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Discussion papers
https://doi.org/10.5194/acp-2019-736
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-736
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 06 Jan 2020

Submitted as: research article | 06 Jan 2020

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

FTIR time series of tropospheric HCN in eastern China: seasonality, interannual variability and source attribution

Youwen Sun1, Cheng Liu1,2,3,4,5, Lin Zhang6, Mathias Palm7, Justus Notholt7, Hao Yin1, Corinne Vigouroux8, Erik Lutsch9, Wei Wang1, Changong Shan1, Thomas Blumenstock10, Tomoo Nagahama11, Isamu Morino12, Emmanuel Mahieu13, Kimberly Strong9, Bavo Langerock8, Martine De Maziere8, Qihou Hu1, Huifang Zhang1, Christoph Petri7, and Jianguo Liu1 Youwen Sun et al.
  • 1Key Laboratory of Environmental Optics and Technology, Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Hefei 230031,China
  • 2Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, China
  • 3University of Science and Technology of China, Hefei, 230026, China
  • 4Key Laboratory of Precision Scientific Instrumentation of Anhui Higher Education Institutes, University of Science and Technology of China
  • 5Anhui Province Key Laboratory of Polar Environment and Global Change, USTC, Hefei, 230026, China
  • 6Department of Atmospheric & Oceanic Sciences, Peking University, Beijing, 100871, China
  • 7University of Bremen, Institute of Environmental Physics, P.O. Box 330440, 28334 Bremen, Germany
  • 8Royal Belgian Institute for Space Aeronomy (BIRA-IASB), Brussels, Belgium
  • 9Department of Physics, University of Toronto, Toronto, Ontario, Canada
  • 10Karlsruhe Institute of Technology (KIT), Institute for Meteorology and Climate Research (IMK-ASF), Karlsruhe, Germany
  • 11Institute for Space-Earth Environmental Research (ISEE), Nagoya University, Nagoya, 464-8601, Japan
  • 12Satellite Observation Center, National Institute for Environmental Studies, Tsukuba, 305-8506, Japan
  • 13Institute of Astrophysics and Geophysics, University of Liège, Belgium

Abstract. We analyzed seasonality and interannual variability of tropospheric HCN column amounts in densely populated eastern China for the first time. The results were derived from solar absorption spectra recorded with ground-based high spectral resolution Fourier transform infrared (FTIR) spectrometer at Hefei (117°10′ E, 31°54′ N) between 2015 and 2018. The tropospheric HCN columns over Hefei, China showed significant seasonal variations with three monthly mean peaks throughout the year. The magnitude of the tropospheric HCN column peak in May > September > December. The tropospheric HCN column reached a maximum of (9.8 ± 0.78) × 1015 molecules/cm2 in May and a minimum of (7.16 ± 0.75) × 1015 molecules/cm2 in November. In most cases, the tropospheric HCN columns at Hefei (32° N) are higher than the FTIR observations at Ny Alesund (79° N), Kiruna (68° N), Bremen (53° N), Jungfraujoch (47° N), Toronto (44° N), Rikubetsu (43° N), Izana (28° N), Mauna Loa (20° N), La Reunion Maido (21° S), Lauder (45° S), and Arrival Heights (78° S) that are affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Enhancements of the tropospheric HCN columns were observed between September 2015 and July 2016 compared to the counterpart measurements in other years. The magnitude of the enhancement ranges from 5 to 46 % with an average of 22 %. Enhancement of tropospheric HCN (ΔHCN) is correlated with the coincident enhancement of tropospheric CO (ΔCO), indicating that enhancements of tropospheric CO and HCN were due to the same sources. The GEOS-Chem tagged CO simulation, the global fire maps and the PSCFs (Potential Source Contribution Function) calculated using back trajectories revealed that the seasonal maxima in May is largely due to the influence of biomass burning in South Eastern Asia (SEAS) (41 ± 13.1 %), Europe and Boreal Asia (EUBA) (21 ± 9.3 %) and Africa (AF) (22 ± 4.7 %). The seasonal maxima in September is largely due to the influence of biomass burnings in EUBA (38 ± 11.3 %), AF (26 ± 6.7 %), SEAS (14 ± 3.3 %), and Northern America (NA) (13.8 ± 8.4 %). For the seasonal maxima in December, dominant contributions are from AF (36 ± 7.1 %), EUBA (21 ± 5.2 %), and NA (18.7 ± 5.2 %). The tropospheric HCN enhancement between September 2015 and July 2016 at Hefei (32° N) were attributed to an elevated influence of biomass burnings in SEAS, EUBA, and Oceania (OCE) in this period. Particularly, an elevated fire number in OCE in the second half of 2015 dominated the tropospheric HCN enhancement in September–December 2015. An elevated fire number in SEAS in the first half of 2016 dominated the tropospheric HCN enhancement in January–July 2016.

Youwen Sun et al.
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Short summary
The first multiyear measurements of HCN in the polluted troposphere in densely populated eastern China have been presented here. The seasonality and interannual variability of tropospheric HCN columns have been investigated. The potential sources that drive the observed HCN seasonality and interannual variability were determined by using the GEOS-Chem tagged CO simulation, the global fire maps and the PSCFs (Potential Source Contribution Function) calculated using HYSPLIT back trajectories.
The first multiyear measurements of HCN in the polluted troposphere in densely populated eastern...
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