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    Formation and growth of nucleated particles into cloud condensation nuclei: Model-measurement comparison
    (München : European Geopyhsical Union, 2013) Westervelt, D.M.; Pierce, J.R.; Riipinen, I.; Trivitayanurak, W.; Hamed, A.; Kulmala, M.; Laaksonen, A.; Decesari, S.; Adams, P.J.
    Aerosol nucleation occurs frequently in the atmosphere and is an important source of particle number. Observations suggest that nucleated particles are capable of growing to sufficiently large sizes that they act as cloud condensation nuclei (CCN), but some global models have reported that CCN concentrations are only modestly sensitive to large changes in nucleation rates. Here we present a novel approach for using long-term size distribution observations to evaluate a global aerosol model's ability to predict formation rates of CCN from nucleation and growth events. We derive from observations at five locations nucleation-relevant metrics such as nucleation rate of particles at diameter of 3 nm (J3), diameter growth rate (GR), particle survival probability (SP), condensation and coagulation sinks, and CCN formation rate (J100). These quantities are also derived for a global microphysical model, GEOS-Chem-TOMAS, and compared to the observations on a daily basis. Using GEOS-Chem-TOMAS, we simulate nucleation events predicted by ternary (with a 10−5 tuning factor) or activation nucleation over one year and find that the model slightly understates the observed annual-average CCN formation mostly due to bias in the nucleation rate predictions, but by no more than 50% in the ternary simulations. At the two locations expected to be most impacted by large-scale regional nucleation, Hyytiälä and San Pietro Capofiume, predicted annual-average CCN formation rates are within 34 and 2% of the observations, respectively. Model-predicted annual-average growth rates are within 25% across all sites but also show a slight tendency to underestimate the observations, at least in the ternary nucleation simulations. On days that the growing nucleation mode reaches 100 nm, median single-day survival probabilities to 100 nm for the model and measurements range from less than 1–6% across the five locations we considered; however, this does not include particles that may eventually grow to 100 nm after the first day. This detailed exploration of new particle formation and growth dynamics adds support to the use of global models as tools for assessing the contribution of microphysical processes such as nucleation to the total number and CCN budget.
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    Chemical composition of cloud water in the puerto rican tropical trade wind cumuli
    (Dordrecht : Springer, 2009) Gioda, A.; Mayol-Bracero, O.L.; Morales-García, F.; Collett, J.; Decesari, S.; Emblico, L.; Facchini, M.C.; Morales-De Jesús, R.J.; Mertes, S.; Borrmann, S.; Walter, S.; Schneider, J.
    As part of the Rain In Cumulus over the Ocean Experiment (RICO) and the Puerto Rico Aerosol and Cloud Study (PRACS), cloud water was collected at East Peak (EP) in Puerto Rico. The main objective of this study was to determine the concentrations of water-soluble species (Cl-, NO3 -, SO4 2-, NH4 +, Ca 2+, H+, Mg2+, K+, and Na +) in water samples taken from clouds influenced by tropical trade winds. The most abundant inorganic species were Na+ (average 465 μeq l-1) and Cl- (434 μeq l-1), followed by Mg2+ (105 μeq l-1), SO4 2- (61 μeq l-1), and NO3 - (25 μeq l -1). High concentrations of nss-SO4 2 (28 μeq l-1), NO3 - (86 μeq l-1), and H+ (14.5 μeq l-1) were measured with a shift in air masses origin from the North Atlantic to North American continent, which reflected a strong anthropogenic influence on cloud chemistry at EP. Long-range transport of particles and acid gases seems to be the factor responsible for fluctuations in concentrations and pH of cloud water at East Peak. When under trade wind influences the liquid phase concentrations of all inorganic substances were similar to those found in clouds in other clean maritime environments. © 2008 Springer Science+Business Media B.V.