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Particle hygroscopicity during atmospheric new particle formation events: Implications for the chemical species contributing to particle growth

2013, Wu, Z., Birmili, W., Poulain, L., Poulain, L., Merkel, M., Fahlbusch, B., Van Pinxteren, D., Herrmann, H., Wiedensohler, A.

This study examines the hygroscopicity of newly formed particles (diameters range 25-45 nm) during two atmospheric new particle formation (NPF) events in the German mid-level mountains during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) field experiment. At the end of the NPF event involving clear particle growth, we measured an unusually high soluble particle fraction of 58.5% at 45 nm particle size. The particle growth rate contributed through sulfuric acid condensation only accounts for around 6.5% of the observed growth rate. Estimations showed that sulfuric acid condensation explained, however, only around 10% of that soluble particle fraction. Therefore, the formation of additional water-soluble matter appears imperative to explain the missing soluble fraction. Although direct evidence is missing, we consider water-soluble organics as candidates for this mechanism. For the case with clear growth process, the particle growth rate was determined by two alternative methods based on tracking the mode diameter of the nucleation mode. The mean particle growth rate obtained from the inter-site data comparison using Lagrangian consideration is 3.8 (± 2.6) nm h-1. During the same period, the growth rate calculated based on one site data is 5.0 nm h-1 using log-normal distribution function method. In light of the fact that considerable uncertainties could be involved in both methods, we consider both estimated growth rates consistent.

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Some insights into the condensing vapors driving new particle growth to CCN sizes on the basis of hygroscopicity measurements

2015, Wu, Z.J., Poulain, L., Birmili, W., Größ, J., Niedermeier, N., Wang, Z.B., Herrmann, H., Wiedensohler, A.

New particle formation (NPF) and growth is an important source of cloud condensation nuclei (CCN). In this study, we investigated the chemical species driving new particle growth to the CCN sizes on the basis of particle hygroscopicity measurements carried out at the research station Melpitz, Germany. Three consecutive NPF events occurred during summertime were chosen as examples to perform the study. Hygroscopicity measurements showed that the (NH4)2SO4-equivalent water-soluble fraction accounts for 20 and 16 % of 50 and 75 nm particles, respectively, during the NPF events. Numerical analysis showed that the ratios of H2SO4 condensational growth to the observed particle growth were 20 and 13 % for 50 and 75 nm newly formed particles, respectively. Aerosol mass spectrometer measurements showed that an enhanced mass fraction of sulfate and ammonium in the newly formed particles was observed when new particles grew to the sizes larger than 30 nm shortly after the particle formation period. At a later time, the secondary organic species played a key role in the particle growth. Both hygroscopicity and aerosol mass spectrometer (AMS) measurements and numerical analysis confirmed that organic compounds were major contributors driving particle growth to CCN sizes. The critical diameters at different supersaturations estimated using AMS data and κ-Köhler theory increased significantly during the later course of NPF events. This indicated that the enhanced organic mass fraction caused a reduction in CCN efficiency of newly formed particles. Our results implied that the CCN production associated with atmospheric nucleation may be overestimated if assuming that newly formed particles can serve as CCN once they grow to a fixed particle size, an assumption made in some previous studies, especially for organic-rich environments. In our study, the enhancement in CCN number concentration associated with individual NPF events were 63, 66, and 69 % for 0.1, 0.4, and 0.6 % supersaturation, respectively.