Fluorescent biological aerosol particles measured with the Waveband Integrated Bioaerosol Sensor WIBS-4: laboratory tests combined with a one year field study

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. <br><br> 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

Can neutral and ionized PAHs be carriers of the UV extinction bump and the diffuse interstellar bands?

Up to now, no laboratory-based study has investigated polycyclic aromatic hydrocarbon (PAH) species as potential carriers of both the diffuse interstellar bands (DIBs) and the 2175 A UV bump. We examined the proposed correlation between these two features by applying experimental and theoretical techniques on two specific medium-sized/large PAHs (dibenzorubicene C30H14 and hexabenzocoronene C42H18) in their neutral and cationic states. It was already shown that mixtures of sufficiently large, neutral PAHs can partly or even completely account for the UV bump. We investigated how the absorption bands are altered upon ionization of these molecules by interstellar UV photons. The experimental studies presented here were realized by performing matrix isolation spectroscopy with subsequent far-UV irradiation. The main effects were found to be a broadening of the absorption bands in the UV combined with slight red shifts. The position of the complete pi - pi* absorption structure around 217.5 nm, however, remains more or less unchanged which could explain the observed position invariance of the interstellar bump for different lines of sight. This favors the assignment of this feature to the interstellar PAH population. As far as the DIBs are concerned, neither our investigations nor the laboratory studies carried out by other research groups support a possible connection with this class of molecules. Instead, there are reasonable arguments that neutral and singly ionized cationic PAHs cannot be made responsible for the DIBs.Comment: 11 pages, 7 figures, 1 tabl

Circular depolarization ratios of single water droplets and finite ice circular cylinders: a modeling study

Computations of the phase matrix elements for single water droplets and ice crystals in fixed orientations are presented to determine if circular depolarization δ<sub>C</sub> is more accurate than linear depolarization for phase discrimination. T-matrix simulations were performed to calculate right-handed and left-handed circular depolarization ratios δ<sub>+C</sub>, respectively δ<sub>−C</sub> and to compare them with linear ones. Ice crystals are assumed to have a circular cylindrical shape where their surface-equivalent diameters range up to 5 μm. The circular depolarization ratios of ice particles were generally higher than linear depolarization and depended mostly on the particle orientation as well as their sizes. The fraction of non-detectable ice crystals (δ<0.05) was smaller considering a circular polarized light source, reaching 4.5%. However, water droplets also depolarized light circularly for scattering angles smaller than 179° and size parameters smaller than 6 at side- and backscattering regions. Differentiation between ice crystals and water droplets might be difficult for experiments performed at backscattering angles which deviate from 180° unlike LIDAR applications. Instruments exploiting the difference in the <I>P</I><sub>44</sub>/<I>P</I><sub>11</sub> ratio at a scattering angle around 115° are significantly constrained in distinguishing between water and ice because small droplets with size parameters between 5 and 10 do cause very high circular depolarizations at this angle. If the absence of the liquid phase is confirmed, the use of circular depolarization in single particle detection is more sensitive and less affected by particle orientation

Strong spectral dependence of light absorption by organic carbon particles formed by propane combustion

International audienceWe have measured the extinction and absorption cross sections of carbon particles emitted by a propane diffusion flame both in an aerosol chamber and on size-segregated samples deposited on optical windows. The absorption cross section, the single scattering albedo, and the Ångström exponent show drastic dependencies both on the C/O ratio and on the particle size. This is interpretated as being due to the appearance of nucleation modes of smaller organic particles at higher C/O ratios, which were detected by SMPS measurements and partially by TEM analysis. The spectral range of the validity of the absorption power-law (Ångström exponent) model is investigated by vacuum ultraviolet extinction measurements. These measurements give also indications for a preferentially aromatic nature of the OC component of the flame products

New cloud chamber experiments on the heterogeneous ice nucleation ability of oxalic acid in the immersion mode

The heterogeneous ice nucleation ability of oxalic acid in the immersion mode has been investigated by controlled expansion cooling runs with airborne, ternary solution droplets composed of, (i), sodium chloride, oxalic acid, and water (NaCl/OA/H₂O) and, (ii), sulphuric acid, oxalic acid, and water (H₂SO₄/OA/H₂O). Polydisperse aerosol populations with median diameters ranging from 0.5–0.7 μm and varying solute concentrations were prepared. The expansion experiments were conducted in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at initial temperatures of 244 and 235 K. In the ternary NaCl/OA/H₂O system, solid inclusions of oxalic acid, presumably nucleated as oxalic acid dihydrate, were formed by temporarily exposing the ternary solution droplets to a relative humidity below the efflorescence point of NaCl. The matrix of the crystallised NaCl particulates triggered the precipitation of the organic crystals which later remained as solid inclusions in the solution droplets when the relative humidity was subsequently raised above the deliquescence point of NaCl. The embedded oxalic acid crystals reduced the critical ice saturation ratio required for the homogeneous freezing of pure NaCl/H₂O solution droplets at a temperature of around 231 K from 1.38 to about 1.32. Aqueous solution droplets with OA inclusions larger than about 0.27 μm in diameter efficiently nucleated ice by condensation freezing when they were activated to micron-sized cloud droplets at 241 K, i.e., they froze well above the homogeneous freezing temperature of pure water droplets of about 237 K. Our results on the immersion freezing potential of oxalic acid corroborate the findings from a recent study with emulsified aqueous solutions containing crystalline oxalic acid. In those experiments, the crystallisation of oxalic acid diyhdrate was triggered by a preceding homogeneous freezing cycle with the emulsion samples. The expansion cooling cycles with ternary H₂SO₄/OA/H₂O solution droplets were aimed to analyse whether those findings can be transferred to ice nucleation experiments with airborne oxalic acid containing aerosol particles. Under our experimental conditions, the efficiency by which the surface of homogeneously nucleated ice crystals triggered the precipitation of oxalic acid dihydrate was very low, i.e., less than one out of a hundred ice crystals that were formed by homogeneous freezing in a first expansion cooling cycle left behind an ice-active organic crystal that acted as immersion freezing nucleus in a second expansion cooling cycle

