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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
© Author(s) 2017. This work is distributed under
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Research article
09 May 2017
Review status
This discussion paper is a preprint. A revision of this manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.
Investigation of global nitrate from the AeroCom Phase III experiment
Huisheng Bian1,2, Mian Chin2, Didier A. Hauglustaine3, Michael Schulz4, Gunnar Myhre5,6, Susanne E. Bauer7,8, Marianne T. Lund6, Vlassis A. Karydis9, Tom L. Kucsera10, Xiaohua Pan11, Andrea Pozzer9, Ragnhild B. Skeie6, Stephen D. Steenrod10, Kengo Sudo12, Kostas Tsigaridis7,8, Alexandra P. Tsimpidi9, and Svetlana G. Tsyro4 1Joint Center for Environmental Technology UMBC, Baltimore, MD, USA
2Laboratory for Atmospheres, NASA Goddard Space Flight Center, Greenbelt, MD, USA
3Laboratoire des Sciences du Climat et de l'Environnement (LSCE), UMR8212, CEA-CNRS-UVSQ, Gif-sur-Yvette, France
4Norwegian Meteorological Institute, Blindern, Norway
5Department of Geosciences, University of Oslo, Oslo, Norway
6Center for International Climate and Environmental Research – Oslo, Oslo, Norway
7The Earth Institute, Center for Climate Systems Research, Columbia University, New York, USA
8NASA Goddard Institute for Space Studies, New York, USA
9Max Planck Institute for Chemistry, 55128 Mainz, Germany
10Universities Space Research Association, GESTAR, Columbia, MD, USA
11School of Computer, Mathematical and Natural Sciences, Morgan State University, Baltimore, MD, USA
12Center for Climate System Research, University of Tokyo, Tokyo, Japan
Abstract. An assessment of global nitrate and ammonium aerosol based on simulations from nine models participating in the AeroCom Phase III study is presented. A budget analyses was conducted to understand the typical magnitude, distribution, and diversity of the aerosols and their precursors among the models. To gain confidence on model performance, the model results were evaluated with various observations globally, including ground station measurements over North America, Europe, and East Asia for tracer concentrations and dry and wet depositions, as well as with aircraft measurements in the Northern Hemisphere mid-high latitudes for tracer vertical distributions. Given the unique chemical and physical features of the nitrate occurrence, we further investigated the similarity and differentiation among the models by examining: (1) the pH-dependent NH3 wet deposition; (2) the nitrate formation via heterogeneous chemistry on the surface of dust and sea-salt particles; and (3) the nitrate coarse mode fraction (i.e., coarse/total). It is found that HNO3, which is simulated explicitly based on full O3–HOx–NOx–aerosol chemistry by all models, differs by up to a factor of 9 among the models in its global tropospheric burden. This partially contributes to a large difference in NO3, whose atmospheric burden differs by up to a factor of 13. Analyses at the process level show that the large diversity in atmospheric burdens of NO3, NH3, and NH4+ is also related to deposition processes. Wet deposition seems to be the dominant process in determining the diversity in NH3 and NH4+ lifetimes. It is critical to correctly account for contributions of heterogeneous chemical production of nitrate on dust and sea-salt, because this process overwhelmingly controls atmospheric nitrate production (typically > 80 %) and determines the coarse and fine mode distribution of nitrate aerosol.

Citation: Bian, H., Chin, M., Hauglustaine, D. A., Schulz, M., Myhre, G., Bauer, S. E., Lund, M. T., Karydis, V. A., Kucsera, T. L., Pan, X., Pozzer, A., Skeie, R. B., Steenrod, S. D., Sudo, K., Tsigaridis, K., Tsimpidi, A. P., and Tsyro, S. G.: Investigation of global nitrate from the AeroCom Phase III experiment, Atmos. Chem. Phys. Discuss.,, in review, 2017.
Huisheng Bian et al.
Interactive discussionStatus: closed
AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment
Printer-friendly Version - Printer-friendly version      Supplement - Supplement
RC1: 'review of Bian et al.', Anonymous Referee #1, 14 Jun 2017 Printer-friendly Version 
RC2: 'Review of Bian et al. Nitrate AEROCOM Comparison', Anonymous Referee #2, 04 Jul 2017 Printer-friendly Version 
AC1: 'Response letter', Huisheng Bian, 19 Jul 2017 Printer-friendly Version 
AC2: 'acp-2017-359-RR.pdf', Huisheng Bian, 22 Aug 2017 Printer-friendly Version Supplement 
Huisheng Bian et al.
Huisheng Bian et al.


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Short summary
Atmospheric nitrate contributes notably to total aerosol mass in the present-day and is likely to be more important over the century with a projected decline in SO2 and NOx emissions and increase in NH3 emissions. This manuscript investigates atmospheric nitrate using multiple global models and measurements. The study is part of the AeroCom phase III activity. The study is the first attempt to look at global atmospheric nitrate simulation at physical and chemical process levels.
Atmospheric nitrate contributes notably to total aerosol mass in the present-day and is likely...