Articles | Volume 15, issue 9
The Cryosphere, 15, 4207–4220, 2021
https://doi.org/10.5194/tc-15-4207-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
The Cryosphere, 15, 4207–4220, 2021
https://doi.org/10.5194/tc-15-4207-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
03 Sep 2021
Research article
| 03 Sep 2021
Impacts of the photo-driven post-depositional processing on snow nitrate and its isotopes at Summit, Greenland: a model-based study
Zhuang Jiang et al.
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Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-417, https://doi.org/10.5194/acp-2022-417, 2022
Preprint under review for ACP
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability of snow accumulation rate and its slight increase after the 1970s masked any signals caused by ozone hole. Meanwhile, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere Discuss., https://doi.org/10.5194/tc-2021-355, https://doi.org/10.5194/tc-2021-355, 2021
Revised manuscript accepted for TC
Short summary
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effects and which should be taken into account when interpreting ice-core nitrate isotope records.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-417, https://doi.org/10.5194/acp-2022-417, 2022
Preprint under review for ACP
Short summary
Short summary
We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability of snow accumulation rate and its slight increase after the 1970s masked any signals caused by ozone hole. Meanwhile, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Saehee Lim, Meehye Lee, Joel Savarino, and Paolo Laj
Atmos. Chem. Phys., 22, 5099–5115, https://doi.org/10.5194/acp-22-5099-2022, https://doi.org/10.5194/acp-22-5099-2022, 2022
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We determined δ15N(NO3−) and Δ17O(NO3−) of PM2.5 in Seoul during 2018–2019 and estimated quantitatively the contribution of oxidation pathways to NO3− formation and NOx emission sources. The nighttime pathway played a significant role in NO3− formation during the winter, and its contribution further increased up to 70 % on haze days when PM2.5 was greater than 75 µg m−3. Vehicle emissions were confirmed as a main NO3− source with an increasing contribution from coal combustion in winter.
Xueyin Ruan, Chun Zhao, Rahul A. Zaveri, Pengzhen He, Xinming Wang, Jingyuan Shao, and Lei Geng
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-62, https://doi.org/10.5194/gmd-2022-62, 2022
Revised manuscript under review for GMD
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Accurate prediction of aerosol pH in chemical transport models is essential to aerosol modeling. This study examines the performance of Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) on aerosol pH predictions and the sensitivities to emissions of nonvolatile cations and NH3, aerosol phase state assumption and heterogeneous sulfate production. Temporal evolution of aerosol pH during haze cycles in Beijing and the driving factors are also presented and discussed.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-44, https://doi.org/10.5194/acp-2022-44, 2022
Revised manuscript under review for ACP
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Radical bromine molecules are seen at higher concentrations during the Arctic Spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Albane Barbero, Joël Savarino, Roberto Grilli, Markus M. Frey, Camille Blouzon, Detlev Helmig, and Nicolas Caillon
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1018, https://doi.org/10.5194/acp-2021-1018, 2021
Revised manuscript under review for ACP
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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 suggests 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.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere Discuss., https://doi.org/10.5194/tc-2021-355, https://doi.org/10.5194/tc-2021-355, 2021
Revised manuscript accepted for TC
Short summary
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effects and which should be taken into account when interpreting ice-core nitrate isotope records.
