Temperature, humidity, and ionisation effect of iodine oxoacid nucleation

IF 2.8 Q3 ENVIRONMENTAL SCIENCES Environmental science: atmospheres Pub Date : 2024-03-21 DOI:10.1039/D4EA00013G
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
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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.

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碘氧化酸成核的温度、湿度和电离效应
碘氧酸盐被认为对海洋和极地大气中新粒子的形成具有重要作用。然而,要将碘氧酸盐成核机制纳入全球模拟,就必须了解该机制在各种大气条件下的变化情况。在这项研究中,我们结合了欧洲核子研究中心 CLOUD(宇宙离开室外液滴)室的测量结果和动力学模型的模拟结果,研究了温度、电离和湿度对碘草酸成核的影响。我们的研究结果表明,离子诱导的粒子形成率基本上不受温度变化的影响。然而,当温度从+10 °C降至-10 °C时,中性粒子的形成率会显著增加。在不同电离率下运行动力学模型的结果表明,只有当碘酸浓度超过 1.5 × 107 cm-3 时,颗粒形成率才会随着电离率的升高而增加,而在原始海洋大气中很少达到这种浓度。因此,我们的模拟结果表明,尽管电离率较高,但在对流层上部,碘酸的带电簇成核途径不太可能因电离率较高而增强。相反,中性成核途径可能是该区域的主要途径。值得注意的是,碘草酸成核机制不受相对湿度从 2% 到 80% 变化的影响。然而,在不切实际的干燥条件下(相对湿度低于 0.008%,温度为 +10 °C),碘氧化物(I2O4 和 I2O5)会显著提高形成率。因此,我们得出结论,碘氧化物成核是海洋和极地边界层大气中碘成核的主要成核机制。
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