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Title: The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere

Abstract

Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40 %–60 % of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003 < Dp < 4.8 µm) in the remote marine troposphere between ~0.18 and 13 km altitude obtained during the NASA Atmospheric Tomography (ATom) mission, we show that high concentrations of newly formed particles in the tropical UT over both themore » Atlantic and Pacific oceans are associated with outflow regions of deep convective clouds. We focus analysis on observations over the remote Pacific Ocean, which is a region less perturbed by continental emissions than the Atlantic. Comparing aerosol size distribution measurements over the remote Pacific with box model simulations for 32 cases shows that none of the NPF schemes most commonly used in global models, including binary nucleation of sulfuric acid and water (neutral and ion-assisted) and ternary involving sulfuric acid, water, and ammonia, are consistent with observations, regardless of precursor concentrations. Through sensitivity studies, we find that the nucleation scheme among those tested that is able to explain most consistently (21 of 32 cases) the observed size distributions is that of Riccobono et al. (2014), which involves both organic species and sulfuric acid. The method of Dunne et al. (2016), involving charged sulfuric acid–water–ammonia nucleation, when coupled with organic growth of the nucleated particles, was most consistent with the observations for 5 of 32 cases. Similarly, the neutral sulfuric acid–water–ammonia method of Napari (2002), when scaled with a tuning factor and with organic growth added, was most consistent for 6 of 32 cases. We find that to best reproduce both nucleation and growth rates, the mixing ratios of gas-phase organic precursors generally need to be at least twice that of SO2, a proxy for dimethyl sulfide (DMS). Unfortunately, we have no information on the nature of oxidized organic species that participated in NPF in this region. Global models rarely include organic-driven nucleation and growth pathways in UT conditions where globally significant NPF takes place, which may result in poor estimates of NPF and CCN abundance and contribute to uncertainties in aerosol–cloud–radiation effects. Furthermore, our results indicate that the organic aerosol precursor vapors may be important in the tropical UT above marine regions, a finding that should guide future observational efforts.« less

