multiple new-particle growth pathways observed at the us doe southern great plains field site
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2016
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Abstract
New-particle formation (NPF) is a significant source of aerosol
particles into the atmosphere. However, these particles are initially too
small to have climatic importance and must grow, primarily through net
uptake of low-volatility species, from diameters ∼ 1 to
30–100 nm in order to potentially impact climate. There are currently
uncertainties in the physical and chemical processes associated with the
growth of these freshly formed particles that lead to uncertainties in
aerosol-climate modeling. Four main pathways for new-particle growth have
been identified: condensation of sulfuric-acid vapor (and associated bases
when available), condensation of organic vapors, uptake of organic acids
through acid–base chemistry in the particle phase, and accretion of organic
molecules in the particle phase to create a lower-volatility compound that
then contributes to the aerosol mass. The relative importance of each
pathway is uncertain and is the focus of this work.
The 2013 New Particle Formation Study (NPFS) measurement campaign took place at the DOE Southern Great Plains (SGP) facility in Lamont, Oklahoma, during spring 2013. Measured gas- and particle-phase compositions during these new-particle growth events suggest three distinct growth pathways: (1) growth by primarily organics, (2) growth by primarily sulfuric acid and ammonia, and (3) growth by primarily sulfuric acid and associated bases and organics. To supplement the measurements, we used the particle growth model MABNAG (Model for Acid–Base chemistry in NAnoparticle Growth) to gain further insight into the growth processes on these 3 days at SGP. MABNAG simulates growth from (1) sulfuric-acid condensation (and subsequent salt formation with ammonia or amines), (2) near-irreversible condensation from nonreactive extremely low-volatility organic compounds (ELVOCs), and (3) organic-acid condensation and subsequent salt formation with ammonia or amines. MABNAG is able to corroborate the observed differing growth pathways, while also predicting that ELVOCs contribute more to growth than organic salt formation. However, most MABNAG model simulations tend to underpredict the observed growth rates between 10 and 20 nm in diameter; this underprediction may come from neglecting the contributions to growth from semi-to-low-volatility species or accretion reactions. Our results suggest that in addition to sulfuric acid, ELVOCs are also very important for growth in this rural setting. We discuss the limitations of our study that arise from not accounting for semi- and low-volatility organics, as well as nitrogen-containing species beyond ammonia and amines in the model. Quantitatively understanding the overall budget, evolution, and thermodynamic properties of lower-volatility organics in the atmosphere will be essential for improving global aerosol models.
The 2013 New Particle Formation Study (NPFS) measurement campaign took place at the DOE Southern Great Plains (SGP) facility in Lamont, Oklahoma, during spring 2013. Measured gas- and particle-phase compositions during these new-particle growth events suggest three distinct growth pathways: (1) growth by primarily organics, (2) growth by primarily sulfuric acid and ammonia, and (3) growth by primarily sulfuric acid and associated bases and organics. To supplement the measurements, we used the particle growth model MABNAG (Model for Acid–Base chemistry in NAnoparticle Growth) to gain further insight into the growth processes on these 3 days at SGP. MABNAG simulates growth from (1) sulfuric-acid condensation (and subsequent salt formation with ammonia or amines), (2) near-irreversible condensation from nonreactive extremely low-volatility organic compounds (ELVOCs), and (3) organic-acid condensation and subsequent salt formation with ammonia or amines. MABNAG is able to corroborate the observed differing growth pathways, while also predicting that ELVOCs contribute more to growth than organic salt formation. However, most MABNAG model simulations tend to underpredict the observed growth rates between 10 and 20 nm in diameter; this underprediction may come from neglecting the contributions to growth from semi-to-low-volatility species or accretion reactions. Our results suggest that in addition to sulfuric acid, ELVOCs are also very important for growth in this rural setting. We discuss the limitations of our study that arise from not accounting for semi- and low-volatility organics, as well as nitrogen-containing species beyond ammonia and amines in the model. Quantitatively understanding the overall budget, evolution, and thermodynamic properties of lower-volatility organics in the atmosphere will be essential for improving global aerosol models.
| Reference Key |
hodshire2016atmosphericmultiple
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| Authors | ;A. L. Hodshire;M. J. Lawler;M. J. Lawler;J. Zhao;J. Zhao;J. Ortega;C. Jen;C. Jen;T. Yli-Juuti;J. F. Brewer;J. K. Kodros;K. C. Barsanti;K. C. Barsanti;D. R. Hanson;P. H. McMurry;J. N. Smith;J. R. Pierce |
| Journal | Journal of agricultural and food chemistry |
| Year | 2016 |
| DOI |
10.5194/acp-16-9321-2016
|
| URL | |
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