Abstract. 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.

Characterization and intercomparison of aerosol absorption photometers: result of two intercomparison workshops [Discussion paper]

. Airborne soot is emitted from combustion processes as aggregates
of primary particles. The size of the primary particles and the overall
aggregate size control soot transport properties, and prior research shows
that these parameters may be related to the soot nanostructure. In this
work, a laminar, inverted nonpremixed burner has been used as a source of
soot that is almost completely elemental carbon. The inverted burner was
connected to an electrical low-pressure impactor, which collected
particles on stages according to the aerodynamic diameter, from 0.03 to 10  µ m. The morphology was analyzed using a transmission electron
microscope followed by image processing to extract projected area and
average primary particle size for each aggregate (approximately 1000
aggregates analyzed in total for the nine impactor stages). Carbon
nanostructure was analyzed using a Raman spectrometer, and five vibrational
bands (D4, D1, D3, G, and D2) were fitted to the spectra to obtain an
estimate of the carbon disorder. The average primary particle diameter
increases from 15 to 30 nm as the impactor stage aerodynamic diameter
increases. The D1, D3, D2, and D4 bands decreased (relative to the G band)
with the particle size, suggesting that the larger aggregates have larger
graphitic domains.

/pdf/morphology-and-raman-spectra-of-aerodynamically-classified-35g7x9m9wf.pdf

Morphology and Raman spectra of aerodynamically-classified soot samples

https://agupubs.onlinelibrary.wiley.com/doi/epdf/10.1029/2019GL086764

Black Carbon Particles Do Not Matter for Immersion Mode Ice Nucleation

Characterization of black carbon particles generated by a propane-fueled miniature inverted soot generator

. Providing reliable observations of aerosol particles' absorption properties at spatial and temporal resolutions suited to climate models is of utter importance to better understand the effects that atmospheric particles have on climate. Nowadays, one of the instruments most widely used in international monitoring networks for in situ surface measurements of light absorption properties of atmospheric aerosol particles is the multi-wavelength dual-spot Aethalometer, AE33. The AE33 derives the absorption coefficients of aerosol particles at seven different wavelengths from the measurements of the optical attenuation of light through a filter where particles are continuously collected. An accurate determination of the absorption coefficients from the AE33 instrument relies on the quantification of the non-linear processes related to the sample collection on the filter. The multiple-scattering correction factor ( C ), which depends on the filter tape used and on the optical properties of the collected particles, is the parameter with both the greatest uncertainty and the greatest impact on the absorption coefficients derived from the AE33 measurements. Here we present an in-depth analysis of the AE33 multiple-scattering correction factor C and its wavelength dependence for two different and widely used filter tapes, namely the old, and most referenced, TFE-coated glass, or M8020, filter tape and the currently, and most widely used, M8060 filter tape. For performing this analysis, we compared the attenuation measurements from AE33 with the absorption coefficients measured with different filter-based techniques. On-line co-located multi-angle absorption photometer (MAAP) measurements and off-line PP_UniMI polar photometer measurements were employed as reference absorption measurements for this work. To this aim, we used data from three different measurement stations located in the north-east of Spain, namely an urban background station (Barcelona, BCN), a regional background station (Montseny, MSY) and a mountaintop station (Montsec d'Ares, MSA). The median C values (at 637 nm) measured at the three stations ranged between 2.29 (at BCN and MSY, lowest 5th percentile of 1.97 and highest 95th percentile of 2.68) and 2.51 (at MSA, lowest 5th percentile of 2.06 and highest 95th percentile of 3.06). The analysis of the cross-sensitivity to scattering, for the two filter tapes considered here, revealed a large increase in the C  factor when the single-scattering albedo (SSA) of the collected particles was above a given threshold, up to a 3-fold increase above the average C values. The SSA threshold appeared to be site dependent and ranged between 0.90 to 0.95 for the stations considered in the study. The results of the cross-sensitivity to scattering displayed a fitted constant multiple-scattering parameter, Cf , of 2.21 and 1.96, and a cross-sensitivity factor, ms , of 1.8 % and 3.4 % for the MSY and MSA stations, respectively, for the TFE-coated glass filter tape. For the M8060 filter tape, Cf values of 2.50, 1.96 and 1.82 and ms values of 1.6 %, 3.0 % and 4.9 % for the BCN, MSY and MSA stations, respectively, were obtained. SSA variations also influenced the spectral dependence of C , which showed an increase with wavelength when SSA was above the site-dependent threshold. Below the SSA threshold, no statistically significant dependence of C on the wavelength was observed. For the measurement stations considered here, the wavelength dependence of C was to some extent driven by the presence of dust particles during Saharan dust outbreaks that had the potential to increase the SSA above the average values. At the mountaintop station, an omission of the wavelength dependence of the C  factor led to an underestimation of the absorption Angstrom exponent (AAE) by up to 12 %. Differences in the absorption coefficient determined from AE33 measurements at BCN, MSY and MSA of around 35 %–40 % can be expected when using the site-dependent experimentally obtained C value instead of the nominal C value. Due to the fundamental role that the SSA of the particles collected on the filter tape has in the multiple-scattering parameter C , we present a methodology that allows the recognition of the conditions upon which the use of a constant and wavelength-independent C is feasible.

