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Characterisation of sub-micron particle number concentrations and formation events in the western Bushveld Igneous Complex, South Africa

South Africa holds significant mineral resources, with a substantial fraction of these reserves occurring and being processed in a large geological structure termed the Bushveld Igneous Complex (BIC). The area is also highly populated by informal, semi-formal and formal residential developments. However, knowledge of air quality and research related to the atmosphere is still very limited in the area. In order to investigate the characteristics and processes affecting sub-micron particle number concentrations and formation events, air ion and aerosol particle size distributions and number concentrations, together with meteorological parameters, trace gases and particulate matter (PM) were measured for over two years at Marikana in the heart of the western BIC. The observations showed that trace gas (i.e. SO2, NOx, CO) and black carbon concentrations were relatively high, but in general within the limits of local air quality standards. The area was characterised by very high condensation sink due to background aerosol particles, PM10 and O3 concentration. The results indicated that high amounts of Aitken and accumulation mode particles originated from domestic burning for heating and cooking in the morning and evening, while during daytime SO2-based nucleation followed by the growth by condensation of vapours from industrial, residential and natural sources was the most probable source for large number concentrations of nucleation and Aitken mode particles. Nucleation event day frequency was extremely high, i.e. 86% of the analysed days, which to the knowledge of the authors is the highest frequency ever reported. The air mass back trajectory and wind direction analyses showed that the secondary particle formation was influenced both by local and regional pollution and vapour sources. Therefore, our observation of the annual cycle and magnitude of the particle formation and growth rates during nucleation events were similar to results previously published for a semi-clean savannah site in South Africa.
The genesis of Typhoon Nuri as observed during the Tropical Cyclone Structure 2008 (TCS08) field experiment – Part 2: Observations of the convective environment

Analyses of thermodynamic data gathered from airborne dropwindsondes during the Tropical Cyclone Structure (2008) experiment are presented for the disturbance that became Typhoon Nuri. Although previous work has suggested that Nuri formed within the protective recirculating "pouch" region of a westward propagating wave-like disturbance and implicated rotating deep convective clouds in driving the inflow to spin up the tangential circulation of the system-scale flow, the nature of the thermodynamic environment that supported the genesis remains a topic of debate. During the genesis phase, vertical profiles of virtual potential temperature show little variability between soundings on a particular day and the system-average soundings likewise show a negligible change. There is a tendency also for the lower and middle troposphere to moisten. However, the data show that, on the scale of the recirculating region of the disturbance, there was no noticeable reduction of virtual temperature in the lower troposphere, but a small warming (less than 1 K) in the upper troposphere. Vertical profiles of pseudo-equivalent potential temperature, θe, during the genesis show a modestly decreasing deficit of θe in the vertical between the surface and the height of minimum θe (between 3 and 4 km), from 17.5 K to 15.2 K. The findings reported here are consistent with those found for developing disturbances observed in the Pre-Depression Investigation of Cloud Systems in the Tropics (PREDICT) experiment in 2010. Some implications of the findings are discussed.
The summer aerosol in the central Arctic 1991–2008: did it change or not?

In the course of global warming dramatic changes are taking place in the Arctic and boreal environments. However, physical aerosol data in from the central summer Arctic taken over the course of 18 yr from 1991 to 2008 do not show systematic year-to-year changes, albeit substantial interannual variations. Besides the limited extent of the data several causes may be responsible for these findings. The processes controlling concentrations and particle size distribution of the aerosol over the central Arctic perennial pack ice area, north of 80°, may not have changed substantially during this time. Environmental changes are still mainly effective in the marginal ice zone, the ice-free waters and continental rims and have not propagated significantly into the central Arctic yet where they could affect the local aerosol and its sources. The analysis of meteorological conditions of the four expedition summers reveal substantial variations which we see as main causes of the measured variations in aerosol parameters. With combined lognormal fits of the hourly number size distributions of the four expeditions representative mode parameters for the summer aerosol in the central Arctic have been calculated. The combined aerosol statistics discussed in the present paper provide comprehensive physical data on the summer aerosol in the central Arctic. These data are the only surface aerosol information from this region.
Black carbon from ships: a review of the effects of ship speed, fuel quality and exhaust gas scrubbing

