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© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 10 Dec 2018

Research article | 10 Dec 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Isotopic Constraints on the Atmospheric Sources and Formation of Nitrogenous Species in Biomass-Burning-Influenced Clouds

Yunhua Chang1, Yanlin Zhang1, Jiarong Li2, Chongguo Tian3, Linlin Song4, Xiaoyao Zhai1, Wenqi Zhang1, Tong Huang1, Yu-Chi Lin1, Chao Zhu2, Yunting Fang4, Moritz F. Lehmann5, and Jianmin Chen2 Yunhua Chang et al.
  • 1Yale-NUIST Center on Atmospheric Environment, Nanjing University of Information Science & Technology, Nanjing 210044, China
  • 2Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Institute of Atmospheric Sciences, Fudan University, Shanghai 200433, China
  • 3Key Laboratory of Coastal Environmental Processes and Ecological Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai 264003, China
  • 4CAS Key Laboratory of Forest Ecology and Management, Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang 110016, China
  • 5Aquatic and Isotope Biogeochemistry, Department of Environmental Sciences, University of Basel, Basel 4056, Switzerland

Abstract. The interpretation of tropospheric cloud formation rests on understanding the sources and processes affecting aerosol constituents of the atmosphere that are preserved in cloudwater. However, this challenge is difficult to be quantitatively addressed based on the sole use of bulk chemical properties. Nitrogenous aerosols, mainly ammonium (NH4+) and nitrate (NO3), play an important role in tropospheric cloud formation. Here we collected cloudwater samples at the summit of Mt. Tai (1545 m above sea level) in Eastern China during a long-lasting biomass burning (BB) event, and measured for the first time the isotopic compositions (mean ± 1σ) of cloudwater nitrogen species (δ15N-NH4+ = −6.53 ± 4.96 ‰, δ15N-NO3 = −2.35 ± 2.00 ‰, δ18O-NO3 = 57.80 ± 4.23 ‰), allowing insights into their sources and potential transformation mechanism within the clouds. Large contributions of BB to the cloudwater NH4+ (32.9 ± 4.6 %) and NO3 (28.2 ± 2.7 %) inventories were confirmed through a Bayesian isotopic mixing model, coupled with our newly-developed computational quantum chemistry module. Despite an overall reduction in total anthropogenic NOx emission due to effective emission control actions and stricter emission standards for vehicles, the observed cloud δ15N-NO3 values suggest that NOx emissions from transportation may have exceeded emissions from coal combustion. δ18O-NO3 values imply that the reaction of OH with NO2 is the dominant pathway of NO3 formation (57 ± 11 %), yet the contribution of heterogeneous hydrolysis of dinitrogen pentoxide was almost as important (43 ± 11 %).

Yunhua Chang et al.
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Status: final response (author comments only)
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Yunhua Chang et al.
Yunhua Chang et al.
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Short summary
The present work underscores the value of cloudwater dissolved inorganic nitrogen isotopes as carrier of quantitative information on regional NOx and NH3 emissions. It sheds light on the origin and production pathways of nitrogenous species in clouds and emphasizes the importance of biomass burning-derived nitrogenous species as cloud condensation nuclei in China’s troposphere. Moreover, it highlights the rapid evolution of NOx emissions in China.
The present work underscores the value of cloudwater dissolved inorganic nitrogen isotopes as...