Technical Note: A numerical test-bed for detailed ice nucleation studies in the AIDA cloud simulation chamber

The AIDA (Aerosol Interactions and Dynamics in the Atmosphere) aerosol and cloud chamber of Forschungszentrum Karlsruhe can be used to test the ice forming ability of aerosols. The AIDA chamber is extensively instrumented including pressure, temperature and humidity sensors, and optical particle counters. Expansion cooling using mechanical pumps leads to ice supersaturation conditions and possible ice formation. In order to describe the evolving chamber conditions during an expansion, a parcel model was modified to account for diabatic heat and moisture interactions with the chamber walls. Model results are shown for a series of expansions where the initial chamber temperature ranged from &minus;20&deg;C to &minus;60&deg;C and which used desert dust as ice forming nuclei. During each expansion, the initial formation of ice particles was clearly observed. For the colder expansions there were two clear ice nucleation episodes. <br><br> In order to test the ability of the model to represent the changing chamber conditions and to give confidence in the observations of chamber temperature and humidity, and ice particle concentration and mean size, ice particles were simply added as a function of time so as to reproduce the observations of ice crystal concentration. The time interval and chamber conditions over which ice nucleation occurs is therefore accurately known, and enables the model to be used as a test bed for different representations of ice formation

The Ice Selective Inlet: a novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds

Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol-cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of supercooled liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterisation. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artifacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the WELAS optical particle size spectrometers and a characterisation of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterisation Experiment (CLACE) 2013 – an extensive international field campaign encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaign provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterisation of its components, as well as a case study demonstrating the ISI performance in the field during CLACE 2013

Heterogeneous ice nucleation activity of bacteria: new laboratory experiments at simulated cloud conditions

The ice nucleation activities of five different &lt;i&gt;Pseudomonas syringae&lt;/i&gt;, &lt;i&gt;Pseudomonas viridiflava&lt;/i&gt; and &lt;i&gt;Erwinia herbicola&lt;/i&gt; bacterial species and of Snomax™ were investigated in the temperature range between &amp;minus;5 and &amp;minus;15&amp;deg;C. Water suspensions of these bacteria were directly sprayed into the cloud chamber of the AIDA facility of Forschungszentrum Karlsruhe at a temperature of &amp;minus;5.7&amp;deg;C. At this temperature, about 1% of the Snomax™ cells induced immersion freezing of the spray droplets before the droplets evaporated in the cloud chamber. The living cells didn&apos;t induce any detectable immersion freezing in the spray droplets at &amp;minus;5.7&amp;deg;C. After evaporation of the spray droplets the bacterial cells remained as aerosol particles in the cloud chamber and were exposed to typical cloud formation conditions in experiments with expansion cooling to about &amp;minus;11&amp;deg;C. During these experiments, the bacterial cells first acted as cloud condensation nuclei to form cloud droplets. Then, only a minor fraction of the cells acted as heterogeneous ice nuclei either in the condensation or the immersion mode. The results indicate that the bacteria investigated in the present study are mainly ice active in the temperature range between &amp;minus;7 and &amp;minus;11&amp;deg;C with an ice nucleation (IN) active fraction of the order of 10&lt;sup&gt;&amp;minus;4&lt;/sup&gt;. In agreement to previous literature results, the ice nucleation efficiency of Snomax™ cells was much larger with an IN active fraction of 0.2 at temperatures around &amp;minus;8&amp;deg;C

Spectral light absorption by ambient aerosols influenced by biomass burning in the Amazon Basin. I: Comparison and field calibration of absorption measurement techniques

International audienceSpectral aerosol light absorption is an important parameter for the assessment of the radiation budget of the atmosphere. Although on-line measurement techniques for aerosol light absorption, such as the Aethalometer and the Particle Soot Absorption Photometer (PSAP), have been available for two decades, they are limited in accuracy and spectral resolution because of the need to deposit the aerosol on a filter substrate before measurement. Recently, a 7-wavelength (?) Aethalometer became commercially available, which covers the visible (VIS) to near-infrared (NIR) spectral range (?=450?950 nm), and laboratory calibration studies improved the degree of confidence in these measurement techniques. However, the applicability of the laboratory calibration factors to ambient conditions has not been investigated thoroughly yet. As part of the LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia ? SMOke aerosols, Clouds, rainfall and Climate) campaign from September to November 2002 in the Amazon basin we performed an extensive field calibration of a 1-? PSAP and a 7-? Aethalometer utilizing a photoacoustic spectrometer (PAS, 532 nm) as reference device. Especially during the dry period of the campaign, the aerosol population was dominated by pyrogenic emissions. The most pronounced artifact of integrating-plate type attenuation techniques (e.g. Aethalometer, PSAP) is due to multiple scattering effects within the filter matrix. For the PSAP, we essentially confirmed the laboratory calibration factor by Bond et al. (1999). On the other hand, for the Aethalometer we found a multiple scattering enhancement of 5.23 (or 4.55, if corrected for aerosol scattering), which is significantly larger than the factors previously reported (~2) for laboratory calibrations. While the exact reason for this discrepancy is unknown, the available data from the present and previous studies suggest aerosol mixing (internal versus external) as a likely cause. For Amazonian aerosol, we found no absorption enhancement due to hygroscopic particle growth in the relative humidity (RH) range between 40% and 80%. However, a substantial bias in PSAP sensitivity that correlated with both RH and temperature (T) was observed for 20%RH<30% and 24°