sea ice is affected by increasing concentrations of crude oils shows that the type of oil, the type of ice, the thickness of the ice, and the size of the oil droplets are important factors. This shows that sea ice is vulnerable to oil pollution.
Albane Barbero, Roberto Grilli, Markus M. Frey, Camille Blouzon, Detlev Helmig, Nicolas Caillon, and Joël Savarino
Atmos. Chem. Phys., 22, 12025–12054, https://doi.org/10.5194/acp-22-12025-2022, https://doi.org/10.5194/acp-22-12025-2022, 2022
Short summary
Short summary
The high reactivity of the summer Antarctic boundary layer results in part from the emissions of nitrogen oxides produced during photo-denitrification of the snowpack, but its underlying mechanisms are not yet fully understood. The results of this study suggest that more NO2 is produced from the snowpack early in the photolytic season, possibly due to stronger UV irradiance caused by a smaller solar zenith angle near the solstice.
David N. Wagner, Matthew D. Shupe, Christopher Cox, Ola G. Persson, Taneil Uttal, Markus M. Frey, Amélie Kirchgaessner, Martin Schneebeli, Matthias Jaggi, Amy R. Macfarlane, Polona Itkin, Stefanie Arndt, Stefan Hendricks, Daniela Krampe, Marcel Nicolaus, Robert Ricker, Julia Regnery, Nikolai Kolabutin, Egor Shimanshuck, Marc Oggier, Ian Raphael, Julienne Stroeve, and Michael Lehning
The Cryosphere, 16, 2373–2402, https://doi.org/10.5194/tc-16-2373-2022, https://doi.org/10.5194/tc-16-2373-2022, 2022
Short summary
Short summary
Based on measurements of the snow cover over sea ice and atmospheric measurements, we estimate snowfall and snow accumulation for the MOSAiC ice floe, between November 2019 and May 2020. For this period, we estimate 98–114 mm of precipitation. We suggest that about 34 mm of snow water equivalent accumulated until the end of April 2020 and that at least about 50 % of the precipitated snow was eroded or sublimated. Further, we suggest explanations for potential snowfall overestimation.
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885, https://doi.org/10.5194/acp-20-5861-2020, https://doi.org/10.5194/acp-20-5861-2020, 2020
Short summary
Short summary
The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Markus M. Frey, Sarah J. Norris, Ian M. Brooks, Philip S. Anderson, Kouichi Nishimura, Xin Yang, Anna E. Jones, Michelle G. Nerentorp Mastromonaco, David H. Jones, and Eric W. Wolff
Atmos. Chem. Phys., 20, 2549–2578, https://doi.org/10.5194/acp-20-2549-2020, https://doi.org/10.5194/acp-20-2549-2020, 2020
Short summary
Short summary
A winter sea ice expedition to Antarctica provided the first direct observations of sea salt aerosol (SSA) production during snow storms above sea ice, thereby validating a model hypothesis to account for winter time SSA maxima in Antarctica not explained otherwise. Defining SSA sources is important given the critical roles that aerosol plays for climate, for air quality and as a potential ice core proxy for sea ice conditions in the past.
Xin Yang, Markus M. Frey, Rachael H. Rhodes, Sarah J. Norris, Ian M. Brooks, Philip S. Anderson, Kouichi Nishimura, Anna E. Jones, and Eric W. Wolff
Atmos. Chem. Phys., 19, 8407–8424, https://doi.org/10.5194/acp-19-8407-2019, https://doi.org/10.5194/acp-19-8407-2019, 2019
Short summary
Short summary
This is a comprehensive model–data comparison aiming to evaluate the proposed mechanism of sea salt aerosol (SSA) production from blowing snow on sea ice. Some key parameters such as snow salinity and blowing-snow size distribution were constrained by data collected in the Weddell Sea. The good agreement between modelled SSA and the cruise data strongly indicates that sea ice surface is a large SSA source in polar regions, a process which has not been considered in current climate models.
Rosalie H. Shepherd, Martin D. King, Amelia A. Marks, Neil Brough, and Andrew D. Ward
Atmos. Chem. Phys., 18, 5235–5252, https://doi.org/10.5194/acp-18-5235-2018, https://doi.org/10.5194/acp-18-5235-2018, 2018
Short summary
Short summary
The refractive index of atmospheric extracts sourced from urban (London), remote (Antarctica), and woodsmoke aerosol was determined by applying optical trapping simultaneously with Mie spectroscopy. In addition, owing to the absorbing nature of woodsmoke and an aqueous humic acid aerosol extract, the absorption Ångström exponent could be determined.The refractive index and absorption Ångström exponent were then applied in a top-of-the-atmosphere albedo radiation transfer model.
Amelia A. Marks, Maxim L. Lamare, and Martin D. King
The Cryosphere, 11, 2867–2881, https://doi.org/10.5194/tc-11-2867-2017, https://doi.org/10.5194/tc-11-2867-2017, 2017
Short summary
Short summary
Arctic sea ice extent is declining rapidly. Prediction of sea ice trends relies on sea ice models that need to be evaluated with real data. A realistic sea ice environment is created in a laboratory by the Royal Holloway sea ice simulator and is used to show a sea ice model can replicate measured properties of sea ice, e.g. reflectance. Black carbon, a component of soot found in atmospheric pollution, is also experimentally shown to reduce the sea ice reflectance, which could exacerbate melting.
Rachael H. Rhodes, Xin Yang, Eric W. Wolff, Joseph R. McConnell, and Markus M. Frey
Atmos. Chem. Phys., 17, 9417–9433, https://doi.org/10.5194/acp-17-9417-2017, https://doi.org/10.5194/acp-17-9417-2017, 2017
Short summary
Short summary
Sea salt aerosol comes from the open ocean or the sea ice surface. In the polar regions, this opens up the possibility of reconstructing sea ice history using sea salt recorded in ice cores. We use a chemical transport model to demonstrate that the sea ice source of aerosol is important in the Arctic. For the first time, we simulate realistic Greenland ice core sea salt in a process-based model. The importance of the sea ice source increases from south to north across the Greenland ice sheet.
Michel Legrand, Susanne Preunkert, Joël Savarino, Markus M. Frey, Alexandre Kukui, Detlev Helmig, Bruno Jourdain, Anna E. Jones, Rolf Weller, Neil Brough, and Hubert Gallée
Atmos. Chem. Phys., 16, 8053–8069, https://doi.org/10.5194/acp-16-8053-2016, https://doi.org/10.5194/acp-16-8053-2016, 2016
Short summary
Short summary
Surface ozone, the most abundant atmospheric oxidant, has been measured since 2004 at the coastal East Antarctic site of Dumont d’Urville, and since 2007 at the Concordia station located on the high East Antarctic plateau. Long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites are discussed. Influences like sea ice extent and outflow from inland Antarctica are discussed.
Joël Savarino, William C. Vicars, Michel Legrand, Suzanne Preunkert, Bruno Jourdain, Markus M. Frey, Alexandre Kukui, Nicolas Caillon, and Jaime Gil Roca
Atmos. Chem. Phys., 16, 2659–2673, https://doi.org/10.5194/acp-16-2659-2016, https://doi.org/10.5194/acp-16-2659-2016, 2016
Short summary
Short summary
Atmospheric nitrate is collected on the East Antarctic ice sheet. Nitrogen and oxygen stable isotopes and concentrations of nitrate are measured. Using a box model, we show that there is s systematic discrepancy between observations and model results. We suggest that this discrepancy probably results from unknown NOx chemistry above the Antarctic ice sheet. However, possible misconception in the stable isotope mass balance is not completely excluded.
M. L. Lamare, J. Lee-Taylor, and M. D. King
Atmos. Chem. Phys., 16, 843–860, https://doi.org/10.5194/acp-16-843-2016, https://doi.org/10.5194/acp-16-843-2016, 2016
Short summary
Short summary
The decrease in reflectivity (albedo) of sea ice and snow containing mineral dusts and volcanic ashes is calculated. The type of snow and sea ice, the thickness and the layering of mineral aerosol deposits are varied. The results show that the response of the albedo of snow and sea ice to mineral aerosol deposits is more sensitive to the type of snow or sea ice than to the properties of the mineral aerosol deposits themselves.
J. Erbland, J. Savarino, S. Morin, J. L. France, M. M. Frey, and M. D. King
Atmos. Chem. Phys., 15, 12079–12113, https://doi.org/10.5194/acp-15-12079-2015, https://doi.org/10.5194/acp-15-12079-2015, 2015
Short summary
Short summary
In this paper, we describe the development of a numerical model which aims at representing nitrate recycling at the air-snow interface on the East Antarctic Plateau. Stable isotopes are used as diagnostic and evaluation tools by comparing the model's results to recent field measurements of nitrate and key atmospheric species at Dome C, Antarctica. From sensitivity tests conducted with the model, we propose a framework for the interpretation of the nitrate isotope record in deep ice cores.
