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New insights into single-particle mixing state using aircraft aerosol time-of-flight mass spectrometry

  • Author(s): Pratt, Kerri Anne
  • et al.
Abstract

Atmospheric aerosols strongly influence the energy balance of the Earth and the hydrological cycle by scattering and absorbing radiation and acting as cloud condensation and ice nuclei. The climate and human health impacts of aerosols are strongly dependent on particle size, chemical composition, and mixing state. During transport in the atmosphere, aerosol particles undergo physical and chemical transformations (atmospheric aging) through heterogeneous reactions with trace gases and gas-particle partitioning of semivolatile species. The size-resolved chemical composition of individual particles may be examined in real-time using aerosol time-of-flight mass spectrometry (ATOFMS). A smaller ATOFMS with increased data acquisition capabilities was developed for aircraft- based studies. Particle volatility was examined through ground-based measurements during the Study of Organic Aerosols in Riverside, CA (SOAR), and vertical mixing state profiles and cloud residues were examined through flight-based measurements during the Ice in Clouds Experiment - Layer Clouds (ICE-L). An automated thermodenuder (TD) was coupled to the aircraft (A)-ATOFMS to provide the first real-time, individual-particle size and volatility-resolved chemical composition measurements. This work provided insight into the volatility of secondary species, as well as the sources and chemistry of ambient particle cores. Seasonal differences in the volatility of amine species were attributed to the formation of aminium sulfate and nitrate salts in the summer. Oligomeric species were detected in real-time for the first time in individual ambient aerosol particles; increased oligomer ion intensities were associated with increased particle acidity and heating. During ICE-L, vertical profiles of particle types, such as soot, mixed with secondary species, such as sulfuric acid, were examined. For cloud sampling, a counterflow virtual impactor was utilized in series with the A-ATOFMS to examine the residues of cloud droplets and ice crystals. This resulted in the first in-situ detection of biological particles in high altitude ice clouds influenced by long- range transported dust. Playa salts were observed to serve as cloud condensation nuclei and were preferentially observed as residues of large droplets

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