Effective density of Aquadag and fullerene soot black carbon reference materials used for SP2 calibration

The mass and effective density of black carbon (BC) particles generated from aqueous suspensions of Aquadag and fullerene soot was measured and parametrized as a function of their mobility diameter. The measurements were made by two independent research groups by operating a differential mobility analyser (DMA) in series with an aerosol particle mass analyser (APM) or a Couette centrifugal particle mass analyser (CPMA). Consistent and reproducible results were found in this study for different production lots of Aquadag, indicating that the effective density of these particles is a stable quantity and largely unaffected by differences in aerosol generation procedures and suspension treatments. The effective density of fullerene soot particles from one production lot was also found to be stable and independent of suspension treatments. Some differences to previous literature data were observed for both Aquadag and fullerene soot at larger particle diameters. Knowledge of the exact relationship between mobility diameter and particle mass is of great importance, as DMAs are commonly used to size-select particles from BC reference materials for calibration of single particle soot photometers (SP2), which quantitatively detect the BC mass in single particles

Mix 'n Match: Integrating Text Matching and Product Substitutability within Product Search

Two products are substitutes if both can satisfy the same consumer need. Intrinsic incorporation of product substitutability - where substitutability is integrated within latent vector space models - is in contrast to the extrinsic re-ranking of result lists. The fusion of text matching and product substitutability objectives allows latent vector space models to mix and match regularities contained within text descriptions and substitution relations. We introduce a method for intrinsically incorporating product substitutability within latent vector space models for product search that are estimated using gradient descent; it integrates flawlessly with state-of-the-art vector space models. We compare our method to existing methods for incorporating structural entity relations, where product substitutability is incorporated extrinsically by re-ranking. Our method outperforms the best extrinsic method on four benchmarks. We investigate the effect of different levels of text matching and product similarity objectives, and provide an analysis of the effect of incorporating product substitutability on product search ranking diversity. Incorporating product substitutability information improves search relevance at the cost of diversity

A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

International audienceAtmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/citric acid and in the ammonium sulfate/glutaric acid cases. However, we observe significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces

Optimized method for black carbon analysis in ice and snow using the Single Particle Soot Photometer

In this study we attempt to optimize the method for measuring black carbon (BC) in snow and ice using a Single Particle Soot Photometer (SP2). Beside the previously applied ultrasonic (CETAC) and Collison-type nebulizers we introduce a jet (Apex Q) nebulizer to aerosolize the aqueous sample for SP2 analysis. Both CETAC and Apex Q require small sample volumes (a few milliliters) which makes them suitable for ice core analysis. The Apex Q shows the least size-dependent nebulizing efficiency in the BC particle diameter range of 100–1000 nm. The CETAC has the advantage that air and liquid flows can be monitored continuously. All nebulizer-types require a calibration with BC standards for the determination of the BC mass concentration in unknown aqueous samples. We found Aquadag to be a suitable material for preparing calibration standards. Further, we studied the influence of different treatments for fresh discrete snow and ice samples as well as the effect of storage. The results show that samples are best kept frozen until analysis. Once melted, they should be sonicated for 25 min, immediately analyzed while being stirred and not be refrozen

The Pagami Creek smoke plume after long-range transport to the upper troposphere over Europe – aerosol properties and black carbon mixing state

During the CONCERT 2011 field experiment with the DLR research aircraft Falcon, an enhanced aerosol layer with particle linear depolarization ratios of 6–8% at 532 nm was observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPILT suggest that the elevated aerosol layer originated from the Pagami Creek forest fire in Minnesota, USA, which caused pyro-convective uplift of particles and gases. The 3–4 day-old smoke plume had high total refractory black carbon (rBC) mass concentrations of 0.03–0.35 μg m⁻³ at standard temperature and pressure (STP) with rBC mass equivalent diameter predominantly smaller than 130 nm. Assuming a core-shell particle structure, the BC cores exhibit very thick (median: 105–136 nm) BC-free coatings. A large fraction of the BC-containing particles disintegrated into a BC-free fragment and a BC fragment while passing through the laser beam of the Single Particle Soot Photometer (SP2). In this study, the disintegration is a result of very thick coatings around the BC cores. This is in contrast to a previous study in a forest-fire plume, where it was hypothesized to be a result of BC cores being attached to a BC-free particle. For the high-altitude forest-fire aerosol layer observed in this study, increased mass specific light-absorption cross sections of BC can be expected due to the very thick coatings around the BC cores, while this would not be the case for the attached-type morphology. We estimate the BC mass import from the Pagami Creek forest fire into the upper troposphere/lower stratosphere (UTLS) region (best estimate: 25 Mg rBC). A comparison to black carbon emission rates from aviation underlines the importance of pyro-convection on the BC load in the UTLS region. Our study provides detailed information on the microphysics and the mixing state of BC in the forest-fire aerosol layer in the upper troposphere that can be used to better understand and investigate the radiative impact of such upper tropospheric aerosol layers

