ALBERT

Description: Airborne measurements of the aerosol hygroscopic and optical properties as well as chemical composition were performed in the Netherlands and northern Italy on board of a Zeppelin NT airship during the PEGASOS field campaigns in 2012. The vertical changes in aerosol properties during the development of the mixing layer were studied. Hygroscopic growth factors (GF) at 95% relative humidity were determined using the white-light humidified optical particles spectrometer (WHOPS) for dry diameters of 300 and 500 nm particles. These measurements were supplemented by an aerosol mass spectrometer (AMS) and an aethalometer providing information on the aerosol chemical composition. Several vertical profiles between 100 and 700 m a.g. were flown just after sunrise close to the San Pietro Capofiume ground station in the Po Valley, Italy. During the early morning hours the lowest layer (newly developing mixing layer) contained a high nitrate fraction (20%) which was coupled with enhanced hygroscopic growth. In the layer above (residual layer) small nitrate fractions of ~ 2% were measured as well as low GFs. After full mixing of the layers, typically around noon and with increased temperature, the nitrate fraction decreased to 2% at all altitudes and led to similar hygroscopicity values as found in the residual layer. These distinct vertical and temporal changes underline the importance of airborne campaigns to study aerosol properties during the development of the mixed layer. The aerosol was externally mixed with 22 and 67% of the 500 nm particles in the range GF 〈 1.1 and GF 〉 1.5, respectively. Contributors to the non-hygroscopic mode in the observed size range are most likely mineral dust and biological material. Mean hygroscopicity parameters (κ) were 0.34, 0.19 and 0.18 for particles in the newly forming mixing layer, residual layer and fully mixed layer, respectively. These results agree well with those from chemical analysis which found values of κ = 0.27, 0.21 and 0.19 for the three layers. The highest κ values in the new mixed layer and lower values in the fully developed mixed layer were additionally confirmed by ground measurements. The aerosol sampled in the Netherlands did not show any altitude dependent characteristics because only the fully mixed layer or the entrainment zone between mixed and the residual layer were probed. The airborne hygroscopicity measurements agreed well with ground based composition measurements. However, the fraction of the hygroscopic particles (GF 〉 1.5) was enhanced compared to the results from Italy amounting to 82%, while 12% showed low hygroscopicity (GF 〈 1.1). The mean κ value measured by the WHOPS was 0.28 and therefore considerably higher than the value measured in the fully mixed layer in Italy. The effective index of refraction reached values of 1.43 and 1.42 for the 500 nm particles in Italy and the Netherlands, respectively. This coincides well with literature data for airmasses with predominant organic contribution as was the case during our flights.

Description: The atmospheric organic aerosol composition is characterized by a great diversity of functional groups and chemical species challenging simple classification schemes. Traditional off-line chemical methods identified chemical classes based on the retention behavior on chromatographic columns and absorbing beds. Such approach led to the isolation of complex mixtures of compounds such as the humic-like substances (HULIS). More recently, on-line aerosol mass spectrometry (AMS) was employed to identify chemical classes by extracting fragmentation patterns from experimental data series using statistical methods (factor analysis), providing simplified schemes for oxygenated organic aerosols (OOAs) classification on the basis of the distribution of oxygen-containing functionalities. The analysis of numerous AMS datasets suggested the occurrence of very oxidized OOAs which were postulated to correspond to the HULIS. However, only a few efforts were made to test the correspondence of the AMS classes of OOAs with the traditional classification from the off-line methods. In this paper, we consider a case study representative for polluted continental regional background environments. We examine the AMS factors for OOAs identified by positive matrix factorization (PMF) and compare to chemical classes of water-soluble organic carbon (WSOC) analysed off-line on a set of filters collected in parallel. WSOC fractionation was performed by means of factor analysis applied to H-NMR spectroscopic data, and by applying an ion-exchange chromatographic method for direct quantification of HULIS. Results show that the very oxidized low-volatility OOAs from AMS correlate with the NMR factor showing HULIS features and also with true "chromatographic" HULIS. On the other hand, UV/VIS-absorbing polyacids (or HULIS sensu stricto) isolated on ion-exchange beds were only a fraction of the AMS and NMR organic carbon fractions showing functional groups attributable to highly substituted carboxylic acids, suggesting that unspeciated low-molecular weight organic acids contribute to HULIS in the broad sense.