M. M. Frey, H. K. Roscoe, A. Kukui, J. Savarino, J. L. France, M. D. King, M. Legrand, and S. Preunkert
Atmos. Chem. Phys., 15, 7859–7875, https://doi.org/10.5194/acp-15-7859-2015, https://doi.org/10.5194/acp-15-7859-2015, 2015
Short summary
Short summary
Surprisingly large concentrations and flux of atmospheric nitrogen oxides were measured at Dome C, East Antarctica. It was found that the surface snow holds a significant reservoir of photochemically produced NOx and is a sink of gas-phase ozone. Main drivers of NOx snow emissions were large snow nitrate concentrations, with contributions of increased UV from decreases in stratospheric ozone. Observed halogen and hydroxyl radical concentrations were too low to explain large NO2:NO ratios.
H. G. Chan, M. D. King, and M. M. Frey
Atmos. Chem. Phys., 15, 7913–7927, https://doi.org/10.5194/acp-15-7913-2015, https://doi.org/10.5194/acp-15-7913-2015, 2015
S. Preunkert, M. Legrand, M. M. Frey, A. Kukui, J. Savarino, H. Gallée, M. King, B. Jourdain, W. Vicars, and D. Helmig
Atmos. Chem. Phys., 15, 6689–6705, https://doi.org/10.5194/acp-15-6689-2015, https://doi.org/10.5194/acp-15-6689-2015, 2015
Short summary
Short summary
During two austral summers HCHO was investigated in air, snow, and interstitial air at the Concordia site located on the East Antarctic Plateau. Snow emission fluxes were estimated to be around 1 to 2 and 3 to 5 x 10^12 molecules m-2 s-1 at night and at noon, respectively. Shading experiments suggest that the photochemical HCHO production in the snowpack at Concordia remains negligible. The mean HCHO level of 130pptv observed at 1m above the surface is quite well reproduced by 1-D simulations.
H. Gallée, S. Preunkert, S. Argentini, M. M. Frey, C. Genthon, B. Jourdain, I. Pietroni, G. Casasanta, H. Barral, E. Vignon, C. Amory, and M. Legrand
Atmos. Chem. Phys., 15, 6225–6236, https://doi.org/10.5194/acp-15-6225-2015, https://doi.org/10.5194/acp-15-6225-2015, 2015
Short summary
Short summary
Regional climate model MAR was run for the region of Dome C located on the East Antarctic plateau, during summer 2011–2012, with a high vertical resolution in the lower troposphere. MAR is generally in very good agreement with the observations and provides sufficiently reliable information about surface turbulent fluxes and vertical profiles of vertical diffusion coefficients when discussing the representativeness of chemical measurements made nearby the ground surface at Dome C.
A. Kukui, M. Legrand, S. Preunkert, M. M. Frey, R. Loisil, J. Gil Roca, B. Jourdain, M. D. King, J. L. France, and G. Ancellet
Atmos. Chem. Phys., 14, 12373–12392, https://doi.org/10.5194/acp-14-12373-2014, https://doi.org/10.5194/acp-14-12373-2014, 2014
Short summary
Short summary
Concentrations of OH radicals and the sum of peroxy radicals, RO2, were measured in the boundary layer for the first time on the East Antarctic Plateau at the Concordia Station during the austral summer 2011/2012. The concentrations of radicals were comparable to those observed at the South Pole, confirming that the elevated oxidative capacity of the Antarctic atmospheric boundary layer found at the South Pole is not restricted to the South Pole but common over the high Antarctic plateau.
M. Legrand, S. Preunkert, M. Frey, Th. Bartels-Rausch, A. Kukui, M. D. King, J. Savarino, M. Kerbrat, and B. Jourdain
Atmos. Chem. Phys., 14, 9963–9976, https://doi.org/10.5194/acp-14-9963-2014, https://doi.org/10.5194/acp-14-9963-2014, 2014
A. A. Marks and M. D. King
The Cryosphere, 8, 1625–1638, https://doi.org/10.5194/tc-8-1625-2014, https://doi.org/10.5194/tc-8-1625-2014, 2014
Q. Libois, G. Picard, J. L. France, L. Arnaud, M. Dumont, C. M. Carmagnola, and M. D. King
The Cryosphere, 7, 1803–1818, https://doi.org/10.5194/tc-7-1803-2013, https://doi.org/10.5194/tc-7-1803-2013, 2013
S. Masclin, M. M. Frey, W. F. Rogge, and R. C. Bales
Atmos. Chem. Phys., 13, 8857–8877, https://doi.org/10.5194/acp-13-8857-2013, https://doi.org/10.5194/acp-13-8857-2013, 2013
A. A. Marks and M. D. King
The Cryosphere, 7, 1193–1204, https://doi.org/10.5194/tc-7-1193-2013, https://doi.org/10.5194/tc-7-1193-2013, 2013
J. Erbland, W. C. Vicars, J. Savarino, S. Morin, M. M. Frey, D. Frosini, E. Vince, and J. M. F. Martins
Atmos. Chem. Phys., 13, 6403–6419, https://doi.org/10.5194/acp-13-6403-2013, https://doi.org/10.5194/acp-13-6403-2013, 2013
M. M. Frey, N. Brough, J. L. France, P. S. Anderson, O. Traulle, M. D. King, A. E. Jones, E. W. Wolff, and J. Savarino
Atmos. Chem. Phys., 13, 3045–3062, https://doi.org/10.5194/acp-13-3045-2013, https://doi.org/10.5194/acp-13-3045-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
The improved Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST): update, validation and applications
Tracing the origins of stratospheric ozone intrusions: direct vs. indirect pathways and their impacts on Central and Eastern China in spring–summer 2019
Flow-dependent observation errors for greenhouse gas inversions in an ensemble Kalman smoother
Observational and model evidence for a prominent stratospheric influence on variability in tropospheric nitrous oxide
Estimation of Canada's methane emissions: inverse modelling analysis using the Environment and Climate Change Canada (ECCC) measurement network
Spatiotemporal source apportionment of ozone pollution over the Greater Bay Area
The importance of moist thermodynamics on neutral buoyancy height for plumes from anthropogenic sources
Partitioning anthropogenic and natural methane emissions in Finland during 2000–2021 by combining bottom-up and top-down estimates
Potential of 14C-based vs. ΔCO-based ΔffCO2 observations to estimate urban fossil fuel CO2 (ffCO2) emissions
On the uncertainty of anthropogenic aromatic volatile organic compound emissions: model evaluation and sensitivity analysis
A mechanism of stratospheric O3 intrusion into the atmospheric environment: a case study of the North China Plain
Influence of atmospheric circulation on the interannual variability of transport from global and regional emissions into the Arctic
The role of OCO-3 XCO2 retrievals in estimating global terrestrial net ecosystem exchanges
Surface networks in the Arctic may miss a future methane bomb
Potential of using CO2 observations over India in a regional carbon budget estimation by improving the modelling system
A bottom-up emission estimate for the 2022 Nord Stream gas leak: derivation, simulations, and evaluation
European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell
Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes
Multidecadal ozone trends in China and implications for human health and crop yields: a hybrid approach combining a chemical transport model and machine learning
On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations
Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling
The sensitivity of Southern Ocean atmospheric dimethyl sulfide (DMS) to modeled oceanic DMS concentrations and emissions
Impacts of maritime shipping on air pollution along the US East Coast
Understanding greenhouse gas (GHG) column concentrations in Munich using the Weather Research and Forecasting (WRF) model
Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions
Estimation of power plant SO2 emissions using the HYSPLIT dispersion model and airborne observations with plume rise ensemble runs
Can we use atmospheric CO2 measurements to verify emission trends reported by cities? Lessons from a 6-year atmospheric inversion over Paris
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons: implication for the influence of the particulate proportion in emissions
An analysis of CMAQ gas-phase dry deposition over North America through grid-scale and land-use-specific diagnostics in the context of AQMEII4
Rethinking the role of transport and photochemistry in regional ozone pollution: insights from ozone concentration and mass budgets
Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport
The effect of anthropogenic emission, meteorological factors, and carbon dioxide on the surface ozone increase in China from 2008 to 2018 during the East Asia summer monsoon season
Development of a CMAQ–PMF-based composite index for prescribing an effective ozone abatement strategy: a case study of sensitivity of surface ozone to precursor volatile organic compound species in southern Taiwan
Comment on “Climate consequences of hydrogen emissions” by Ocko and Hamburg (2022)
Constraining emissions of volatile organic compounds from western US wildfires with WE-CAN and FIREX-AQ airborne observations
Satellite quantification of methane emissions and oil–gas methane intensities from individual countries in the Middle East and North Africa: implications for climate action
Coupled mesoscale–microscale modeling of air quality in a polluted city using WRF-LES-Chem
Impact of aerosol optics on vertical distribution of ozone in autumn over Yangtze River Delta
A view of the European carbon flux landscape through the lens of the ICOS atmospheric observation network
Technical note: The CAMS greenhouse gas reanalysis from 2003 to 2020
Evaluation of simulated CO2 power plant plumes from six high-resolution atmospheric transport models
Impacts of urbanization on air quality and the related health risks in a city with complex terrain
Optimizing 4 years of CO2 biospheric fluxes from OCO-2 and in situ data in TM5: fire emissions from GFED and inferred from MOPITT CO data
Development and application of a multi-scale modeling framework for urban high-resolution NO2 pollution mapping
Towards monitoring the CO2 source–sink distribution over India via inverse modelling: quantifying the fine-scale spatiotemporal variability in the atmospheric CO2 mole fraction
Methane emissions from China: a high-resolution inversion of TROPOMI satellite observations
Estimated regional CO2 flux and uncertainty based on an ensemble of atmospheric CO2 inversions
Assessing the representativity of NH3 measurements influenced by boundary-layer dynamics and the turbulent dispersion of a nearby emission source
Analysis of CO2, CH4, and CO surface and column concentrations observed at Réunion Island by assessing WRF-Chem simulations
Technical note: Interpretation of field observations of point-source methane plume using observation-driven large-eddy simulations
Zhou Zang, Jane Liu, David Tarasick, Omid Moeini, Jianchun Bian, Jinqiang Zhang, Anne M. Thompson, Roeland Van Malderen, Herman G. J. Smit, Ryan M. Stauffer, Bryan J. Johnson, and Debra E. Kollonige
Atmos. Chem. Phys., 24, 13889–13912, https://doi.org/10.5194/acp-24-13889-2024, https://doi.org/10.5194/acp-24-13889-2024, 2024
Short summary
Short summary
The Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST) provides a global-scale, long-term ozone climatology that is horizontally and vertically resolved. In this study, we improved, updated and validated TOST from 1970 to 2021. Based on this TOST dataset, we characterized global ozone variations spatially in both the troposphere and stratosphere and temporally by season and decade. We also showed a stagnant lower stratospheric ozone variation since the late 1990s.
