TY - JOUR
T1 - Temperature, humidity, and ionisation effect of iodine oxoacid nucleation
AU - Rörup, Birte
AU - He, Xucheng
AU - Shen, Jiali
AU - Baalbaki, Rima
AU - Dada, Lubna
AU - Sipilä, Mikko
AU - Kirkby, Jasper
AU - Kulmala, Markku
AU - Amorim, Antonio
AU - Baccarini, Andrea
AU - Bell, David M.
AU - Caudillo-Plath, Lucía
AU - Duplissy, Jonathan
AU - Finkenzeller, Henning
AU - Kürten, Andreas
AU - Lamkaddam, Houssni
AU - Lee, Chuan Ping
AU - Makhmutov, Vladimir
AU - Manninen, Hanna E.
AU - Marie, Guillaume
AU - Marten, Ruby
AU - Mentler, Bernhard
AU - Onnela, Antti
AU - Philippov, Maxim
AU - Scholz, Carolin Wiebke
AU - Simon, Mario
AU - Stolzenburg, Dominik
AU - Tham, Yee Jun
AU - Tomé, António
AU - Wagner, Andrea C.
AU - Wang, Mingyi
AU - Wang, Dongyu
AU - Wang, Yonghong
AU - Weber, Stefan K.
AU - Zauner-Wieczorek, Marcel
AU - Baltensperger, Urs
AU - Curtius, Joachim
AU - Donahue, Neil M.
AU - Haddad, Imad El
AU - Flagan, Richard C.
AU - Hansel, Armin
AU - Möhler, Ottmar
AU - Petäjä, Tuukka
AU - Volkamer, Rainer
AU - Worsnop, Douglas
AU - Lehtipalo, Katrianne
PY - 2024
Y1 - 2024
N2 - 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.
AB - 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.
KW - 114 Physical sciences
U2 - 10.1039/d4ea00013g
DO - 10.1039/d4ea00013g
M3 - Article
SN - 2634-3606
VL - 4
SP - 531
EP - 546
JO - Environmental science: Atmospheres
JF - Environmental science: Atmospheres
IS - 5
ER -