Description: Remote sensing of aerosols provides important information on the atmospheric aerosol abundance. However, due to the hygroscopic nature of aerosol particles observed aerosol optical properties are influenced by atmospheric humidity, and the measurements do not unambiguously characterize the aerosol dry mass and composition which complicates the comparison with aerosol models. In this study we derive aerosol water and chemical composition by a modeling approach that combines individual measurements of remotely sensed aerosol properties (e.g. optical thickness, single scattering albedo, refractive index and size distribution) from an AERONET (Aerosol Robotic Network) sun-photometer with radiosonde measurements of relative humidity. The model simulates water uptake by aerosols based on the chemical composition and size distribution. A minimization method is used to calculate aerosol composition and concentration, which are then compared to in situ measurements from the Intensive Measurement Campaign At the Cabauw Tower (IMPACT, May 2008, the Netherlands). Computed concentrations show reasonable agreement with surface observations and follow the day-to-day variability in observations. Total dry mass (33 ± 12 μg m−3) and black carbon concentrations (0.7 ± 0.3 μg m−3) are generally accurately computed. The uncertainty in the AERONET (real) refractive index (0.025–0.05) introduces larger uncertainty in the modeled aerosol composition (e.g. sulfates, ammonium nitrate or organic matter) and leads to an uncertainty of 0.1–0.25 in aerosol water volume fraction. Water volume fraction is highly variable depending on composition, up to 〉0.5 at 70–80% and

Description: A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM). Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models. The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where substantial reductions in sulphur dioxide emissions have yet to occur. Anticipated reductions in sulphur dioxide in polluted regions will result in an increase in the availability of ammonia to form ammonium nitrate as opposed to ammonium sulphate. This will be most important where intensive agricultural practises occur. Our observations over North-Western Europe, a region where sulphur dioxide emissions have already been reduced, indicate that failure to include the semi-volatile behaviour of ammonium nitrate will result in significant errors in predicted aerosol direct radiative forcing. Such errors will be particularly significant on regional scales.

Description: The aerosol light absorption coefficient is an essential parameter involved in atmospheric radiation budget calculations. The Aethalometer (AE) has the great advantage of measuring the aerosol light absorption coefficient at several wavelengths, but the derived absorption coefficients are systematically too high when compared to reference methods. Up to now, four different correction algorithms of the AE absorption coefficients have been proposed by several authors. A new correction scheme based on these previously published methods has been developed, which accounts for the optical properties of the aerosol particles embedded in the filter. All the corrections have been tested on six datasets representing different aerosol types and loadings and include multi-wavelength AE and white-light AE. All the corrections have also been evaluated through comparison with a Multi-Angle Absorption Photometer (MAAP) for four datasets lasting between 6 months and five years. The modification of the wavelength dependence by the different corrections is analyzed in detail. The performances and the limits of all AE corrections are determined and recommendations are given.

Description: A size dependent parameterization for the removal of aerosol particles by falling rain droplets is developed. Scavenging coefficients are calculated explicitly as a function of aerosol particle size and precipitation intensity including the full interaction of rain droplet size distribution and aerosol particles. The actual parameterization is a simple and accurate three-parameter fit through these pre-calculated scavenging coefficients. The parameterization is applied in the global chemistry transport model TM4 and the importance of below-cloud scavenging relative to other removal mechanisms is investigated for sea salt aerosol. For a full year run (year 2000), we find that below-cloud scavenging accounts for 12% of the total removal of super-micron aerosol. At mid-latitudes of both hemispheres the fractional contribution of below-cloud scavenging to the total removal of super-micron sea salt is about 30% with regional maxima exceeding 50%. Below-cloud scavenging reduces the global average super-micron aerosol lifetime from 2.47 to 2.16 days in our simulations. Despite large uncertainties in precipitation, relative humidity, and water uptake by aerosol particles, we conclude that below cloud scavenging is likely an important sink for super-micron sized sea salt aerosol particles that needs to be included in size-resolved aerosol models.