Kai Meng, Tianliang Zhao, Yongqing Bai, Ming Wu, Le Cao, Xuewei Hou, Yuehan Luo, and Yongcheng Jiang
Atmos. Chem. Phys., 24, 12623–12642, https://doi.org/10.5194/acp-24-12623-2024, https://doi.org/10.5194/acp-24-12623-2024, 2024
Short summary
Short summary
We studied the impact of stratospheric intrusions (SIs) on tropospheric and near-surface ozone in Central and Eastern China from a stratospheric source tracing perspective. SIs contribute the most in the eastern plains, with a contribution exceeding 15 %, and have a small contribution to the west and south. Western Siberia and Mongolia are the most critical source areas for indirect and direct SIs, with the Rossby wave and northeast cold vortex being important driving circulation systems.
Michael Steiner, Luca Cantarello, Stephan Henne, and Dominik Brunner
Atmos. Chem. Phys., 24, 12447–12463, https://doi.org/10.5194/acp-24-12447-2024, https://doi.org/10.5194/acp-24-12447-2024, 2024
Short summary
Short summary
Atmospheric greenhouse gas inversions have great potential to independently check reported bottom-up emissions; however they are subject to large uncertainties. It is paramount to address and reduce the largest source of uncertainty, which stems from the representation of atmospheric transport in the models. In this study, we show that the use of a temporally varying flow-dependent atmospheric transport uncertainty can enhance the accuracy of emission estimation in an idealized experiment.
Cynthia D. Nevison, Qing Liang, Paul A. Newman, Britton B. Stephens, Geoff Dutton, Xin Lan, Roisin Commane, Yenny Gonzalez, and Eric Kort
Atmos. Chem. Phys., 24, 10513–10529, https://doi.org/10.5194/acp-24-10513-2024, https://doi.org/10.5194/acp-24-10513-2024, 2024
Short summary
Short summary
This study examines the drivers of interannual variability in tropospheric N2O. New insights are obtained from aircraft data and a chemistry–climate model that explicitly simulates stratospheric N2O. The stratosphere is found to be the dominant driver of N2O variability in the Northern Hemisphere, while both the stratosphere and El Niño cycles are important in the Southern Hemisphere. These results are consistent with known atmospheric dynamics and differences between the hemispheres.
Misa Ishizawa, Douglas Chan, Doug Worthy, Elton Chan, Felix Vogel, Joe R. Melton, and Vivek K. Arora
Atmos. Chem. Phys., 24, 10013–10038, https://doi.org/10.5194/acp-24-10013-2024, https://doi.org/10.5194/acp-24-10013-2024, 2024
Short summary
Short summary
Methane (CH4) emissions in Canada for 2007–2017 were estimated using Canada’s surface greenhouse gas measurements. The estimated emissions show no significant trend, but emission uncertainty was reduced as more measurement sites became available. Notably for climate change, we find the wetland CH4 emissions show a positive correlation with surface air temperature in summer. Canada’s measurement network could monitor future CH4 emission changes and compliance with climate change mitigation goals.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
Atmos. Chem. Phys., 24, 8847–8864, https://doi.org/10.5194/acp-24-8847-2024, https://doi.org/10.5194/acp-24-8847-2024, 2024
Short summary
Short summary
This study investigates the contribution of pollutants from different emitting periods to ozone episodes over the Greater Bay Area. The analysis reveals the variation in major spatiotemporal contributors to the O3 pollution under the influence of typhoons and subtropical high pressure. Through temporal contribution analysis, our work offers a new perspective on the evolution of O3 pollution and can aid in developing effective and timely control policies under unfavorable weather conditions.
Sepehr Fathi, Paul Makar, Wanmin Gong, Junhua Zhang, Katherine Hayden, and Mark Gordon
EGUsphere, https://doi.org/10.5194/egusphere-2024-1655, https://doi.org/10.5194/egusphere-2024-1655, 2024
Short summary
Short summary
Our study explores the influence of water phase changes in plumes from industrial sources on atmospheric dispersion of emitted pollutants and air quality. Employing PRISM (Plume-Rise-Iterative-Stratified-Moist), a new method, we found that considering these effects significantly improves predictions of pollutant dispersion. This insight enhances our understanding of environmental impacts, enabling more accurate air quality modeling, and fostering more effective pollution management strategies.
Maria K. Tenkanen, Aki Tsuruta, Hugo Denier van der Gon, Lena Höglund-Isaksson, Antti Leppänen, Tiina Markkanen, Ana Maria Roxana Petrescu, Maarit Raivonen, and Tuula Aalto
EGUsphere, https://doi.org/10.5194/egusphere-2024-1953, https://doi.org/10.5194/egusphere-2024-1953, 2024
Short summary
Short summary
Accurate national methane (CH4) emission estimates are essential for tracking progress towards climate goals. This study compares estimates from Finland, which use different methods and scales, and shows how well a global model estimates emissions within a country. The bottom-up estimates vary a lot but constraining them with atmospheric CH4 measurements brought the estimates closer together. We also highlight the importance of quantifying natural emissions alongside anthropogenic emissions.
Fabian Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
Atmos. Chem. Phys., 24, 8183–8203, https://doi.org/10.5194/acp-24-8183-2024, https://doi.org/10.5194/acp-24-8183-2024, 2024
Short summary
Short summary
We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates vs. continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of ffCO2 emissions in an urban region with an inverse modeling framework. We find that the CO-based ffCO2 estimates allow us to reconstruct robust seasonal cycles, which show the distinct COVID-19 drawdown in 2020 and can be used to validate emission inventories.
Kevin Oliveira, Marc Guevara, Oriol Jorba, Hervé Petetin, Dene Bowdalo, Carles Tena, Gilbert Montané Pinto, Franco López, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7137–7177, https://doi.org/10.5194/acp-24-7137-2024, https://doi.org/10.5194/acp-24-7137-2024, 2024
Short summary
Short summary
In this work, we assess and evaluate benzene, toluene, and xylene primary emissions and air quality levels in Spain by combining observations, emission inventories, and air quality modelling techniques. The comparison between modelled and observed levels allows identifying uncertainty sources within the emission input. This contributes to improving air quality models' performance when simulating these compounds, leading to better support for the design of effective pollution control strategies.
