A global vertically resolved aerosol data set covering more than 10 years of observations at more than 20 measurement sites distributed from 63° N to 52° S and 72° W to 124° E has been achieved within the Raman and polarization lidar network Polly^NET. This network consists of portable, remote-controlled multiwavelength-polarization-Raman lidars (Polly) for automated and continuous 24/7 observations of clouds and aerosols. Polly^NET is an independent, voluntary, and scientific network. All Polly lidars feature a standardized instrument design with different capabilities ranging from single wavelength to multiwavelength systems, and now apply unified calibration, quality control, and data analysis. The observations are processed in near-real time without manual intervention, and are presented online at http://polly.tropos.de/. The paper gives an overview of the observations on four continents and two research vessels obtained with eight Polly systems. The specific aerosol types at these locations (mineral dust, smoke, dust-smoke and other dusty mixtures, urban haze, and volcanic ash) are identified by their Ångström exponent, lidar ratio, and depolarization ratio. The vertical aerosol distribution at the Polly^NET locations is discussed on the basis of more than 55 000 automatically retrieved 30 min particle backscatter coefficient profiles at 532 nm as this operating wavelength is available for all Polly lidar systems. A seasonal analysis of measurements at selected sites revealed typical and extraordinary aerosol conditions as well as seasonal differences. These studies show the potential of Polly^NET to support the establishment of a global aerosol climatology that covers the entire troposphere.

Atmospheric aerosol particles serving as Cloud Condensation Nuclei (CCN) are key elements of the hydrological cycle and climate. We measured and characterized CCN in polluted air and biomass burning smoke during the PRIDE-PRD2006 campaign from 1–30 July 2006 at a rural site ~60 km northwest of the mega-city Guangzhou in southeastern China. CCN efficiency spectra (activated fraction vs. dry particle diameter; 20–290 nm) were recorded at water vapor supersaturations (S) in the range of 0.068% to 1.27%. The corresponding effective hygroscopicity parameters describing the influence of particle composition on CCN activity were in the range of κ≈0.1–0.5. The campaign average value of κ=0.3 equals the average value of κ for other continental locations. During a strong local biomass burning event, the average value of κ dropped to 0.2, which can be considered as characteristic for freshly emitted smoke from the burning of agricultural waste. At low S (≤0.27%), the maximum activated fraction remained generally well below one, indicating substantial portions of externally mixed CCN-inactive particles with much lower hygroscopicity – most likely soot particles (up to ~60% at ~250 nm). The mean CCN number concentrations (N_CCN,S) ranged from 1000 cm⁻³ at S=0.068% to 16 000 cm⁻³ at S=1.27%, which is about two orders of magnitude higher than in pristine air. Nevertheless, the ratios between CCN concentration and total aerosol particle concentration (integral CCN efficiencies) were similar to the ratios observed in pristine continental air (~6% to ~85% at S=0.068% to 1.27%). Based on the measurement data, we have tested different model approaches for the approximation/prediction of N_CCN,S. Depending on S and on the model approach, the relative deviations between observed and predicted N_CCN,S ranged from a few percent to several hundred percent. The largest deviations occurred at low S with a simple power law. With a Köhler model using variable κ values obtained from individual CCN efficiency spectra, the relative deviations were on average less than ~10% and hardly exceeded 20%, confirming the applicability of the κ-Köhler model approach for efficient description of the CCN activity of atmospheric aerosols. Note, however, that different types of κ-parameters must be distinguished for external mixtures of CCN-active and -inactive aerosol particles (κ_a, κ_t, κ_cut). Using a constant average hygroscopicity parameter (κ=0.3) and variable size distributions as measured, the deviations between observed and predicted CCN concentrations were on average less than 20%. In contrast, model calculations using variable hygroscopicity parameters as measured and constant size distributions led to much higher deviations: ~70% for the campaign average size distribution, ~80% for a generic rural size distribution, and ~140% for a generic urban size distribution. These findings confirm earlier studies suggesting that aerosol particle number and size are the major predictors for the variability of the CCN concentration in continental boundary layer air, followed by particle composition and hygroscopicity as relatively minor modulators. Depending on the required and applicable level of detail, the information and parameterizations presented in this study should enable efficient description of the CCN activity of atmospheric aerosols in detailed process models as well as in large-scale atmospheric and climate models.

This study was part of the international field measurement Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing‐2006). We investigated a new particle formation event in a highly polluted air mass at a regional site south of the megacity Beijing and its impact on the abundance and properties of cloud condensation nuclei (CCN). During the 1‐month observation, particle nucleation followed by significant particle growth on a regional scale was observed frequently (∼30%), and we chose 23 August 2006 as a representative case study. Secondary aerosol mass was produced continuously, with sulfate, ammonium, and organics as major components. The aerosol mass growth rate was on average 19 μg m⁻³ h⁻¹ during the late hours of the day. This growth rate was observed several times during the 1‐month intensive measurements. The nucleation mode grew very quickly into the size range of CCN, and the CCN size distribution was dominated by the growing nucleation mode (up to 80% of the total CCN number concentration) and not as usual by the accumulation mode. At water vapor supersaturations of 0.07–0.86%, the CCN number concentrations reached maximum values of 4000–19,000 cm⁻³ only 6–14 h after the nucleation event. During particle formation and growth, the effective hygroscopicity parameter κ increased from about 0.1–0.3 to 0.35–0.5 for particles with diameters of 40–90 nm, but it remained nearly constant at ∼0.45 for particles with diameters of ∼190 nm. This result is consistent with aerosol chemical composition data, showing a pronounced increase of sulfate.

