Articles | Volume 24, issue 8
https://doi.org/10.5194/acp-24-4895-2024
© Author(s) 2024. 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-24-4895-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
25 Apr 2024
Research article |
| 25 Apr 2024
| 25 Apr 2024
An inverse model to correct for the effects of post-depositional processing on ice-core nitrate and its isotopes: model framework and applications at Summit, Greenland, and Dome C, Antarctica
Zhuang Jiang
School of Earth and Space Sciences, University of Science and Technology of China, Hefei, Anhui, China
Becky Alexander
Department of Atmospheric Sciences, University of Washington, Seattle WA, USA
Joel Savarino
IGE, Univ. Grenoble Alpes, CNRS, IRD, Grenoble INP, INRAE, Grenoble, France
School of Earth and Space Sciences, University of Science and Technology of China, Hefei, Anhui, China
Deep Space Exploration Laboratory, Hefei, Anhui, China
CAS Center for Excellence in Comparative Planetology, University of Science and Technology of China, Hefei, Anhui, China
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We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
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We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851, https://doi.org/10.5194/acp-16-13837-2016, https://doi.org/10.5194/acp-16-13837-2016, 2016
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This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Josué Bock, Joël Savarino, and Ghislain Picard
Atmos. Chem. Phys., 16, 12531–12550, https://doi.org/10.5194/acp-16-12531-2016, https://doi.org/10.5194/acp-16-12531-2016, 2016
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We develop a physically based parameterisation of the co-condensation process. Our model includes solid-state diffusion within a snow grain. It reproduces with good agreement the nitrate measurement in surface snow. Winter and summer concentrations are driven respectively by thermodynamic equilibrium and co-condensation. Adsorbed nitrate likely accounts for a minor part. This work shows that co-condensation is required to explain the chemical composition of snow undergoing temperature gradient.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
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
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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.
Alexandra Touzeau, Amaëlle Landais, Barbara Stenni, Ryu Uemura, Kotaro Fukui, Shuji Fujita, Sarah Guilbaud, Alexey Ekaykin, Mathieu Casado, Eugeni Barkan, Boaz Luz, Olivier Magand, Grégory Teste, Emmanuel Le Meur, Mélanie Baroni, Joël Savarino, Ilann Bourgeois, and Camille Risi
The Cryosphere, 10, 837–852, https://doi.org/10.5194/tc-10-837-2016, https://doi.org/10.5194/tc-10-837-2016, 2016
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The relationship between water isotope ratios and temperature is investigated in precipitation snow at Vostok and Dome C, as well as in surface snow along traverses. The temporal slope of the linear regression for the precipitation is smaller than the geographical slope. Thus, using the latter could lead to an underestimation of past temperature changes. The processes active at remote sites (best glacial analogs) are explored through a combination of water isotopes in short snow pits.
Michael Sigl, Tyler J. Fudge, Mai Winstrup, Jihong Cole-Dai, David Ferris, Joseph R. McConnell, Ken C. Taylor, Kees C. Welten, Thomas E. Woodruff, Florian Adolphi, Marion Bisiaux, Edward J. Brook, Christo Buizert, Marc W. Caffee, Nelia W. Dunbar, Ross Edwards, Lei Geng, Nels Iverson, Bess Koffman, Lawrence Layman, Olivia J. Maselli, Kenneth McGwire, Raimund Muscheler, Kunihiko Nishiizumi, Daniel R. Pasteris, Rachael H. Rhodes, and Todd A. Sowers
Clim. Past, 12, 769–786, https://doi.org/10.5194/cp-12-769-2016, https://doi.org/10.5194/cp-12-769-2016, 2016
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Here we present a chronology (WD2014) for the upper part (0–2850 m; 31.2 ka BP) of the West Antarctic Ice Sheet (WAIS) Divide ice core, which is based on layer counting of distinctive annual cycles preserved in the elemental, chemical and electrical conductivity records. We validated the chronology by comparing it to independent high-accuracy, absolutely dated chronologies. Given its demonstrated high accuracy, WD2014 can become a reference chronology for the Southern Hemisphere.
Maria Zatko, Lei Geng, Becky Alexander, Eric Sofen, and Katarina Klein
Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, https://doi.org/10.5194/acp-16-2819-2016, 2016
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We have incorporated an idealized snowpack with a nitrate photolysis parameterization into a global chemical transport model (GEOS-Chem) to examine the implications of snow nitrate photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core nitrate in ice cores across Antarctica and Greenland. We also examine the sensitivity of these processes to meteorological parameters and chemical, optical, and physical snow properties.
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
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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.
E. Gautier, J. Savarino, J. Erbland, A. Lanciki, and P. Possenti
Clim. Past, 12, 103–113, https://doi.org/10.5194/cp-12-103-2016, https://doi.org/10.5194/cp-12-103-2016, 2016
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We evaluate the local-scale variability of a sulfate profile at a low-accumulation site (Dome C, Antarctica) to assess the representativeness of one ice core for volcanic reconstructions. Peak statistical occurrence, depth and flux variability are evaluated from five cores. Due to local-scale variability, 64 volcanic peaks can be identified by a five-cores analysis, while only half of them can be assessed from two cores. Using five cores, the uncertainty of the mean flux is reduced to 29 %.