Yuehan Luo, Tianliang Zhao, Kai Meng, Jun Hu, Qingjian Yang, Yongqing Bai, Kai Yang, Weikang Fu, Chenghao Tan, Yifan Zhang, Yanzhe Zhang, and Zhikuan Li
Atmos. Chem. Phys., 24, 7013–7026, https://doi.org/10.5194/acp-24-7013-2024, https://doi.org/10.5194/acp-24-7013-2024, 2024
Short summary
Short summary
We reveal a significant mechanism of stratospheric O3 intrusion (SI) into the atmospheric environment induced by an extratropical cyclone system. This system facilitates the downward transport of stratospheric O3 to the near-surface layer by vertical coupling, involving the upper westerly trough, the middle northeast cold vortex, and the lower extratropical cyclone in the troposphere. On average, stratospheric O3 contributed 26.77 % to near-surface O3 levels over the North China Plain.
Cheng Zheng, Yutian Wu, Mingfang Ting, and Clara Orbe
Atmos. Chem. Phys., 24, 6965–6985, https://doi.org/10.5194/acp-24-6965-2024, https://doi.org/10.5194/acp-24-6965-2024, 2024
Short summary
Short summary
Trace gases and aerosols in the Arctic, which typically originate from midlatitude and tropical emission regions, modulate the Arctic climate via their radiative and chemistry impacts. Thus, long-range transport of these substances is important for understanding the current and the future change of Arctic climate. By employing chemistry–climate models, we explore how year-to-year variations in the atmospheric circulation modulate atmospheric long-range transport into the Arctic.
Xingyu Wang, Fei Jiang, Hengmao Wang, Zhengqi Zhang, Mousong Wu, Jun Wang, Wei He, Weimin Ju, and Jingming Chen
EGUsphere, https://doi.org/10.5194/egusphere-2024-1568, https://doi.org/10.5194/egusphere-2024-1568, 2024
Short summary
Short summary
The role of Orbital Carbon Observatory 3 (OCO-3) satellites in estimating the global terrestrial near-Earth environment is unclear. So we study it by assimilating OCO-3 XCO2 alone and with OCO-2 XCO2 inversion. We found that assimilation OCO-3 XCO2 underestimated land sinks at high latitudes by retrieval alone. Joint assimilation of OCO-2 and OCO-3 XCO2 needs to be retrieved to better estimate global terrestrial NEEs.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
Short summary
Short summary
The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Vishnu Thilakan, Dhanyalekshmi Pillai, Jithin Sukumaran, Christoph Gerbig, Haseeb Hakkim, Vinayak Sinha, Yukio Terao, Manish Naja, and Monish Vijay Deshpande
Atmos. Chem. Phys., 24, 5315–5335, https://doi.org/10.5194/acp-24-5315-2024, https://doi.org/10.5194/acp-24-5315-2024, 2024
Short summary
Short summary
This study investigates the usability of CO2 mixing ratio observations over India to infer regional carbon sources and sinks. We demonstrate that a high-resolution modelling system can represent the observed CO2 variations reasonably well by improving the transport and flux variations at a fine scale. Future carbon data assimilation systems can thus benefit from these recently available CO2 observations when fine-scale variations are adequately represented in the models.
Rostislav Kouznetsov, Risto Hänninen, Andreas Uppstu, Evgeny Kadantsev, Yalda Fatahi, Marje Prank, Dmitrii Kouznetsov, Steffen Manfred Noe, Heikki Junninen, and Mikhail Sofiev
Atmos. Chem. Phys., 24, 4675–4691, https://doi.org/10.5194/acp-24-4675-2024, https://doi.org/10.5194/acp-24-4675-2024, 2024
Short summary
Short summary
By relying solely on publicly available media reports, we were able to infer the temporal evolution and the injection height for the Nord Stream gas leaks in September 2022. The inventory specifies locations, vertical distributions, and temporal evolution of the methane sources. The inventory can be used to simulate the event with atmospheric transport models. The inventory is supplemented with a set of observational data tailored to evaluate the results of the simulated atmospheric dispersion.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
Short summary
Short summary
The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Nan Wang, Hongyue Wang, Xin Huang, Xi Chen, Yu Zou, Tao Deng, Tingyuan Li, Xiaopu Lyu, and Fumo Yang
Atmos. Chem. Phys., 24, 1559–1570, https://doi.org/10.5194/acp-24-1559-2024, https://doi.org/10.5194/acp-24-1559-2024, 2024
Short summary
Short summary
This study explores the influence of extreme-weather-induced natural processes on ozone pollution, which is often overlooked. By analyzing meteorological factors, natural emissions, chemistry pathways and atmospheric transport, we discovered that these natural processes could substantially exacerbate ozone pollution. The findings contribute to a deeper understanding of ozone pollution and offer valuable insights for controlling ozone pollution in the context of global warming.
Jia Mao, Amos P. K. Tai, David H. Y. Yung, Tiangang Yuan, Kong T. Chau, and Zhaozhong Feng
Atmos. Chem. Phys., 24, 345–366, https://doi.org/10.5194/acp-24-345-2024, https://doi.org/10.5194/acp-24-345-2024, 2024
Short summary
Short summary
Surface ozone (O3) is well-known for posing great threats to both human health and agriculture worldwide. However, a multidecadal assessment of the impacts of O3 on public health and agriculture in China is lacking without sufficient O3 observations. We used a hybrid approach combining a chemical transport model and machine learning to provide a robust dataset of O3 concentrations over the past 4 decades in China, thereby filling the gap in the long-term O3 trend and impact assessment in China.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
Short summary
Short summary
NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Ondřej Tichý, Sabine Eckhardt, Yves Balkanski, Didier Hauglustaine, and Nikolaos Evangeliou
Atmos. Chem. Phys., 23, 15235–15252, https://doi.org/10.5194/acp-23-15235-2023, https://doi.org/10.5194/acp-23-15235-2023, 2023
Short summary
Short summary
We show declining trends in NH3 emissions over Europe for 2013–2020 using advanced dispersion and inverse modelling and satellite measurements from CrIS. Emissions decreased by −26% since 2013, showing that the abatement strategies adopted by the European Union have been very efficient. Ammonia emissions are low in winter and peak in summer due to temperature-dependent soil volatilization. The largest decreases were observed in central and western Europe in countries with high emissions.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
Short summary
Short summary
Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Maryam Golbazi and Cristina Archer
Atmos. Chem. Phys., 23, 15057–15075, https://doi.org/10.5194/acp-23-15057-2023, https://doi.org/10.5194/acp-23-15057-2023, 2023
Short summary
Short summary
We use scientific models to study the impact of ship emissions on air quality along the US East Coast. We find an increase in three major pollutants (PM2.5, NO2, and SO2) in coastal regions. However, we detect a reduction in ozone (O3) levels in major coastal cities. This reduction is linked to the significant emissions of nitrogen oxides (NOx) from ships, which scavenged O3, especially in highly polluted urban areas experiencing an NOx-limited regime.
Xinxu Zhao, Jia Chen, Julia Marshall, Michal Gałkowski, Stephan Hachinger, Florian Dietrich, Ankit Shekhar, Johannes Gensheimer, Adrian Wenzel, and Christoph Gerbig
Atmos. Chem. Phys., 23, 14325–14347, https://doi.org/10.5194/acp-23-14325-2023, https://doi.org/10.5194/acp-23-14325-2023, 2023
Short summary
Short summary
We develop a modeling framework using the Weather Research and Forecasting model at a high spatial resolution (up to 400 m) to simulate atmospheric transport of greenhouse gases and interpret column observations. Output is validated against weather stations and column measurements in August 2018. The differential column method is applied, aided by air-mass transport tracing with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, also for an exploratory measurement interpretation.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
Short summary
Short summary
The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
Short summary
Short summary
The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
Short summary
Short summary
This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Fu-Jie Zhu, Peng-Tuan Hu, and Wan-Li Ma
Atmos. Chem. Phys., 23, 8583–8590, https://doi.org/10.5194/acp-23-8583-2023, https://doi.org/10.5194/acp-23-8583-2023, 2023
Short summary
Short summary
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons was established based on the level-III multimedia fugacity model, which proved that the particulate proportion of PAHs in emissions was a crucial factor for G–P partitioning of PAHs. In addition, gaseous and particulate interference was also derived in the new steady-state model determined by the particulate proportion in emission that could derivate the G–P partitioning quotients from the equilibrium state.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
Short summary
Short summary
Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
Short summary
Short summary
Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
Short summary
Short summary
Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Danyang Ma, Tijian Wang, Hao Wu, Yawei Qu, Jian Liu, Jane Liu, Shu Li, Bingliang Zhuang, Mengmeng Li, and Min Xie
Atmos. Chem. Phys., 23, 6525–6544, https://doi.org/10.5194/acp-23-6525-2023, https://doi.org/10.5194/acp-23-6525-2023, 2023
Short summary
Short summary
Increasing surface ozone (O3) concentrations have long been a significant environmental issue in China, despite the Clean Air Action Plan launched in 2013. Most previous research ignores the contributions of CO2 variations. Our study comprehensively analyzed O3 variation across China from various perspectives and highlighted the importance of considering CO2 variations when designing long-term O3 control policies, especially in high-vegetation-coverage areas.