/pdf/determination-of-the-multiple-scattering-correction-factor-52gctd85ps.pdf

Determination of the multiple-scattering correction factor and its cross-sensitivity to scattering and wavelength dependence for different AE33 Aethalometer filter tapes: a multi-instrumental approach

Flame-generated soot from miniCAST burners is increasingly being used in academia and industry as engine exhaust soot surrogate for atmospheric studies and instrument calibration. Previous studies have found that elemental carbon (EC) content of miniCAST soot is proportional to the mean particle size. Here, the characterization of a prototype miniCAST generator (5201 Type BC), which was designed to decouple the soot composition from the particle size and produce soot particles with high EC and BC content in a large size range, is reported. This prototype may operate either in a diffusion-flame or a partially premixed-flame mode, an option that was not available in former models. It was confirmed that soot properties, such as EC content and Angstrom absorption exponent (AAE), were linked to the overall flame composition. In particular, combustion under fuel-rich conditions provided particles with size coupled to the EC fraction and AAE, i.e. smaller particles exhibited a lower EC fraction and highe...

Characterization of a new miniCAST with diffusion flame and premixed flame options: Generation of particles with high EC content in the size range 30 nm to 200 nm

The miniCAST 5201 black carbon (BC) generator is a novel soot generator able to produce soot particles with a wide range of properties in a stable and reproducible manner. In this study, particles ...

Optical and morphological properties of soot particles generated by the miniCAST 5201 BC generator

Abstract. Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parametrization schemes for the optical properties of BC using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. In the first step, the modeling techniques were examined for bare BC particles, and in the second step, for BC particles with organic material. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. The BC fractal aggregate is usually modelled using monodispersed particles since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25 % uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the discrepancy between modelled and measured particle light absorption coefficient σabs to 10 %, for particles with volume mean mobility diameters between 60–160 nm. However, for particles larger than 100 nm, the Absorption Ångström Exponent (AAE) calculated by using a spherical morphology was more consistent with the measured value. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 to 2; mim between 0.50 to 1; Df from 1.7 to 1.9, and app between 10 to 14 nm. Overall, this study provides experimental support for emphasizing the use of an appropriate size representation (polydisperse size method) and an appropriate morphological representation (aggregate morphology) for optical modelling and parametrization scheme development of BC. 

Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations

Michaela N. Ess

Papers

Characterization of a new miniCAST with diffusion flame and premixed flame options: Generation of particles with high EC content in the size range 30 nm to 200 nm

Optical and morphological properties of soot particles generated by the miniCAST 5201 BC generator

Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations