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Title: Spring and summer contrast in new particle formation over nine forest areas in North America

Abstract

Recent laboratory chamber studies indicate a significant role for highly oxidized low-volatility organics in new particle formation (NPF), but the actual role of these highly oxidized low-volatility organics in atmospheric NPF remains uncertain. Here, particle size distributions (PSDs) measured in nine forest areas in North America are used to characterize the occurrence and intensity of NPF and to evaluate model simulations using an empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low-volatility organics from alpha-pinene oxidation (Nucl-Org), and using an ion-mediated nucleation mechanism (excluding organics) (Nucl-IMN). On average, NPF occurred on ~ 70 % of days during March for the four forest sites with springtime PSD measurements, while NPF occurred on only ~ 10 % of days in July for all nine forest sites. Both Nucl-Org and Nucl-IMN schemes capture the observed high frequency of NPF in spring, but the Nucl-Org scheme significantly overpredicts while the Nucl-IMN scheme slightly underpredicts NPF and particle number concentrations in summer. Statistical analyses of observed and simulated ultrafine particle number concentrations and frequency of NPF events indicate that the scheme without organics agrees better overall with observations. The two schemes predict quite different nucleation rates (includingmore » their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America, highlighting the need to reduce NPF uncertainties in regional and global earth system models.« less

Authors:
 [1];  [1]; ORCiD logo [2];  [3];  [4];  [5];  [1];  [6];  [7];  [3];  [8];  [9];  [1];  [1]
  1. State Univ. of New York (SUNY), Albany, NY (United States). Atmospheric Sciences Research Center
  2. Cornell Univ., Ithaca, NY (United States). Dept. of Earth and Athospheric Sciences
  3. North Carolina State Univ., Raleigh, NC (United States). Dept. of Marine, Earth, and Atmospheric Sciences
  4. Kent State Univ., Kent, OH (United States). College of Public Health
  5. National Center for Atmospheric Research, Boulder, CO (United States)
  6. Desert Research Inst. (DRI), Steamboat Springs, CO (United States). Storm Peak Lab.
  7. Environment Canada, Toronto, ON (Canada). Science and Technology Branch
  8. National Center for Atmospheric Research, Boulder, CO (United States); Univ. of Eastern Finland, Kuopio (Finland). Applied Physics Dept.
  9. North Carolina State Univ., Raleigh, NC (United States). Dept. of Marine, Earth, and Atmospheric Sciences; US Environmental Protection Agency (EPA), Durham, NC (United States)
Publication Date:
Research Org.:
National Center for Atmospheric Research, Boulder, CO (United States); State Univ. of New York (SUNY), Albany, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Aeronautic and Space Administration (NASA); National Science Foundation (NSF)
OSTI Identifier:
1233973
Alternate Identifier(s):
OSTI ID: 1455172
Grant/Contract Number:  
SC0011664; NNX13AK20G; NNX11AQ72G; 1517365
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 15; Journal Issue: 24; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Yu, F., Luo, G., Pryor, S. C., Pillai, P. R., Lee, S. H., Ortega, J., Schwab, J. J., Hallar, A. G., Leaitch, W. R., Aneja, V. P., Smith, J. N., Walker, J. T., Hogrefe, O., and Demerjian, K. L. Spring and summer contrast in new particle formation over nine forest areas in North America. United States: N. p., 2015. Web. doi:10.5194/acp-15-13993-2015.
Yu, F., Luo, G., Pryor, S. C., Pillai, P. R., Lee, S. H., Ortega, J., Schwab, J. J., Hallar, A. G., Leaitch, W. R., Aneja, V. P., Smith, J. N., Walker, J. T., Hogrefe, O., & Demerjian, K. L. Spring and summer contrast in new particle formation over nine forest areas in North America. United States. doi:10.5194/acp-15-13993-2015.
Yu, F., Luo, G., Pryor, S. C., Pillai, P. R., Lee, S. H., Ortega, J., Schwab, J. J., Hallar, A. G., Leaitch, W. R., Aneja, V. P., Smith, J. N., Walker, J. T., Hogrefe, O., and Demerjian, K. L. Fri . "Spring and summer contrast in new particle formation over nine forest areas in North America". United States. doi:10.5194/acp-15-13993-2015.
@article{osti_1233973,
title = {Spring and summer contrast in new particle formation over nine forest areas in North America},
author = {Yu, F. and Luo, G. and Pryor, S. C. and Pillai, P. R. and Lee, S. H. and Ortega, J. and Schwab, J. J. and Hallar, A. G. and Leaitch, W. R. and Aneja, V. P. and Smith, J. N. and Walker, J. T. and Hogrefe, O. and Demerjian, K. L.},
abstractNote = {Recent laboratory chamber studies indicate a significant role for highly oxidized low-volatility organics in new particle formation (NPF), but the actual role of these highly oxidized low-volatility organics in atmospheric NPF remains uncertain. Here, particle size distributions (PSDs) measured in nine forest areas in North America are used to characterize the occurrence and intensity of NPF and to evaluate model simulations using an empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low-volatility organics from alpha-pinene oxidation (Nucl-Org), and using an ion-mediated nucleation mechanism (excluding organics) (Nucl-IMN). On average, NPF occurred on ~ 70 % of days during March for the four forest sites with springtime PSD measurements, while NPF occurred on only ~ 10 % of days in July for all nine forest sites. Both Nucl-Org and Nucl-IMN schemes capture the observed high frequency of NPF in spring, but the Nucl-Org scheme significantly overpredicts while the Nucl-IMN scheme slightly underpredicts NPF and particle number concentrations in summer. Statistical analyses of observed and simulated ultrafine particle number concentrations and frequency of NPF events indicate that the scheme without organics agrees better overall with observations. The two schemes predict quite different nucleation rates (including their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America, highlighting the need to reduce NPF uncertainties in regional and global earth system models.},
doi = {10.5194/acp-15-13993-2015},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 24,
volume = 15,
place = {United States},
year = {2015},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.5194/acp-15-13993-2015

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Cited by: 5 works
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