Size-dependent influence of NO x  on the growth rates of organic aerosol particles

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Abstract

NO _x is important for particle growth as it can participate in HOM formation and alter the HOM volatility distribution.

Abstract

Atmospheric new-particle formation (NPF) affects climate by contributing to a large fraction of the cloud condensation nuclei (CCN). Highly oxygenated organic molecules (HOMs) drive the early particle growth and therefore substantially influence the survival of newly formed particles to CCN. Nitrogen oxide (NO _x) is known to suppress the NPF driven by HOMs, but the underlying mechanism remains largely unclear. Here, we examine the response of particle growth to the changes of HOM formation caused by NO _x. We show that NO _x suppresses particle growth in general, but the suppression is rather nonuniform and size dependent, which can be quantitatively explained by the shifted HOM volatility after adding NO _x. By illustrating how NO _x affects the early growth of new particles, a critical step of CCN formation, our results help provide a refined assessment of the potential climatic effects caused by the diverse changes of NO _x level in forest regions around the globe.

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Most cited references 53

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Direct observations of atmospheric aerosol nucleation.

Markku Kulmala, Jenni Kontkanen, Heikki Junninen … (2013)

Atmospheric nucleation is the dominant source of aerosol particles in the global atmosphere and an important player in aerosol climatic effects. The key steps of this process occur in the sub-2-nanometer (nm) size range, in which direct size-segregated observations have not been possible until very recently. Here, we present detailed observations of atmospheric nanoparticles and clusters down to 1-nm mobility diameter. We identified three separate size regimes below 2-nm diameter that build up a physically, chemically, and dynamically consistent framework on atmospheric nucleation--more specifically, aerosol formation via neutral pathways. Our findings emphasize the important role of organic compounds in atmospheric aerosol formation, subsequent aerosol growth, radiative forcing and associated feedbacks between biogenic emissions, clouds, and climate.

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Impact of nucleation on global CCN

J Merikanto, D. Spracklen, G. W. Mann … (2009)

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The role of low-volatility organic compounds in initial particle growth in the atmosphere

Jasmin Tröstl, Wayne Chuang, Hamish Gordon … (2016)

The growth of nucleated organic particles has been investigated in controlled laboratory experiments under atmospheric conditions; initial growth is driven by organic vapours of extremely low volatility, and accelerated by more abundant vapours of slightly higher volatility, leading to markedly different modelled concentrations of atmospheric cloud condensation nuclei when this growth mechanism is taken into account. Supplementary information The online version of this article (doi:10.1038/nature18271) contains supplementary material, which is available to authorized users. The effect of atmospheric aerosols on clouds and the radiative forcing of the climate system remains poorly understood. It is thought that nucleation of aerosol particles from atmospheric vapours rarely proceeds in the absence of sulfuric acid. Now two papers in this week’s Nature point to a previously unappreciated role for highly oxygenated molecules (HOMs) in promoting new particle formation and growth, essentially a mechanism that produces aerosols in the absence of pollution. Jasper Kirkby et al . show that aerosol particles can form as a result of ion-induced nucleation of HOMs in the absence of sulfuric acid under conditions relevant to the atmosphere in the CLOUD chamber at CERN. Jasmin Tröstl et al . examined the role of organic vapours in the initial growth of nucleated organic particles in the absence of sulfuric acid in the CERN CLOUD chamber under atmospheric conditions. They find that the organic vapours driving initial growth have extremely low volatilities. With increasing particle size, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility. Supplementary information The online version of this article (doi:10.1038/nature18271) contains supplementary material, which is available to authorized users. About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday 1 . Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres 2 , 3 . In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles 4 , thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth 5 , 6 , leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer 7 , 8 , 9 , 10 . Although recent studies 11 , 12 , 13 predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon 2 , and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory) 2 , 14 , has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown 15 that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10 −4.5 micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10 −4.5 to 10 −0.5 micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations. Supplementary information The online version of this article (doi:10.1038/nature18271) contains supplementary material, which is available to authorized users.

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Author and article information

Journal

Journal ID (nlm-ta): Sci Adv

Journal ID (iso-abbrev): Sci Adv

Journal ID (publisher-id): SciAdv

Journal ID (hwp): advances

Title: Science Advances

Publisher: American Association for the Advancement of Science

ISSN (Electronic): 2375-2548

Publication date Collection: May 2020

Publication date (Electronic): 27 May 2020

Volume: 6

Issue: 22

Electronic Location Identifier: eaay4945

Affiliations

[1 ]Institute for Atmospheric and Earth System Research/INAR–Physics, Faculty of Science, University of Helsinki, 00560 Helsinki, Finland.

[2 ]Joint International Research Laboratory of Atmospheric and Earth System Sciences, School of Atmospheric Sciences, Nanjing University, Nanjing, China.

