Antarctic Aerosol Research Articles

Australian Black summer smoke signal on Antarctic aerosol collected between New Zealand and the Ross sea

Open biomass burning (BB) events are a well-known primary aerosol source, resulting in the emission of significant amount of gaseous and particulate matter and affecting Earth's radiation budget. The 2019–2020 summer, known as “Australian Black Summer”, showed exceptional duration and intensity of seasonal wildfires, triggered by high temperatures and severe droughts. Since increasing megafires are predicted due to expected climate changes, it is critical to study the impact of BB aerosol on a large scale and evaluate related transport processes. In this study, five aerosol samples (total suspended particles with a diameter >1 μm) were collected during the XXXV Italian Expedition in Antarctica on board of the R/V Laura Bassi from 6th of January to February 16, 2020, along the sailing route from Lyttelton harbor (New Zealand) to Terra Nova Bay (Antarctica). Levoglucosan and its isomers have been analyzed as markers of BB, together with polycyclic aromatic hydrocarbons (PAHs), sucrose and alcohol sugars. Ionic species and carboxylic acids have been analyzed to support the identification of aerosol sources and its aging. Results showed high levoglucosan concentrations (325–1266 pg m−3) during the campaign, suggesting the widespread presence of smoke in the region, because of huge wildfire releases. Backward trajectories indicated the presence of long-range atmospheric transport from South America, probably carrying wildfires plume, in agreement with literature. Regional sources have been suggested for PAHs, particularly for 3–4 rings' compounds; monosaccharides, sucrose, arabitol, and mannitol were related to marine and biogenic contributions. In a warming climate scenario, more frequent and extensive wildfire episodes are expected in Australia, potentially altering albedo, aerosol radiative properties, and cloud interactions. Therefore, it is crucial to strengthens the investigations on the regional climatic effects of these events in Antarctica.

Theoretical derivation of aerosol lidar ratio using Mie theory for CALIOP-CALIPSO and OPAC aerosol models

Abstract. The extinction-to-backscattering ratio, popularly known as lidar (light detection and ranging) ratio of atmospheric aerosols is an important optical property, which is essential to retrieve the extinction profiles of atmospheric aerosols. Lidar satellite observations can provide the global coverage of atmospheric aerosols along with their vertical extent. NASA's Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite is the only space-based platform available, so far, that provides the vertical profiles of extinction due to atmospheric aerosols. A physics-based theoretical approach is presented in the present paper that estimates lidar ratio values for CALIPSO aerosol models, which can be used as inputs to determine the extinction profiles of aerosols using CALIPSO data. The developed methodology was also qualified by comparing it with the lidar ratio values derived using AERONET (AErosol RObotic NETwork) datasets. Lidar ratio values for CALIPSO aerosol models were estimated in the range of 38.72 to 85.98 sr at 532 nm, whereas at 1064 nm lidar ratio varied between 20.11 to 71.11 sr depending upon the aerosol type and their size distributions. Aerosols are compositions of various particles; thus, the presence of water vapour in the atmosphere can affect the optical properties of the aerosols. Thus, the effect of relative humidity on lidar ratio was studied using Optical Properties of Aerosols and Clouds (OPAC) aerosol models, which are the standard aerosol models against the cluster-classified AERONET and CALIPSO aerosol models. Water-soluble particles contribute substantially in clean continental, clean marine, tropical marine and desert aerosol models and are hygroscopic in nature. Hygroscopic sulfate particles dominate the Antarctic aerosols during summertime. In the presence of relative humidity between 0 %–80 %, the lidar ratio values were observed to decrease from 53.59 to 47.13, from 53.66 to 47.15, from 53.70 to 47.16, and from 55.32 to 48.78 sr at 532 nm for clean continental, clean marine, tropical marine, and desert aerosols, respectively, whereas lidar ratio gradually increased from 47.13 to 51, from 47.15 to 51, from 47.16 to 51, and from 48.78 to 51.68 sr, respectively, for these aerosol models when relative humidity was between 80 %–99 %, due to constituent hygroscopic particles. In the case of Antarctic aerosols, the lidar ratio was observed to increase from 57.73 to 97.64 sr due to hygroscopic sulfate particles that backscattered heavily in the presence of water vapour at 532 nm. The soot particles dominate the polluted continental and polluted marine particles, causing an increase in lidar ratio over its corresponding clean counterpart. Similar results were observed at 1064 nm for OPAC aerosol models.

A Review of Atmospheric Aerosols in Antarctica: From Characterization to Data Processing

One of the major problems of the present era is air pollution, not only for its impact on climate change but also for the diseases provoked by this scourge. Among the most concerning air pollutants is particulate matter, since it can travel long distances and affect the entire globe. Antarctica is extremely sensitive to climate change and essential for regulating temperature and permitting life on Earth. Therefore, air quality studies in this region are extremely important. The aim of this review is to present the work conducted on the identification and detection of aerosols and particulate matter in the Antarctic region in the last 20 years. These studies revealed a large number of organic and inorganic species. Organochlorine pesticides or polychlorinated biphenyls represent almost 50% of the organic fraction detected in Antarctica. Furthermore, heavy metals such as Hg and Pb were also found in the region related to anthropogenic activities. To summarize, this work detailed different analytical techniques and data processing to help characterize Antarctic aerosols and their potential sources.

Summertime High Abundances of Succinic, Citric, and Glyoxylic Acids in Antarctic Aerosols: Implications to Secondary Organic Aerosol Formation

AbstractObservations of organic compounds associated with natural sources are scarce in Antarctica, which limits our understanding of their sources and formation processes over the pristine region. Summertime Antarctic PM10 samples collected from Bharati station were studied for a homologous series of dicarboxylic acids (C2‐C12), ω‐oxoacids (C2‐C9), α‐dicarbonyls (C2‐C3) as well as citric and pyruvic acids by employing a water‐extraction followed by dibutyl ester derivatization technique and analyzed using capillary gas chromatography (GC). Results show that succinic (C4) and citric acids are the foremost abundant among the measured organic acids followed by glyoxylic (ωC2), azelaic (C9), and adipic (C6) acids. Such a typical molecular distribution of organic acids suggests the dominance of natural sources over the Antarctic. Two distinct air masses arrived from different altitudes, high and low altitude‐troposphere (HTAs and LTAs), showed a significant difference in mass concentrations of organic acids with higher values in LTAs. Total diacids‐C accounted for ∼9% of total carbon in HTAs, which is linked to chemical aging during long‐range transport. The higher abundance of C4 and citric acids are likely produced through secondary photooxidation of marine‐derived organic precursors, such as unsaturated fatty acids, phenolic, and biogenic isoprene compounds enriched in sea‐surface microlayer, via sea‐to‐air emission as confirmed by the significant (p < 0.05) correlations among the organic tracer compounds. Minor concentrations of oxalic and malonic (C2 and C3) acids were attributed to photo iron‐complex reactions in the aqueous‐phase atmosphere. These findings may help in reducing model uncertainties and present new insights into the secondary formation of organic aerosols in the polar environment.

Ammonium in Antarctic Aerosol: Marine Biological Activity Versus Long‐Range Transport of Biomass Burning

AbstractYear‐round records of the ionic composition of Antarctic aerosol were obtained at the inland Dome C (DC) and coastal Neumayer (NM) sites, with additional observations of black carbon (BC) at NM. Discussions focus on the origin of ammonium in Antarctica. This first Antarctic atmospheric study of several species emitted by biomass burning (BB) indicates that BC and oxalate reach a maximum in October in relation to BB activity in the southern hemisphere. Ammonium reaches a maximum 2 months later, suggesting that BB remains a minor ammonium source there. The ammonium maximum in December coincides with the occurrence of diatom blooms in the austral ocean, suggesting that oceanic ammonia emissions are the main source of ammonium in Antarctica. The ammonium to sulfur‐derived biogenic species molar ratio of 0.15 in summer suggests far lower ammonia emissions from the Antarctic oceans than midlatitude southern oceans.

Determination of Cd, Pb, and Cu in the Atmospheric Aerosol of Central East Antarctica at Dome C (Concordia Station).

Trace heavy metals Cd, Pb, and Cu were determined (by square wave anodic stripping voltammetry) in aerosol samples collected at Dome C (the Italo-French Station Concordia), a remote site of the Central East Antarctic plateau, for which no data are available until now. During the Austral Summer 2005–2006, three PM10 high-volume impactors were installed in two locations nearby of Concordia station: the first one very close and downwind of the station (about 50 m north), the other two (very close to each other) in a ‘distant’ site, upwind of the station and close to the astrophysics tent (not used in that expedition) at ~800 m south of Station Concordia. For each sample, the availability of the mass of the aerosol collected (obtained by differential weighing carried out on site), in addition to the volume of the filtered air, allowed us to express results both in terms of metal mass fractions in the aerosol and in the usual way of metal atmospheric concentrations. Metal contents increased in the order Cd < Pb < Cu with the following ranges of values: Cd 1.0–8.4 µg g−1 (0.09–3.1 pg m−3), Pb 96–470 µg g−1 (12–62 pg m−3), and Cu 0.17–20 mg g−1 (0.027–2.4 ng m−3). From the metal temporal profiles obtained we estimated the following background values for the area of Dome C, expressed both in mass fractions and in atmospheric concentrations: Cd 1.2 ± 0.2 µg g−1 (0.24 ± 0.13 pg m−3), Pb (here fixed as upper limit) 113 ± 13 µg g−1 (21 ± 8 pg m−3), and Cu 0.91 ± 0.48 mg g−1 (0.12 ± 0.07 ng m−3). The highest values were observed in the first part of the season, and particularly for the site close to the station, possibly related to sample contamination linked to intense activity at the Concordia station connected with the beginning of the expedition, including aircraft arrivals/departures. Increments of up to 10 times (and even 20 times for Cu) were recorded with respect to the background values. The metal excesses of the contaminated over background samples were found approximately, except for Cu, in the same proportion of the metal contents of the special Antarctic blend (SAB) diesel fuel, which is used almost exclusively at Concordia Station. The effect of the wind direction was also observed. Thus in the intermediate period of the campaign, when the wind direction reversed for several days with respect to the prevailing one, Cd and Pb metal contents decreased at the sampling point installed close to the station, now upwind of Concordia station, and increased at the ‘clean’ site astrophysics tent, turned downwind at the main station. No simple and easily interpretable effect of the wind direction was observed for Cu, which suggests that some other extemporaneous and not clearly identified factor may have intervened in this case. These results suggest that the human impact at Dome C influences mainly the zone very close to the station, but also the area in the neighborhood, including the supposed clean site of the astrophysics tent (about 800 m far from the station), when the wind direction reverses with respect to the prevailing one, leaving the site downwind of the station Concordia. Since no other data are reported for the Dome C area, our results are compared with literature data referred to the South Pole Station (the only other plateau site for which data are available) and several other coastal Antarctic sites, observing that our results (excluding Cu) are the lowest ever observed for Antarctic aerosol.

AWARE: The Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment

AbstractThe U.S. Department of Energy Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment (AWARE) performed comprehensive meteorological and aerosol measurements and ground-based atmospheric remote sensing at two Antarctic stations using the most advanced instrumentation available. A suite of cloud research radars, lidars, spectral and broadband radiometers, aerosol chemical and microphysical sampling equipment, and meteorological instrumentation was deployed at McMurdo Station on Ross Island from December 2015 through December 2016. A smaller suite of radiometers and meteorological equipment, including radiosondes optimized for surface energy budget measurement, was deployed on the West Antarctic Ice Sheet between 4 December 2015 and 17 January 2016. AWARE provided Antarctic atmospheric data comparable to several well-instrumented high Arctic sites that have operated for many years and that reveal numerous contrasts with the Arctic in aerosol and cloud microphysical properties. These include persistent differences in liquid cloud occurrence, cloud height, and cloud thickness. Antarctic aerosol properties are also quite different from the Arctic in both seasonal cycle and composition, due to the continent’s isolation from lower latitudes by Southern Ocean storm tracks. Antarctic aerosol number and mass concentrations are not only non-negligible but perhaps play a more important role than previously recognized because of the higher sensitivities of clouds at the very low concentrations caused by the large-scale dynamical isolation. Antarctic aerosol chemical composition, particularly organic components, has implications for local cloud microphysics. The AWARE dataset, fully available online in the ARM Program data archive, offers numerous case studies for unique and rigorous evaluation of mixed-phase cloud parameterization in climate models.