The International Maritime Organization (IMO) has moved to address the health and climate impact of the emissions from the combustion of low-quality residual fuels within the commercial shipping industry. Fuel sulfur content (FS) limits and an efficiency design index for future ships are examples of such IMO actions. The impacts of black carbon (BC) emissions from shipping are now under review by the IMO, with a particular focus on the potential impacts of future Arctic shipping. Recognizing that associating impacts with BC emissions requires both ambient and onboard observations, we provide recommendations for the measurement of BC. We also evaluate current insights regarding the effect of ship speed (engine load), fuel quality and exhaust gas scrubbing on BC emissions from ships. Observations demonstrate that BC emission factors (EFBC) increases 3 to 6 times at very low engine loads (<25% compared to EFBC at 85–100% load); absolute BC emissions (per nautical mile of travel) also increase up to 100% depending on engine load, even with reduced load fuel savings. If fleets were required to operate at lower maximum engine loads, presumably associated with reduced speeds, then engines could be re-tuned, which would reduce BC emissions. Ships operating in the Arctic are likely running at highly variable engine loads (25–100%) depending on ice conditions and ice breaking requirements. The ships operating at low load may be emitting up to 50% more BC than they would at their rated load. Such variable load conditions make it difficult to assess the likely emissions rate of BC. Current fuel sulfur regulations have the effect of reducing EFBC by an average of 30% and potentially up to 80% regardless of engine load; a removal rate similar to that of scrubbers. Uncertainties among current observations demonstrate there is a need for more information on a) the impact of fuel quality on EFBC using robust measurement methods and b) the efficacy of scrubbers for the removal of particulate matter by size and composition.
Optical-microphysical properties of Saharan dust aerosols and composition relationship using a multi-wavelength Raman lidar, in situ sensors and modelling: a case study analysis

A strong Saharan dust event that occurred over the city of Athens, Greece (37.9° N, 23.6° E) between 27 March and 3 April 2009 was followed by a synergy of three instruments: a 6-wavelength Raman lidar, a CIMEL sun-sky radiometer and the MODIS sensor. The BSC-DREAM model was used to forecast the dust event and to simulate the vertical profiles of the aerosol concentration. Due to mixture of dust particles with low clouds during most of the reported period, the dust event could be followed by the lidar only during the cloud-free day of 2 April 2009. The lidar data obtained were used to retrieve the vertical profile of the optical (extinction and backscatter coefficients) properties of aerosols in the troposphere. The aerosol optical depth (AOD) values derived from the CIMEL ranged from 0.33–0.91 (355 nm) to 0.18–0.60 (532 nm), while the lidar ratio (LR) values retrieved from the Raman lidar ranged within 75–100 sr (355 nm) and 45–75 sr (532 nm). Inside a selected dust layer region, between 1.8 and 3.5 km height, mean LR values were 83 ± 7 and 54 ± 7 sr, at 355 and 532 nm, respectively, while the Ångström-backscatter-related (ABR355/532) and Ångström-extinction-related (AER355/532) were found larger than 1 (1.17 ± 0.08 and 1.11 ± 0.02, respectively), indicating mixing of dust with other particles. Additionally, a retrieval technique representing dust as a mixture of spheres and spheroids was used to derive the mean aerosol microphysical properties (mean and effective radius, number, surface and volume density, and mean refractive index) inside the selected atmospheric layers. Thus, the mean value of the retrieved refractive index was found to be 1.49( ± 0.10) + 0.007( ± 0.007)i, and that of the effective radiuses was 0.30 ± 0.18 μm. The final data set of the aerosol optical and microphysical properties along with the water vapor profiles obtained by Raman lidar were incorporated into the ISORROPIA II model to provide a possible aerosol composition consistent with the retrieved refractive index values. Thus, the inferred chemical properties showed 12–40% of dust content, sulfate composition of 16–60%, and organic carbon content of 15–64%, indicating a possible mixing of dust with haze and smoke. PM10 concentrations levels, PM10 composition results and SEM-EDX (Scanning Electron Microscope-Energy Dispersive X-ray) analysis results on sizes and mineralogy of particles from samples during the Saharan dust transport event were used to evaluate the retrieval.
Distributions, long term trends and emissions of four perfluorocarbons in remote parts of the atmosphere and firn air

