Birte Rörup, Xu-Cheng He, Jiali Shen, Rima Baalbaki, Lubna Dada, Mikko Sipilä, Jasper Kirkby, Markku Kulmala, Antonio Amorim, Andrea Baccarini, David M. Bell, Lucía Caudillo-Plath, Jonathan Duplissy, Henning Finkenzeller, Andreas Kürten, Houssni Lamkaddam, Chuan Ping Lee, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Antti Onnela, Maxim Philippov, Carolin Wiebke Scholz, Mario Simon, Dominik Stolzenburg, Yee Jun Tham, António Tomé, Andrea C. Wagner, Mingyi Wang, Dongyu Wang, Yonghong Wang, Stefan K. Weber, Marcel Zauner-Wieczorek, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Imad El Haddad, Richard C. Flagan, Armin Hansel, Ottmar Möhler, Tuukka Petäjä, Rainer Volkamer, Douglas Worsnop and Katrianne Lehtipalo
{"title":"Temperature, humidity, and ionisation effect of iodine oxoacid nucleation","authors":"Birte Rörup, Xu-Cheng He, Jiali Shen, Rima Baalbaki, Lubna Dada, Mikko Sipilä, Jasper Kirkby, Markku Kulmala, Antonio Amorim, Andrea Baccarini, David M. Bell, Lucía Caudillo-Plath, Jonathan Duplissy, Henning Finkenzeller, Andreas Kürten, Houssni Lamkaddam, Chuan Ping Lee, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Antti Onnela, Maxim Philippov, Carolin Wiebke Scholz, Mario Simon, Dominik Stolzenburg, Yee Jun Tham, António Tomé, Andrea C. Wagner, Mingyi Wang, Dongyu Wang, Yonghong Wang, Stefan K. Weber, Marcel Zauner-Wieczorek, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Imad El Haddad, Richard C. Flagan, Armin Hansel, Ottmar Möhler, Tuukka Petäjä, Rainer Volkamer, Douglas Worsnop and Katrianne Lehtipalo","doi":"10.1039/D4EA00013G","DOIUrl":null,"url":null,"abstract":"<p >Iodine oxoacids are recognised for their significant contribution to the formation of new particles in marine and polar atmospheres. Nevertheless, to incorporate the iodine oxoacid nucleation mechanism into global simulations, it is essential to comprehend how this mechanism varies under various atmospheric conditions. In this study, we combined measurements from the CLOUD (Cosmic Leaving OUtdoor Droplets) chamber at CERN and simulations with a kinetic model to investigate the impact of temperature, ionisation, and humidity on iodine oxoacid nucleation. Our findings reveal that ion-induced particle formation rates remain largely unaffected by changes in temperature. However, neutral particle formation rates experience a significant increase when the temperature drops from +10 °C to −10 °C. Running the kinetic model with varying ionisation rates demonstrates that the particle formation rate only increases with a higher ionisation rate when the iodic acid concentration exceeds 1.5 × 10<small><sup>7</sup></small> cm<small><sup>−3</sup></small>, a concentration rarely reached in pristine marine atmospheres. Consequently, our simulations suggest that, despite higher ionisation rates, the charged cluster nucleation pathway of iodic acid is unlikely to be enhanced in the upper troposphere by higher ionisation rates. Instead, the neutral nucleation channel is likely to be the dominant channel in that region. Notably, the iodine oxoacid nucleation mechanism remains unaffected by changes in relative humidity from 2% to 80%. However, under unrealistically dry conditions (below 0.008% RH at +10 °C), iodine oxides (I<small><sub>2</sub></small>O<small><sub>4</sub></small> and I<small><sub>2</sub></small>O<small><sub>5</sub></small>) significantly enhance formation rates. Therefore, we conclude that iodine oxoacid nucleation is the dominant nucleation mechanism for iodine nucleation in the marine and polar boundary layer atmosphere.</p>","PeriodicalId":72942,"journal":{"name":"Environmental science: atmospheres","volume":" 5","pages":" 531-546"},"PeriodicalIF":2.8000,"publicationDate":"2024-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ea/d4ea00013g?page=search","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental science: atmospheres","FirstCategoryId":"1085","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/ea/d4ea00013g","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
引用次数: 0
Abstract
Iodine oxoacids are recognised for their significant contribution to the formation of new particles in marine and polar atmospheres. Nevertheless, to incorporate the iodine oxoacid nucleation mechanism into global simulations, it is essential to comprehend how this mechanism varies under various atmospheric conditions. In this study, we combined measurements from the CLOUD (Cosmic Leaving OUtdoor Droplets) chamber at CERN and simulations with a kinetic model to investigate the impact of temperature, ionisation, and humidity on iodine oxoacid nucleation. Our findings reveal that ion-induced particle formation rates remain largely unaffected by changes in temperature. However, neutral particle formation rates experience a significant increase when the temperature drops from +10 °C to −10 °C. Running the kinetic model with varying ionisation rates demonstrates that the particle formation rate only increases with a higher ionisation rate when the iodic acid concentration exceeds 1.5 × 107 cm−3, a concentration rarely reached in pristine marine atmospheres. Consequently, our simulations suggest that, despite higher ionisation rates, the charged cluster nucleation pathway of iodic acid is unlikely to be enhanced in the upper troposphere by higher ionisation rates. Instead, the neutral nucleation channel is likely to be the dominant channel in that region. Notably, the iodine oxoacid nucleation mechanism remains unaffected by changes in relative humidity from 2% to 80%. However, under unrealistically dry conditions (below 0.008% RH at +10 °C), iodine oxides (I2O4 and I2O5) significantly enhance formation rates. Therefore, we conclude that iodine oxoacid nucleation is the dominant nucleation mechanism for iodine nucleation in the marine and polar boundary layer atmosphere.