Laura Crick, Andrea Burke, William Hutchison, Mika Kohno, Kathryn A. Moore, Joel Savarino, Emily A. Doyle, Sue Mahony, Sepp Kipfstuhl, James W. B. Rae, Robert C. J. Steele, R. Stephen J. Sparks, and Eric W. Wolff
Clim. Past, 17, 2119–2137, https://doi.org/10.5194/cp-17-2119-2021, https://doi.org/10.5194/cp-17-2119-2021, 2021
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The ~ 74 ka eruption of Toba was one of the largest eruptions of the last 100 ka. We have measured the sulfur isotopic composition for 11 Toba eruption candidates in two Antarctic ice cores. Sulfur isotopes allow us to distinguish between large eruptions that have erupted material into the stratosphere and smaller ones that reach lower altitudes. Using this we have identified the events most likely to be Toba and place the eruption on the transition into a cold period in the Northern Hemisphere.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, and Nicolas Caillon
Atmos. Chem. Phys., 21, 10477–10497, https://doi.org/10.5194/acp-21-10477-2021, https://doi.org/10.5194/acp-21-10477-2021, 2021
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We report an efficient method to collect atmospheric NO2 adapted for multi-isotopic analysis and present the first NO2 triple oxygen and double nitrogen isotope measurements. Atmospheric samplings carried out in Grenoble, France, highlight the NO2 isotopic signature sensitivity to the local NOx emissions and chemical regimes. These preliminary results are very promising for using the combination of Δ17O and δ15N of NO2 as a probe of the atmospheric NOx emissions and chemistry.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Albane Barbero, Camille Blouzon, Joël Savarino, Nicolas Caillon, Aurélien Dommergue, and Roberto Grilli
Atmos. Meas. Tech., 13, 4317–4331, https://doi.org/10.5194/amt-13-4317-2020, https://doi.org/10.5194/amt-13-4317-2020, 2020
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In this paper, we present a compact, affordable and robust instrument for in situ measurements of different trace gases: NOx, IO, CHOCHO and O3 with very low detection limits. The device weighs 15 kg and has a total electrical power consumption of < 300 W. Its very low detection limits and its design make it suitable for field applications to address different questions such as how to better constrain the oxidative capacity of the atmosphere and study the chemistry of highly reactive species.
Jiayue Huang, Lyatt Jaeglé, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mat J. Evans, Nicolas Theys, and Sungyeon Choi
Atmos. Chem. Phys., 20, 7335–7358, https://doi.org/10.5194/acp-20-7335-2020, https://doi.org/10.5194/acp-20-7335-2020, 2020
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Large-scale enhancements of tropospheric BrO and the depletion of surface ozone are often observed in the springtime Arctic. Here, we use a chemical transport model to examine the role of sea salt aerosol from blowing snow in explaining these phenomena. We find that our simulation can account for the spatiotemporal variability of satellite observations of BrO. However, the model has difficulty in producing the magnitude of observed ozone depletion events.
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
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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.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
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Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Detlev Helmig, Daniel Liptzin, Jacques Hueber, and Joel Savarino
The Cryosphere, 14, 199–209, https://doi.org/10.5194/tc-14-199-2020, https://doi.org/10.5194/tc-14-199-2020, 2020
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We present 15 months of trace gas observations from air withdrawn within the snowpack and from above the snow at Concordia Station in Antarctica. The data show occasional positive spikes, indicative of pollution from the station generator. The pollution signal can be seen in snowpack air shortly after it is observed above the snow surface, and lasting for up to several days, much longer than above the surface.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Jingyuan Shao, Qianjie Chen, Yuxuan Wang, Xiao Lu, Pengzhen He, Yele Sun, Viral Shah, Randall V. Martin, Sajeev Philip, Shaojie Song, Yue Zhao, Zhouqing Xie, Lin Zhang, and Becky Alexander
Atmos. Chem. Phys., 19, 6107–6123, https://doi.org/10.5194/acp-19-6107-2019, https://doi.org/10.5194/acp-19-6107-2019, 2019
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Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Tommaso Galeazzo, Slimane Bekki, Erwan Martin, Joël Savarino, and Stephen R. Arnold
Atmos. Chem. Phys., 18, 17909–17931, https://doi.org/10.5194/acp-18-17909-2018, https://doi.org/10.5194/acp-18-17909-2018, 2018
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Volcanic sulfur can have climatic impacts for the planet via sulfate aerosol formation, leading also to pollution events. We provide model constraints on tropospheric volcanic sulfate formation, with implications for its lifetime and impacts on regional air quality. Oxygen isotope investigations from our model suggest that in the poor tropospheric plumes of halogens, the O2/TMI sulfur oxidation pathway might significantly control sulfate production. The produced sulfate has no isotopic anomaly.
