1Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720-8226, USA
2Department of Physics, University of Würzburg, Am Hu-bland, 97074 Würzburg, Germany
3W. R. Wiley Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington, 99352, USA
4Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland, Washington, 99352, USA
5Department of Applied Sciences, University of California, Davis, California, USA
6Department of Meteorology, University of Utah, Salt Lake City, Utah, USA
*now at: Department of Chemistry, University of Iowa, Iowa City, Iowa 52242, USA
**now at: Department of Atmospheric Science, Colorado State University, Fort Collins, Colorado, 80523-1371, USA
Received: 29 Jul 2009 – Discussion started: 12 Aug 2009
Abstract. This study was part of the Megacities Initiative: Local and Global Research Observations (MILAGRO) field campaign conducted in Mexico City metropolitan area during spring 2006. The physical and chemical transformations of particles aged in the outflow from Mexico City were investigated for the transport event of 22 March 2006. A detailed chemical analysis of individual particles was performed using a combination of complementary microscopy and micro-spectroscopy techniques. The applied techniques included scanning transmission X-ray microscopy (STXM) coupled with near edge X-ray absorption fine structure spectroscopy (NEXAFS) and computer controlled scanning electron microscopy with an energy dispersive X-ray analyzer (CCSEM/EDX). As the aerosol plume evolves from the city center, the organic mass per particle increases and the fraction of carbon-carbon double bonds (associated with elemental carbon) decreases. Organic functional groups enhanced with particle age include: carboxylic acids, alkyl groups, and oxygen bonded alkyl groups. At the city center (T0) the most prevalent aerosol type contained inorganic species (composed of sulfur, nitrogen, oxygen, and potassium) coated with organic material. At the T1 and T2 sites, located northeast of T0 (~29 km and ~65 km, respectively), the fraction of homogenously mixed organic particles increased in both size and number. These observations illustrate the evolution of the physical mixing state and organic bonding in individual particles in a photochemically active environment.
Revised: 03 Dec 2009 – Accepted: 05 Jan 2010 – Published: 01 Feb 2010
Moffet, R. C., Henn, T. R., Tivanski, A. V., Hopkins, R. J., Desyaterik, Y., Kilcoyne, A. L. D., Tyliszczak, T., Fast, J., Barnard, J., Shutthanandan, V., Cliff, S. S., Perry, K. D., Laskin, A., and Gilles, M. K.: Microscopic characterization of carbonaceous aerosol particle aging in the outflow from Mexico City, Atmos. Chem. Phys., 10, 961-976, doi:10.5194/acp-10-961-2010, 2010.