[3 ]CERN, CH-1211, Geneva, Switzerland.

[4 ]Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.

[5 ]Finnish Meteorological Institute, Erik Palménin aukio 1, 00560 Helsinki, Finland.

[6 ]University of Vienna, Faculty of Physics, Boltzmanngasse 5, 1090 Wien, Austria.

[7 ]University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria.

[8 ]Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China.

[9 ]University of Leeds, Leeds LS2 9JT, UK.

[10 ]Goethe University Frankfurt, Institute for Atmospheric and Environmental Sciences, Altenhöferallee 1, 60438 Frankfurt am Main, Germany.

[11 ]Division of Nuclear Physics, Department of Physics, Lund University, P. O. Box 118, SE-221 00 Lund, Sweden.

[12 ]CENTRA and FCUL, Universidade de Lisboa, Campo Grande, 1749-016 Lisboa, Portugal.

[13 ]Carnegie Mellon University Center for Atmospheric Particle Studies, 5000 Forbes Ave., Pittsburgh, PA 15213, USA.

[14 ]Aerodyne Research Inc., Billerica, MA 01821, USA.

[15 ]University of Eastern Finland, Department of Applied Physics, P.O. Box 1627, 70211 Kuopio, Finland.

[16 ]Department of Chemistry, University of California, Irvine, CA 92697, USA.

[17 ]California Institute of Technology, 210-41, Pasadena, CA 91125, USA.

[18 ]Department of Chemistry and Biochemistry, University of Colorado, Boulder, CO 80309, USA.

[19 ]School of Earth and Environmental Science, University of Manchester, Manchester M13 9PL, UK

[20 ]IDL Universidade da Beira Interior, Covilhã, Portugal.

[21 ]IONICON GesmbH, Innsbruck, Austria.

[22 ]Department of Environmental Science and Analytical Chemistry (ACES) and Bolin Centre for Climate Research, Stockholm University, 10691 Stockholm, Sweden.

[23 ]Helsinki Institute of Physics, FI-00014 Helsinki, Finland.

Author notes

[*]

These authors contributed equally to this work.

[† ]Corresponding author. Email: chao.yan@ 123456helsinki.fi (C.Y.); katrianne.lehtipalo@ 123456helsinki.fi (K.L.)

[‡]

Present address: Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany.

[§]

Present address: Université Clermont Auvergne, CNRS, Laboratoire de Météorologie Physique (LaMP), F-63000 Clermont-Ferrand, France.

[||]

Present address: Carnegie Mellon University, Forbes Avenue, Pittsburgh, PA 15213, USA.

[¶]

Present address: Harvard University, 18 Oxford Street, Cambridge, MA 02138, USA.

[#]

Present address: Institute of Physics, University of Tartu, W. Ostwaldi 1, EE-50411 Tartu, Estonia.

[**]

Present address: Institute for Atmospheric and Climate Science, ETH Zurich, Switzerland.

[††]

Present address: Flight Research Laboratory, National Research Council of Canada, Ottawa K1V 9B4, Canada.

[‡‡]

Present address: NASA Langley Research Center, Hampton, VA 23681, USA.

[§§]

Present address: Department of Chemistry, University of Oslo, 0315 Oslo, Norway.

[||||]

Present address: Atmospheric Composition Research, Finnish Meteorological Institute, 00101 Helsinki, Finland.

[¶¶ ]

Present address: Department of Chemistry & CIRES, University of Colorado Boulder, 215 UCB, Boulder, CO 80309-0215, USA.