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. CCN properties were measured and characterized during the CAREBeijing-2006 campaign at a regional site south of the megacity of Beijing, China. Size-resolved CCN efficiency spectra recorded for a supersaturation range of S=0.07% to 0.86% yielded average activation diameters in the range of 190 nm to 45 nm. The corresponding effective hygroscopicity parameters (κ) exhibited a strong size dependence ranging from ~0.25 in the Aitken size range to ~0.45 in the accumulation size range. The campaign average value (κ =0.3 ± 0.1) was similar to the values observed and modeled for other populated continental regions. The hygroscopicity parameters derived from the CCN measurements were consistent with chemical composition data recorded by an aerosol mass spectrometer (AMS) and thermo-optical measurements of apparent elemental and organic carbon (EC and OC). The CCN hygroscopicity and its size dependence could be parameterized as a function of only AMS based organic and inorganic mass fractions (f_org, f_inorg) using the simple mixing rule κ_p ≈ 0.1 · f_org + 0.7 · f_inorg. When the measured air masses originated from the north and passed rapidly over the center of Beijing (fresh city pollution), the average particle hygroscopicity was reduced (κ = 0.2 ± 0.1), which is consistent with enhanced mass fractions of organic compounds (~50%) and EC (~30%) in the fine particulate matter (PM₁). Moreover, substantial fractions of externally mixed weakly CCN-active particles were observed at low supersaturation (S=0.07%), which can be explained by the presence of freshly emitted soot particles with very low hygroscopicity (κ < 0.1). Particles in stagnant air from the industrialized region south of Beijing (aged regional pollution) were on average larger and more hygroscopic, which is consistent with enhanced mass fractions (~60%) of soluble inorganic ions (mostly sulfate, ammonium, and nitrate). Accordingly, the number concentration of CCN in aged air from the megacity region was higher than in fresh city outflow ((2.5–9.9) × 10³ cm⁻³ vs. (0.4–8.3) × 10³ cm⁻³ for S=0.07–0.86%) although the total aerosol particle number concentration was lower (1.2 × 10⁴ cm⁻³ vs. 2.3 × 10⁴ cm⁻³). A comparison with related studies suggests that the fresh outflow from Chinese urban centers generally may contain more, but smaller and less hygroscopic aerosol particles and thus fewer CCN than the aged outflow from megacity regions.

Size-resolved chemical composition, mixing state, and cloud condensation nucleus (CCN) activity of aerosol particles in polluted mega-city air and biomass burning smoke were measured during the PRIDE-PRD2006 campaign near Guangzhou, China, using an aerosol mass spectrometer (AMS), a volatility tandem differential mobility analyzer (VTDMA), and a continuous-flow CCN counter (DMT-CCNC). The size-dependence and temporal variations of the effective average hygroscopicity parameter for CCN-active particles (κ_a) could be parameterized as a function of organic and inorganic mass fractions (f_org, f_inorg) determined by the AMS: κ_a,p=κ_org·f_org + κ_inorg·f_inorg. The characteristic κ values of organic and inorganic components were similar to those observed in other continental regions of the world: κ_org≈0.1 and κ_inorg≈0.6. The campaign average κ_a values increased with particle size from ~0.25 at ~50 nm to ~0.4 at ~200 nm, while f_org decreased with particle size. At ~50 nm, f_org was on average 60% and increased to almost 100% during a biomass burning event. The VTDMA results and complementary aerosol optical data suggest that the large fractions of CCN-inactive particles observed at low supersaturations (up to 60% at S≤0.27%) were externally mixed weakly CCN-active soot particles with low volatility (diameter reduction <5% at 300 °C) and effective hygroscopicity parameters around κ_LV≈0.01. A proxy for the effective average hygroscopicity of the total ensemble of CCN-active particles including weakly CCN-active particles (κ_t) could be parameterized as a function of κ_a,p and the number fraction of low volatility particles determined by VTDMA (φ_LV): κ_t,p=κ_a,p−φ_LV·(κ_a,p−κ_LV). Based on κ values derived from AMS and VTDMA data, the observed CCN number concentrations (N_CCN,S≈10²–10⁴ cm⁻³ at S = 0.068–0.47%) could be efficiently predicted from the measured particle number size distribution. The mean relative deviations between observed and predicted CCN concentrations were ~10% when using κ_t,p, and they increased to ~20% when using only κ_a,p. The mean relative deviations were not higher (~20%) when using an approximate continental average value of κ≈0.3, although the constant κ value cannot account for the observed temporal variations in particle composition and mixing state (diurnal cycles and biomass burning events). Overall, the results confirm that on a global and climate modeling scale an average value of κ≈0.3 can be used for approximate predictions of CCN number concentrations in continental boundary layer air when aerosol size distribution data are available without information about chemical composition. Bulk or size-resolved data on aerosol chemical composition enable improved CCN predictions resolving regional and temporal variations, but the composition data need to be highly accurate and complemented by information about particle mixing state to achieve high precision (relative deviations <20%).

Direct observations during intense warm‐air advection over the East Siberian Sea reveal a period of rapid sea‐ice melt. A semistationary, high‐pressure system north of the Bering Strait forced northward advection of warm, moist air from the continent. Air‐mass transformation over melting sea ice formed a strong, surface‐based temperature inversion in which dense fog formed. This induced a positive net longwave radiation at the surface while reducing net solar radiation only marginally; the inversion also resulted in downward turbulent heat flux. The sum of these processes enhanced the surface energy flux by an average of ~15 W m⁻² for a week. Satellite images before and after the episode show sea‐ice concentrations decreasing from > 90% to ~50% over a large area affected by the air‐mass transformation. We argue that this rapid melt was triggered by the increased heat flux from the atmosphere due to the warm‐air advection.