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Air–snow Transfer of Nitrate on the East Antarctic Plateau – Part 2: an Isotopic Model for the Interpretation of Deep Ice-core Records : Volume 15, Issue 5 (10/03/2015)

By Erbland, J.

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Book Id: WPLBN0003997185
Format Type: PDF Article :
File Size: Pages 80
Reproduction Date: 2015

Title: Air–snow Transfer of Nitrate on the East Antarctic Plateau – Part 2: an Isotopic Model for the Interpretation of Deep Ice-core Records : Volume 15, Issue 5 (10/03/2015)  
Author: Erbland, J.
Volume: Vol. 15, Issue 5
Language: English
Subject: Science, Atmospheric, Chemistry
Collections: Periodicals: Journal and Magazine Collection, Copernicus GmbH
Historic
Publication Date:
2015
Publisher: Copernicus Gmbh, Göttingen, Germany
Member Page: Copernicus Publications

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Morin, S., King, M. D., France, J. L., Savarino, J., Frey, M. M., & Erbland, J. (2015). Air–snow Transfer of Nitrate on the East Antarctic Plateau – Part 2: an Isotopic Model for the Interpretation of Deep Ice-core Records : Volume 15, Issue 5 (10/03/2015). Retrieved from http://community.ebooklibrary.org/


Description
Description: Université Grenoble Alpes, LGGE, 38000 Grenoble, France. Unraveling the modern budget of reactive nitrogen on the Antarctic plateau is critical for the interpretation of ice core records of nitrate. This requires accounting for nitrate recycling processes occurring in near surface snow and the overlying atmospheric boundary layer. Not only concentration measurements, but also isotopic ratios of nitrogen and oxygen in nitrate, provide constraints on the processes at play. However, due to the large number of intertwined chemical and physical phenomena involved, numerical modelling is required to test hypotheses in a~quantitative manner. Here we introduce the model TRansfer of Atmospheric Nitrate Stable Isotopes To the Snow (TRANSITS), a~novel conceptual, multi-layer and one-dimensional model representing the impact of processes operating on nitrate at the air–snow interface on the East Antarctic plateau, in terms of concentrations (mass fraction) and the nitrogen (δ15N) and oxygen isotopic composition (17O}-excess, Δ17O) in nitrate. At the air–snow interface at Dome C (DC, 75°06' S, 123°19' E), the model reproduces well the values of δ15N in atmospheric and surface snow (skin layer) nitrate as well as in the δ15N profile in DC snow including the observed extraordinary high positive values (around +300 ‰) below 20 \unit{cm}. The model also captures the observed variability in nitrate mass fraction in the snow. While oxygen data are qualitatively reproduced at the air–snow interface at DC and in East Antarctica, the simulated Δ17O values underestimate the observed Δ17O values by a~few~‰. This is explained by the simplifications made in the description of the atmospheric cycling and oxidation of NO2. The model reproduces well the sensitivity of δ15N, Δ17O and the apparent fractionation constants (15ϵapp, 17Eapp) to the snow accumulation rate. Building on this development, we propose a~framework for the interpretation of nitrate records measured from ice cores. Measurement of nitrate mass fractions and δ15N in the nitrate archived in an ice core, may be used to derive information about past variations in the total ozone column and/or the primary inputs of nitrate above Antarctica as well as in nitrate trapping efficiency (defined as the ratio between the archived nitrate flux and the primary nitrate input flux). The Δ17O of nitrate could then be corrected from the impact of cage recombination effects associated with the photolysis of nitrate in snow. Past changes in the relative contributions of the Δ17O in the primary inputs of nitrate and the Δ17O in the locally cycled NO2 could then be determined. Therefore, information about the past variations in the local and long range processes operating on reactive nitrogen species could be obtained from ice cores collected in low accumulation regions such as the Antarctic plateau.

Summary
Air–snow transfer of nitrate on the East Antarctic plateau – Part 2: An isotopic model for the interpretation of deep ice-core records

Excerpt
Alexander, B., Hastings, M. G., Allman, D. J., Dachs, J., Thornton, J. A., and Kunasek, S. A.: Quantifying atmospheric nitrate formation pathways based on a global model of the oxygen isotopic composition ($\Delta ^17$O) of atmospheric nitrate, Atmos. Chem. Phys., 9, 5043–5056, doi:10.5194/acp-9-5043-2009, 2009.; Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., and Troe, J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I – gas phase reactions of Ox, HOx, NOx and SOx species, Atmos. Chem. Phys., 4, 1461–1738, doi:10.5194/acp-4-1461-2004, 2004.; Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., Troe, J., and IUPAC Subcommittee: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II – gas phase reactions of organic species, Atmos. Chem. Phys., 6, 3625–4055, doi:10.5194/acp-6-3625-2006, 2006.; Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., and Troe, J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume III – gas phase reactions of inorganic halogens, Atmos. Chem. Phys., 7, 981–1191, doi:10.5194/acp-7-981-2007, 2007.; Berhanu, T. A., Meusinger, C., Erbland, J., Jost, R., Bhattacharya, S. K., Johnson, M. S., and Savarino, J.: Laboratory study of nitrate photolysis in Antarctic snow. II. Isotope effects and wavelength dependence, J. Chem. Phys., 140, 244306, doi:10.1063/1.4882899, 2014a.; Berhanu, T. A., Savarino, J., Erbland, J., Vicars, W. C., Preunkert, S., Martins, J. F., and Johnson, M. S.: Isotopic effects of nitrate photochemistry in snow: a field study at Dome C, Antarctica, Atmos. Chem. Phys. Discuss., 14, 33045–33088, doi:10.5194/acpd-14-33045-2014, 2014b.; Blunier, T., Floch, G. L., Jacobi, H.-W., and Quansah, E.: Isotopic view on nitrate loss in Antarctic surface snow, Geophys. Res. Lett., 32, L13501, doi:10.1029/2005GL023011, 2005.; 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, doi:10.5194/acp-8-4855-2008, 2008.; Legrand, M. R. and Delmas, R. J.: Relative contributions of tropospheric and stratospheric sources to nitrate in Antarctic snow, Tellus B, 38, 236–249, 1986.; Brizzi, G., Arnone, E., Carlotti, M., Dinelli, B. M., Flaud, J.-M., Papandrea, E., Perrin, A., and Ridolfi, M.: Retrieval of atmospheric $\chemH^{15NO_3}/\chemH^{14NO_3}$ isotope ratio profile from MIPAS/ENVISAT limb-scanning measurements, J. Geophys. Res., 114, D16301, doi:10.1029/2008JD011504, 2009.; Chance, K. and Kurucz, R. L.: An improved high-resolution solar reference spectrum for Earth's atmosphere measurements in the ultraviolet, visible, and near infrared, J. Quant. Spectrosc. Ra., 111, 1289–1295, 2010.; Chu, L. and Anastasio, C.: Quantum yields of hydroxyl radical and nitrogen dioxide from the photolysis of nitrate on ice, J. Phys. Chem. A, 107, 9594–9602, 2003.; Chu, L. and Anastasio, C.: Temperature and wavelength depen- dence of nitrite photolysis in frozen and aqueous solutions, Environ. Sci. Technol., 41, 3

 

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