Airborne minerals and related aerosol particles: Effects on climate and the environment

Aerosol particles are ubiquitous in the troposphere and exert an important influence on global climate and the environment. They affect climate through scattering, transmission, and absorption of radiation as well as by acting as nuclei for cloud formation. A significant fraction of the aerosol particle burden consists of minerals, and most of the remainder— whether natural or anthropogenic—consists of materials that can be studied by the same methods as are used for fine-grained minerals. Our emphasis is on the study and character of the individual particles. Sulfate particles are the main cooling agents among aerosols; we found that in the remote oceanic atmosphere a significant fraction is aggregated with soot, a material that can diminish the cooling effect of sulfate. Our results suggest oxidization of SO2 may have occurred on soot surfaces, implying that even in the remote marine troposphere soot provided nuclei for heterogeneous sulfate formation. Sea salt is the dominant aerosol species (by mass) above the oceans. In addition to being important light scatterers and contributors to cloud condensation nuclei, sea-salt particles also provide large surface areas for heterogeneous atmospheric reactions. Minerals comprise the dominant mass fraction of the atmospheric aerosol burden. As all geologists know, they are a highly heterogeneous mixture. However, among atmospheric scientists they are commonly treated as a fairly uniform group, and one whose interaction with radiation is widely assumed to be unpredictable. Given their abundances, large total surface areas, and reactivities, their role in influencing climate will require increased attention as climate models are refined.

Comment on “Low time resolution analysis of polar ice cores cannot detect impulsive nitrate events” by D.F. Smart et al.

Smart et al. (2014) suggested that the detection of nitrate spikes in polar ice cores from solar energetic particle (SEP) events could be achieved if an analytical system with sufficiently high resolution was used. Here we show that the spikes they associate with SEP events are not reliably recorded in cores from the same location, even when the resolution is clearly adequate. We explain the processes that limit the effective resolution of ice cores. Liquid conductivity data suggest that the observed spikes are associated with sodium or another nonacidic cation, making it likely that they result from deposition of sea salt or similar aerosol that has scavenged nitrate, rather than from a primary input of nitrate in the troposphere. We consider that there is no evidence at present to support the identification of any spikes in nitrate as representing SEP events. Although such events undoubtedly create nitrate in the atmosphere, we see no plausible route to using nitrate spikes to document the statistics of such events.

Size exclusion chromatogram of the Tannermoor 2009 sample after saltout experiments

Samples from a pristine raised peat bog runoff in Austria, the Tannermoor creek, were analysed for their iron linked to natural organic matter (NOM) content. Dissolved organic carbon < 0.45 µm (DOC) was 41 to 64 mg/L, iron 4.4 to 5.5 mg/L. Samples were analysed applying asymmetric field flow fractionation (AsFlFFF) coupled to UV-Vis absorption, fluorescence and inductively coupled plasma mass spectrometry (ICP-MS). The samples showed an iron peak associated with the NOM peak, one sample exhibiting a second peak of iron independent from the NOM peak. As highland peat bogs with similar climatic conditions and vegetation to the Tanner Moor are found throughout the world, including areas adjacent to the sea, we examined the behaviour of NOM and iron in samples brought to euhaline (35 per mil) conditions with artificial sea salt. The enhanced ionic strength reduced NOM by 53% and iron by 82%. Size exclusion chromatography (SEC) of the samples at sea-like salinity revealed two major fractions of NOM associated with different iron concentrations. The larger one, eluting sharply after the upper exclusion limits of 4000-5000 g/mol, seems to be most important for iron chelating. The results outline the global importance of sub-mountainous and mountainous raised peat bogs as a source of iron chelators to the marine environment at sites where such peat bogs release their run-offs into the sea.

Halogen deposition in polar snow and ice

The atmospheric chemistry of iodine and bromine in polar regions is of interest due to the key role of halogens in many atmospheric processes, particularly tropospheric ozone destruction. Bromine is emitted from the open ocean but is enriched above first-year sea ice during springtime bromine explosion events, whereas iodine is emitted from biological communities hosted by sea ice. It has been previously demonstrated that bromine and iodine are present in Antarctic ice over glacial-interglacial cycles. Here we investigate seasonal variability of bromine and iodine in polar snow and ice, to evaluate their emission, transport and deposition in Antarctica and the Arctic and better understand potential links to sea ice. We find that bromine enrichment (relative to sea salt content) and iodine concentrations in polar ice do vary seasonally in Arctic snow and Antarctic ice and we relate such variability to satellite-based observations of tropospheric halogen concentrations. Peaks of bromine enrichment in Arctic snow and Antarctic ice occur in spring and summer, when sunlight is present. Iodine concentrations are largest in winter Antarctic ice strata, contrary to contemporary observations of summer maxima in iodine emissions.

Dust and calcium record in calculated for ice core EPICA Dome C

Ice core data from Antarctica provide detailed insights into the characteristics of past climate, atmospheric circulation, as well as changes in the aerosol load of the atmosphere. We present high-resolution records of soluble calcium (Ca2+), non-sea-salt soluble calcium (nssCa2+), and particulate mineral dust aerosol from the East Antarctic Plateau at a depth resolution of 1 cm, spanning the past 800 000 years. Despite the fact that all three parameters are largely dust-derived, the ratio of nssCa2+ to particulate dust is dependent on the particulate dust concentration itself. We used principal component analysis to extract the joint climatic signal and produce a common high-resolution record of dust flux. This new record is used to identify Antarctic warming events during the past eight glacial periods. The phasing of dust flux and CO2 changes during glacial-interglacial transitions reveals that iron fertilization of the Southern Ocean during the past nine glacial terminations was not the dominant factor in the deglacial rise of CO2 concentrations. Rapid changes in dust flux during glacial terminations and Antarctic warming events point to a rapid response of the southern westerly wind belt in the region of southern South American dust sources on changing climate conditions. The clear lead of these dust changes on temperature rise suggests that an atmospheric reorganization occurred in the Southern Hemisphere before the Southern Ocean warmed significantly.