Jackson Hian-Wui Chang, Stephen M. Griffith, Steven Soon-Kai Kong, Ming-Tung Chuang, and Neng-Huei Lin
Atmos. Chem. Phys., 23, 6357–6382, https://doi.org/10.5194/acp-23-6357-2023, https://doi.org/10.5194/acp-23-6357-2023, 2023
Short summary
Short summary
A novel CMAQ–PMF-based composite index is developed to identify the key VOC source species for an effective ozone abatement strategy. The index provides information as to which VOC species are key to ozone formation and where to reduce sources of these VOC species. Using the composite index, we recommended the VOC control measures in southern Taiwan should prioritize solvent usage, vehicle emissions, and the petrochemical industry.
Lei Duan and Ken Caldeira
Atmos. Chem. Phys., 23, 6011–6020, https://doi.org/10.5194/acp-23-6011-2023, https://doi.org/10.5194/acp-23-6011-2023, 2023
Short summary
Short summary
Ocko and Hamburg (2022) emphasize the short-term climate impact of hydrogen, and we present an analysis that places greater focus on long-term outcomes. We have derived equations that describe the time-evolving impact of hydrogen and show that higher methane leakage is primarily responsible for the warming potential of blue hydrogen, while hydrogen leakage plays a less critical role. Fossil fuels show more prominent longer-term climate impacts than clean hydrogen under all emission scenarios.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
Short summary
Short summary
Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
Short summary
Short summary
We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Jianing Dai, Cathy Wing Yi Li, Pablo Lichtig, Roy Chun-Wang Tsang, Chun-Ho Liu, Tao Wang, and Guy Pierre Brasseur
Atmos. Chem. Phys., 23, 5905–5927, https://doi.org/10.5194/acp-23-5905-2023, https://doi.org/10.5194/acp-23-5905-2023, 2023
Short summary
Short summary
Air quality in urban areas is difficult to simulate in coarse-resolution models. This work exploits the WRF (Weather Research and Forecasting) model coupled with a large-eddy simulation (LES) component and online chemistry to perform high-resolution (33.3 m) simulations of air quality in a large city. The evaluation of the simulations with observations shows that increased model resolution improves the representation of the chemical species near the pollution sources.
Shuqi Yan, Bin Zhu, Shuangshuang Shi, Wen Lu, Jinhui Gao, Hanqing Kang, and Duanyang Liu
Atmos. Chem. Phys., 23, 5177–5190, https://doi.org/10.5194/acp-23-5177-2023, https://doi.org/10.5194/acp-23-5177-2023, 2023
Short summary
Short summary
We analyze ozone response to aerosol mixing states in the vertical direction by WRF-Chem simulations. Aerosols generally lead to turbulent suppression, precursor accumulation, low-level photolysis reduction, and upper-level photolysis enhancement under different underlying surface and pollution conditions. Thus, ozone decreases within the entire boundary layer during the daytime, and the decrease is the least in aerosol external mixing states compared to internal and core shell mixing states.
Ida Storm, Ute Karstens, Claudio D'Onofrio, Alex Vermeulen, and Wouter Peters
Atmos. Chem. Phys., 23, 4993–5008, https://doi.org/10.5194/acp-23-4993-2023, https://doi.org/10.5194/acp-23-4993-2023, 2023
Short summary
Short summary
In this study, we evaluate what is in the influence regions of the ICOS atmospheric measurement stations to gain insight into what land cover types and land-cover-associated fluxes the network represents. Subsequently, insights about strengths, weaknesses, and potential gaps can assist in future network expansion decisions. The network is concentrated in central Europe, which leads to a general overrepresentation of coniferous forest and cropland and underrepresentation of grass and shrubland.
Anna Agustí-Panareda, Jérôme Barré, Sébastien Massart, Antje Inness, Ilse Aben, Melanie Ades, Bianca C. Baier, Gianpaolo Balsamo, Tobias Borsdorff, Nicolas Bousserez, Souhail Boussetta, Michael Buchwitz, Luca Cantarello, Cyril Crevoisier, Richard Engelen, Henk Eskes, Johannes Flemming, Sébastien Garrigues, Otto Hasekamp, Vincent Huijnen, Luke Jones, Zak Kipling, Bavo Langerock, Joe McNorton, Nicolas Meilhac, Stefan Noël, Mark Parrington, Vincent-Henri Peuch, Michel Ramonet, Miha Razinger, Maximilian Reuter, Roberto Ribas, Martin Suttie, Colm Sweeney, Jérôme Tarniewicz, and Lianghai Wu
Atmos. Chem. Phys., 23, 3829–3859, https://doi.org/10.5194/acp-23-3829-2023, https://doi.org/10.5194/acp-23-3829-2023, 2023
Short summary
Short summary
We present a global dataset of atmospheric CO2 and CH4, the two most important human-made greenhouse gases, which covers almost 2 decades (2003–2020). It is produced by combining satellite data of CO2 and CH4 with a weather and air composition prediction model, and it has been carefully evaluated against independent observations to ensure validity and point out deficiencies to the user. This dataset can be used for scientific studies in the field of climate change and the global carbon cycle.
Dominik Brunner, Gerrit Kuhlmann, Stephan Henne, Erik Koene, Bastian Kern, Sebastian Wolff, Christiane Voigt, Patrick Jöckel, Christoph Kiemle, Anke Roiger, Alina Fiehn, Sven Krautwurst, Konstantin Gerilowski, Heinrich Bovensmann, Jakob Borchardt, Michal Galkowski, Christoph Gerbig, Julia Marshall, Andrzej Klonecki, Pascal Prunet, Robert Hanfland, Margit Pattantyús-Ábrahám, Andrzej Wyszogrodzki, and Andreas Fix
Atmos. Chem. Phys., 23, 2699–2728, https://doi.org/10.5194/acp-23-2699-2023, https://doi.org/10.5194/acp-23-2699-2023, 2023
Short summary
Short summary
We evaluated six atmospheric transport models for their capability to simulate the CO2 plumes from two of the largest power plants in Europe by comparing the models against aircraft observations collected during the CoMet (Carbon Dioxide and Methane Mission) campaign in 2018. The study analyzed how realistically such plumes can be simulated at different model resolutions and how well the planned European satellite mission CO2M will be able to quantify emissions from power plants.
Chenchao Zhan, Min Xie, Hua Lu, Bojun Liu, Zheng Wu, Tijian Wang, Bingliang Zhuang, Mengmeng Li, and Shu Li
Atmos. Chem. Phys., 23, 771–788, https://doi.org/10.5194/acp-23-771-2023, https://doi.org/10.5194/acp-23-771-2023, 2023
Short summary
Short summary
With the development of urbanization, urban land use and anthropogenic
emissions increase, affecting urban air quality and, in turn, the health risks associated with air pollutants. In this study, we systematically evaluate the impacts of urbanization on air quality and the corresponding health risks in a highly urbanized city with severe air pollution and complex terrain. This work focuses on the health risks caused by urbanization and can provide valuable insight for air pollution strategies.
Hélène Peiro, Sean Crowell, and Berrien Moore III
Atmos. Chem. Phys., 22, 15817–15849, https://doi.org/10.5194/acp-22-15817-2022, https://doi.org/10.5194/acp-22-15817-2022, 2022
Short summary
Short summary
CO data can provide a powerful constraint on fire fluxes, supporting more accurate estimation of biospheric CO2 fluxes. We converted CO fire flux into CO2 fire prior, which is then used to adjust CO2 respiration. We applied this to two other fire flux products. CO2 inversions constrained by satellites or in situ data are then performed. Results show larger variations among the data assimilated than across the priors, but tropical flux from in situ inversions is sensitive to priors.