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
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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.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256, https://doi.org/10.5194/acp-15-11243-2015, https://doi.org/10.5194/acp-15-11243-2015, 2015
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In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
P. Achakulwisut, L. J. Mickley, L. T. Murray, A. P. K. Tai, J. O. Kaplan, and B. Alexander
Atmos. Chem. Phys., 15, 7977–7998, https://doi.org/10.5194/acp-15-7977-2015, https://doi.org/10.5194/acp-15-7977-2015, 2015
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The atmosphere’s oxidative capacity determines the lifetime of many trace gases important to climate, chemistry, and human health. Yet uncertainties remain about its past variations, its controlling factors, and the radiative forcing of short-lived species it influences. To reduce these uncertainties, we must better quantify the natural emissions and chemical reaction mechanisms of organic compounds in the atmosphere, which play a role in governing the oxidative capacity.
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
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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.
L. Geng, J. Cole-Dai, B. Alexander, J. Erbland, J. Savarino, A. J. Schauer, E. J. Steig, P. Lin, Q. Fu, and M. C. Zatko
Atmos. Chem. Phys., 14, 13361–13376, https://doi.org/10.5194/acp-14-13361-2014, https://doi.org/10.5194/acp-14-13361-2014, 2014
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Examinations on snowpit and firn core results from Summit, Greenland suggest that there are two mechanisms leading to the observed double nitrate peaks in some years in the industrial era: 1) long-rang transport of nitrate and 2) enhanced local photochemical production of nitrate. Both of these mechanisms are related to pollution transport, as the additional nitrate from either direct transport or enhanced local photochemistry requires enhanced nitrogen sources from anthropogenic emissions.
J.-C. Gallet, F. Domine, J. Savarino, M. Dumont, and E. Brun
The Cryosphere, 8, 1205–1215, https://doi.org/10.5194/tc-8-1205-2014, https://doi.org/10.5194/tc-8-1205-2014, 2014
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769, https://doi.org/10.5194/acp-14-5749-2014, https://doi.org/10.5194/acp-14-5749-2014, 2014
L. T. Murray, L. J. Mickley, J. O. Kaplan, E. D. Sofen, M. Pfeiffer, and B. Alexander
Atmos. Chem. Phys., 14, 3589–3622, https://doi.org/10.5194/acp-14-3589-2014, https://doi.org/10.5194/acp-14-3589-2014, 2014
Related subject area
Subject: Climate and Earth System | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Opinion: Exploring potential atmospheric methane removal approaches: an example research roadmap for chlorine radical enhancement
The carbon sink in China as seen from GOSAT with a regional inversion system based on the Community Multi-scale Air Quality (CMAQ) and ensemble Kalman smoother (EnKS)
Katrine A. Gorham, Sam Abernethy, Tyler R. Jones, Peter Hess, Natalie M. Mahowald, Daphne Meidan, Matthew S. Johnson, Maarten M. J. W. van Herpen, Yangyang Xu, Alfonso Saiz-Lopez, Thomas Röckmann, Chloe A. Brashear, Erika Reinhardt, and David Mann
EGUsphere, https://doi.org/10.22541/essoar.169755495.51174285/v1, https://doi.org/10.22541/essoar.169755495.51174285/v1, 2023
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Rapid reduction of atmospheric methane is needed to slow the rate of global warming. Reducing anthropogenic methane emissions is the top priority. However, atmospheric methane is also impacted by rising natural emissions and changing sinks. Study of possible atmospheric methane removal approaches, such as iron salt aerosols to increase the chlorine radical sink, benefit from a roadmapped approach to understand if there may be viable and socially acceptable ways to decrease future risk.
Xingxia Kou, Zhen Peng, Meigen Zhang, Fei Hu, Xiao Han, Ziming Li, and Lili Lei
Atmos. Chem. Phys., 23, 6719–6741, https://doi.org/10.5194/acp-23-6719-2023, https://doi.org/10.5194/acp-23-6719-2023, 2023
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A CMAQ EnSRF-based regional inversion system was extended to resolve satellite retrievals into biogenic source–sink changes. The size of the assimilated biosphere sink in China inferred from GOSAT was −0.47 Pg C yr−1. The biosphere flux at the provincial scale was re-estimated following the refined description in the regional inversion.
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Short summary
Ice-core nitrate could track the past atmospheric NOx and oxidant level, but its interpretation is hampered by the post-depositional processing. In this work, an inverse model was developed and tested against two polar sites and was shown to well reproduce the observed nitrate signals in snow and atmosphere, suggesting that the model can properly correct for the effect of post-depositional processing. This model offers a very useful tool for future studies on ice-core nitrate records.
Ice-core nitrate could track the past atmospheric NOx and oxidant level, but its interpretation...
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