(Table 1, pages 283), Elemental concentrations of ferromanganese crusts from Lake Biwa, Japan

Ferromanganese crusts were sampled from the surface of a stone collected at a depth of 20 m in the northern part of Lake Biwa, Japan. These samples were analysed for 37 elements by neutron activation, X-ray fluorescence, and ICP-AE. The crusts were found to be enriched with Ba, P, B, As, and sometimes with Co, Ni, Cu and Sb. The elements were classified into 4 groups based on the varieties of host minerals (Fe-oxides, Mn-oxides or allochthonous materials) in which they were incorporated : elements mainly associated with 1) Mn-oxides : Ba, Ni, Cs, Sr and Co ; 2) Fe-oxides : P, B and As; 3) allochthonous materials : Na, K, Rb, Al, Ti, Sc, Hf and Th ; and 4) Mn-oxides plus allochthonous materials : rare earth elements and major heavy metals. The elemental compositions in the Lake Biwa concretions, including the crusts and Mn-deposits studied previously by these authors, were compared with those in other freshwater and oceanic concretions. As a result, the concentrations of rare earth elements and major heavy metals were found to be much lower, whereas those of B, P and As were higher in the Lake Biwa than in the oceanic concretions. These differences could be well explained in terms of the effects of sea salt, growth rates of the concretions, and pH of the formation environment.

Source/receptor reconciliation of ambient organic fine particulate matter in Palm Beach County

Airborne particulate matter (PM) is of environmental concern not only in urban but also rural areas that are easily inhalable and have been considered responsible, together with gaseous pollutants, for possible health effects. The objectives of this research study is to generate an extensive data set for ambient PM collected at Belle Glade and Delray Beach that ultimately was used together with published source profiles to predict the contributions of major sources to the overall airborne particle burden in Belle Glade and Delray Beach. ^ The size segregated particle sampling was conducted for one entire year. The samples collected during the months of January and May were further subjected to chemical analysis for organic compounds by Gas Chromatography-Mass Spectrometry. Additional, PM10 sampling was conducted simultaneously with size segregated particle sampling during January and May to analyze for trace elements using Instrumental Neutron Activation Analysis technique. Elements and organic marker compounds were used in Chemical Mass Balance modeling to determine the major source contribution to the ambient fine particle matter burden. ^ Size segregated particle distribution results show bimodal in both sampling sites. Sugarcane pre-harvest burning in the rural site elevated PM10 concentration by about 30% during the sugarcane harvest season compared to sugarcane growing season. Sea salt particles and Saharan dust particles accounted for the external sources. ^ The results of trace element analysis show that Al, Ca, Cs, Eu, Lu, Nd, Sc, Sm, Th, and Yb are more abundant at the rural sampling site. The trace elements Ba, Br, Ce, Cl, Cr, Fe, Gd, Hf, Na, Sb, Ta, V, and W show high abundance at the urban site due to anthropogenic activities except for Na and Cl, which are from sea salt spray. On the other hand, size segregated trace organic compounds measurements show that organic compounds mainly from combustion process were accumulated in PM0.95. ^ In conclusion, major particle sources were determined by the CMB8.2 software as follows: road dust, sugarcane leaf burning, diesel-powered and gasoline powered vehicle exhaust, leaf surface abrasion particles, and a very small fraction of meat cooking. ^

Age model of firn core DML03C98_09

The influence of atmospheric circulation patterns on sea salt aerosol deposition in the study area of the new EPICA (European Project for Ice Coring in Antarctica) deep drilling in Dronning Maud Land (DML), Antarctica, has been investigated. Comparison of ice core records with reanalysis data showed that recent sea salt concentrations are strongly influenced by the occurrence of a blocking high pressure ridge over the eastern and enhanced storm activity over the western Atlantic sector of the Southern Ocean (SO) leading to marine intrusions, thus enhanced sea salt export, into DML. These variations occur with periods of 4-5 and 12-14 yr, the prior being associated with the Antarctic Circumpolar Wave (ACW). The prevalence of these periodicities in a 2000 year ice core record from DML shows for the first time that the ACW is a prevalent feature of SO atmosphere dynamics over the last two millennia.

Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June, 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the N. E. Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm(-3), while background marine air aerosol concentrations were between 400-600 cm(-3). The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm(-3), was observed and attributed to open ocean particle formation. Continental air submicron chemical composition (excluding refractory sea salt) was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF) and cloud condensation nuclei (CCN) to total condensation nuclei (CN) concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40-50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by methanesulphonic acid (MSA). Sulphate concentrations were highest in marine tropical air - even higher than in continental air. MSA was present at twice the concentrations of previously-reported concentrations at the same location and the same season. Both continental and marine air exhibited aerosol GFs significantly less than ammonium sulphate aerosol pointing to a significant organic contribution to all air mass aerosol properties.