Zhaofeng Lv, Zhenyu Luo, Fanyuan Deng, Xiaotong Wang, Junchao Zhao, Lucheng Xu, Tingkun He, Yingzhi Zhang, Huan Liu, and Kebin He
Atmos. Chem. Phys., 22, 15685–15702, https://doi.org/10.5194/acp-22-15685-2022, https://doi.org/10.5194/acp-22-15685-2022, 2022
Short summary
Short summary
This study developed a hybrid model, CMAQ-RLINE_URBAN, to predict the urban NO2 concentrations at a high spatial resolution. To estimate the influence of various street canyons on the dispersion of air pollutants, a new parameterization scheme was established based on computational fluid dynamics and machine learning methods. This work created a new method to identify the characteristics of vehicle-related air pollution at both city and street scales simultaneously and accurately.
Vishnu Thilakan, Dhanyalekshmi Pillai, Christoph Gerbig, Michal Galkowski, Aparnna Ravi, and Thara Anna Mathew
Atmos. Chem. Phys., 22, 15287–15312, https://doi.org/10.5194/acp-22-15287-2022, https://doi.org/10.5194/acp-22-15287-2022, 2022
Short summary
Short summary
This paper demonstrates how we can use atmospheric observations to improve the CO2 flux estimates in India. This is achieved by improving the representation of terrain, mesoscale transport, and flux variations. We quantify the impact of the unresolved variations in the current models on optimally estimated fluxes via inverse modelling and quantify the associated flux uncertainty. We illustrate how a parameterization scheme captures this variability in the coarse models.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
Short summary
Short summary
We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Naveen Chandra, Prabir K. Patra, Yousuke Niwa, Akihiko Ito, Yosuke Iida, Daisuke Goto, Shinji Morimoto, Masayuki Kondo, Masayuki Takigawa, Tomohiro Hajima, and Michio Watanabe
Atmos. Chem. Phys., 22, 9215–9243, https://doi.org/10.5194/acp-22-9215-2022, https://doi.org/10.5194/acp-22-9215-2022, 2022
Short summary
Short summary
This paper is intended to accomplish two goals: (1) quantify mean and uncertainty in non-fossil-fuel CO2 fluxes estimated by inverse modeling and (2) provide in-depth analyses of regional CO2 fluxes in support of emission mitigation policymaking. CO2 flux variability and trends are discussed concerning natural climate variability and human disturbances using multiple lines of evidence.
Ruben B. Schulte, Margreet C. van Zanten, Bart J. H. van Stratum, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 22, 8241–8257, https://doi.org/10.5194/acp-22-8241-2022, https://doi.org/10.5194/acp-22-8241-2022, 2022
Short summary
Short summary
We present a fine-scale simulation framework, utilizing large-eddy simulations, to assess NH3 measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source. The minimum required distance from an emission source differs for concentration and flux measurements, from 0.5–3.0 km and 0.75–4.5 km, respectively. The simulation framework presented here proves to be a powerful and versatile tool for future NH3 research at high spatio-temporal resolutions.
Sieglinde Callewaert, Jérôme Brioude, Bavo Langerock, Valentin Duflot, Dominique Fonteyn, Jean-François Müller, Jean-Marc Metzger, Christian Hermans, Nicolas Kumps, Michel Ramonet, Morgan Lopez, Emmanuel Mahieu, and Martine De Mazière
Atmos. Chem. Phys., 22, 7763–7792, https://doi.org/10.5194/acp-22-7763-2022, https://doi.org/10.5194/acp-22-7763-2022, 2022
Short summary
Short summary
A regional atmospheric transport model is used to analyze the factors contributing to CO2, CH4, and CO observations at Réunion Island. We show that the surface observations are dominated by local fluxes and dynamical processes, while the column data are influenced by larger-scale mechanisms such as biomass burning plumes. The model is able to capture the measured time series well; however, the results are highly dependent on accurate boundary conditions and high-resolution emission inventories.
Anja Ražnjević, Chiel van Heerwaarden, Bart van Stratum, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, and Maarten Krol
Atmos. Chem. Phys., 22, 6489–6505, https://doi.org/10.5194/acp-22-6489-2022, https://doi.org/10.5194/acp-22-6489-2022, 2022
Short summary
Short summary
Mobile measurement techniques (e.g., instruments placed in cars) are often employed to identify and quantify individual sources of greenhouse gases. Due to road restrictions, those observations are often sparse (temporally and spatially). We performed high-resolution simulations of plume dispersion, with realistic weather conditions encountered in the field, to reproduce the measurement process of a methane plume emitted from an oil well and provide additional information about the plume.
Cited articles
Abbatt, J. P. D.: Interaction of HNO3 with water-ice surfaces at temperatures of the free troposphere, Geophys. Res. Lett., 24, 1479–1482, https://doi.org/10.1029/97GL01403, 1997.
Akinfiev, N. N., Mironenko, M. V., and Grant, S. A.: Thermodynamic Properties of NaCl Solutions at Subzero Temperatures, J. Solut. Chem., 30, 1065–1080, https://doi.org/10.1023/A:1014445917207, 2001.
Ammann, M., Cox, R. A., Crowley, J. N., Jenkin, M. E., Mellouki, A., Rossi, M. J., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VI – heterogeneous reactions with liquid substrates, Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, 2013.
Bartels-Rausch, T., Jacobi, H.-W., Kahan, T. F., Thomas, J. L., Thomson, E. S., Abbatt, J. P. D., Ammann, M., Blackford, J. R., Bluhm, H., Boxe, C., Domine, F., Frey, M. M., Gladich, I., Guzmán, M. I., Heger, D., Huthwelker, T., Klán, P., Kuhs, W. F., Kuo, M. H., Maus, S., Moussa, S. G., McNeill, V. F., Newberg, J. T., Pettersson, J. B. C., Roeselová, M., and Sodeau, J. R.: A review of air ice chemical and physical interactions (AICI): liquids, quasi-liquids, and solids in snow, Atmo. Chem. Phys., 14, 1587–1633, https://doi.org/10.5194/acp-14-1587-2014, 2014.
Beine, H. J., Honrath, R. E., Dominè, F., Simpson, W. R., and Fuentes, J. D.: NOx during background and ozone depletion periods at Alert: Fluxes above the snow surface, J. Geophys. Res.-Atmos., 107, 4584, https://doi.org/10.1029/2002JD002082, 2002.
Beine, H. J., Dominè, F., Ianniello, A., Nardino, M., Allegrini, I., Teinilä, K., and Hillamo, R.: Fluxes of nitrates between snow surfaces and the atmosphere in the European high Arctic, Atmos. Chem. Phys., 3, 335–346, https://doi.org/10.5194/acp-3-335-2003, 2003.
Beyer, K. D. and Hansen, A. R.: Phase Diagram of the Nitric Acid/Water System: Implications for Polar Stratospheric Clouds, J. Phys. Chem. A, 106, 10275–10284, https://doi.org/10.1021/jp025535o, 2002.
Bock, J., Savarino, J., and Picard, G.: Air–snow exchange of nitrate: a modelling approach to investigate physicochemical processes in surface snow at Dome C, Antarctica, Atmos. Chem. Phys., 16, 12531–12550, https://doi.org/10.5194/acp-16-12531-2016, 2016.
Boxe, C. S. and Saiz-Lopez, A.: Multiphase modeling of nitrate photochemistry in the quasi-liquid layer (QLL): implications for NOx release from the Arctic and coastal Antarctic snowpack, Atmos. Chem. Phys., 8, 4855–4864, https://doi.org/10.5194/acp-8-4855-2008, 2008.
Brimblecombe, P. and Clegg, S. L.: The solubility and behaviour of acid gases in the marine aerosol, J. Atmos. Chem., 7, 1–18, https://doi.org/10.1007/BF00048251, 1988.
Burkholder, J. B., Sander, S. P., Abbatt, J. P., Barker, J. R., Huie, R. E., Kolb, C. E., Kurylo, M. J., Orkin, V. L., Wilmouth, D. M., and Wine, P. H.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation No. 18, JPL Publication 15-10, Jet Propulsion Laboratory, Pasadena, 2015.
Cho, H., Shepson, P. B., Barrie, L. A., Cowin, J. P., Zaveri, R.: NMR Investigation of the Quasi-Brine Layer in Ice/Brine Mixtures, J. Phys. Chem. B, 106, 11226–11232, https://doi.org/10.1021/jp020449, 2002.
Conde, M. M., Vega, C., and Patrykiejew, A.: The thickness of a liquid layer on the free surface of ice as obtained from computer simulation, J. Chem. Phys., 129, 014702, https://doi.org/10.1063/1.2940195, 2008.
Cox, R. A., Fernandez, M. A., Symington, A., Ullerstam, M., and Abbatt, J. P. D.: A kinetic model for uptake of HNO3 and HCl on ice in a coated wall flow system, Phys. Chem. Chem. Phys., 7, 3434–3442, https://doi.org/10.1039/B506683B, 2005.