We report the first data set of atmospheric abundances for the following four perfluoroalkanes: n-decafluorobutane (n-C4F10), n-dodecafluoropentane (n-C5F12), n-tetradecafluorohexane (n-C6F14) and n-hexadecafluoroheptane (n-C7F16). All four compounds could be detected and quantified in air samples from remote locations in the Southern Hemisphere (at Cape Grim, Tasmania, archived samples dating back to 1978) and the upper troposphere (a passenger aircraft flying from Germany to South Africa). Further observations originate from air samples extracted from deep firn in Greenland and allow trends of atmospheric abundances in the earlier 20th century to be inferred. All four compounds were not present in the atmosphere prior to the 1960s. n-C4F10 and n-C5F12 were also measured in samples collected in the stratosphere with the data indicating that they have no significant sinks in this region. Emissions were inferred from these observations and found to be comparable with emissions from the EDGAR database for n-C6F14. However, emissions of n-C4F10, n-C5F12 and n-C7F16 were found to differ by up to five orders of magnitude between our approach and the database. Although the abundances of the four perfluorocarbons reported here are currently small (less than 0.3 parts per trillion) they have strong Global Warming Potentials several thousand times higher than carbon dioxide (on a 100-yr time horizon) and continue to increase in the atmosphere. We estimate that the sum of their cumulative emissions reached 325 million metric tonnes CO2 equivalent at the end of 2009.
Observation of atmospheric aerosols at Mt. Hua and Mt. Tai in central and east China during spring 2009 – Part 2: Impact of dust storm on organic aerosol composition and size distribution

PM10 and size-resolved particles (9-stage) were simultaneously collected at Mt. Hua and Mt. Tai in central and east China during the spring of 2009 including a massive dust storm occurring on 24 April (named as DS II), and determined for organic compounds to investigate the impact of dust storm on organic aerosols. High molecular weight (HMW) n-alkanes, fatty acids, and fatty alcohols and trehalose sharply increased and almost entirely stayed in coarse particles when dust storm was present, suggesting that high level of organic aerosols in the mountain atmospheres during the event largely originated from Gobi desert plants. However, most anthropogenic aerosols (e.g. PAHs, and aromatic and dicarboxylic acids) during the event significantly decreased due to a dilution effect, indicating that anthropogenic aerosols in the mountain atmospheres during the nonevent period largely originated from local/regional sources rather than from long-range transport. Trehalose, a metabolism product enriched in biota in dry conditions, was 62 ± 78 and 421 ± 181 ng m−3 at Mt. Hua and Mt. Tai during DS II, 10–30 times higher than that in the nonevent time, indicating that trehalose may be a tracer for dust emissions from Gobi desert regions. Molecular compositions of organic aerosols in the mountain samples demonstrate that domestic coal burning is still the major source of PAHs in China. n-Alkanes and fatty acids showed a bimodal size distribution during the nonevent with a major peak in fine mode (<2.1 μm) and a small peak in coarse mode (>2.1 μm). The coarse mode significantly increased and even dominated over the whole size range when dust was present. Glucose and trehalose were also dominant in the coarse mode especially in the DS II time. PAHs and levoglucosan concentrated in fine particles with no significant changes in size distribution when dust storm occurred. However, phthalic and succinic acids showed bimodal size distribution pattern with an increase in coarse mode during the event, because both are formed via a gas phase oxidation and a subsequent condensation/adsorption onto aerosol phase. In contrast, terephthalic and malic acids are mostly emitted from combustion process as fine particles, thus both showed a fine mode pattern during the whole campaign with a minor peak in coarse mode caused by an increased coagulation with dust during the event. Geometric mean diameters (GMDs) of the organic aerosols above are in general larger at Mt.~Hua than at Mt. Tai during the nonevent period. We found that during the event GMD of the fine mode organics that derived mostly from the local/regional sources rather than Gobi desert became smaller while GMD of them in coarse mode became larger. Such a splitting in sizes during the event is most likely caused by decreased fine particle coagulation due to dilution and increased adsorption/coagulation with dust.
Saharan dust event impacts on cloud formation and radiation over Western Europe

