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In this paper bioaerosol measurements conducted with the Waveband Integrated Bioaerosol Sensor mark 4 (WIBS-4) are presented. The measurements comprise aerosol chamber characterization experiments and a one-year ambient measurement period at a semi-rural site in South Western Germany. This study aims to investigate the sensitivity of WIBS-4 to biological and non-biological aerosols and detection of biological particles in the ambient aerosol. Several types of biological and non-biological aerosol samples, including fungal spores, bacteria, mineral dust, ammonium sulphate, combustion soot, and fluorescent polystyrene spheres, were analyzed by WIBS-4 in the laboratory. The results confirm the sensitivity of the ultraviolet light-induced fluorescence (UV-LIF) method to biological fluorophores and show the good discrimination capabilities of the two excitation wavelengths/detection wavebands method applied in WIBS-4. However, a weak cross-sensitivity to non-biological fluorescent interferers remains and is discussed in this paper. All the laboratory studies have been undertaken in order to prepare WIBS-4 for ambient aerosol measurements. According to the one-year ambient aerosol study, number concentration of fluorescent biological aerosol particles (FBAP) show strong seasonal and diurnal variability. The highest number concentration of FBAP was measured during the summer term and decreased towards the winter period when colder and drier conditions prevail. Diurnal FBAP concentrations start to increase after sunset and reach maximum values during the late night and early morning hours. On the other hand, the total aerosol number concentration was almost always higher during daytime than during nighttime and a sharp decrease after sunset was observed. There was no correlation observed between the FBAP concentration and the meteorological parameters temperature, precipitation, wind direction and wind speed. However, a clear correlation was identified between the FBAP number concentration and the relative humidity. Humidity-controlled release mechanisms of some fungal spore species are discussed as a possible explanation.

We have retrieved the wavelength-dependent imaginary parts of the complex refractive index for five different Saharan dust aerosol particles of variable mineralogical composition at wavelengths between 305 and 955 nm. The dust particles were generated by dispersing soil samples into a laboratory aerosol chamber, typically yielding particle sizes with mean diameters ranging from 0.3 to 0.4 μm and maximum diameters from 2 to 4 μm. The extinction and absorption coefficients as well as the number size distribution of the dust particles were simultaneously measured by various established techniques. An inversion scheme based on a spheroidal dust model was employed to deduce the refractive indices. The retrieved imaginary parts of the complex refractive index were in the range from 0.003 to 0.005, 0.005 to 0.011, and 0.016 to 0.050 at the wavelengths 955, 505, and 305 nm. The hematite content of the dust particles was determined by electron-microscopical single particle analysis. Hematite volume fractions in the range from 1.1 to 2.7% were found for the different dusts, a range typical for atmospheric mineral dust. We have performed a sensitivity study to assess how accurately the retrieved imaginary refractive indices could be reproduced by calculations with mixing rule approximations using the experimentally determined hematite contents as input.

Atmospheric secondary organic aerosol (SOA) is likely to exist in a semi-solid or glassy state, particularly at low temperatures and humidities. Previously, it has been shown that glassy aqueous citric acid aerosol is able to nucleate ice heterogeneously under conditions relevant to cirrus in the tropical tropopause layer (TTL). In this study we test if glassy aerosol distributions with a range of chemical compositions heterogeneously nucleate ice under cirrus conditions. Three single component aqueous solution aerosols (raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA) and levoglucosan) and one multi component aqueous solution aerosol (raffinose mixed with five dicarboxylic acids and ammonium sulphate) were studied in both the liquid and glassy states at a large cloud simulation chamber. The investigated organic compounds have similar functionality to oxidised organic material found in atmospheric aerosol and have estimated temperature/humidity induced glass transition thresholds that fall within the range predicted for atmospheric SOA. A small fraction of aerosol particles of all compositions were found to nucleate ice heterogeneously in the deposition mode at temperatures relevant to the TTL (<200 K). Raffinose and HMMA, which form glasses at higher temperatures, nucleated ice heterogeneously at temperatures as high as 214.6 and 218.5 K respectively. We present the calculated ice active surface site density, ns, of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RHi). We also propose a parameterisation which can be used to estimate heterogeneous ice nucleation by glassy aerosol for use in cirrus cloud models up to ~220 K. Finally, we show that heterogeneous nucleation by glassy aerosol may compete with ice nucleation on mineral dust particles in mid-latitudes cirrus.