On the annual variability of Antarctic aerosol size distributions at Halley Research Station

Abstract. The Southern Ocean and Antarctic region currently best represent one of the few places left on our planet with conditions similar to the preindustrial age. Currently, climate models have a low ability to simulate conditions forming the aerosol baseline; a major uncertainty comes from the lack of understanding of aerosol size distributions and their dynamics. Contrasting studies stress that primary sea salt aerosol can contribute significantly to the aerosol population, challenging the concept of climate biogenic regulation by new particle formation (NPF) from dimethyl sulfide marine emissions. We present a statistical cluster analysis of the physical characteristics of particle size distributions (PSDs) collected at Halley (Antarctica) for the year 2015 (89 % data coverage; 6–209 nm size range; daily size resolution). By applying the Hartigan–Wong k-mean method we find eight clusters describing the entire aerosol population. Three clusters show pristine average low particle number concentrations (&lt; 121–179 cm−3) with three main modes (30, 75–95 and 135–160 nm) and represent 57 % of the annual PSD (up to 89 %–100 % during winter and 34 %–65 % during summer based on monthly averages). Nucleation and Aitken mode PSD clusters dominate summer months (September–January, 59 %–90 %), whereas a clear bimodal distribution (43 and 134 nm, respectively; Hoppel minimum at mode 75 nm) is seen only during the December–April period (6 %–21 %). Major findings of the current work include: (1) NPF and growth events originate from both the sea ice marginal zone and the Antarctic plateau, strongly suggesting multiple vertical origins, including the marine boundary layer and free troposphere; (2) very low particle number concentrations are detected for a substantial part of the year (57 %), including summer (34 %–65 %), suggesting that the strong annual aerosol concentration cycle is driven by a short temporal interval of strong NPF events; (3) a unique pristine aerosol cluster is seen with a bimodal size distribution (75 and 160 nm, respectively), strongly associated with high wind speed and possibly associated with blowing snow and sea spray sea salt, dominating the winter aerosol population (34 %–54 %). A brief comparison with two other stations (Dome C – Concordia – and King Sejong Station) during the year 2015 (240 d overlap) shows that the dynamics of aerosol number concentrations and distributions are more complex than the simple sulfate–sea-spray binary combination, and it is likely that an array of additional chemical components and processes drive the aerosol population. A conceptual illustration is proposed indicating the various atmospheric processes related to the Antarctic aerosols, with particular emphasis on the origin of new particle formation and growth.

The importance of blowing snow to halogen-containing aerosol in coastal Antarctica: influence of source region versus wind speed

Abstract. A fundamental understanding of the processes that control Antarctic aerosols is necessary in determining the aerosol impacts on climate-relevant processes from Antarctic ice cores to clouds. The first in situ observational online composition measurements by an aerosol mass spectrometer (AMS) of Antarctic aerosols were only recently performed during the Two-Season Ozone Depletion and Interaction with Aerosols Campaign (2ODIAC). 2ODIAC was deployed to sea ice on the Ross Sea near McMurdo Station over two field seasons: austral spring–summer 2014 and winter–spring 2015. The results presented here focus on the overall trends in aerosol composition primarily as functions of air masses and local meteorological conditions. The results suggest that the impact of long-range air mass back trajectories on either the absolute or relative concentrations of the aerosol constituents measured by (and inferred from) an AMS at a coastal location is small relative to the impact of local meteorology. However, when the data are parsed by wind speed, two observations become clear. First, a critical wind speed is required to loft snow from the surface, which, in turn, increases particle counts in all measured size bins. Second, elevated wind speeds showed increased aerosol chloride and sodium. Further inspection of the AMS data shows that the increased chloride concentrations have more of a “fast-vaporizing” nature than chloride measured at low wind speed. Also presented are the Cl:Na ratios of snow samples and aerosol filter samples, as measured by ion chromatography, as well as non-chloride aerosol constituents measured by the AMS. Additionally, submicron aerosol iodine and bromine concentrations as functions of wind speed are also presented. The results presented here suggest that aerosol composition in coastal Antarctica is a strong function of wind speed and that the mechanisms determining aerosol composition are likely linked to blowing snow.