We investigated the impact of mineral dust particles on clouds, radiation and atmospheric state during a strong Saharan dust event over Europe in May 2008, applying a comprehensive online-coupled regional model framework that explicitly treats particle microphysics and chemical composition. Sophisticated parameterizations for aerosol activation and ice nucleation, together with two-moment cloud microphysics are used to calculate the interaction of the different particles with clouds depending on their physical and chemical properties. The impact of dust on cloud droplet number concentration was found to be low, with just a slight increase in cloud droplet number concentration for both uncoated and coated dust. For temperatures lower than the level of homogeneous freezing, no significant impact of dust on the number and mass concentration of ice crystals was found, though the concentration of frozen dust particles reached up to 100 l−1 during the ice nucleation events. Mineral dust particles were found to have the largest impact on clouds in a temperature range between freezing level and the level of homogeneous freezing, where they determined the number concentration of ice crystals due to efficient heterogeneous freezing of the dust particles and modified the glaciation of mixed phase clouds. Our simulations show that during the dust events, ice crystals concentrations were increased twofold in this temperature range (compared to if dust interactions are neglected). This had a significant impact on the cloud optical properties, causing a reduction in the incoming short-wave radiation at the surface up to −75 W m−2. Including the direct interaction of dust with radiation caused an additional reduction in the incoming short-wave radiation by 40 to 80 W m−2, and the incoming long-wave radiation at the surface was increased significantly in the order of +10 W m−2. The strong radiative forcings associated with dust caused a reduction in surface temperature in the order of −0.2 to −0.5 K for most parts of France, Germany, and Italy during the dust event. The maximum difference in surface temperature was found in the East of France, the Benelux, and Western Germany with up to −1 K. This magnitude of temperature change was sufficient to explain a systematic bias in numerical weather forecasts during the period of the dust event.
Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF

The first ambient measurements using nitrate ion based Chemical Ionization with the Atmospheric Pressure interface Time-Of-Flight mass spectrometer (CI-APi-TOF) for sulphuric acid and neutral cluster detection are presented. We have found CI-APi-TOF a highly stable and sensitive tool for molecular sulphuric acid detection. The lowest limit of detection for sulphuric acid was determined to be 3.6 × 104 molecules cm−3 for 15 min averaging. Signals from sulphuric acid clusters up to tetramer containing ammonia were also obtained but these were found to result from naturally charged clusters formed by ion induced clustering in the atmosphere during nucleation. Opposite to earlier studies with cluster mass spectrometers, we had no indication of neutral clusters. The reason is either less efficient charging of clusters in comparison to molecular sulphuric acid, or the low concentration of neutral clusters at our measurement site during these particular nucleation events. We show that utilizing high resolution mass spectrometry is crucial in separating the weak sulfuric acid cluster signal from other compounds.
Changes in black carbon deposition to Antarctica from two high-resolution ice core records, 1850–2000 AD

Refractory black carbon aerosols (rBC) emitted by biomass burning (fires) and fossil fuel combustion, affect global climate and atmospheric chemistry. In the Southern Hemisphere (SH), rBC is transported in the atmosphere from low- and mid-latitudes to Antarctica and deposited to the polar ice sheet preserving a history of emissions and atmospheric transport. Here, we present two high-resolution Antarctic rBC ice core records drilled from the West Antarctic Ice Sheet divide and Law Dome on the periphery of the East Antarctic ice sheet. Separated by ~3500 km, the records span calendar years 1850–2001 and reflect the rBC distribution over the Indian and Pacific ocean sectors of the Southern Ocean. Concentrations of rBC in the ice cores displayed significant variability at annual to decadal time scales, notably in ENSO-QBO and AAO frequency bands. The delay observed between rBC and ENSO variability suggested that ENSO does not directly affect rBC transport, but rather continental hydrology, subsequent fire regimes, and aerosol emissions. From 1850 to 1950, the two ice core records were uncorrelated but were highly correlated from 1950 to 2002 (cross-correlation coefficient at annual resolution: r = 0.54, p < 0.01) due to a common decrease in rBC variability. The decrease in ice-core rBC from the 1950s to late 1980s displays similarities with inventories of SH rBC grass fires and biofuel emissions, which show reduced emission estimates over that period.