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840, https://doi.org/10.5194/acp-18-15825-2018, https://doi.org/10.5194/acp-18-15825-2018, 2018
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Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
Qianjie Chen, Tomás Sherwen, Mathew Evans, and Becky Alexander
Atmos. Chem. Phys., 18, 13617–13637, https://doi.org/10.5194/acp-18-13617-2018, https://doi.org/10.5194/acp-18-13617-2018, 2018
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Uncertainty in the natural tropospheric sulfur cycle represents the largest source of uncertainty in radiative forcing estimates of sulfate aerosol. This study investigates the natural sulfur cycle in the marine troposphere using the GEOS-Chem model. We found that BrO is important for DMS oxidation and multiphase chemistry is important for MSA production and loss, which have implications for the yield of SO2 and MSA from DMS oxidation and the radiative effect of DMS-derived sulfate aerosol.
Prasad Kasibhatla, Tomás Sherwen, Mathew J. Evans, Lucy J. Carpenter, Chris Reed, Becky Alexander, Qianjie Chen, Melissa P. Sulprizio, James D. Lee, Katie A. Read, William Bloss, Leigh R. Crilley, William C. Keene, Alexander A. P. Pszenny, and Alma Hodzic
Atmos. Chem. Phys., 18, 11185–11203, https://doi.org/10.5194/acp-18-11185-2018, https://doi.org/10.5194/acp-18-11185-2018, 2018
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Recent measurements of NOx and HONO suggest that photolysis of particulate nitrate in sea-salt aerosols is important in terms of marine boundary layer oxidant chemistry. We present the first global-scale assessment of the significance of this new chemical pathway for NOx, O3, and OH in the marine boundary layer. We also present a preliminary assessment of the potential impact of photolysis of particulate nitrate associated with other aerosol types on continental boundary layer chemistry.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528, https://doi.org/10.5194/acp-18-5515-2018, https://doi.org/10.5194/acp-18-5515-2018, 2018
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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
Discipline: Snow | Subject: Snow Chemistry
Temporal variation of bacterial community and nutrients in Tibetan glacier snowpack
Atmospheric and snow nitrate isotope systematics at Summit, Greenland: the reality of the post-depositional effect
Brief communication: Spatial and temporal variations in surface snow chemistry along a traverse from coastal East Antarctica to the ice sheet summit (Dome A)
Brief communication: An alternative method for estimating the scavenging efficiency of black carbon by meltwater over sea ice
Quantifying the light absorption and source attribution of insoluble light-absorbing particles on Tibetan Plateau glaciers between 2013 and 2015
Mercury in the Arctic tundra snowpack: temporal and spatial concentration patterns and trace gas exchanges
Variability of sea salts in ice and firn cores from Fimbul Ice Shelf, Dronning Maud Land, Antarctica
Yuying Chen, Keshao Liu, Yongqin Liu, Trista J. Vick-Majors, Feng Wang, and Mukan Ji
The Cryosphere, 16, 1265–1280, https://doi.org/10.5194/tc-16-1265-2022, https://doi.org/10.5194/tc-16-1265-2022, 2022
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We investigated the bacterial communities in surface and subsurface snow samples in a Tibetan Plateau glacier using 16S rRNA gene sequences. Our results revealed rapid temporal changes in nitrogen (including nitrate and ammonium) and bacterial communities in both surface and subsurface snow. These findings advance our understanding of bacterial community variations and bacterial interactions after snow deposition and provide a possible biological explanation for nitrogen dynamics in snow.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere Discuss., https://doi.org/10.5194/tc-2021-355, https://doi.org/10.5194/tc-2021-355, 2021
Revised manuscript accepted for TC
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effects and which should be taken into account when interpreting ice-core nitrate isotope records.