Real-time detection of airborne fluorescent bioparticles in Antarctica

Abstract. We demonstrate, for the first time, continuous real-time observations of airborne bio-fluorescent aerosols recorded at the British Antarctic Survey's Halley VI Research Station, located on the Brunt Ice Shelf close to the Weddell Sea coast (lat 75°34′59′′ S, long 26°10′0′′ W) during Antarctic summer, 2015. As part of the NERC MAC (Microphysics of Antarctic Clouds) aircraft aerosol cloud interaction project, observations with a real-time ultraviolet-light-induced fluorescence (UV-LIF) spectrometer were conducted to quantify airborne biological containing particle concentrations along with dust particles as a function of wind speed and direction over a 3-week period. Significant, intermittent enhancements of both non- and bio-fluorescent particles were observed to varying degrees in very specific wind directions and during strong wind events. Analysis of the particle UV-induced emission spectra, particle sizes and shapes recorded during these events suggest the majority of particles were likely a subset of dust with weak fluorescence emission responses. A minor fraction, however, were likely primary biological particles that were very strongly fluorescent, with a subset identified as likely being pollen based on comparison with laboratory data obtained using the same instrument. A strong correlation of bio-fluorescent particles with wind speed was observed in some, but not all, periods. Interestingly, the fraction of fluorescent particles to total particle concentration also increased significantly with wind speed during these events. The enhancement in concentrations of these particles could be interpreted as due to resuspension from the local ice surface but more likely due to emissions from distal sources within Antarctica as well as intercontinental transport. Likely distal sources identified by back trajectory analyses and dispersion modelling were the coastal ice margin zones in Halley Bay consisting of bird colonies with likely associated high bacterial activity together with contributions from exposed ice margin bacterial colonies but also long-range transport from the southern coasts of Argentina and Chile. Dispersion modelling also demonstrated emissions from shipping lanes, and therefore marine anthropogenic sources cannot be ruled out. Average total concentrations of total fluorescent aerosols were found to be 1.9 ± 2.6 L−1 over a 3-week period crossing over from November into December, but peak concentrations during intermittent enhancement events could be up to several tens per litre. While this short pilot study is not intended to be generally representative of Antarctic aerosol, it demonstrates the usefulness of the UV-LIF measurement technique for quantification of airborne bioaerosol concentrations and to understand their dispersion. The potential importance for microbial colonisation of Antarctica is highlighted.

Aerosol and snow transfer processes: An investigation on the behavior of water-soluble organic compounds and ionic species

The concentrations of water-soluble compounds (ions, carboxylic acids, amino acids, sugars, phenolic compounds) in aerosol and snow have been determined at the coastal Italian base “Mario Zucchelli” (Antarctica) during the 2014–2015 austral summer. The main aim of this research was to investigate the air-snow transfer processes of a number of classes of chemical compounds and investigate their potential as tracers for specific sources.The composition and particle size distribution of Antarctic aerosol was measured, and water-soluble compounds accounted for 66% of the PM10 total mass concentration. The major ions Na+, Mg2+, Cl− and SO42− made up 99% of the total water soluble compound concentration indicating that sea spray input was the main source of aerosol. These ionic species were found mainly in the coarse fraction of the aerosol resulting in enhanced deposition, as reflected by the snow composition.Biogenic sources were identified using chemical markers such as carboxylic acids, amino acids, sugars and phenolic compounds. This study describes the first characterization of amino acids and sugar concentrations in surface snow. High concentrations of amino acids were found after a snowfall event, their presence is probably due to the degradation of biological material scavenged during the snow event. Alcohol sugars increased in concentration after the snow event, suggesting a deposition of primary biological particles, such as airborne fungal spores.

A missing source of aerosols in Antarctica – beyond long-range transport, phytoplankton, and photochemistry

Abstract. Understanding the sources and evolution of aerosols is crucial for constraining the impacts that aerosols have on a global scale. An unanswered question in atmospheric science is the source and evolution of the Antarctic aerosol population. Previous work over the continent has primarily utilized low temporal resolution aerosol filters to answer questions about the chemical composition of Antarctic aerosols. Bulk aerosol sampling has been useful in identifying seasonal cycles in the aerosol populations, especially in populations that have been attributed to Southern Ocean phytoplankton emissions. However, real-time, high-resolution chemical composition data are necessary to identify the mechanisms and exact timing of changes in the Antarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion and Interaction with Aerosols Campaign) field campaign saw the first ever deployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS – soot particle aerosol mass spectrometer – or AMS) to the continent. Data obtained from the AMS, and a suite of other aerosol, gas-phase, and meteorological instruments, are presented here. In particular, this paper focuses on the aerosol population over coastal Antarctica and the evolution of that population in austral spring. Results indicate that there exists a sulfate mode in Antarctica that is externally mixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtime increases in sulfate aerosol are observed and attributed to biogenic sources, in agreement with previous research identifying phytoplankton activity as the source of the aerosol. Furthermore, the total Antarctic aerosol population is shown to undergo three distinct phases during the winter to summer transition. The first phase is dominated by highly aged sulfate particles comprising the majority of the aerosol mass at low wind speed. The second phase, previously unidentified, is the generation of a sub-250 nm aerosol population of unknown composition. The second phase appears as a transitional phase during the extended polar sunrise. The third phase is marked by an increased importance of biogenically derived sulfate to the total aerosol population (photolysis of dimethyl sulfate and methanesulfonic acid (DMS and MSA)). The increased importance of MSA is identified both through the direct, real-time measurement of aerosol MSA and through the use of positive matrix factorization on the sulfur-containing ions in the high-resolution mass-spectral data. Given the importance of sub-250 nm particles, the aforementioned second phase suggests that early austral spring is the season where new particle formation mechanisms are likely to have the largest contribution to the aerosol population in Antarctica.

Particle size distribution of inorganic and organic ions in coastal and inland Antarctic aerosol.

The concentration and particle-size distribution of ionic species in Antarctic aerosol samples were determined to investigate their potential sources, chemical evolution, and transport. We analyzed aerosol samples collected at two different Antarctic sites: a coastal site near Victoria Land close to the Italian Research Base "Mario Zucchelli", and another site located on the Antarctic plateau, close to Italian-French Concordia Research Station. We investigated anionic compounds using ion-chromatography coupled to mass spectrometry, and cationic species through capillary ion chromatography with conductometry. Aerosol collected close to the coast was mainly characterized by sea salt species such as Na+, Mg2+, and SO42-. These species represented a percentage of 88% of the total sum of all detected ionic species in the aerosol samples from the coastal site. These species were mainly distributed in the coarse fraction, confirming the presence of primary aerosol near the ocean source. Aerosol collected over the Antarctic plateau was characterized by high acidity, with nss-SO42-, NO3-, and methanesulfonic acid as the most abundant species. These species were mainly distributed in the <0.49μm fraction, and they had a behavior of a typical secondary aerosol, where several chemical and physical processes occurred.

Single-particle investigation of summertime and wintertime Antarctic sea spray aerosols using low-&amp;lt;i&amp;gt;Z&amp;lt;/i&amp;gt; particle EPMA, Raman microspectrometry, and ATR-FTIR imaging techniques

