Diurnal Evolution of Aerosol Optical Properties and Morphology at Pico Tres Padres: A Phenomenological Analysis

Aerosol optical properties affect planetary radiative balance and therefore climate. The optical properties are related to chemical composition, size distribution, and morphology, which also have implications for human health and environmental degradation. During the MILAGRO field campaign, we measured ensemble aerosol absorption and angle-integrated scattering in Mexico City. These measurements were performed using the Los Alamos aerosol photoacoustic instrument with an integrated nephelometer (LAPA) operating at 781 nm. The LAPA was mounted on-board the Aerodyne Inc. mobile laboratory, which hosted a wide variety of gaseous and aerosol instruments. During the campaign, the Aerodyne mobile laboratory was moved to different sites, capturing the influence of spatial and temporal parameters including location, aging, elevation, and sources on ambient air pollution. The LAPA operated almost continuously between the 3rd and the 28th of March 2006. During the same period we collected ambient aerosols on more than 100 Nuclepore filters for scanning electron microscopy (SEM) analysis. Filter samples were collected during specific pollution events and different times of the day. Subsequently, SEM images of selected filters were taken to study particle morphology. The elemental composition of a few individual particles was also qualitatively assessed by energy dispersive X-ray spectroscopy. Between March 7th and 19th the laboratory was sampling air close to the top of the Pico Tres Padres, a ~3000 m high mountain on the north side of the Mexico City. Daily changes of aerosol loading and pollutant concentrations followed the expected diurnal variations of the boundary layer height. Here we report a preliminary analysis of aerosol absorption, scattering, and morphology at Pico Tres Padres for three specific days (9th, 11th and 12th of March 2006). The single scattering albedo (ratio of scattering to total extinction) during these three days showed a characteristic drop in the tens-of-minutes-to-hour time frame immediately following the growth of the boundary layer above the sampling site. Later in the day the single scattering albedo grew steadily to reach a maximum in the late afternoon. The SEM images show a wide variety of aerosol shapes including fractal-like chain aggregates (possibly soot), spherical particles (possibly tar balls), cylinders, and irregular non-fractal shapes. The increased afternoon single scattering albedo in the hottest part of the day qualitatively correlated with a relative increase in spherical particles that typically are not strongly light absorbing relative to fractal-like chain aggregates that are typically strongly light absorbing. These changes in optical properties and/or morphology can be explained by multiple mechanisms such as the collapse of fractal-like chain aggregates due to thermal effects and/or condensation of volatile compounds, coating by organic compounds, and photochemical secondary organic particle formation. Elemental analysis of a few individual particles yielded a relative large carbon abundance combined with smaller fractions of oxygen, silicon, metals, and other elements.