Guitao Shi, Hongmei Ma, Zhengyi Hu, Zhenlou Chen, Chunlei An, Su Jiang, Yuansheng Li, Tianming Ma, Jinhai Yu, Danhe Wang, Siyu Lu, Bo Sun, and Meredith G. Hastings
The Cryosphere, 15, 1087–1095, https://doi.org/10.5194/tc-15-1087-2021, https://doi.org/10.5194/tc-15-1087-2021, 2021
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It is important to understand atmospheric chemistry over Antarctica under a changing climate. Thus snow collected on a traverse from the coast to Dome A was used to investigate variations in snow chemistry. The non-sea-salt fractions of K+, Mg2+, and Ca2+ are associated with terrestrial inputs, and nssCl− is from HCl. In general, proportions of non-sea-salt fractions of ions to the totals are higher in the interior areas than on the coast, and the proportions are higher in summer than in winter.
Tingfeng Dou, Zhiheng Du, Shutong Li, Yulan Zhang, Qi Zhang, Mingju Hao, Chuanjin Li, Biao Tian, Minghu Ding, and Cunde Xiao
The Cryosphere, 13, 3309–3316, https://doi.org/10.5194/tc-13-3309-2019, https://doi.org/10.5194/tc-13-3309-2019, 2019
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The meltwater scavenging coefficient (MSC) determines the BC enrichment in the surface layer of melting snow and therefore modulates the BC-snow-albedo feedbacks. This study presents a new method for MSC estimation over the sea-ice area in Arctic. Using this new method, we analyze the spatial variability of MSC in the western Arctic and demonstrate that the value in Canada Basin (23.6 % ± 2.1 %) ≈ that in Greenland (23.0 % ± 12.5 %) > that in Chukchi Sea (17.9 % ± 5.0 %) > that in Elson Lagoon (14.5 % ± 2.6 %).
Xin Wang, Hailun Wei, Jun Liu, Baiqing Xu, Mo Wang, Mingxia Ji, and Hongchun Jin
The Cryosphere, 13, 309–324, https://doi.org/10.5194/tc-13-309-2019, https://doi.org/10.5194/tc-13-309-2019, 2019
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A large survey on measuring optical and chemical properties of insoluble light-absorbing impurities (ILAPs) from seven glaciers was conducted on the Tibetan Plateau (TP) during 2013–2015. The results indicated that the mixing ratios of black carbon (BC), organic carbon (OC), and iron (Fe) all showed a tendency to decrease from north to south, and the industrial pollution (33.1 %), biomass and biofuel burning (29.4 %), and soil dust (37.5 %) were the major sources of the ILAPs on the TP.
Yannick Agnan, Thomas A. Douglas, Detlev Helmig, Jacques Hueber, and Daniel Obrist
The Cryosphere, 12, 1939–1956, https://doi.org/10.5194/tc-12-1939-2018, https://doi.org/10.5194/tc-12-1939-2018, 2018
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In this study, we investigated mercury dynamics in an interior arctic tundra at Toolik Field Station (200 km from the Arctic Ocean) during two full snow seasons. We continuously measured atmospheric, snow gas phase, and soil pores mercury concentrations. We observed consistent concentration declines from the atmosphere to snowpack to soils, indicating that soils are continuous sinks of mercury. We suggest that interior arctic snowpacks may be negligible sources of mercury.
Carmen Paulina Vega, Elisabeth Isaksson, Elisabeth Schlosser, Dmitry Divine, Tõnu Martma, Robert Mulvaney, Anja Eichler, and Margit Schwikowski-Gigar
The Cryosphere, 12, 1681–1697, https://doi.org/10.5194/tc-12-1681-2018, https://doi.org/10.5194/tc-12-1681-2018, 2018
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Ions were measured in firn and ice cores from Fimbul Ice Shelf, Antarctica, to evaluate sea-salt loads. A significant sixfold increase in sea salts was found in the S100 core after 1950s which suggests that it contains a more local sea-salt signal, dominated by processes during sea-ice formation in the neighbouring waters. In contrast, firn cores from three ice rises register the larger-scale signal of atmospheric flow conditions and transport of sea-salt aerosols produced over open water.
