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Published November 11, 2020 | Supplemental Material + Published
Journal Article Open

Determination of the collision rate coefficient between charged iodic acid clusters and iodic acid using the appearance time method

Abstract

Ions enhance the formation rate of atmospheric aerosol particles, which play an important role in Earth's radiative balance. Ion-induced nucleation involves the stepwise accretion of neutral monomers onto a molecular cluster containing an ion, which helps to stabilize the cluster against evaporation. Although theoretical frameworks exist to calculate the collision rate coefficients between neutral molecules and ions, they need to be experimentally confirmed, ideally under atmospherically relevant conditions of around 1000 ion pairs cm⁻³. Here, in experiments performed under atmospheric conditions in the CERN CLOUD chamber, we have measured the collision rate coefficients between neutral iodic acid (HIO₃) monomers and charged iodic acid molecular clusters containing up to 11 iodine atoms. Three methods were analytically derived to calculate ion-polar molecule collision rate coefficients. After evaluation with a kinetic model, the 50% appearance time method is found to be the most robust. The measured collision rate coefficient, averaged over all iodine clusters, is (2.4 ± 0.8)×10⁻⁹ cm³ s⁻¹, which is close to the expectation from the surface charge capture theory.

Additional Information

© 2020 The Author(s). Published with license by Taylor & Francis Group, LLC. This is an Open Access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. Received 27 Jun 2020, Accepted 09 Oct 2020, Accepted author version posted online: 28 Oct 2020, Published online: 11 Nov 2020. X.-C.H., S.I., V.-M.K, R.C.F., J.Kon., J.Kir., T.K. and M.K. wrote and/or edited the manuscript. X.-C.H., M.Sip., J.Kir. and M.K. designed the experiments. X.-C.H. and J.P. derived equations. X.-C.H. designed, wrote and ran the kinetic model. S.I., T.K. and X.-C.H. performed quantum chemical calculations. X.-C.H., A.Y., M.P., R.B., M.Sim. analyzed data. All other authors participated in either the development and preparations of the CLOUD facility and the instruments, and/or collecting and analysing the data. We thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with important technical and financial resources and for providing a particle beam from the CERN Proton Synchrotron. This research has received supports from the Academy of Finland projects (316114, 307331, 310682, 266388, 306853, 296628, 299574, 326948); The European Research Council projects (692891, 616075, 764991, 316662, 742206, 714621); CSC – Finnish IT center; Austrian Science fund (FWF, J3951-N36, P27295-N20); the Swiss National Science Foundation (20FI20_159851, 200021_169090, 200020_172602, 20FI20_172622); the U.S. National Science Foundation Grants (AGS1447056, AGS1439551, AGS1801897, AGS1649147, AGS1801280, AGS1602086, AGS1801329); MSCA H2020 COFUND-FP-CERN-2014 fellowship (665779); German Federal Ministry of Education and Research: CLOUD-16 (01LK1601A); Academy of Finland Centre of Excellence in Atmospheric Sciences (grant no. 272041).

Attached Files

Published - Determination_of_the_collision_rate_coefficient_between_charged_iodic_acid_clusters_and_iodic_acid_using_the_appearance_time_method.pdf

Supplemental Material - uast_a_1839013_sm8224.docx

Files

Determination_of_the_collision_rate_coefficient_between_charged_iodic_acid_clusters_and_iodic_acid_using_the_appearance_time_method.pdf

Additional details

Created:
August 20, 2023
Modified:
October 23, 2023