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Abstract Aircraft observations have revealed ubiquitous new particle formation in the tropical upper troposphere over the Amazon1,2and the Atlantic and Pacific oceans3,4. Although the vapours involved remain unknown, recent satellite observations have revealed surprisingly high night-time isoprene mixing ratios of up to 1 part per billion by volume (ppbv) in the tropical upper troposphere5. Here, in experiments performed with the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber, we report new particle formation initiated by the reaction of hydroxyl radicals with isoprene at upper-tropospheric temperatures of −30 °C and −50 °C. We find that isoprene-oxygenated organic molecules (IP-OOM) nucleate at concentrations found in the upper troposphere, without requiring any more vapours. Moreover, the nucleation rates are enhanced 100-fold by extremely low concentrations of sulfuric acid or iodine oxoacids above 105 cm−3, reaching rates around 30 cm−3 s−1at acid concentrations of 106 cm−3. Our measurements show that nucleation involves sequential addition of IP-OOM, together with zero or one acid molecule in the embryonic molecular clusters. IP-OOM also drive rapid particle growth at 3–60 nm h−1. We find that rapid nucleation and growth rates persist in the presence of NOxat upper-tropospheric concentrations from lightning. Our laboratory measurements show that isoprene emitted by rainforests may drive rapid new particle formation in extensive regions of the tropical upper troposphere1,2, resulting in tens of thousands of particles per cubic centimetre.more » « less
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Zhang, Yue; Katira, Shachi; Lee, Andrew; Lambe, Andrew T.; Onasch, Timothy B.; Xu, Wen; Brooks, William A.; Canagaratna, Manjula R.; Freedman, Andrew; Jayne, John T.; et al (, Atmospheric Measurement Techniques)Glass transitions from liquid to semi-solid and solid phase states have important implications for reactivity, growth, and cloud-forming (cloud condensation nuclei and ice nucleation) capabilities of secondary organic aerosols (SOAs). The small size and relatively low mass concentration of SOAs in the atmosphere make it difficult to measure atmospheric SOA glass transitions using conventional methods. To circumvent these difficulties, we have adapted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols. Aerosol particles to be studied are deposited in the form of a thin film onto an interdigitated electrode (IDE) using electrostatic precipitation. Dielectric spectroscopy provides dipole relaxation rates for organic aerosols as a function of temperature (373 to 233 K) that are used to calculate the glass transition temperatures for several cooling or heating rates. IDE-enabled broadband dielectric spectroscopy (BDS) was successfully used to measure the kinetically controlled glass transition temperatures of aerosols consisting of glycerol and four other compounds with selected cooling and heating rates. The glass transition results agree well with available literature data for these five compounds. The results indicate that the IDE-BDS method can provide accurate glass transition data for organic aerosols under atmospheric conditions. The BDS data obtained with the IDE-BDS technique can be used to characterize glass transitions for both simulated and ambient organic aerosols and to model their climate effects.more » « less
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