Crowley, J. N., Ammann, M., Cox, R. A., Hynes, R. G., Jenkin, M. E., Mellouki, A., Rossi, M. J., Troe, J., and Wallington, T. J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume V heterogeneous reactions on solid substrates, Atmos. Chem. Phys., 10, 9059–9223, https://doi.org/10.5194/acp-10-9059-2010, 2010.
Dasgupta, P. K., Campbell, S. W., Al-Horr, R. S., Ullah, S. R., Li, J., Amalfitano, C., and Poor, N. D.: Conversion of sea salt aerosol to NaNO3 and the production of HCl: Analysis of temporal behavior of aerosol chloride/nitrate and gaseous HCl/HNO3 concentrations with {AIM}, Atmos. Environ., 41, 4242–4257, https://doi.org/10.1016/j.atmosenv.2006.09.054, 2007.
Dash, J. G., Rempel, A. W. and Wettlaufer, J. S.: The physics of premelted ice and its geophysical consequences, Rev. Mod. Phys., 78, 695–741, https://doi.org/10.1103/RevModPhys.78.695, 2006.
Domine, F., Bock, J., Voisin, D., and Donaldson, D. J.: Can We Model Snow Photochemistry? Problems with the Current Approaches, J. Phys. Chem. A, 117, 4733–4749, https://doi.org/10.1021/jp3123314, 2013.
Erbland, J., Vicars, W. C., Savarino, J., Morin, S., Frey, M. M., Frosini, D., Vince, E., and Martins, J. M. F.: Air–snow transfer of nitrate on the East Antarctic Plateau – Part 1: Isotopic evidence for a photolytically driven dynamic equilibrium in summer, Atmos. Chem. Phys., 13, 6403–6419, https://doi.org/10.5194/acp-13-6403-2013, 2013.
Finlayson-Pitts, B. J. and Pitts, J. N. (Eds.): Chapter 5 – Kinetics and Atmospheric Chemistry, in: Chemistry of the Upper and Lower Atmosphere, Academic Press, San Diego, 130–178, https://doi.org/10.1016/B978-012257060-5/50007-1, 2000.
Flanner, M. G. and Zender, C. S.: Linking snowpack microphysics and albedo evolution, J. Geophys. Res.-Atmos., 111, d12208, https://doi.org/10.1029/2005JD006834, 2006.
Fowler, D., Amann, M., Anderson, F., Ashmore, M., Cox, P., Depledge, M., Derwent, D., Grennfelt, P., Hewitt, N., Hov, O., Jenkin, M., Kelly, F., Liss, P. S., Pilling, M., Pyle, J., Slingo, J., and Stevenson, D.: Ground-level ozone in the 21st century: future trends, impacts and policy implications, in: vol. 15/08 of Science Policy, The Royal Society, London, http://nora.nerc.ac.uk/8577/ (last access: August 2017), 2008.
France, J. L., King, M. D., Frey, M. M., Erbland, J., Picard, G., Preunkert, S., MacArthur, A., and Savarino, J.: Snow optical properties at Dome C (Concordia), Antarctica; implications for snow emissions and snow chemistry of reactive nitrogen, Atmos. Chem. Physics, 11, 9787–9801, https://doi.org/10.5194/acp-11-9787-2011, 2011.
Frey, M. M., Savarino, J., Morin, S., Erbland, J., and Martins, J. M. F.: Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling, Atmos. Chem. Phys., 9, 8681–8696, https://doi.org/10.5194/acp-9-8681-2009, 2009.
Frey, M. M., Brough, N., France, J. L., Anderson, P. S., Traulle, O., King, M. D., Jones, A. E., Wolff, E. W., and Savarino, J.: The diurnal variability of atmospheric nitrogen oxides (NO and NO2) above the Antarctic Plateau driven by atmospheric stability and snow emissions, Atmos. Chem. Phys., 13, 3045–3062, https://doi.org/10.5194/acp-13-3045-2013, 2013.
Gligorovski, S., Strekowski, R., Barbati, S., and Vione, D.: Environmental Implications of Hydroxyl Radicals (OH), Chem. Rev., 115, 13051–13092, https://doi.org/10.1021/cr500310b, 2015.
Grannas, A. M., Jones, A. E., Dibb, J., Ammann, M., Anastasio, C., Beine, H. J., Bergin, M., Bottenheim, J., Boxe, C. S., Carver, G., Chen, G., Crawford, J. H., Dominé, F., Frey, M. M., Guzmán, M. I., Heard, D. E., Helmig, D., Hoffmann, M. R., Honrath, R. E., Huey, L. G., Hutterli, M., Jacobi, H. W., Klán, P., Lefer, B., McConnell, J., Plane, J., Sander, R., Savarino, J., Shepson, P. B., Simpson, W. R., Sodeau, J. R., von Glasow, R., Weller, R., Wolff, E. W., and Zhu, T.: An overview of snow photochemistry: evidence, mechanisms and impacts, Atmos. Chem. Phys., 7, 4329–4373, https://doi.org/10.5194/acp-7-4329-2007, 2007.
Honrath, R. E., Peterson, M. C., Dziobak, M. P., Dibb, J. E., Arsenault, M. A., and Green, S. A.: Release of NOx from sunlight-irradiated midlatitude snow, Geophys. Res. Lett., 27, 2237–2240, https://doi.org/10.1029/1999GL011286, 2000.
Hudson, P. K., Zondlo, M. A., and Tolbert, M. A.: The Interaction of Methanol, Acetone, and Acetaldehyde with Ice and Nitric Acid-Doped Ice: Implications for Cirrus Clouds, J. Phys. Chem. A, 106, 2882–2888, https://doi.org/10.1021/jp012718m, 2002.
Huthwelker, T., Malmström, M. E., Helleis, F., Moortgat, G. K., and Peter, T.: Kinetics of HCl Uptake on Ice at 190 and 203 K: Implications for the Microphysics of the Uptake Process, J. Phys. Chem. A, 30, 6302–6318, https://doi.org/10.1021/jp0309623, 2004.
Huthwelker, T. and Ammann, M. and Peter, T.: The Uptake of Acidic Gases on Ice, Chem. Rev., 106, 1375–1444, https://doi.org/10.1021/cr020506v, 2006.
Hutterli, M. A. and Röthlisberger, R.: Atmosphere-to-snow-to-firn transfer studies of HCHO at Summit, Greenland, Geophys. Res. Lett., 26, 1691–1694, 1999.
Hutterli, M. A., McConnell, J. R., Bales, R. C., and Stewart, R. W.: Sensitivity of hydrogen peroxide (H2O2) and formaldehyde (HCHO) preservation in snow to changing environmental conditions: Implications for ice core records, J. Geophys. Res.-Atmos., 108, 4023, https://doi.org/10.1029/2002JD002528, 2003.
Jacobson, M. Z.: Fundamentals of Atmospheric Modeling, 2nd Edn., Cambridge University Press, Cambridge, UK, 2005.
Jones, A. E., Weller, R., Anderson, P. S., Jacobi, H.-W., Wolff, E. W., Schrems, O., and Miller, H.: Measurements of NOx emissions from the Antarctic snowpack, Geophys. Res. Lett., 28, 1499–1502, https://doi.org/10.1029/2000GL011956, 2001.
Jones, A. E., Wolff, E. W., Salmon, R. A., Bauguitte, S. J.-B., Roscoe, H. K., Anderson, P. S., Ames, D., Clemitshaw, K. C., Fleming, Z. L., Bloss, W. J., Heard, D. E., Lee, J. D., Read, K. A., Hamer, P., Shallcross, D. E., Jackson, A. V., Walker, S. L., Lewis, A. C., Mills, G. P., Plane, J. M. C., Saiz-Lopez, A., Sturges, W. T., and Worton, D. R.: Chemistry of the Antarctic Boundary Layer and the Interface with Snow: an overview of the CHABLIS campaign, Atmos. Chem. Phys., 8, 3789–3803, https://doi.org/10.5194/acp-8-3789-2008, 2008.
Jones, A. E., Wolff, E. W., Ames, D., Bauguitte, S. J.-B., Clemitshaw, K. C., Fleming, Z., Mills, G. P., Saiz-Lopez, A., Salmon, R. A., Sturges, W. T., and Worton, D. R.: The multi-seasonal NOy budget in coastal Antarctica and its link with surface snow and ice core nitrate: results from the CHABLIS campaign, Atmos. Chem. Phys., 11, 9271–9285, https://doi.org/10.5194/acp-11-9271-2011, 2011.