Cirrus clouds and their impact on the Earth's radiative budget are subjects of current research. The processes governing the growth of cirrus ice particles are central to the radiative properties of cirrus clouds. At temperatures relevant to cirrus clouds, the growth of ice crystals smaller than a few microns in size is strongly influenced by the accommodation coefficient of water molecules on ice, αice, making this parameter relevant for cirrus cloud modeling. However, the experimentally determined magnitude of αice for cirrus temperatures is afflicted with uncertainties of almost three orders of magnitude, and values for αice derived from cirrus cloud data lack significance so far. This has motivated dedicated experiments at the cloud chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) to determine αice in the cirrus-relevant temperature interval between 190 K and 235 K under realistic cirrus ice particle growth conditions. The experimental data sets have been evaluated independently with two model approaches: the first relying on the newly developed model SIGMA (Simple Ice Growth Model for determining Alpha), the second one on an established model, ACPIM (Aerosol-Cloud-Precipitation Interaction Model). Within both approaches a careful uncertainty analysis of the obtained αice values has been carried out for each AIDA experiment. The results show no significant dependence of αice on temperature between 190 K and 235 K. In addition, we find no evidence for a dependence of αice on ice particle size or on water vapor supersaturation for ice particles smaller than 20 μm and supersaturations of up to 70%. The temperature-averaged and combined result from both models is αice = 0.7−0.5+0.3, which implies that αice may only exert a minor impact on cirrus clouds and their characteristics when compared to the assumption of αice =1. Impact on prior calculations of cirrus cloud properties, e.g., in climate models, with αice typically chosen in the range 0.2–1 is thus expected to be negligible. In any case, we provide a well-constrained αice which future cirrus model studies can rely on.

The article presents the laser scattering and depolarisation instrument SIMONE that is installed at the large aerosol and cloud chamber facility AIDA of the Karlsruhe Institute of Technology. SIMONE uses a 488 nm cw laser to probe simulated atmospheric clouds by measuring the scattered light from the 1.8° and 178.2° directions. At 178.2°, the scattered light is analysed for the linear polarisation state to deduce the particle linear depolarisation ratio δp which is a common measurement parameter of atmospheric lidar applications. The optical setup and the mathematical formalism of the depolarisation detection concept are given. SIMONE depolarisation measurements in spheroidal hematite aerosol and supercooled liquid clouds are used to validate the instrument. SIMONE data from a series of AIDA ice nucleation experiments at temperatures between 195 and 225 K were analysed in terms of the impact of the ice particle microphysics on δp. We found strong depolarisation values of up to 0.4 in case of small growing and sublimating ice particles with volume equivalent diameters of only a few micrometers. Modelling runs with the T-matrix method showed that the measured depolarisation ratios can be accurately reproduced assuming spheroidal and cylindrical particles with a size distribution that has been constrained by IR extinction spectroscopy. Based on the T-matrix modelling runs, we demonstrate that in case of small ice crystals the SIMONE depolarisation results are representative for the lidar depolarisation ratio which is measured at exact backscattering direction of 180°. The relevance of our results for the interpretation of recent lidar observations in cirrus and contrails is discussed. In view of our results, the high depolarisation ratios observed by the spaceborne lidar CALIOP in the tropical upper troposphere might be a hint for the presence of small (sublimating) ice particles in the outflows of deep convective systems.

Fungal spores as a prominent type of primary biological aerosol particles (PBAP) have been incorporated into the COSMO-ART (Consortium for Small-scale Modelling-Aerosols and Reactive Trace gases) regional atmospheric model. Two literature-based emission rates for fungal spores derived from fungal spore colony counts and chemical tracer measurements were used as a parameterization baseline for this study. A third, new emission parameterization for fluorescent biological aerosol particles (FBAP) was adapted to field measurements from four locations across Europe. FBAP concentrations can be regarded as a lower estimate of total PBAP concentrations. Size distributions of FBAP often show a distinct mode at approx. 3 μm, corresponding to a diameter range characteristic for many fungal spores. Previous studies for several locations have suggested that FBAP are in many cases dominated by fungal spores. Thus, we suggest that simulated FBAP and fungal spore concentrations obtained from the three different emission parameterizations can be compared to FBAP measurements. The comparison reveals that simulated fungal spore concentrations based on literature emission parameterizations are lower than measured FBAP concentrations. In agreement with the measurements, the model results show a diurnal cycle in simulated fungal spore concentrations, which may develop partially as a consequence of a varying boundary layer height between day and night. Temperature and specific humidity, together with leaf area index (LAI), were chosen to drive the new emission parameterization which is fitted to the FBAP observations. The new parameterization results in similar root mean square errors (RMSEs) and correlation coefficients compared to the FBAP observations as the previously existing fungal spore emission parameterizations, with some improvements in the bias. Using the new emission parameterization on a model domain covering western Europe, FBAP in the lowest model layer comprise a fraction of 15% of the total aerosol mass over land and reach average number concentrations of 26 L−1. The results confirm that fungal spores and biological particles may account for a major fraction of supermicron aerosol particle number and mass concentration over vegetated continental regions and should thus be explicitly considered in air quality and climate studies.

