Martin Schnaiter

Absorption of light by soot particles: determination of the absorption coefficient by means of aethalometers

Duringa soot aerosol measurement campaig n the response of two di*erent aethalometers (AE10 with white light and AE30 with multiwavelength capability) to several types of soot was investigated. Diesel soot, spark-generated carbon particles, and mixtures of these soot particles with ammonium sulfate and oxidation products of � -pinene were used in this evaluation. The determination of the particles light absorption coe%cient (babs) with the AE10 aethalometer is a di%cult task because of an ill-de7ned spectral sensitivity of this instrument. Provided that the proper numerical corrections are performed, the AE30 instrument allows for the measurement of babs over a wide spectral range (� = 450–950 nm). Duringall experiments it was found that with increasing7lter load the optical path in the aethalometer 7lter decreased. As a result, an increased underestimation of the measured aethalometer signals (babs or black carbon mass concentrations) occurs with increasing7lter loads. This e*ect, which is attributed to a “shadowing ” of the particles in the 7ber matrix, is very pronounced for “pure” soot particles while almost negligible for aged atmospheric aerosols. An empirical correction for this bias is presented and requires information on the light scattering behavior (i.e. light scattering coe%cient) of the sampled particles. Without this additional information, the applicability of the instruments is limited. Comparison with a reference method shows that multiple scatteringin the nearly unloaded 7ber 7lter is responsible for enhanced light absorption by a factor of about 2.14. ? 2003 Elsevier Ltd. All rights reserved.

UV-VIS-NIR spectral optical properties of soot and soot-containing aerosols

Abstract The UV-VIS-NIR spectral optical properties of soot and soot containing aerosols were investigated in detail during the AIDA Soot Aerosol Campaign 1999. One aim of the campaign was a comprehensive comparison of the microphysical properties of Diesel and spark generator soot. The mass specific extinction cross section at λ=450 nm of Diesel soot is 10.6±0.5 m 2 g −1 which is almost a factor of two larger than the corresponding value of 5.7±0.3 m 2 g −1 measured for spark generator soot. Coagulation-induced particle growth does not affect the soot extinction cross section and has a weak influence on the scattering properties of the soot aggregates. Atmospheric processing of freshly emitted soot was simulated in mixing experiments. The formation of mixed Diesel soot and dry ammonium sulfate particles by coagulation has only a minor effect on the soot absorption cross section. The coating of spark generated soot with organic material results in a strong increase of the single scattering albedo. A significant increase of the absorption coefficient at λ=473 nm during the coating process can be attributed to an enhancement of the specific soot absorption cross section by more than 30%.

The effect of organic coating on the heterogeneous ice nucleation efficiency of mineral dust aerosols

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 3.7?m3 aerosol vessel and either directly transferred into the 84?m3 cloud simulation chamber or coated before with the semi-volatile products from the reaction of ?-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 210?K. Almost all uncoated dust particles with diameters between 0.1 and 1.0??m 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 17?wt% were ice-active at RHi between 115 and 130%, and only 10% of the illite particles coated with an SOA mass fraction of 41?wt% 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.

Coating of soot and (NH4)2SO4 particles by ozonolysis products of α-pinene

The ozonolysis of � -pinene in a large aerosol chamber was usedto generate second ary organic aerosol (SOA) mass by homogeneous nucleation, or by heterogeneous nucleation, either on soot, or on (NH4)2SO4 seedaerosols. The rate of the � -pinene + ozone reaction andthe aerosol yieldof ∼19% are in goodagreement with literature data. The organic coating of soot particles leads to a compaction of the fractal agglomerates expressedby an increase in fractal d imension from 1.9 to 2.1 for Diesel soot, andfrom 2.0 to 2.3 for spark generated“Palas” soot. The d ielectric coating of the soot particles with SOA layers between 2 to 11 nm gives rise to a substantial enhancement of their single scattering albedo, from about 0.2 to 0.5, and increases the e+ective absorption coeCcients of both soot types by ca. 30%. The coating of both soot types increases the hygroscopic growth factors (HGF) to values close below the HGF measuredfor pure SOA material d=d0∼1:12 at 90% RH. ? 2003 Elsevier Ltd. All rights reserved.

Matrix-isolated Nano-sized Carbon Grains as an Analog for the 217.5 Nanometer Feature Carrier

The effect of particle shape or particle clustering on the extinction behavior of nano-sized hydrogenated carbon grains is investigated experimentally. The particles were extracted by a molecular beam technique at different condensation and clustering states and isolated in an argon matrix for UV spectroscopy. The state of clustering in the samples was controlled by transmission electron microscopy analysis. The simple spherical morphology of the matrix-isolated nonagglomerated particles permitted the derivation of reliable optical constants. A clear correlation was found between the measured UV feature width and the degree of particle clustering, in agreement with theoretical investigations based on the derived optical data. Therefore, the results prove unambiguously the expectation that the optical properties of carbonaceous grain material are strongly influenced by the particle shape and the clustering degree. For particles produced in hydrogen-containing atmospheres, the UV extinction peak was shifted blueward to a position close to the 217.5 nm hump. This shift was found to be nearly independent of the amount of hydrogen in the condensation zone. We also discuss the infrared spectra of the hydrogenated carbon materials. The astrophysical implications of the results are discussed with regard to the observational as well as the elemental abundance constraints.

