Multicomponent new particle formation from sulfuric acid, ammonia, and biogenic vapors

Creators: Lehtipalo, Katrianne; Kim, Changhyuk; Mai, Huajun; Flagan, Richard C.

Abstract

A major fraction of atmospheric aerosol particles, which affect both air quality and climate, form from gaseous precursors in the atmosphere. Highly oxygenated organic molecules (HOMs), formed by oxidation of biogenic volatile organic compounds, are known to participate in particle formation and growth. However, it is not well understood how they interact with atmospheric pollutants, such as nitrogen oxides (NO_x) and sulfur oxides (SO_x) from fossil fuel combustion, as well as ammonia (NH_3) from livestock and fertilizers. Here, we show how NO_x suppresses particle formation, while HOMs, sulfuric acid, and NH3 have a synergistic enhancing effect on particle formation. We postulate a novel mechanism, involving HOMs, sulfuric acid, and ammonia, which is able to closely reproduce observations of particle formation and growth in daytime boreal forest and similar environments. The findings elucidate the complex interactions between biogenic and anthropogenic vapors in the atmospheric aerosol system.

Additional Information

© 2018 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 License 4.0 (CC BY). Submitted 20 June 2018; Accepted 15 November 2018; Published 12 December 2018. We thank CERN for supporting CLOUD with technical and financial resources, and for providing a particle beam from the CERN Proton Synchrotron. We thank P. Carrie, L.-P. De Menezes, J. Dumollard, K. Ivanova, F. Josa, I. Krasin, R. Kristic, A. Laassiri, O. S. Maksumov, B. Marichy, H. Martinati, S. V. Mizin, R. Sitals, A. Wasem, and M. Wilhelmsson for their contributions to the experiment. We thank tofTools team for providing programs for mass spectrometry analysis. This research has received funding from the EC Seventh Framework Programme and European Union's Horizon 2020 Programme [Marie Curie ITN (no. 316662 "CLOUD-TRAIN") MSCA-IF (no. 656994 "nano-CAVa"), MC-COFUND (grant nos. 600377 and 665779), and ERC (project no. 692891 "DAMOCLES," no. 638703 "COALA," no. 616075 "NANODYNAMITE," no. 335478 "QAPPA," no. 742206 "ATM-GP," and no. 714621 "GASPARCON")], the German Federal Ministry of Education and Research (project nos. 01LK0902A, 01LK1222A, and 01LK1601A), the Swiss National Science Foundation [project nos. 200021_140663, 206021_144947/1, 20FI20_159851, 200020_172602, 20FI20_172622, 200021_169090, and the Starting Grant IPR-SHOP (BSSGI0_155846)], the Academy of Finland (Center of Excellence no. 307331 and project nos. 139995, 137749, 299574, 251007, 296628, and 306853), the Finnish Funding Agency for Technology and Innovation, the Väisälä Foundation, the Nessling Foundation, the Austrian Science Fund (FWF; project no. J3951-N36), the Austrian research funding association (FFG, project no. 846050), the Portuguese Foundation for Science and Technology (project no. CERN/FP/116387/2010), the Swedish Research Council Formas (project no. 2015-749), Knut and Alice Wallenberg Foundation (Academy Fellowship AtmoRemove), Vetenskapsrådet (grant no. 2011-5120), the Presidium of the Russian Academy of Sciences and Russian Foundation for Basic Research (grant nos. 08-02-91006-CERN and 12-02-91522-CERN), the U.S. National Science Foundation (grant nos. AGS1136479, AGS1447056, AGS1439551, CHE1012293, AGS1649147, and AGS1602086), the Wallace Research Foundation, the U.S. Department of Energy (grant DE-SC0014469), the NERC GASSP (project no. NE/J024252/1m), the Royal Society (Wolfson Merit Award), UK Natural Environment Research Council (grant no. NE/K015966/1), Dreyfus Award (EP-11-117), the French National Research Agency, the Nord-Pas de Calais, and European Funds for Regional Economic Development Labex-Cappa (grant no. ANR-11-LABX-0005-01). Author contributions: K.L., C.Y., D.R.W., and M.K. designed the experiments and wrote the paper. K.L., C.Y., L.D., F.B., M.X., R.W., and D.S. analyzed the main datasets. All other authors contributed to the design of the facility and preparation of the instruments or data collection and analysis and commented on the manuscript. The authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. Additional data related to this paper may be requested from the authors.

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