ALBERT

Description: Arctic sea ice has decreased dramatically in the past few decades and the Arctic is increasingly open to transit shipping and natural resource extraction. However, large knowledge gaps exist regarding composition and impacts of emissions associated with these activities. Arctic hydrocarbon extraction is currently under development owing to the large oil and gas reserves in the region. Transit shipping through the Arctic as an alternative to the traditional shipping routes is currently underway. These activities are expected to increase emissions of air pollutants and climate forcers (e.g., aerosols, ozone) in the Arctic troposphere significantly in the future. The authors present the first measurements of these activities off the coast of Norway taken in summer 2012 as part of the European Arctic Climate Change, Economy, and Society (ACCESS) project. The objectives include quantifying the impact that anthropogenic activities will have on regional air pollution and understanding the connections to Arctic climate. Trace gas and aerosol concentrations in pollution plumes were measured, including emissions from different ship types and several offshore extraction facilities. Emissions originating from industrial activities (smelting) on the Kola Peninsula were also sampled. In addition, pollution plumes originating from Siberian biomass burning were probed in order to put the emerging local pollution within a broader context. In the near future these measurements will be combined with model simulations to quantify the influence of local anthropogenic activities on Arctic composition. Here the authors present the scientific objectives of the ACCESS aircraft experiment and the the meteorological conditions during the campaign, and they highlight first scientific results from the experiment.

Description: 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 has been observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPLIT suggest that the elevated aerosol layer originated from the pyro-convective Pagami Creek forest fire in Minnesota, USA. The 3–4 days old smoke plume has 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 diameters predominantly smaller than 130 nm. Assuming a core-shell particle structure, the BC cores exhibit very thick (median: 105–136 nm) BC-free coatings, which modify the radiative transfer through this layer. A large fraction of the BC-containing particles disintegrate while passing the laser beam of the Single Particle Soot Photometer (SP2). This is shown for the first time for high-altitude aerosol layers in this study, giving evidence for heterogeneous mixing structures and possibly modified light-scattering and light-absorbing properties of the particles. This case study estimates the rBC mass import from the Pagami Creek forest fire into the upper troposphere/lower stratosphere (UTLS) region (best estimate: 25 Mg BC). A comparison to black carbon emission rates from aviation underlines the relevance of the import of forest fire aerosol on the BC load in the UTLS region. Our detailed information on the microphysics and the mixing state of the BC forest fire aerosol layer will help to better understand and investigate its radiative impact.

Description: 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.

Description: 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 ~0.3 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 were 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 datasets 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 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, compared also well (within ±17%). The estimated coating thickness values were consistent with thermo-optical analysis of OC and 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.

Description: 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.