Author information

C. Yan http://orcid.org/0000-0002-5735-9597

W. Nie http://orcid.org/0000-0002-6048-0515

A. L. Vogel http://orcid.org/0000-0002-1293-6370

L. Dada http://orcid.org/0000-0003-1105-9043

K. Lehtipalo http://orcid.org/0000-0002-1660-2706

D. Stolzenburg http://orcid.org/0000-0003-1014-1360

R. Wagner http://orcid.org/0000-0001-7365-8020

M. P. Rissanen http://orcid.org/0000-0003-0463-8098

L. Ahonen http://orcid.org/0000-0002-2534-6898

L. Fischer http://orcid.org/0000-0002-3141-9088

C. Rose http://orcid.org/0000-0002-4524-221X

F. Bianchi http://orcid.org/0000-0003-2996-3604

H. Gordon http://orcid.org/0000-0002-1822-3224

O. Garmash http://orcid.org/0000-0002-9675-3271

P. Roldin http://orcid.org/0000-0002-4223-4708

A. Dias http://orcid.org/0000-0002-0842-4639

P. Ye http://orcid.org/0000-0002-6954-4028

V. Hofbauer http://orcid.org/0000-0001-9036-4446

A. Amorim http://orcid.org/0000-0003-0638-2321

P. S. Bauer http://orcid.org/0000-0002-0014-3082

A. Bergen http://orcid.org/0000-0003-1647-5513

A.-K. Bernhammer http://orcid.org/0000-0002-0614-3649

S. Buenrostro Mazon http://orcid.org/0000-0002-6788-7828

X. Chen http://orcid.org/0000-0002-7731-6842

A. Ding http://orcid.org/0000-0003-4481-5386

J. Dommen http://orcid.org/0000-0002-0006-0009

D. C. Draper http://orcid.org/0000-0002-2027-8822

J. Duplissy http://orcid.org/0000-0001-8819-0264

C. Frege http://orcid.org/0000-0001-7833-8771

L. Heikkinen http://orcid.org/0000-0001-7837-967X

C. R. Hoyle http://orcid.org/0000-0002-1369-9143

T. Jokinen http://orcid.org/0000-0002-1280-1396

J. Kangasluoma http://orcid.org/0000-0002-1639-1187

J. Kirkby http://orcid.org/0000-0003-2341-9069

J. Kontkanen http://orcid.org/0000-0002-5373-3537

A. Kürten http://orcid.org/0000-0002-8955-4450

M. J. Lawler http://orcid.org/0000-0003-0421-6629

R. L. Mauldin III http://orcid.org/0000-0002-8569-8561

U. Molteni http://orcid.org/0000-0002-1623-1933

L. Nichman http://orcid.org/0000-0003-3923-1589

T. Nieminen http://orcid.org/0000-0002-2713-715X

J. Nowak http://orcid.org/0000-0002-5697-9807

T. Petäjä http://orcid.org/0000-0002-1881-9044

F. Piel http://orcid.org/0000-0002-8191-8029

N. Sarnela http://orcid.org/0000-0003-1874-3235

A. Tomé http://orcid.org/0000-0001-9144-7120

J. Tröstl http://orcid.org/0000-0002-2807-0348

Q. Zha http://orcid.org/0000-0001-6301-7086

K. S. Carslaw http://orcid.org/0000-0002-6800-154X

J. Curtius http://orcid.org/0000-0003-3153-4630

R. C. Flagan http://orcid.org/0000-0001-5690-770X

A. Hansel http://orcid.org/0000-0002-1062-2394

A. Virtanen http://orcid.org/0000-0002-2917-5344

N. M. Donahue http://orcid.org/0000-0003-3054-2364

V.-M. Kerminen http://orcid.org/0000-0002-0706-669X

M. Kulmala http://orcid.org/0000-0003-3464-7825

M. Ehn http://orcid.org/0000-0002-0215-4893

D. R. Worsnop http://orcid.org/0000-0002-8928-8017

Article

Publisher ID: aay4945

DOI: 10.1126/sciadv.aay4945

PMC ID: 7253163

PubMed ID: 32518819

SO-VID: aa7f3f0d-3c11-41c3-a579-cf4580e9ae9d

Copyright © Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

License:

This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

History

Date received : 01 July 2019

Date accepted : 19 March 2020

Funding

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 316662

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 656994

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 600337

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

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Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

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Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 257360

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 227463

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 227463

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 616075

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 335478

Funded by: doi http://dx.doi.org/10.13039/100010661, Horizon 2020 Framework Programme;

Award ID: 742206

Funded by: doi http://dx.doi.org/10.13039/501100001711, Swiss National Science Foundation;

Award ID: 200020_135307

Funded by: doi http://dx.doi.org/10.13039/501100001711, Swiss National Science Foundation;

Award ID: 206620_141278

Funded by: doi http://dx.doi.org/10.13039/501100001711, Swiss National Science Foundation;

Award ID: 200021_140663

Funded by: doi http://dx.doi.org/10.13039/501100001711, Swiss National Science Foundation;

Award ID: 206021_144947/1

Funded by: doi http://dx.doi.org/10.13039/501100001862, Swedish Research Council Formas;

Award ID: 2015-749

Funded by: doi http://dx.doi.org/10.13039/501100002428, Austrian Science Fund;

Award ID: J3951-N36

Funded by: doi http://dx.doi.org/10.13039/501100004359, Vetenskapsrådet;

Award ID: 2011-5120

Funded by: doi http://dx.doi.org/10.13039/501100009999, Jiangsu Collaborative Innovation Center for Climate Change;

Funded by: the National Natural Science Foundation of China;

Award ID: D0512/41675145

Funded by: US Department of Energy;

Award ID: DE-SC0014469

Funded by: German Federal Ministry of Education and Research;

Award ID: 01LK0902A

Funded by: German Federal Ministry of Education and Research;

Award ID: 01LK1222A

Funded by: German Federal Ministry of Education and Research;

Award ID: 01LK1601A