Impact of humidity on aerosol growth from methanesulfonic acid.
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Yu Wenjuan, Baalbaki Rima, Shen Jiali, DeVivo Jenna, Caudillo-Plath Lucía, Sommer Eva, Heitto Arto, Klebach Hannah, Russell Douglas M, Amorim António, Beckmann Hannah, Bhattacharyya Nirvan, Blankenship Vine, Chassaing Anouck, Cruz-Simbron Romulo, Dada Lubna, Jacobshagen Aenne, Judmaier Bernhard, Kaniyodical Sebastian Milin, Konrat Ruth, Krüger Timm, Kunkler Felix, Lietzke Clara J, Liu Lu, Mauldin Roy, Mentler Bernhard, Morawiec Aleksandra, Rato Pedro, Rörup Birte, Ruhl Samuel, Scholz Wiebke, Simon Mario, Stinchfield Alexandria, Tomé António, Tong Yandong, Top Jens, Umo Nsikanabasi Silas, Unfer Gabriela R, Vettikkat Lejish, Weissbacher Jakob, Xenofontos Christos, Yang Boxing, Zauner-Wieczorek Marcel, Zhang Jiangyi, Zheng Zhensen, Christoudias Theodoros, Curtius Joachim, El Haddad Imad, Flagan Richard, Hansel Armin, Harder Hartwig, Kürten Andreas, Möhler Ottmar, Petäjä Tuukka, Volkamer Rainer, Winkler Paul M, Worsnop Douglas R, Kulmala Markku, Donahue Neil M, Kirkby Jasper, Yli-Juuti Taina, Riipinen Ilona, He Xu-Cheng, Lehtipalo Katrianne
Аннотация
Methanesulfonic acid (MSA; CH3SO3H), produced by oxidation of dimethylsulfide (DMS; CH3SCH3), is a key precursor for aerosols in the marine boundary layer and free troposphere. Laboratory experiments show that MSA contributes to both particle nucleation and subsequent growth, often together with sulfuric acid (H2SO4) and base vapours such as ammonia (NH3). However, the influence of relative humidity (RH) on MSA condensation to particles remains uncertain. Here, in experiments conducted under low NH3 conditions (<4 parts per trillion by volume, pptv) at the CERN Cosmics Leaving OUtdoor Droplets (CLOUD) chamber, we find that RH critically regulates the participation of MSA in the initial growth of newly formed particles. Between +10 °C and -10 °C, MSA drives rapid particle growth at high RH (>50%), whereas its contribution at low RH (<16%) is negligible. When comparing with aerosol process models such as the Model for Acid-Base Chemistry in Nanoparticle Growth (MABNAG), we find that the model fails to match our laboratory results. In particular, our measurements show that MSA drives rapid particle growth at substantially warmer temperatures and lower relative humidities than predicted by the Extended Aerosol Inorganic Model (E-AIM). This highlights the importance of further experiments to fully quantify the effect of RH on MSA particle growth and evaporation, and incorporating these measurements in aerosol models. This will be essential for accurately representing the important role of MSA in marine aerosols in global models, particularly in cold, low-NH3 environments like polar regions and the free troposphere.