4.8 Article

Using Novel Molecular-Level Chemical Composition Observations of High Arctic Organic Aerosol for Predictions of Cloud Condensation Nuclei

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 56, Issue 19, Pages 13888-13899

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.2c02162

Keywords

aerosol-cloud interactions; cloud droplet activation; CCN closure; atmospheric aerosol; aerosol chemistry; chemical ionization mass spectrometry (CIMS); High Arctic

Funding

  1. Swedish Research Council [2015- 00748, 2017-00567, 2016.0024]
  2. Swedish Research Council for Sustainable Development FORMAS [2017.0165, 865799]
  3. Knut and Alice Wallenberg Foundation (ACAS project) [865799, 821205]
  4. Knut and Alice Wallenberg Foundation [821205, 200021_169090]
  5. European Research Council [2016-03518]
  6. European Commission [2018-04255]
  7. Swiss National Science Foundation [2016-05100]
  8. Swiss Polar Institute
  9. Ocean Frontier Institute
  10. Natural Sciences and Engineering Research Council of Canada (NSERC)
  11. NSERC CREATE Transatlantic Ocean System Science and Technology (TOSST)
  12. strategic research area MERGE at Lund University, Sweden
  13. Bolin Centre for Climate Research at Stockholm University, Sweden
  14. Formas [2015-00748, 2017-00567] Funding Source: Formas

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Predictions of cloud droplet activation in the late summertime Arctic Ocean show that the aerosol in the High Arctic late summer is acidic and highly cloud active, with a substantial contribution from Aitken mode particles. The forecast underestimated the cloud condensation nuclei (CCN) number concentration by 4-8%.
Predictions of cloud droplet activation in the late summertime (September) central Arctic Ocean are made using kappa- Ko''hler theory with novel observations of the aerosol chemical composition from a high-resolution time-of-flight chemical ionization mass spectrometer with a filter inlet for gases and aerosols (FIGAERO-CIMS) and an aerosol mass spectrometer (AMS), deployed during the Arctic Ocean 2018 expedition onboard the Swedish icebreaker Oden. We find that the hygroscopicity parameter kappa of the total aerosol is 0.39 & PLUSMN; 0.19 (mean & PLUSMN; std). The predicted activation diameter of & SIM;25 to 130 nm particles is overestimated by 5%, leading to an underestimation of the cloud condensation nuclei (CCN) number concentration by 4-8%. From this, we conclude that the aerosol in the High Arctic late summer is acidic and therefore highly cloud active, with a substantial CCN contribution from Aitken mode particles. Variability in the predicted activation diameter is addressed mainly as a result of uncertainties in the aerosol size distribution measurements. The organic kappa was on average 0.13, close to the commonly assumed kappa of 0.1, and therefore did not significantly influence the predictions. These conclusions are supported by laboratory experiments of the activation potential of seven organic compounds selected as representative of the measured aerosol.

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