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Environ Sci Technol. 2018 Jun 19;52(12):6807-6815. doi: 10.1021/acs.est.8b01011. Epub 2018 May 30.

Spatial Variability of Sources and Mixing State of Atmospheric Particles in a Metropolitan Area.

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Center for Atmospheric Particle Studies , Carnegie Mellon University , Pittsburgh , Pennsylvania 15213 , United States.
Department of Mechanical Engineering , Carnegie Mellon University , Pittsburgh , Pennsylvania 15213 , United States.
Penn State Greater Allegheny , 4000 University Drive , McKeesport , Pennsylvania 15132 , United States.
Department of Civil and Environmental Engineering , National University of Singapore , Singapore 117576.
Department of Civil, Architectural and Environmental Engineering , University of Texas , Austin , Texas 78712 , United States.


Characterizing intracity variations of atmospheric particulate matter has mostly relied on fixed-site monitoring and quantifying variability in terms of different bulk aerosol species. In this study, we performed ground-based mobile measurements using a single-particle mass spectrometer to study spatial patterns of source-specific particles and the evolution of particle mixing state in 21 areas in the metropolitan area of Pittsburgh, PA. We selected sampling areas based on traffic density and restaurant density with each area ranging from 0.2 to 2 km2. Organics dominate particle composition in all of the areas we sampled while the sources of organics differ. The contribution of particles from traffic and restaurant cooking varies greatly on the neighborhood scale. We also investigate how primary and aged components in particles mix across the urban scale. Lastly we quantify and map the particle mixing state for all areas we sampled and discuss the overall pattern of mixing state evolution and its implications. We find that in the upwind and downwind of the urban areas, particles are more internally mixed while in the city center, particle mixing state shows large spatial heterogeneity that is mostly driven by emissions. This study is to our knowledge, the first study to perform fine spatial scale mapping of particle mixing state using ground-based mobile measurement and single-particle mass spectrometry.

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