Role of Iodine-Assisted Aerosol Particle Formation in Antarctica

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Abstract

New particle formation via the ion-mediated sulfuric acid and ammonia molecular clustering mechanism remains the most widely observed and experimentally verified pathway. Recent laboratory and molecular level observations indicate iodine-driven nucleation as a potentially important source of new particles, especially in coastal areas. In this study, we assess the role of iodine species in particle formation using the best available molecular thermochemistry data and coupled to a detailed 1-d column model which is run along air mass trajectories over the Southern Ocean and the coast of Antarctica. In the air masses traversing the open ocean, ion-mediated SA-NH ₃ clustering appears insufficient to explain the observed particle size distribution, wherein the simulated Aitken mode is lacking. Including the iodine-assisted particle formation improves the modeled Aitken mode representation with an increase in the number of freshly formed particles. This implies that more particles survive and grow to Aitken mode sizes via condensation of gaseous precursors and heterogeneous reactions. Under certain meteorological conditions, iodine-assisted particle formation can increase cloud condensation nuclei concentrations by 20%–100%.

Abstract

The impact of iodine-assisted particle formation in the Southern Ocean marine air masses is assessed. The study reports that iodine-assisted particle formation can play a significant role over open oceans, with potential implications to CCN concentrations.

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Most cited references 54

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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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W. A. Hoppel, R LARSON, G. M. Frick (1986)

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Author and article information

Journal

Journal ID (nlm-ta): Environ Sci Technol

Journal ID (iso-abbrev): Environ Sci Technol

Journal ID (publisher-id): es

Journal ID (coden): esthag

Title: Environmental Science & Technology

Publisher: American Chemical Society

ISSN (Print): 0013-936X

ISSN (Electronic): 1520-5851

Publication date (Electronic): 16 April 2024

Publication date Collection: 30 April 2024

Volume: 58

Issue: 17

Pages: 7314-7324

Affiliations

[† ]Department of Physics, Lund University , Professorsgatan 1, Lund SE-22363, Sweden

[‡ ]Swedish Meteorological and Hydrological Institute (SMHI) , Norrköping SE-60176, Sweden

[§ ]Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki , P.O. Box 64, Helsinki 00014, Finland

[∥ ]Climate & Atmosphere Research Centre (CARE-C), The Cyprus Institute , P.O. Box 27456, Nicosia 1645, Cyprus

[⊥ ]Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt , Frankfurt am Main 60438, Germany

[# ]Swedish Environmental Research Institute IVL , Malmö SE-21119, Sweden

Author notes

[* ]Email: carlton.xavier@ 123456fysik.lu.se .

Author information

Carlton Xavier https://orcid.org/0000-0001-8120-0431

Article

DOI: 10.1021/acs.est.3c09103

PMC ID: 11064213

PubMed ID: 38626432

SO-VID: ee6f4ef3-9202-455a-8c54-8c3e1fe59e21

License:

Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

History

Date received : 03 November 2023

Date accepted : 04 April 2024

Date revision received : 03 April 2024

Funding

Funded by: VetenskapsrÃ¥det, doi 10.13039/501100004359;

Award ID: 2019-04853

Funded by: H2020 European Research Council, doi 10.13039/100010663;

Award ID: 714621

Funded by: VetenskapsrÃ¥det, doi 10.13039/501100004359;

Award ID: 2019-05006

Funded by: Crafoordska Stiftelsen, doi 10.13039/501100003173;

Award ID: 20210969

Funded by: Lunds Universitet, doi 10.13039/501100003252;

Award ID: NA