Abstract. Two aerosol samples collected at King Sejong Korean scientific research station, Antarctica, on 9 December 2011 in the austral summer (sample S1) and 23 July 2012 in the austral winter (sample S2), when the oceanic chlorophyll a levels on the collection days of the samples were quite different, by ∼ 19 times (2.46 vs. 0.13 µg L−1, respectively), were investigated on a single-particle basis using quantitative energy-dispersive electron probe X-ray microanalysis (ED-EPMA), called low-Z particle EPMA, Raman microspectrometry (RMS), and attenuated total reflection Fourier transform infrared (ATR-FTIR) imaging techniques to obtain their characteristics based on the elemental chemical compositions, molecular species, and mixing state. X-ray analysis showed that the supermicron summertime and wintertime Antarctic aerosol samples have different elemental chemical compositions, even though all the individual particles analyzed were sea spray aerosols (SSAs); i.e., the contents of C, O, Ca, S, and Si were more elevated, whereas Cl was more depleted, for sample S1 than for sample S2. Based on qualitative analysis of the chemical species present in individual SSAs by the combined application of RMS and ATR-FTIR imaging, different organic species were observed in samples S1 and S2; i.e., Mg hydrate salts of alanine were predominant in samples S1 and S2, whereas Mg salts of fatty acids internally mixed with Mg hydrate salts of alanine were significant in sample S2. Although CaSO4 was observed significantly in both samples S1 and S2, other inorganic species, such as Na2SO4, NaNO3, Mg(NO3)2, SiO2, and CH3SO3Mg, were observed more significantly in sample S1, suggesting that those compounds may be related to the higher phytoplankton activity in summer.

Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice

Abstract. Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm−3 – higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of cloud and aerosol over the Southern Ocean.

An integrated study of the chemical composition of Antarctic aerosol to investigate natural and anthropogenic sources

Environmental contextOwing to its remoteness, Antarctica is an excellent natural laboratory for conducting studies on the behavior of marine aerosols and for monitoring the impact of global human activities. The aim of this study is to provide an extensive chemical characterization of Antarctic aerosol and to investigate its sources. A distinction among anthropogenic, crustal, and biogenic sources was defined using several chemical markers. AbstractDuring the 2010–11 austral summer, an aerosol sampling campaign was carried out at a coastal Antarctic site (Terra Nova Bay, Victoria Land). In this work, previously published data about water-soluble organic compounds and major and trace elements were merged with novel measurements of major ions, carboxylic acids and persistent organic pollutants (polychlorobiphenyls, polycyclic aromatic hydrocarbons, polychlorinated naphthalenes, polybrominated diphenylethers and organochlorine pesticides) in order to provide a chemical characterisation of Antarctic aerosol and to investigate its sources. The persistent organic pollutants were determined using a high-volume sampler, able to collect both particulate and gaseous fractions, whereas remaining compounds were determined by performing an aerosol size fractionation with a PM10 cascade impactor. Ionic species represented 58% (350ng m–3) of the sum of concentrations of all detected compounds (596ng m–3) in our Antarctic PM10 aerosol samples due to natural emission. Trace concentrations of persistent organic pollutants highlighted that the occurrence of these species can be due to long-range atmospheric transport or due to the research base. Factor analysis was applied to the dataset obtained from the samples collected with the PM10 sampler in order to make a distinction between anthropogenic, crustal and biogenic sources using specific chemical markers.

Levoglucosan and phenols in Antarctic marine, coastal and plateau aerosols

Due to its isolated location, Antarctica is a natural laboratory for studying atmospheric aerosols and pollution in remote areas. Here, we determined levoglucosan and phenolic compounds (PCs) at diverse Antarctic sites: on the plateau, a coastal station and during an oceanographic cruise. Levoglucosan and PCs reached the Antarctic plateau where they were observed in accumulation mode aerosols (with median levoglucosan concentrations of 6.4pgm−3 and 4.1pgm−3, and median PC concentrations of 15.0pgm−3 and 7.3pgm−3). Aged aerosols arrived at the coastal site through katabatic circulation with the majority of the levoglucosan mass distributed on larger particulates (24.8pgm−3), while PCs were present in fine particles (34.0pgm−3). The low levoglucosan/PC ratios in Antarctic aerosols suggest that biomass burning aerosols only had regional, rather than local, sources. General acid/aldehyde ratios were lower at the coastal site than on the plateau. Levoglucosan and PCs determined during the oceanographic cruise were 37.6pgm−3 and 58.5pgm−3 respectively. Unlike levoglucosan, which can only be produced by biomass burning, PCs have both biomass burning and other sources. Our comparisons of these two types of compounds across a range of Antarctic marine, coastal, and plateau sites demonstrate that local marine sources dominate Antarctic PC concentrations.

