Particle hygroscopic growth at 90% RH (relative humidity), cloud condensation nuclei (CCN) activity, and size-resolved chemical composition were concurrently measured in the Thüringer Wald mid-level mountain range in central Germany in the fall of 2010. The median hygroscopicity parameter values, κ, of 50, 75, 100, 150, 200, and 250 nm particles derived from hygroscopicity measurements are respectively 0.14, 0.14, 0.17, 0.21, 0.24, and 0.28 during the sampling period. The closure between HTDMA (Hygroscopicity Tandem Differential Mobility Analyzers)-measured (κ_HTDMA) and chemical composition-derived (κ_chem) hygroscopicity parameters was performed based on the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. Using size-averaged chemical composition, the κ values are substantially overpredicted (30 and 40% for 150 and 100 nm particles). Introducing size-resolved chemical composition substantially improved closure. We found that the evaporation of NH₄NO₃, which may happen in a HTDMA system, could lead to a discrepancy in predicted and measured particle hygroscopic growth. The hygroscopic parameter of the organic fraction, κ_org, is positively correlated with the O : C ratio (κ_org = 0.19 × (O : C) − 0.03). Such correlation is helpful to define the κ_org value in the closure study. κ derived from CCN measurement was around 30% (varied with particle diameters) higher than that determined from particle hygroscopic growth measurements (here, hydrophilic mode is considered only). This difference might be explained by the surface tension effects, solution non-ideality, gas-particle partitioning of semivolatile compounds, and the partial solubility of constituents or non-dissolved particle matter. Therefore, extrapolating from HTDMA data to properties at the point of activation should be done with great care. Finally, closure study between CCNc (cloud condensation nucleus counter)-measured (κ_CCN) and chemical composition (κ_{CCN, chem}) was performed using CCNc-derived κ values for individual components. The results show that the κ_CCN can be well predicted using particle size-resolved chemical composition and the ZSR mixing rule

Abstract. The marine aerosol arriving at Barbados (Ragged Point) was characterized during two 3-week long measurement periods in November 2010 and April 2011, in the context of the measurement campaign CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados). Through a comparison between groundbased and airborne measurements it was shown that the former are representative of the marine boundary layer at least up to cloud base. In general, total particle number concentrations (N total ) ranged from as low as 100 up to 800 cm −3 , while number concentrations for cloud condensation nuclei (N CCN ) at a supersaturation of 0.26 % ranged from some 10 to 600 cm −3 . N total and N CCN depended on the air mass origin. Three distinct types of air masses were found. One type showed elevated values for both N total and N CCN and could be attributed to long-range transport from Africa, by which biomass burning particles from the Sahel region and/or mineral dust particles from the Sahara were advected. The second and third type both had values for N CCN below 200 cm −3 and a clear minimum in the particle number size distribution (NSD) around 70 to 80 nm (Hoppel minimum). While for one of these two types the accumulation mode was dominating (albeit less so than for air masses advected from Africa), the Aitken mode dominated the other and contributed more than 50 % of all particles. These Aitken mode particles likely were formed by new particle formation no more than 3 days prior to the measurements. Hygroscopicity of particles in the CCN size range was determined from CCN measurements to be κ = 0.66 on average, which suggests that these particles contain mainly sulfate and do not show a strong influence from organic material, which might generally be the case for the months during which measurements were made. The average κ could be used to derive N CCN from measured number size distributions, showing that this is a valid approach to obtain N CCN . Although the total particulate mass sampled on filters was found to be dominated by Na + and Cl − , this was found to be contributed by a small number of large particles (> 500 nm, mostly even in the super-micron size range). Based on a three-modal fit, a sea spray mode observed in the NSDs was found to contribute 90 % to the total particulate mass but only 4 to 10 % to N total and up to 15 % to N CCN . This is in accordance with finding no correlation between N total and wind speed.

.[1] Humic-like substances (HULIS) constitute a significant fraction of aerosol particles in different environments. Studies of the role of HULIS in hygroscopic growth and cloud condensation nuclei (CCN) activity of aerosol particles are scarce, and results differ significantly. In this work the hygroscopic growth and CCN activity of water extracts (WE) and HULIS extracted from particulate matter (PM) collected at a polluted urban site (Copenhagen, Denmark), a rural site (Melpitz, Germany) and the remote site Storm Peak Laboratory (Colorado, USA) were investigated. Measurements of inorganic ions, elemental carbon, organic carbon and water soluble organic carbon (WSOC) within the PM confirmed that the sources of aerosol particles most likely differed for the three samples. The hygroscopic properties of the filtered WE were characterized by hygroscopicity parameters for subsaturated conditions (k GF ) of 0.25, 0.41 and 0.22, and for supersaturated conditions k CCN were 0.23, 0.29 and 0.22 respectively for the urban, rural and remote WE samples. The measured hygroscopic growth and CCN activity were almost identical for the three HULIS samples and could be well represented by k GF = 0.07 and k CCN = 0.08-0.10 respectively. Small amounts of inorganic ions were present in the HULIS samples so the actual values for pure HULIS are expected to be slightly lower (k GF * = 0.04-0.06 and k CCN * = 0.07-0.08). The HULIS samples are thus less hygroscopic compared to most previous studies. To aid direct comparison of hygroscopic properties of HULIS from different studies, we recommend that the fraction of inorganic species in the HULIS samples always is measured and reported.Citation: Kristensen, T. B., et al. (2012), Hygroscopic growth and CCN activity of HULIS from different environments,

Abstract. The CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados) project, focused on high resolution and collocated measurements of thermodynamic, turbulent, microphysical, and radiative properties of trade wind cumuli over Barbados, is introduced. The project is based on two one-month field campaigns in November 2010 (climatic wet season) and April 2011 (climatic dry season). Observations are based on helicopterborne and ground-based measurements in an area of 100 km 2 off the coast of Barbados. CARRIBA is accompanied by long-term observations at the Barbados Cloud Observatory located at the East coast of Barbados since early in 2010 and which provides a longer-term context for the CARRIBA measurements. The deployed instrumentation and sampling strategy are presented together with a classification of the meteorological conditions. The two campaigns were influenced by different air masses advected from the Caribbean area, the Atlantic Ocean, and the African continent which led to distinct aerosol conditions. Pristine conditions with low aerosol particle number concentrations of ∼100 cm 3 were alternating with periods influenced by Saharan dust or aerosol from biomass burning resulting in comparably high number concentrations of ∼ 500 cm 3 . The biomass burning aerosol was originating from both the Caribbean area and Africa. The shallow cumulus clouds responded to the different aerosol conditions with a wide range of mean droplet sizes and number concentrations. Two days with different aerosol and cloud microphysical properties but almost identical meteorological conditions have been analyzed in detail. The differences in the droplet number concentration and droplet sizes appear not to show any significant change for turbulent cloud mixing, but the relative roles of droplet inertia and sedimentation in initiating coalescence, as well as the cloud reflectivity, do change substantially.