The effect of organic coating on the heterogeneous ice nucleation (IN) efficiency of dust particles was investigated at simulated cirrus cloud conditions in the AIDA cloud chamber of Forschungszentrum Karlsruhe. Arizona test dust (ATD) and the clay mineral illite were used as surrogates for atmospheric dust aerosols. The dry dust samples were dispersed into a 3.7m3 aerosol vessel and either directly transferred into the 84m3 cloud simulation chamber or coated before with the semi-volatile products from the reaction of α-pinene with ozone in order to mimic the coating of atmospheric dust particles with secondary organic aerosol (SOA) substances. The ice-active fraction was measured in AIDA expansion cooling experiments as a function of the relative humidity with respect to ice, RHi, in the temperature range from 205 to 210K. Almost all uncoated dust particles with diameters between 0.1 and 1.0µm acted as efficient deposition mode ice nuclei at RHi between 105 and 120%. This high ice nucleation efficiency was markedly suppressed by coating with SOA. About 20% of the ATD particles coated with a SOA mass fraction of 17wt% were ice-active at RHi between 115 and 130%, and only 10% of the illite particles coated with an SOA mass fraction of 41wt% were ice-active at RHi between 160 and 170%. Only a minor fraction of pure SOA particles were ice-active at RHi between 150 and 190%. Strong IN activation of SOA particles was observed only at RHi above 200%, which is clearly above water saturation at the given temperature. The IN suppression and the shift of the heterogeneous IN onset to higher RHi seem to depend on the coating thickness or the fractional surface coverage of the mineral particles. The results indicate that the heterogeneous ice nucleation potential of atmospheric mineral particles may also be suppressed if they are coated with secondary organics.

The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA), levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition) before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosol particles that have re-vitrified in contact with the ice crystals during the preceding homogeneous freezing cycle exhibit pre-activation: they may retain small ice embryos in pores, have footprints on their surface which match the ice lattice, or simply have a much greater surface area or different surface microstructure compared to the unprocessed glassy aerosol particles. Pre-activation must be considered for the correct interpretation of experimental results on the heterogeneous ice nucleation ability of glassy aerosol particles and may provide a mechanism of producing a population of extremely efficient ice nuclei in the upper troposphere.

Soot particles, consisting of black carbon (BC), organic carbon (OC), inorganic salts, and trace elements, are emitted into the atmosphere during incomplete combustion. Accurate measurements of atmospheric BC are important as BC particles cause adverse health effects and impact the climate. Unfortunately, the accurate measurement of the properties and mass concentrations of BC particles remains difficult. The Single Particle Soot Photometer (SP2) can contribute to improving this situation by measuring the mass of refractory BC in individual particles as well as its mixing state. Here, the results of the first detailed SP2 intercomparison, involving 6 SP2s from 6 different research groups, are presented, including the most evolved data products that can presently be calculated from SP2 measurements. It was shown that a detection efficiency of almost 100% down to 1 fg BC per particle can readily be achieved, and that this limit can be pushed down to ∼0.2 fg BC with optimal SP2 setup. Number and mass size distributions of BC cores agreed within ±5% and ±10%, respectively, in between the SP2s, with larger deviations in the range below 1 fg BC. The accuracy of the SP2's mass concentration measurement depends on the calibration material chosen. The SP2 has previously been shown to be equally sensitive to fullerene soot and ambient BC from sources where fossil fuel was dominant and less sensitive to fullerene soot than to Aquadag. Fullerene soot was therefore chosen as the standard calibration material by the SP2 user community; however, many data sets rely solely on Aquadag calibration measurements. The difference in SP2 sensitivity was found to be almost equal (fullerene soot to Aquadag response ratio of ∼0.75 at 8.9 fg BC) for all SP2s. This allows the calculation of a fullerene soot equivalent calibration curve from a measured Aquadag calibration, when no fullerene soot calibration is available. It could be shown that this approach works well for all SP2s over the mass range of 1–10 fg. This range is suitable for typical BC mass size distributions in the ambient air far from sources. The number size distribution of purely scattering particles optically measured by the 6 SP2s also agreed within 15%. Measurements of the thickness of non-refractory coatings (i.e. product from α-pinene ozonolysis) on the BC particles, relying on BC mass optical size and on an additional particle position measurement, also compared well (within ±17%). The estimated coating thickness values were consistent with thermo-optical analysis of OC and elemental carbon (EC) content, though absolutely accurate values cannot be expected given all the assumptions that have to be made regarding refractive index, particle morphology, etc. This study showed that the SP2 provides accurate and reproducible data, but also that high data quality is only achieved if the SP2 is carefully tuned and calibrated. It has to be noted that the agreement observed here does not account for additional variability in output data that could result from the differences in the potentially subjective assumptions made by different SP2 users in the data processing.

Mixed phase clouds (MPCs) represent a great source of uncertainty for both climate predictions and weather forecasts. In particular, there is still a lack of understanding on how ice forms in these clouds. In this work we present a technique to analyze in situ measurements of MPCs performed with the latest instruments from the Small Ice Detector family. These instruments record high-resolution scattering patterns of individual small cloud particles. For the analysis of the scattering patterns we developed an algorithm that can discriminate the phase of the cloud particles. In the case of a droplet, a Mie solution is fitted to the recorded pattern and the size of the corresponding particle is obtained, which allows for a size calibration of the instrument. In the case of an ice particle, its shape is deduced from the scattering pattern. We apply our data analysis method to measurements from three distinct MPC types. The results from laboratory measurements demonstrate that our technique can discriminate between droplets and ice particles in the same optical size range. This ability was verified by measurements at a mountain top station where we found an alternation of liquid- and ice-dominated cloud regions. The analysis of results from aircraft-based measurements illustrates the ice detection threshold of the technique.