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Title: Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site

Abstract

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 sulfuricmore » 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.« less

Authors:
; ; ORCiD logo; ; ORCiD logo; ; ; ORCiD logo; ORCiD logo; ; ; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Colorado State Univ., Fort Collins, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1274820
Alternate Identifier(s):
OSTI ID: 1360124
Grant/Contract Number:  
SC0011780
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 16 Journal Issue: 14; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hodshire, Anna L., Lawler, Michael J., Zhao, Jun, Ortega, John, Jen, Coty, Yli-Juuti, Taina, Brewer, Jared F., Kodros, Jack K., Barsanti, Kelley C., Hanson, Dave R., McMurry, Peter H., Smith, James N., and Pierce, Jeffery R. Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site. Germany: N. p., 2016. Web. doi:10.5194/acp-16-9321-2016.
Hodshire, Anna L., Lawler, Michael J., Zhao, Jun, Ortega, John, Jen, Coty, Yli-Juuti, Taina, Brewer, Jared F., Kodros, Jack K., Barsanti, Kelley C., Hanson, Dave R., McMurry, Peter H., Smith, James N., & Pierce, Jeffery R. Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site. Germany. https://doi.org/10.5194/acp-16-9321-2016
Hodshire, Anna L., Lawler, Michael J., Zhao, Jun, Ortega, John, Jen, Coty, Yli-Juuti, Taina, Brewer, Jared F., Kodros, Jack K., Barsanti, Kelley C., Hanson, Dave R., McMurry, Peter H., Smith, James N., and Pierce, Jeffery R. Thu . "Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site". Germany. https://doi.org/10.5194/acp-16-9321-2016.
@article{osti_1274820,
title = {Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site},
author = {Hodshire, Anna L. and Lawler, Michael J. and Zhao, Jun and Ortega, John and Jen, Coty and Yli-Juuti, Taina and Brewer, Jared F. and Kodros, Jack K. and Barsanti, Kelley C. and Hanson, Dave R. and McMurry, Peter H. and Smith, James N. and Pierce, Jeffery R.},
abstractNote = {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.},
doi = {10.5194/acp-16-9321-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 14,
volume = 16,
place = {Germany},
year = {2016},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.5194/acp-16-9321-2016

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  • Environmental Science & Technology, Vol. 45, Issue 20
  • DOI: 10.1021/es201819a

Atmospheric Measurements of Sub-20 nm Diameter Particle Chemical Composition by Thermal Desorption Chemical Ionization Mass Spectrometry
journal, February 2004


Molecular understanding of sulphuric acid–amine particle nucleation in the atmosphere
journal, October 2013

  • Almeida, João; Schobesberger, Siegfried; Kürten, Andreas
  • Nature, Vol. 502, Issue 7471
  • DOI: 10.1038/nature12663

Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer
conference, January 2013

  • Chen, Modi; Titcombe, Mari; Jiang, Jingkun
  • NUCLEATION AND ATMOSPHERIC AEROSOLS: 19th International Conference, AIP Conference Proceedings
  • DOI: 10.1063/1.4803354

The Formation of Highly Oxidized Multifunctional Products in the Ozonolysis of Cyclohexene
journal, October 2014

  • Rissanen, Matti P.; Kurtén, Theo; Sipilä, Mikko
  • Journal of the American Chemical Society, Vol. 136, Issue 44
  • DOI: 10.1021/ja507146s

Observations of aminium salts in atmospheric nanoparticles and possible climatic implications
journal, January 2010

  • Smith, J. N.; Barsanti, K. C.; Friedli, H. R.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 15
  • DOI: 10.1073/pnas.0912127107

Thermodynamic Models of Aqueous Solutions Containing Inorganic Electrolytes and Dicarboxylic Acids at 298.15 K. 1. The Acids as Nondissociating Components
journal, May 2006

  • Clegg, Simon L.; Seinfeld, John H.
  • The Journal of Physical Chemistry A, Vol. 110, Issue 17
  • DOI: 10.1021/jp056149k

H 2 SO 4 vapor pressure of sulfuric acid and ammonium sulfate solutions
journal, February 1997

  • Marti, James J.; Jefferson, Anne; Cai, Xiao Ping
  • Journal of Geophysical Research: Atmospheres, Vol. 102, Issue D3
  • DOI: 10.1029/96JD03064

Dicarboxylic acids in the Arctic aerosols and snowpacks collected during ALERT 2000
journal, May 2002


Formation and growth of nucleated particles into cloud condensation nuclei: model–measurement comparison
journal, January 2013

  • Westervelt, D. M.; Pierce, J. R.; Riipinen, I.
  • Atmospheric Chemistry and Physics, Vol. 13, Issue 15
  • DOI: 10.5194/acp-13-7645-2013

Low-Molecular-Weight Dicarboxylic Acids in an Urban and Rural Atmosphere
journal, March 2000


Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature)
journal, January 2006

  • Guenther, A.; Karl, T.; Harley, P.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 11
  • DOI: 10.5194/acp-6-3181-2006

Dynamics of atmospheric nucleation mode particles: a timescale analysis
journal, April 2004