Journal cover Journal topic
Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
Atmos. Chem. Phys., 16, 9321-9348, 2016
© Author(s) 2016. This work is distributed
under the Creative Commons Attribution 3.0 License.
Research article
28 Jul 2016
Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site
Anna L. Hodshire1, Michael J. Lawler2,a, Jun Zhao3,b, John Ortega2, Coty Jen3,c, Taina Yli-Juuti4, Jared F. Brewer1, Jack K. Kodros1, Kelley C. Barsanti5,d, Dave R. Hanson6, Peter H. McMurry3, James N. Smith7, and Jeffery R. Pierce1 1Department of Atmospheric Science, Colorado State University, Fort Collins, 80523, USA
2Atmospheric Chemistry Observations & Modeling, National Center for Atmospheric Research, Boulder, 80305, USA
3Department of Mechanical Engineering, University of Minnesota-Twin Cities, Minneapolis, 55455, USA
4Department of Applied Physics, University of Eastern Finland, Kupio, 70211, Finland
5Department of Civil and Environmental Engineering, Portland State University, Portland, 97201, USA
6Department of Chemistry, Augsburg College, Minneapolis, 55454, USA
7Department of Chemistry, University of California, Irvine, 92697-2025, USA
anow at: Department of Chemistry, University of California, Irvine, 92697-2025, USA
bnow at: School of Atmospheric Sciences, Sun Yat-sen University, Guangzhou, 510275, China
cnow at: Environmental Science, Policy, and Management, University of California, Berkeley, 94720-3114, USA
dnow at: Chemical and Environmental Engineering, University of California, Riverside, 92521, USA
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.

Citation: Hodshire, A. L., Lawler, M. J., Zhao, J., Ortega, J., Jen, C., Yli-Juuti, T., Brewer, J. F., Kodros, J. K., Barsanti, K. C., Hanson, D. R., McMurry, P. H., Smith, J. N., and Pierce, J. R.: Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site, Atmos. Chem. Phys., 16, 9321-9348, doi:10.5194/acp-16-9321-2016, 2016.
Publications Copernicus
Short summary
Processes that control the growth of newly formed particles are not well understood and limit predictions of aerosol climate impacts. We combine state-of-the-art measurements at a central-US site with a particle-growth model to investigate the species and processes contributing to growth. Observed growth was dominated by organics, sulfate salts, or a mixture of these two. The model qualitatively captures the variability between different days.
Processes that control the growth of newly formed particles are not well understood and limit...