Measurement of Wavelength-Resolved Light Absorption by Aerosols Utilizing a UV-VIS Extinction Cell

The principle, technical details, and performance of the long path extinction spectrometer (LOPES), a new folded–path extinction cell with a spectral range from the mid–UV (200 nm) to the near infrared (1015 nm), is presented. Using nonabsorbing glass beads the measured extinction spectrum of LOPES was validated by Mie calculations and was compared with scattering coefficients in the visible measured by a three–color integrating nephelometer (TSI, mod. 3563). For absorbing aerosols (here soot and biomass burning aerosol with single–scattering albedos of about 0.2 and 0.74 at 550 nm), LOPES was combined with a TSI 3563 nephelometer to determine the wavelength–dependent absorption coefficients from the difference of the extinction and scattering coefficients. These absorption coefficients were found to agree with the measurements by two state–of–the–art absorption techniques, the multiangle absorption photometry (MAAP) and photoacoustic spectrometry (PAS), which measure the absorption coefficient at the single wavelength of 532 nm and 670 nm, respectively. Finally, based on a comprehensive analysis of the TSI 3563 nephelometer errors and their propagation into the determination of the absorption coefficients from the LOPES and nephelometer data, we discuss implications for improving in situ measurements of the optical properties of atmospheric aerosols.

Ice nucleation on flame soot aerosol of different organic carbon content

The aerosol chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) was used as a moderate expansion cloud chamber to investigate the effect of the organic carbon (OC) content on the ice nucleation properties of soot aerosol particles. Two different soot samples with OC contents of 16 % (CS16) and 40 % (CS40) where produced with the CAST (Combustion Aerosol Standard) burner operated at different air/fuel (propane) ratios. In dynamic expansion experiments with about 30 %/min increase of relative humidity with respect to ice, the CS16 sample started to nucleate ice crystals at an ice saturation ratio S in of 1.45 (at a temperature of 207 K). This value is very close to the ice saturation ratio of ice nucleation onset on carbon spark generator soot particles coated with a significant amount of sulphuric acid investigated in previous AIDA expansion experiments. A second experiment with CS40 soot performed at almost identical thermodynamic conditions showed ice nucleation onset to occur at S in between 1.5 and 1.7. The formation rate of ice crystals was at least two orders of magnitude less than for CS16 soot, even at ice saturation ratios up to values of 1.9, which is very close to water saturation at a temperature of 207 K. Therefore, increasing the amount of OC seems to significantly suppress the ice nucleation on flame soot particles. In contrast, similar expansion experiments with dry and untreated mineral dust particles (Arizona test dust) in the temperature range 194 to 241 K showed ice nucleation to occur at much lower ice saturation ratios of only 1.05 to 1.15.

Fluorescent biological aerosol particles (FBAPs) 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. 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.

Infrared Spectroscopy of Nano-sized Carbon Grains Produced by Laser Pyrolysis of Acetylene: Analog Materials for Interstellar Grains

The infrared spectroscopic behavior of nano-sized carbon grains produced by laser-driven pyrolysis of acetylene (C2H2) is presented with respect to the internal structure of the particles investigated by electron energy loss spectroscopy and high-resolution transmission electron microscopy. Carbon grain samples were synthesized at different condensation conditions, and the effect of the pyrolysis temperature and pyrolysis mode (pulsed versus continuous wave) on the carbon structure was investigated. The size distribution of the carbon clusters synthesized in the flow reactor was determined by means of time-of-flight mass spectroscopy. Despite the CH absorption features attributed to saturated aliphatic hydrocarbons adsorbed by the grain surfaces, the infrared spectra of the neat carbon grains show only weak CH features. The investigations show that the formation and growth of polycyclic aromatic structural units are involved in the carbon grain condensation process. We conclude that the low feature-to-continuum ratio in the IR spectra of the grains is a typical property of carbonaceous dust formed by the pyrolysis of acetylene. The lack of observational evidence for hydrocarbon dust in the outflows of carbon-rich asymptotic giant branch (AGB) stars can be rationalized by our spectroscopic results. An evolutionary sequence of the circumstellar carbonaceous material during the AGB to planetary nebula (PN) phase transition can be deduced from our results by comparison with the IR spectral behavior of carbonaceous grain materials synthesized in other condensation systems.

ACRIDICON–CHUVA Campaign: Studying Tropical Deep Convective Clouds and Precipitation over Amazonia Using the New German Research Aircraft HALO

AbstractBetween 1 September and 4 October 2014, a combined airborne and ground-based measurement campaign was conducted to study tropical deep convective clouds over the Brazilian Amazon rain forest. The new German research aircraft, High Altitude and Long Range Research Aircraft (HALO), a modified Gulfstream G550, and extensive ground-based instrumentation were deployed in and near Manaus (State of Amazonas). The campaign was part of the German–Brazilian Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON– CHUVA) venture to quantify aerosol–cloud–precipitation interactions and their thermodynamic, dynamic, and radiative effects by in situ and remote sensing measurements over Amazonia. The ACRIDICON–CHUVA field observations were carried out in cooperation with the second intensive operating period...