Authors:
ORCiD logo; ; ORCiD logo; ORCiD logo; ; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); European Research Council (ERC)
OSTI Identifier:
1731017
Alternate Identifier(s):
OSTI ID: 1751937
Grant/Contract Number:  
SC0019000; 640458
Resource Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 20 Journal Issue: 23; Journal ID: ISSN 1680-7324
Publisher:
Copernicus GmbH
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Kupc, Agnieszka, Williamson, Christina J., Hodshire, Anna L., Kazil, Jan, Ray, Eric, Bui, T. Paul, Dollner, Maximilian, Froyd, Karl D., McKain, Kathryn, Rollins, Andrew, Schill, Gregory P., Thames, Alexander, Weinzierl, Bernadett B., Pierce, Jeffrey R., and Brock, Charles A. The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere. Germany: N. p., 2020. Web. doi:10.5194/acp-20-15037-2020.
Kupc, Agnieszka, Williamson, Christina J., Hodshire, Anna L., Kazil, Jan, Ray, Eric, Bui, T. Paul, Dollner, Maximilian, Froyd, Karl D., McKain, Kathryn, Rollins, Andrew, Schill, Gregory P., Thames, Alexander, Weinzierl, Bernadett B., Pierce, Jeffrey R., & Brock, Charles A. The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere. Germany. https://doi.org/10.5194/acp-20-15037-2020
Kupc, Agnieszka, Williamson, Christina J., Hodshire, Anna L., Kazil, Jan, Ray, Eric, Bui, T. Paul, Dollner, Maximilian, Froyd, Karl D., McKain, Kathryn, Rollins, Andrew, Schill, Gregory P., Thames, Alexander, Weinzierl, Bernadett B., Pierce, Jeffrey R., and Brock, Charles A. Fri . "The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere". Germany. https://doi.org/10.5194/acp-20-15037-2020.
@article{osti_1731017,
title = {The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere},
author = {Kupc, Agnieszka and Williamson, Christina J. and Hodshire, Anna L. and Kazil, Jan and Ray, Eric and Bui, T. Paul and Dollner, Maximilian and Froyd, Karl D. and McKain, Kathryn and Rollins, Andrew and Schill, Gregory P. and Thames, Alexander and Weinzierl, Bernadett B. and Pierce, Jeffrey R. and Brock, Charles A.},
abstractNote = {Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40 %–60 % of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003 < Dp < 4.8 µm) in the remote marine troposphere between ~0.18 and 13 km altitude obtained during the NASA Atmospheric Tomography (ATom) mission, we show that high concentrations of newly formed particles in the tropical UT over both the Atlantic and Pacific oceans are associated with outflow regions of deep convective clouds. We focus analysis on observations over the remote Pacific Ocean, which is a region less perturbed by continental emissions than the Atlantic. Comparing aerosol size distribution measurements over the remote Pacific with box model simulations for 32 cases shows that none of the NPF schemes most commonly used in global models, including binary nucleation of sulfuric acid and water (neutral and ion-assisted) and ternary involving sulfuric acid, water, and ammonia, are consistent with observations, regardless of precursor concentrations. Through sensitivity studies, we find that the nucleation scheme among those tested that is able to explain most consistently (21 of 32 cases) the observed size distributions is that of Riccobono et al. (2014), which involves both organic species and sulfuric acid. The method of Dunne et al. (2016), involving charged sulfuric acid–water–ammonia nucleation, when coupled with organic growth of the nucleated particles, was most consistent with the observations for 5 of 32 cases. Similarly, the neutral sulfuric acid–water–ammonia method of Napari (2002), when scaled with a tuning factor and with organic growth added, was most consistent for 6 of 32 cases. We find that to best reproduce both nucleation and growth rates, the mixing ratios of gas-phase organic precursors generally need to be at least twice that of SO2, a proxy for dimethyl sulfide (DMS). Unfortunately, we have no information on the nature of oxidized organic species that participated in NPF in this region. Global models rarely include organic-driven nucleation and growth pathways in UT conditions where globally significant NPF takes place, which may result in poor estimates of NPF and CCN abundance and contribute to uncertainties in aerosol–cloud–radiation effects. Furthermore, our results indicate that the organic aerosol precursor vapors may be important in the tropical UT above marine regions, a finding that should guide future observational efforts.},
doi = {10.5194/acp-20-15037-2020},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 23,
volume = 20,
place = {Germany},
year = {Fri Dec 04 00:00:00 EST 2020},
month = {Fri Dec 04 00:00:00 EST 2020}
}

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A comparative study of nucleation parameterizations: 1. Examination and evaluation of the formulations
journal, January 2010

  • Zhang, Yang; McMurry, Peter H.; Yu, Fangqun
  • Journal of Geophysical Research, Vol. 115, Issue D20
  • DOI: 10.1029/2010JD014150

Ion-induced nucleation of pure biogenic particles
journal, May 2016

  • Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika
  • Nature, Vol. 533, Issue 7604
  • DOI: 10.1038/nature17953

Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms
journal, January 2006

  • Sihto, S. -L.; Kulmala, M.; Kerminen, V. -M.
  • Atmospheric Chemistry and Physics, Vol. 6, Issue 12
  • DOI: 10.5194/acp-6-4079-2006

Methane sulfonic acid-enhanced formation of molecular clusters of sulfuric acid and dimethyl amine
journal, January 2014


Atmospheric Degradation of Volatile Organic Compounds
journal, December 2003

  • Atkinson, Roger; Arey, Janet
  • Chemical Reviews, Vol. 103, Issue 12
  • DOI: 10.1021/cr0206420

Deep convection as a source of new particles in the midlatitude upper troposphere: DEEP CONVECTION AS A SOURCE OF NEW PARTICLES
journal, November 2002

  • Twohy, Cynthia H.; Clement, Charles F.; Gandrud, Bruce W.
  • Journal of Geophysical Research: Atmospheres, Vol. 107, Issue D21
  • DOI: 10.1029/2001JD000323

A large source of cloud condensation nuclei from new particle formation in the tropics
journal, October 2019


Pollution and the planetary albedo
journal, December 1974


Predicting global aerosol size distributions in general circulation models
journal, January 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

Molecular understanding of new-particle formation from α-pinene between −50 and +25 °C
journal, January 2020

  • Simon, Mario; Dada, Lubna; Heinritzi, Martin
  • Atmospheric Chemistry and Physics, Vol. 20, Issue 15
  • DOI: 10.5194/acp-20-9183-2020