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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 12 Sep 2018

Research article | 12 Sep 2018

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

Seasonal study of stable carbon and nitrogen isotopic composition in fine aerosols at a Central European rural background station

Petr Vodička1,2, Kimitaka Kawamura1, Jaroslav Schwarz2, Bhagawati Kunwar1, and Vladimír Ždímal2 Petr Vodička et al.
  • 1Chubu Institute for Advanced Studies, Chubu University, 1200 Matsumoto-cho, Kasugai 487–8501, Japan
  • 2Institute of Chemical Process Fundamentals of the Czech Academy of Science, Rozvojová 2/135, 165 02, Prague 6, Czech Republic

Abstract. Determinations of stable carbon isotope ratios (δ13C) of total carbon (TC) and nitrogen isotope ratios (δ15N) of total nitrogen (TN) were carried out for fine aerosol particles (PM1) collected on a daily basis at a rural background site in Košetice (Central Europe) between 27 September 2013 and 9 August 2014 (n=146). We found a seasonal pattern for both δ13C and δ15N. The seasonal variation in δ15N was more pronounced, with 15N-depleted values (av. 13.1±4.5‰) in winter and 15N-enriched values (25.0±1.6‰) in summer. Autumn and spring are transition periods when the isotopic composition gradually changed due to different sources and the ambient temperature. The seasonal variation in δ13C was less pronounced but more depleted in 13C in summer (−27.8±0.4‰) compared to winter (−26.7±0.5‰).

Major controls of the seasonal dependencies were found based on a comparative analysis with water-soluble ions, organic carbon, elemental carbon, trace gases and meteorological parameters (mainly ambient temperature). A comparison of δ15N with NO3, NH4+ and organic nitrogen (OrgN) revealed that although a higher content of NO3 was associated with a decrease in δ15N values in TN, NH4+ and OrgN had the opposite influences. The highest concentrations of nitrate, mainly represented by NH4NO3, originated from the emissions from biomass burning, leading to lower δ15N values of approximately 14‰ in winter. During spring, the percentage of NO3 in PM1 decreased, and 15N enrichment was probably driven by equilibrium exchange between the gas and aerosol phases (NH3(g)NH4+(p)) as supported by the increased ambient temperature. This equilibrium was suppressed in early summer when the NH4+/SO42− molar ratios reached 2, and nitrate partitioning in aerosol was negligible. During summer, kinetic reactions probably were the primary processes as opposed to gas-aerosol equilibrium on a nitrogen level. However, summertime δ15N values were some of the highest observed, probably suggesting the aging of ammonium sulfate and OrgN aerosols. Such aged aerosols can be coated by organics in which 13C enrichment takes place by photooxidation process. This result was supported by the positive correlation of δ13C with temperature and ozone, as observed in the summer season.

During winter, we observed an event with the lowest δ15N and highest δ13C values. The winter Event was connected with prevailing southeast winds. Although higher δ13C values probably originated from biomass burning particles, the lowest δ15N values were associated with agriculture emissions of NH3 under low temperature conditions that were below 0°C.

Petr Vodička et al.
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Petr Vodička et al.
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Short summary
Measurements of stable carbon and nitrogen isotopic compositions in the PM1 atmospheric aerosol provide partial insight into the possible sources of aerosol at this station but mainly offers a deeper insight into the physical and chemical processes taking place between the gas phase and particulate matter. These processes are probably valid in general (not only at this site), especially for nitrogen compounds.
Measurements of stable carbon and nitrogen isotopic compositions in the PM1 atmospheric aerosol...