Recent increase in black carbon concentrations from a Mt. Everest ice core spanning 1860–2000 AD

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/95622/1/grl27751.pd

The Pagami Creek smoke plume after long-range transport to the upper troposphere over Europe – Aerosol properties and black carbon mixing state

During the CONCERT 2011 field experiment with the DLR research aircraft Falcon, an enhanced aerosol layer with particle linear depolarization ratios of 6–8% at 532 nm was observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPILT suggest that the elevated aerosol layer originated from the Pagami Creek forest fire in Minnesota, USA, which caused pyro-convective uplift of particles and gases. The 3–4 day-old smoke plume had high total refractory black carbon (rBC) mass concentrations of 0.03–0.35 μg m−3 at standard temperature and pressure (STP) with rBC mass equivalent diameter predominantly smaller than 130 nm. Assuming a core-shell particle structure, the BC cores exhibit very thick (median: 105–136 nm) BC-free coatings. A large fraction of the BC-containing particles disintegrated into a BC-free fragment and a BC fragment while passing through the laser beam of the Single Particle Soot Photometer (SP2). In this study, the disintegration is a result of very thick coatings around the BC cores. This is in contrast to a previous study in a forest-fire plume, where it was hypothesized to be a result of BC cores being attached to a BC-free particle. For the high-altitude forest-fire aerosol layer observed in this study, increased mass specific light-absorption cross sections of BC can be expected due to the very thick coatings around the BC cores, while this would not be the case for the attached-type morphology. We estimate the BC mass import from the Pagami Creek forest fire into the upper troposphere/lower stratosphere (UTLS) region (best estimate: 25 Mg rBC). A comparison to black carbon emission rates from aviation underlines the importance of pyro-convection on the BC load in the UTLS region. Our study provides detailed information on the microphysics and the mixing state of BC in the forest-fire aerosol layer in the upper troposphere that can be used to better understand and investigate the radiative impact of such upper tropospheric aerosol layers

On the effects of organic matter and sulphur-containing compounds on the CCN activation of combustion particles

The European PartEmis project (Measurement and prediction of emissions of aerosols and gaseous precursors from gas turbine engines) was focussed on the characterisation and quantification of exhaust emissions from a gas turbine engine. The combustion aerosol characterisation included on-line measurements of mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, cloud condensation nuclei (CCN) activation potential, and off-line analysis of chemical composition. Based on this extensive data set, the role of sulphuric acid coating and of the organic fraction of the combustion particles for the CCN activation was investigated. Modelling of CCN activation was conducted using microphysical and chemical properties obtained from the measurements as input data. Coating the combustion particles with water-soluble sulphuric acid, increases the potential CCN activation, or lowers the activation diameter, respectively. The adaptation of a Köhler model to the experimental data yielded coatings from 0.1 to 3 vol-% of water-soluble matter, which corresponds to an increase in the fraction of CCN-activated combustion particles from ≤10^−4 to ≌10^−2 at a water vapour saturation ratio S_w=1.006. Additional particle coating by coagulation of combustion particles and aqueous sulphuric acid particles formed by nucleation further reduces the CCN activation diameter. In contrast, particles containing a large fraction of non-volatile organic compounds grow significantly less at high relative humidity than particles with a lower content of non-volatile OC. The resulting reduction in the potential CCN activation with an increasing fraction of non-volatile OC becomes visible as a trend in the experimental data. While a coating of water-soluble sulphuric acid increases the potential CCN activation, or lowers the activation diameter, respectively, the non-volatile organic compounds, mainly found at lower combustion temperatures, can partially compensate this sulphuric acid-related enhancement of CCN activation of carbonaceous combustion aerosol particles