Description: Absorption photometers for real time application have been available since the 1980s, but the use of filter-based instruments to derive information on aerosol properties (absorption coefficient and black carbon, BC) is still a matter of debate. Several workshops have been conducted to investigate the performance of individual instruments over the intervening years. Two workshops with large sets of aerosol absorption photometers were conducted in 2005 and 2007. The data from these instruments were corrected using existing methods before further analysis. The inter-comparison shows a large variation between the responses to absorbing aerosol particles for different types of instruments. The unit to unit variability between instruments can be up to 30% for Particle Soot Absorption Photometers (PSAPs) and Aethalometers. Multi Angle Absorption Photometers (MAAPs) showed a variability of less than 5%. Reasons for the high variability were identified to be variations in sample flow and spot size. It was observed that different flow rates influence system performance with respect to response to absorption and instrumental noise. Measurements with non absorbing particles showed that the current corrections of a cross sensitivity to particle scattering are not sufficient. Remaining cross sensitivities were found to be a function of the total particle load on the filter. The large variation between the response to absorbing aerosol particles for different types of instruments indicates that current correction functions for absorption photometers are not adequate.

Description: Characterization of atmospheric aerosols is important for understanding their impact on health and climate. A wealth of aerosol parameters can be retrieved from multi-angle, multi-wavelength radiance and polarization measurements of the clear sky. We developed a ground-based SPEX instrument (groundSPEX) for accurate spectropolarimetry, based on the passive, robust, athermal, and snapshot spectral polarization modulation technique, and is hence ideal for field deployment. It samples the scattering phase function in the principal plane in an automated fashion, using a motorized pan/tilt unit and automatic exposure time detection. Extensive radiometric and polarimetric calibrations were performed, yielding values for both random noise and systematic uncertainties. The absolute polarimetric accuracy at low degrees of polarization is established to be ~5 × 10−3. About 70 measurement sequences have been performed throughout four clear-sky days at Cabauw, the Netherlands. Several aerosol parameters were retrieved: aerosol optical thickness, effective radius, and complex refractive index for fine and coarse mode. The results are in good agreement with the colocated AERONET products, with a correlation coefficient of ρ = 0.932 for the total aerosol optical thickness at 550 nm.

Description: In this paper, the use of a neural network algorithm for the retrieval of the aerosol properties from ground-based spectropolarimetric measurements is discussed. The neural network is able to retrieve the aerosol properties with an accuracy that is almost comparable to that of an iterative retrieval. By using the outcome of the neural network as first guess in the iterative retrieval scheme, the accuracy of the retrieved fine- and coarse-mode optical thickness is further improved, while for the other parameters the improvement is small or absent. The resulting scheme (neural network + iterative retrieval) is compared to the original one (look-up table + iterative retrieval) on a set of simulated ground-based measurements, and on a small set of real observations carried out by an accurate ground-based spectropolarimeter. The results show that the use of a neural-network-based first guess leads to an increase in the number of converging retrievals, and possibly to more accurate estimates of the aerosol effective radius and complex refractive index.

Description: The fact that polarisation lidars measure a depolarisation signal in liquid clouds due to the occurrence of multiple scattering is well known. The degree of measured depolarisation depends on the lidar characteristics (e.g. wavelength and receiver field of view) as well as the cloud macrophysical (e.g. cloud-base altitude) and microphysical (e.g. effective radius, liquid water content) properties. Efforts seeking to use depolarisation information in a quantitative manner to retrieve cloud properties have been undertaken with, arguably, limited practical success. In this work we present a retrieval procedure applicable to clouds with (quasi-)linear liquid water content (LWC) profiles and (quasi-)constant cloud-droplet number density in the cloud-base region. Thus limiting the applicability of the procedure allows us to reduce the cloud variables to two parameters (namely the derivative of the liquid water content with height and the extinction at a fixed distance above cloud base). This simplification, in turn, allows us to employ a fast and robust optimal-estimation inversion using pre-computed look-up tables produced using extensive lidar Monte Carlo (MC) multiple-scattering simulations. In this paper, we describe the theory behind the inversion procedure and successfully apply it to simulated observations based on large-eddy simulation (LES) model output. The inversion procedure is then applied to actual depolarisation lidar data corresponding to a range of cases taken from the Cabauw measurement site in the central Netherlands. The lidar results were then used to predict the corresponding cloud-base region radar reflectivities. In non-drizzling condition, it was found that the lidar inversion results can be used to predict the observed radar reflectivities with an accuracy within the radar calibration uncertainty (2–3 dBZ). This result strongly supports the accuracy of the lidar inversion results. Results of a comparison between ground-based aerosol number concentration and lidar-derived cloud-droplet number densities are also presented and discussed. The observed relationship between the two quantities is seen to be consistent with the results of previous studies based on aircraft-based in situ measurements.