Cited articles
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Dibb, J. E., Arsenault, M., Peterson, M. C., and Honrath, R. E.: Fast nitrogen oxide photochemistry in Summit, Greenland snow, Atmos. Environ, 36, 2501–2511, https://doi.org/10.1016/S1352-2310(02)00130-9, 2002.
Dibb, J. E., Whitlow, S. I., and Arsenault, M.: Seasonal variations in the soluble ion content of snow at Summit. Greenland: Constraints from three years of daily surface snow samples, Atmos. Environ., 41, 5007–5019, https://doi.org/10.1016/j.atmosenv.2006.12.010, 2007.
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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.
Erbland, J., Savarino, J., Morin, S., France, J. L., Frey, M. M., and King, M. D.: Air–snow transfer of nitrate on the East Antarctic Plateau – Part 2: An isotopic model for the interpretation of deep ice-core records, Atmos. Chem. Phys., 15, 12079–12113, https://doi.org/10.5194/acp-15-12079-2015, 2015.
Fibiger, D. L., Hastings, M. G., Dibb, J. E., and Huey, L. G.: The
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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.
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Noro, K., Hattori, S., Uemura, R., Fukui, K., Hirabayashi, M., Kawamura, K., Motoyama, H., Takenaka, N., and Yoshida, N.: Spatial variation of isotopic compositions of snowpack nitrate related to post-depositional processes in eastern Dronning Maud Land, East Antarctica, Geochem. J., 52, e7–e14, https://doi.org/10.2343/geochemj.2.0519, 2018.
Shi, G., Buffen, A. M., Hastings, M. G., Li, C., Ma, H., Li, Y., Sun, B., An, C., and Jiang, S.: Investigation of post-depositional processing of nitrate in East Antarctic snow: isotopic constraints on photolytic loss, re-oxidation, and source inputs, Atmos. Chem. Phys., 15, 9435–9453, https://doi.org/10.5194/acp-15-9435-2015, 2015.
Sjostedt, S. J., Huey, L. G., Tanner, D. J., Peischl, J., Chen, G., Dibb, J. E., Lefer, B., Hutterli, M. A., Beyersdorf, A. J., Blake, N. J., Blake, D. R., Sueper, D., Ryerson, T., Burkhart, J., and Stohl, A.: Observations of hydroxyl and the sum of peroxy radicals at Summit, Greenland during summer 2003, Atmos. Environ., 41, 5122–5137, https://doi.org/10.1016/j.atmosenv.2006.06.065, 2007.
Thomas, J. L., Dibb, J. E., Huey, L. G., Liao, J., Tanner, D., Lefer, B., von Glasow, R., and Stutz, J.: Modeling chemistry in and above snow at Summit, Greenland – Part 2: Impact of snowpack chemistry on the oxidation capacity of the boundary layer, Atmos. Chem. Phys., 12, 6537–6554, https://doi.org/10.5194/acp-12-6537-2012, 2012.
Vicars, W. C. and Savarino, J.: Quantitative constraints on the 17O-excess (Δ17O) signature of surface ozone: Ambient measurements from 50∘ N to 50∘ S using the nitrite-coated filter technique, Geochim. Cosmochim. Ac., 135, 270–287, https://doi.org/10.1016/j.gca.2014.03.023, 2014.
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.
Zatko, M., Geng, L., Alexander, B., Sofen, E., and Klein, K.: The impact of snow nitrate photolysis on boundary layer chemistry and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland in a global chemical transport model, Atmos. Chem. Phys., 16, 2819–2842, https://doi.org/10.5194/acp-16-2819-2016, 2016.
Zatko, M. C., Grenfell, T. C., Alexander, B., Doherty, S. J., Thomas, J. L., and Yang, X.: The influence of snow grain size and impurities on the vertical profiles of actinic flux and associated NOx emissions on the Antarctic and Greenland ice sheets, Atmos. Chem. Phys., 13, 3547–3567, https://doi.org/10.5194/acp-13-3547-2013, 2013.
Short summary
We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at...
