Published December 15, 2023 | Version Published
Journal Article Open

Iodine oxoacids enhance nucleation of sulfuric acid particles in the atmosphere

Abstract

The main nucleating vapor in the atmosphere is thought to be sulfuric acid (H₂SO₄), stabilized by ammonia (NH₃). However, in marine and polar regions, NH₃ is generally low, and H₂SO₄ is frequently found together with iodine oxoacids [HIOₓ, i.e., iodic acid (HIO₃) and iodous acid (HIO₂)]. In experiments performed with the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we investigated the interplay of H₂SO₄and HIOₓ during atmospheric particle nucleation. We found that HIOₓ greatly enhances H₂SO₄(-NH₃) nucleation through two different interactions. First, HIO₃ strongly binds with H₂SO₄ in charged clusters so they drive particle nucleation synergistically. Second, HIO₂ substitutes for NH₃ , forming strongly bound H₂SO₄-HIO₂ acid-base pairs in molecular clusters. Global observations imply that HIO x is enhancing H₂SO₄(-NH₃) nucleation rates 10- to 10,000-fold in marine and polar regions.

Copyright and License

© 2023 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. This is an article distributed under the terms of the Science Journals Default License.

Acknowledgement

We thank CERN for supporting CLOUD with important technical and financial resources and for providing a particle beam from the CERN Proton Synchrotron. We thank the CSC IT Center for Science in Espoo, Finland, for computing time.

Funding

This work was supported by Research Council of Finland ACCC Flagship nos. 337549 and 337552; Research Council of Finland professorship (302958); Research Council of Finland Centre of Excellence nos. 346371, 346372, and 346373; Research Council of Finland project nos. 335844, 334514, 345125, 325656, 316114, 314798, 325647, 353836, 341349, 346372, 296628, and 349659; European Research Council (ERC) project nos. 742206, 714621, 616075, and 101002728; Marie Skłodowska-Curie grant agreement nos. 316662, 701647, 895875, and 764991; National Natural Science Foundation of China grant nos. 42175118 and 22236004; the National Key Research and Development Program of China (2022YFC3701000, Task 1); Swiss National Science Foundation grant nos. 200021_169090, 200021_213071, 206021_198140, 200020_172602, and 20FI20_172622; US National Science Foundation grants nos. AGS-2132089, AGS-1801897, AGS-1801574, AGS-1801280, AGS-2027252, AGS-2215522, AGS-1602086, AGS-1801329, and AGS-2215527; German Federal Ministry of Education and Research (BMBF) project no. 01LK1601A; and Portuguese Science Foundation project CERN/FIS-COM/0028/2019. R.C.T. and M.K. thank the Jane and Aatos Erkko Foundation for funding. M.K. received funding from Prince Albert Foundation contract no. 2859. M.W. thanks the Schmidt Science Fellowship for support. X.-C.H. and M.K. thank the Jenny and Antti Wihuri Foundation for funding.

Contributions

X.-C.H., J.Kir., M.Sip., and M.K. planned the experiments. X.-C.H., M.Sim., B.R., J.S., H.F., D.S., A.B., Y.J.T., M.W., S.A., A.A.P., A.A., R.B., Z.B., L.C., B.C., L.D., J.D., I.E.H., R.C.F., M.G., M.H., V.H., W.K., J.Kre., A.K., H.L., B.L., N.G.A.M., V.M., H.E.M., G.M., R.M., D.M., R.L.M., B.M., A.O., T.P., J.P., M.P., M.P.R., S.S., W.S., B.S., M.Sur., A.T., A.C.W., D.W., Y.W., S.K.W., A.W., P.M.W., M.Z.-W., J.Kir., U.B., K.L., J.C., R.V., M.Sip., and M.K. prepared the CLOUD facility or measuring instruments. X.-C.H., M.Sim., S.I., B.R., J.S., H.F., D.S., A.B., Y.J.T., A.A., R.B., L.C., L.D., J.D., I.E.H., M.G., M.H., V.H., T.J., D.K., W.K., J.Kre., H.L., B.L., N.G.A.M., V.M., H.E.M., G.M., R.M., D.M., R.LM., B.M., J.P., A.R., W.S., R.C.T., A.C.W., D.W., S.K.W., M.Z.-W., J.Kir., J.C., and R.V. collected the data. X.-C.H., S.I., H.-B.X., H.F., D.S., R.Z., Y.J.T., L.C., L.D., R.C.F., F.M., W.S., R.C.T., S.K.W., P.M.W., T.K. and D.R.W. analyzed the data. X.-C.H., N.M.D. and J.Kir. wrote the manuscript with contributions from S.I., H.-B.X., B.R. and R.Z. X.-C.H., M.Sim., S.I., H.-B.X., B.R., J.S., H.F., D.S., R.Z., A.B., L.D., J.D., I.E.H., R.C.F., A.H., H.L., N.G.A.M., T.P., S.S., W.S., R.C.T., A.C.W., J.Kir., U.B., K.L., J.C., T.K., D.R.W., R.V., N.M.D., M.Sip. and M.K. commented on and edited the manuscript.

Data Availability

Data for all figures in the main text and supplementary materials are available at the Zenodo repository (43). Correspondence and additional requests for materials should be addressed to X.-C.H. (institutional email: xucheng.he@helsinki.fi; permanent email: xuchenghe93@gmail.com).

Conflict of Interest

The authors declare that they have no competing interests.

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Additional details

Identifiers

ISSN
1095-9203

Funding

European Research Council
742206
European Research Council
714621
European Research Council
616075
European Research Council
101002728
European Research Council
Marie Skłodowska-Curie fellowship 316662
European Research Council
Marie Skłodowska-Curie fellowship 701647
European Research Council
Marie Skłodowska-Curie fellowship 895875
European Research Council
Marie Skłodowska-Curie fellowship 764991
National Natural Science Foundation of China
42175118
National Natural Science Foundation of China
22236004
Swiss National Science Foundation
200021_169090
Swiss National Science Foundation
200021_213071
Swiss National Science Foundation
206021_198140
Swiss National Science Foundation
200020_172602
Swiss National Science Foundation
20FI20_172622
National Science Foundation
AGS-2132089
National Science Foundation
AGS-1801897
National Science Foundation
AGS-1801574
National Science Foundation
AGS-1801280
National Science Foundation
AGS-2027252
National Science Foundation
AGS-2215522
National Science Foundation
AGS-1602086
National Science Foundation
AGS-1801329
National Science Foundation
AGS-2215527
Fundação para a Ciência e Tecnologia
CERN/FIS-COM/0028/2019
Jane and Aatos Erkko Foundation
Prince Albert II of Monaco Foundation
2859
Schmidt Family Foundation
Jenny ja Antti Wihurin Rahasto