Jourdain, B., Preunkert, S., Cerri, O., Castebrunet, H, Udisti, R., and Legrand, M.: Year-round record of size-segregated aerosol composition in central Antarctica (Concordia station): Implications for the degree of fractionation of sea-salt particles, J. Geophys. Res.-Atmos., 113, D14308, https://doi.org/10.1029/2007JD009584, 2008.
Kuo, M. H., Moussa, S. G., and McNeill, V. F.: Modeling interfacial liquid layers on environmental ices, Atmos. Chem. Phys., 11, 9971–9982, https://doi.org/10.5194/acp-11-9971-2011, 2011.
Legrand, M., Yang, X., Preunkert, S., and Theys, N.: Year-round records of sea salt, gaseous, and particulate inorganic bromine in the atmospheric boundary layer at coastal (Dumont d'Urville) and central (Concordia) East Antarctic sites, J. Geophys. Res.-Atmos., 121, 997–1023, https://doi.org/10.1002/2015JD024066, 2016.
McConnell, J. R., Bales, R. C., Stewart, R. W., Thompson, A. M., Albert, M. R., and Ramos, R.: Physically based modeling of atmosphere-to-snow-to-firn transfer of H2O2 at South Pole, J. Geophys. Res.-Atmos., 103, 10561–10570, https://doi.org/10.1029/98JD00460, 1998.
McNeill, V. F., Grannas, A. M., Abbatt, J. P. D., Ammann, M., Ariya, P., Bartels-Rausch, T., Domine, F., Donaldson, D. J., Guzman, M. I., Heger, D., Kahan, T. F., Klán, P., Masclin, S., Toubin, C., and Voisin, D.: Organics in environmental ices: sources, chemistry, and impacts, Atmos. Chem. Phys., 12, 9653–9678, https://doi.org/10.5194/acp-12-9653-2012, 2012.
Morin, S., Savarino, J., Frey, M. M., Yan, N., Bekki, S., Bottenheim, J. W., and Martins, J. M. F.: Tracing the Origin and Fate of NOx in the Arctic Atmosphere Using Stable Isotopes in Nitrate, Science, 322, 730–732, https://doi.org/10.1126/science.1161910, 2008.
Murray, K. A., Kramer, L. J., Doskey, P. V., Ganzeveld, L., Seok, B., Dam, B. V., and Helmig, D.: Dynamics of ozone and nitrogen oxides at Summit, Greenland. II. Simulating snowpack chemistry during a spring high ozone event with a 1-D process-scale model, Atmos. Environ., 117, 110–123, https://doi.org/10.1016/j.atmosenv.2015.07.004, 2015.
Picard, G., Libois, Q., Arnaud, L., Vérin, G., and Dumont, M.: Time-series of snow spectral albedo and superficial snow specific surface area at Dome C in Antarctica, 2012–2015, https://doi.org/10.1594/PANGAEA.860945, supplement to: Picard, G. et al. (2016): Development and calibration of an automatic spectral albedometer to estimate near-surface snow SSA time series, The Cryosphere, 10, 1297–1316, https://doi.org/10.5194/tc-10-1297-2016, 2016.
Pinzer, B. R., Schneebeli, M., and Kaempfer, T. U.: Vapor flux and recrystallization during dry snow metamorphism under a steady temperature gradient as observed by time-lapse micro-tomography, The Cryosphere, 6, 1141–1155, https://doi.org/10.5194/tc-6-1141-2012, 2012.
Press, W. H., Teukolsky, S. A., Vetterling, W. T., and Flannery, B. P.: Numerical Recipe in Fortran 90, 2nd Edn., Cambridge Univeristy Press, Cambridge, 1996.
Pruppacher, H. R. and Klett, J. D.: Microphysics of clouds and precipitation, in: With an introduction to cloud chemistry and cloud electricity, 2nd rev. and enl. ed Edn., Kluwer Academic Publishers, Dordrecht, Boston, 1997.
Rankin, A. M. and Wolff, E. W.: A year-long record of size-segregated aerosol composition at Halley, Antarctica, J. Geophys. Res.-Atmos., 108, D244775, https://doi.org/10.1029/2003JD003993, 2003.
Röthlisberger, R., Hutterli, M. A., Sommer, S., Wolff, E. W., and Mulvaney, R.: Factors controlling nitrate in ice cores: Evidence from the Dome C deep ice core, J. Geophys. Res.-Atmos., 105, 20565–20572, https://doi.org/10.1029/2000JD900264, 2000.
Sander, R.: Modeling Atmospheric Chemistry: Interactions between Gas-Phase Species and Liquid Cloud/Aerosol Particles, Surv. Geophys., 20, 1–31, https://doi.org/10.1023/A:1006501706704, 1999.
Tang, M. J., Cox, R. A., and Kalberer, M.: Compilation and evaluation of gas phase diffusion coefficients of reactive trace gases in the atmosphere: volume 1. Inorganic compounds, Atmos. Chem. Phys., 14, 9233–9247, https://doi.org/10.5194/acp-14-9233-2014, 2014.
Thibert, E. and Dominé, F.: Thermodynamics and Kinetics of the Solid Solution of HNO3 in Ice, J. Phys. Chem. B, 102, 4432–4439, https://doi.org/10.1021/jp980569a, 1998.
Thomas, J. L., Stutz, J., Lefer, B., Huey, L. G., Toyota, K., Dibb, J. E., and von Glasow, R.: Modeling chemistry in and above snow at Summit, Greenland – Part 1: Model description and results, Atmos. Chem. Phys., 11, 4899–4914, https://doi.org/10.5194/acp-11-4899-2011, 2011.
Toyota, K., McConnell, J. C., Staebler, R. M., and Dastoor, A. P.: Air-snowpack exchange of bromine, ozone and mercury in the springtime Arctic simulated by the 1-D model PHANTAS – Part 1: In-snow bromine activation and its impact on ozone, Atmos. Chem. Phys., 14, 4101–4133, https://doi.org/10.5194/acp-14-4101-2014, 2014.
Traversi, R., Udisti, R., Frosini, D., Becagli, S., Ciardini, V., Funke, B., Lanconelli, C., Petkov, B., Scarchilli, C., Severi, M., and Vitale, V.: Insights on nitrate sources at Dome C (East Antarctic Plateau) from multi-year aerosol and snow records, Tellus B, 66, 22550, https://doi.org/10.3402/tellusb.v66.22550, 2014.
Udisti, R., Becagli, S., Benassai, S., Castellano, E., Fattori, I., Innocenti, M., Migliori, A., and Traversi, R.: Atmospheresnow interaction by a comparison between aerosol and uppermost snow-layers composition at Dome C, East Antarctica, Ann. Glaciol., 39, 53–61, https://doi.org/10.3189/172756404781814474, 2004.
Ullerstam, M. and Abbatt, J. P. D.: Burial of gas-phase HNO3 by growing ice surfaces under tropospheric conditions, Phys. Chem. Chem. Phys., 7, 3596–3600, https://doi.org/10.1039/B507797D, 2005a.
Ullerstam, M., Thornberry, T., and Abbatt, J. P. D.: Uptake of gas-phase nitric acid to ice at low partial pressures: evidence for unsaturated surface coverage, Faraday Discuss., 130, 211–226, https://doi.org/10.1039/B417418F, 2005b.
Waddington, E. D., Cunningham, J., and Harder, S. L.: The Effects Of Snow Ventilation on Chemical Concentrations, Springer, Berlin, Heidelberg, 403–451, https://doi.org/10.1007/978-3-642-61171-1_18, 1996.
Wolff, E. W., Jones, A. E., Bauguitte, S. J.-B., and Salmon, R. A.: The interpretation of spikes and trends in concentration of nitrate in polar ice cores, based on evidence from snow and atmospheric measurements, Atmos. Chem. Phys., 8, 5627–5634, https://doi.org/10.5194/acp-8-5627-2008, 2008.
Yuan-Hui, L. and Gregory, S.: Diffusion of ions in sea water and in deep-sea sediments, Geochim. Cosmochim. Ac., 38, 703–714, https://doi.org/10.1016/0016-7037(74)90145-8, 1974.
Short summary
Emissions of reactive nitrogen from snowpacks influence remote air quality. Two physical air–snow models for nitrate were developed. One assumes that below a threshold temperature the air–snow grain interface is pure ice and above it a disordered interface emerges. The other assumes an air–ice interface below melting and that any liquid present is concentrated in micropockets. Only the latter matches observations at two Antarctic lcoations covering a wide range of environmental conditions.
Emissions of reactive nitrogen from snowpacks influence remote air quality. Two physical...
Altmetrics
Final-revised paper
Preprint