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Volume 17, issue 3 | Copyright
Atmos. Chem. Phys., 17, 1653-1672, 2017
https://doi.org/10.5194/acp-17-1653-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 02 Feb 2017

Research article | 02 Feb 2017

Contributions of nitrated aromatic compounds to the light absorption of water-soluble and particulate brown carbon in different atmospheric environments in Germany and China

Monique Teich1, Dominik van Pinxteren1, Michael Wang2, Simonas Kecorius1, Zhibin Wang1,a, Thomas Müller1, Griša Močnik3,4, and Hartmut Herrmann1 Monique Teich et al.
  • 1Leibniz Institute for Tropospheric Research, TROPOS, 04315 Leipzig, Germany
  • 2McMaster University, Hamilton, ON L8S 4L8, Canada
  • 3Aerosol d.o.o., 1000 Ljubljana, Slovenia
  • 4Condensed Physics Department, Jožef Stefan Institute, Ljubljana, Slovenia
  • anow at: Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany

Abstract. The relative contributions of eight nitrated aromatic compounds (NACs: nitrophenols and nitrated salicylic acids) to the light absorption of aqueous particle extracts and particulate brown carbon were determined from aerosol particle samples collected in Germany and China.

High-volume filter samples were collected during six campaigns, performed at five locations in two seasons: (I) two campaigns with strong influence of biomass-burning (BB) aerosol at the TROPOS institute (winter, 2014, urban background, Leipzig, Germany) and the Melpitz research site (winter, 2014, rural background); (II) two campaigns with strong influence from biogenic emissions at Melpitz (summer, 2014) and the forest site Waldstein (summer, 2014, Fichtelgebirge, Germany); and (III) two CAREBeijing-NCP campaigns at Xianghe (summer, 2013, anthropogenic polluted background) and Wangdu (summer, 2014, anthropogenic polluted background with a distinct BB episode), both in the North China Plain.

The filter samples were analyzed for NAC concentrations and the light absorption of aqueous filter extracts was determined. Light absorption properties of particulate brown carbon were derived from a seven-wavelength aethalometer during the campaigns at TROPOS (winter) and Waldstein (summer). The light absorption of the aqueous filter extracts was found to be pH dependent, with larger values at higher pH. In general, the aqueous light absorption coefficient (Abs370) ranged from 0.21 to 21.8Mm−1 under acidic conditions and 0.63 to 27.2Mm−1 under alkaline conditions, over all campaigns. The observed mass absorption efficiency (MAE370) was in a range of 0.10–1.79m2g−1 and 0.24–2.57m2g−1 for acidic and alkaline conditions, respectively. For MAE370 and Abs370, the observed values were higher in winter than in summer, in agreement with other studies. The lowest MAE was observed for the Waldstein (summer) campaign (average of 0.17±0.03m2g−1), indicating that freshly emitted biogenic aerosols are only weakly absorbing. In contrast, a strong relationship was found between the light absorption properties and the concentrations of levoglucosan, corroborating findings from other studies.

Regarding the particulate light absorption at 370nm, a mean particulate light absorption coefficient babs, 370 of 54Mm−1 and 6.0Mm−1 was determined for the TROPOS (winter) and Waldstein (summer) campaigns, respectively, with average contributions of particulate brown carbon to babs, 370 of 46% at TROPOS (winter) and 15% at Waldstein (summer). Thus, the aethalometer measurements support the findings from aqueous filter extracts of only weakly absorbing biogenic aerosols in comparison to the more polluted and BB influenced aerosol at TROPOS (winter).

The mean contribution of NACs to the aqueous extract light absorption over all campaigns ranged from 0.10 to 1.25% under acidic conditions and 0.13 to 3.71% under alkaline conditions. The high variability among the measurement sites showed that the emission strengths of light-absorbing compounds and the composition of brown carbon were very different for each site. The mean contribution of NACs to the particulate brown carbon light absorption was 0.10±0.06% (acidic conditions) and 0.13±0.09% (alkaline conditions) during the Waldstein (summer) campaign and 0.25±0.21% (acidic conditions) and 1.13±1.03% (alkaline conditions) during the TROPOS (winter) campaign.

The average contribution of NACs to the aqueous extract light absorption over all campaigns was found to be 5 times higher than their mass contribution to water-soluble organic carbon indicating that even small amounts of light-absorbing compounds can have a disproportionately high impact on the light absorption properties of particles.

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This study provides a large data set on concentrations of individual brown carbon constituents, i.e., nitrated aromatic compounds, in diverse atmospheric environments and their relative contribution to water-soluble and particulate light absorption. It extends the existing knowledge on the abundance of brown carbon and its molecular composition and provides scientific motivation for further studies on ambient brown carbon constituents.
This study provides a large data set on concentrations of individual brown carbon constituents,...
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