[1] The recently developed immersion mode cooling chamber has been used as an extension of the Zurich ice nucleation chamber (ZINC) in order to measure the ice nucleation efficiency of size-selected kaolinite particles in the immersion mode. Particles with selected diameters of 200, 400, and 800 nm have been activated as cloud condensation nuclei in order to obtain water droplets with single immersed particles. After continuous cooling of the droplets to the experimental temperature in ZINC, the frozen fraction of the droplets was measured with a recently developed depolarization detector, the ice optical detector (IODE). Temperatures below −30°C were necessary to freeze 50% of the droplets throughout the investigated size range. Although not very strong, a size dependence of the freezing efficiency has been observed. The median freezing temperature increases from −35°C for 200 nm kaolinite particles to −33°C for 800 nm particles. An experiment with 200 nm ammonium sulfate particles in the same temperature range resulted in no significant frozen fraction of the droplets. This suggests that the ice crystals observed in experiments with kaolinite particles nucleated heterogeneously. The temperature-dependent frozen fraction of water droplets has been fitted with different theoretical models. Comparison of the resulting fit curves with the data suggests that including the concept of active sites in the description of the ice nucleus surface is more appropriate than the approximation of a constant contact angle.Citation: Lüönd, F., O. Stetzer, A. Welti, and U. Lohmann (2010), Experimental study on the ice nucleation ability of size-selected kaolinite particles in the immersion mode,

Abstract. Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental parameters associated with these techniques.Within the framework of INUIT (Ice Nuclei Research Unit), we distributed an illite-rich sample (illite NX) as a representative surrogate for atmospheric mineral dust particles to investigators to perform immersion freezing experiments using different IN measurement methods and to obtain Published by Copernicus Publications on behalf of the European Geosciences Union. N. Hiranuma et al.: A comparison of 17 IN measurement techniquesIN data as a function of particle concentration, temperature (T ), cooling rate and nucleation time. A total of 17 measurement methods were involved in the data intercomparison. Experiments with seven instruments started with the test sample pre-suspended in water before cooling, while 10 other instruments employed water vapor condensation onto drydispersed particles followed by immersion freezing. The resulting comprehensive immersion freezing data set was evaluated using the ice nucleation active surface-site density, n s , to develop a representative n s (T ) spectrum that spans a wide temperature range (−37 • C < T < −11 • C) and covers 9 orders of magnitude in n s .In general, the 17 immersion freezing measurement techniques deviate, within a range of about 8 • C in terms of temperature, by 3 orders of magnitude with respect to n s . In addition, we show evidence that the immersion freezing efficiency expressed in n s of illite NX particles is relatively independent of droplet size, particle mass in suspension, particle size and cooling rate during freezing. A strong temperature dependence and weak time and size dependence of the immersion freezing efficiency of illite-rich clay mineral particles enabled the n s parameterization solely as a function of temperature. We also characterized the n s (T ) spectra and identified a section with a steep slope between −20 and −27 • C, where a large fraction of active sites of our test dust may trigger immersion freezing. This slope was followed by a region with a gentler slope at temperatures below −27 • C. While the agreement between different instruments was reasonable below ∼ −27 • C, there seemed to be a different trend in the temperature-dependent ice nucleation activity from the suspension and dry-dispersed particle measurements for this mineral dust, in particular at higher temperatures. For instance,...

Abstract. We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer–fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5–3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42−] + [NO3−]) is only 0.5–0.7 mol mol−1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8–28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD and we attribute this in part to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available.

The recently developed Zurich Ice Nucleation Chamber (ZINC) was used to explore ice nucleation of size-selected mineral dust particles at temperatures between −20 • C and −55 • C. Four different mineral dust species have been tested: montmorillonite, kaolinite, illite and Arizona test dust (ATD). The selected particle diameters are 100 nm, 200 nm, 400 nm and 800 nm. Relative humidities with respect to ice (RH i ) required to activate 1% of the dust particles as ice nuclei (IN) are reported as a function of temperature. An explicit size dependence of the ice formation efficiency has been observed for all dust types. 800 nm particles required the lowest RH i to activate. Deposition nucleation below water saturation was found only below −30 • C or −35 • C dependent on particle size. Minimum RH i for 1% activation were 105% for illite, kaolinite and montmorillonite at −40 • C, respectively 110% for ATD at −45 • C. In addition, a possible parameterisation for the measured activation spectra is proposed, which could be used in modeling studies.