References

ACP

Atmospheric Chemistry and Physics

ACP

Atmos. Chem. Phys.

1680-7324

Copernicus Publications

Göttingen, Germany

10.5194/acp-12-4477-2012

Size-resolved measurement of the mixing state of soot in the megacity Beijing, China: diurnal cycle, aging and parameterization

Cheng

Y. F.

¹ ² ⁷ Su

³ Rose

³ Gunthe

S. S.

³ ⁸ Berghof

² Wehner

² Achtert

² Nowak

² Takegawa

⁴ Kondo

⁵ Shiraiwa

³ ⁹ Gong

Y. G.

⁶ Shao

¹ Hu

¹ Zhu

¹ Zhang

Y. H.

¹ Carmichael

G. R.

⁷ Wiedensohler

² Andreae

M. O.

³ Pöschl

College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China

Leibniz Institute for Tropospheric Research, Leipzig 04318, Germany

Biogeochemistry Department, Max Planck Institute for Chemistry, Mainz 55020, Germany

Research Center for Advanced Science and Technology, the University of Tokyo, Tokyo, Japan

Department of Earth and Planetary Science, Graduate School of Science, the University of Tokyo, Tokyo 1130033, Japan

Research Institute of Chemical Defence, Beijing 102205, China

Center for Global and Regional Environment Research, University of Iowa, IA 52242, USA

now at: EWRE Division, Department of Civil Engineering, Indian Institute of Technology Madras, Chennai 600036, India

now at: Department of Chemical Engineering, California Institute of Technology, Pasadena, USA

22 05 2012

12 10 4477 4491

2012

This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/

This article is available from https://acp.copernicus.org/articles/12/4477/2012/acp-12-4477-2012.html

The full text article is available as a PDF file from https://acp.copernicus.org/articles/12/4477/2012/acp-12-4477-2012.pdf

Soot particles are the most efficient light absorbing aerosol species in the atmosphere, playing an important role as a driver of global warming. Their climate effects strongly depend on their mixing state, which significantly changes their light absorbing capability and cloud condensation nuclei (CCN) activity. Therefore, knowledge about the mixing state of soot and its aging mechanism becomes an important topic in the atmospheric sciences. The size-resolved (30–320 nm diameter) mixing state of soot particles in polluted megacity air was measured at a suburban site (Yufa) during the CAREBeijing 2006 campaign in Beijing, using a volatility tandem differential mobility analyzer (VTDMA). Particles in this size range with non-volatile residuals at 300 °C were considered to be soot particles. On average, the number fraction of internally mixed soot in total soot particles (Fin), decreased from 0.80 to 0.57 when initial Dp increased from 30 to 320 nm. Further analysis reveals that: (1) Fin was well correlated with the aerosol hygroscopic mixing state measured by a CCN counter. More externally mixed soot particles were observed when particles showed more heterogeneous features with regard to hygroscopicity. (2) Fin had pronounced diurnal cycles. For particles in the accumulation mode (Dp at 100–320 nm), largest Fin were observed at noon time, with "apparent" turnover rates (kex → in) up to 7.8% h−1. (3) Fin was subject to competing effects of both aging and emissions. While aging increases Fin by converting externally mixed soot particles into internally mixed ones, emissions tend to reduce Fin by emitting more fresh and externally mixed soot particles. Similar competing effects were also found with air mass age indicators. (4) Under the estimated emission intensities, actual turnover rates of soot (kex → in) up to 20% h−1 were derived, which showed a pronounced diurnal cycle peaking around noon time. This result confirms that (soot) particles are undergoing fast aging/coating with the existing high levels of condensable vapors in the megacity Beijing. (5) Diurnal cycles of Fin were different between Aitken and accumulation mode particles, which could be explained by the faster growth of smaller Aitken mode particles into larger size bins. To improve the Fin prediction in regional/global models, we suggest parameterizing Fin by an air mass aging indicator, i.e., Fin = a + bx, where a and b are empirical coefficients determined from observations, and x is the value of an air mass age indicator. At the Yufa site in the North China Plain, fitted coefficients (a, b) were determined as (0.57, 0.21), (0.47, 0.21), and (0.52, 0.0088) for x (indicators) as [NOz]/[NOy], [E]/[X] ([ethylbenzene]/[m,p-xylene]) and ([IM] + [OM])/[EC] ([inorganic + organic matter]/[elemental carbon]), respectively. Such a parameterization consumes little additional computing time, but yields a more realistic description of Fin compared with the simple treatment of soot mixing state in regional/global models.

European Commission

PEGASOS - Pan-European Gas-AeroSol-climate interaction Study (265148)

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