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

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 acidmore » 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:
 [1];  [2];  [3];  [4];  [5];  [6];  [1];  [1];  [7];  [8];  [9];  [10];  [1]
  1. Colorado State Univ., Fort Collins, CO (United States)
  2. National Center for Atmospheric Research, Boulder, CO (United States); Univ. of California, Irvine, CA (United States)
  3. Univ. of Minnesota-Twin Cities, Minneapolis, MN (United States); Sun Yat-sen Univ., Guangzhou (China)
  4. National Center for Atmospheric Research, Boulder, CO (United States)
  5. Univ. of Minnesota-Twin Cities, Minneapolis, MN (United States); Univ. of California, Berkeley, CA (United States)
  6. Univ. of Eastern Finland, Kupio (Finland)
  7. Portland State Univ., Portland, OR (United States); Univ. of California, Riverside, CA (United States)
  8. Augsburg College, Minneapolis, MN (United States)
  9. Univ. of Minnesota-Twin Cities, Minneapolis, MN (United States)
  10. Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
Colorado State Univ., Fort Collins, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1274820
Grant/Contract Number:
SC0011780
Resource Type:
Journal Article: 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:
European Geosciences Union
Country of Publication:
United States
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. United States: 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. United States. 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., and Pierce, Jeffery R. 2016. "Multiple new-particle growth pathways observed at the US DOE Southern Great Plains field site". United States. doi: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 = {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 = {United States},
year = 2016,
month = 7
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.5194/acp-16-9321-2016

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  • 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–basemore » 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. Furthermore, the relative importance of each pathway is uncertain and is the focus of this work.« less
  • The Weather Research and Forecasting (WRF) model is used to investigate choice of land surface model (LSM) on the near-surface wind profile, including heights reached by multi-megawatt wind turbines. Simulations of wind profiles and surface energy fluxes were made using five LSMs of varying degrees of sophistication in dealing with soil-plant-atmosphere feedbacks for the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Southern Great Plains (SGP) Central Facility in Oklahoma. Surface-flux and wind-profile measurements were available for validation. The WRF model was run for three two-week periods during which varying canopy and meteorological conditions existed. Themore » LSMs predicted a wide range of energy-flux and wind-shear magnitudes even during the cool autumn period when we expected less variability. Simulations of energy fluxes varied in accuracy by model sophistication, whereby LSMs with very simple or no soil-plant-atmosphere feedbacks were the least accurate; however, the most complex models did not consistently produce more accurate results. Errors in wind shear also were sensitive to LSM choice and were partially related to the accuracy of energy flux data. The variability of LSM performance was relatively high, suggesting that LSM representation of energy fluxes in the WRF model remains a significant source of uncertainty for simulating wind turbine inflow conditions.« less
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  • Although shallow cumuli are common over large areas of the globe, their impact on the surface radiative forcing has not been carefully evaluated. This study addresses this shortcoming by analyzing data from days with shallow cumuli collected over eight summers (2000-2007) at the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) Climate Research Facility (collectively ACRF) Southern Great Plains site. During periods with clouds, the average shortwave and longwave radiative forcings are 45.5 W m-2 and +11.6 W m-2, respectively. The forcing has been defined so that a negative (positive) forcing indicates a surface cooling (warming). On average, the shortwavemore » forcing is negative, however, instances with positive shortwave forcing are observed approximately 20% of the time. These positive values of shortwave forcing are associated with three-dimensional radiative effects of the clouds. The three-dimensional effects are shown to be largest for intermediate cloud amounts. The magnitude of the three-dimensional effects decreased with averaging time, but it is not negligibly small even for large averaging times as long as four hours.« less