Trajectory modeling of modern dust transport to the Southern Ocean and Antarctica

AbstractAerosol deposition over the Southern Ocean and Antarctica has the potential to alter marine productivity and thus ocean carbon uptake while also impacting radiative balance due to scattering and absorption from atmospheric particulates. Quantification of modern emission, transport, and deposition of terrestrial dust and other airborne material from Southern Hemisphere sources is challenging due to low emission levels and poor detection from remote sensing platforms. Here forward trajectory modeling is used to explore atmospheric transport, independent of deposition processes, from 1979 to 2013. Trajectories are initiated from known arid dust source areas in South America (Patagonia), Australia, and southern Africa, with detailed consideration of New Zealand as a potential source. Results suggest that Patagonian and New Zealand dust and other aerosol emissions share strong atmospheric transport during all seasons, allowing even potentially small New Zealand emissions to contribute significantly to Southern Ocean and Antarctic aerosol loading. We find that atmospheric transport controlling distribution of dust and other aerosols shows distinct spatial variability. New Zealand and Patagonia rapidly contribute a high proportion of trajectories to West Antarctica, while in interior East Antarctica, source contributions are limited and highly mixed. The sensitivity of existing deep ice core sites to modern atmospheric transport is discussed. Finally, interannual variability of poleward trajectory extension over the Pacific and Atlantic sectors of the Southern Ocean highlights the association of both tropical Pacific sea‐surface temperature and high‐latitude wind variability (e.g., the Southern Annular Mode) with transport of dust and other aerosols to the Southern Ocean and Antarctica.

Sugars in Antarctic aerosol

The processes and transformations occurring in the Antarctic aerosol during atmospheric transport were described using selected sugars as source tracers.Monosaccharides (arabinose, fructose, galactose, glucose, mannose, ribose, xylose), disaccharides (sucrose, lactose, maltose, lactulose), alcohol-sugars (erythritol, mannitol, ribitol, sorbitol, xylitol, maltitol, galactitol) and anhydrosugars (levoglucosan, mannosan and galactosan) were measured in the Antarctic aerosol collected during four different sampling campaigns.For quantification, a sensitive high-pressure anion exchange chromatography was coupled with a single quadrupole mass spectrometer. The method was validated, showing good accuracy and low method quantification limits.This study describes the first determination of sugars in the Antarctic aerosol. The total mean concentration of sugars in the aerosol collected at the “Mario Zucchelli” coastal station was 140 pg m−3; as for the aerosol collected over the Antarctic plateau during two consecutive sampling campaigns, the concentration amounted to 440 and 438 pg m−3.The study of particle-size distribution allowed us to identify the natural emission from spores or from sea-spray as the main sources of sugars in the coastal area. The enrichment of sugars in the fine fraction of the aerosol collected on the Antarctic plateau is due to the degradation of particles during long-range atmospheric transport. The composition of sugars in the coarse fraction was also investigated in the aerosol collected during the oceanographic cruise.

Determination of water-soluble, acid-extractable and inert fractions of Cd, Pb and Cu in Antarctic aerosol by square wave anodic stripping voltammetry after sequential extraction and microwave digestion

A two-step microwave (MW) digestion (ramps to 135°C and to 185°C) was set up for the subsequent voltammetric determination of the inert fraction of Cd, Pb and Cu in Antarctic aerosol (PM10), after a sequential extraction with water (soluble fraction) and dilute HCl (acid extractable fraction) of the filter samples. A digestion mixture of 5.0mL HNO3, 1.0mL H2O2, and 1.0mL HF was used. The amount of H2O2 was adjusted at a compromise value to avoid interferences from organic substances or from the reagent itself. Hydrogen fluoride was used at the maximum quantity suggested in the literature, since there were no interferences due to excess HF with the voltammetric measurement. Our procedure did not provide for a third digestion step with H3BO3, as generally required in order to eliminate excess HF when subsequent spectrochemical analyses are to be carried out. Thus the total digestion time was reduced from ~5h to ~1.5h. The ultrasensitive technique of square wave anodic stripping voltammetry (SWASV) was used and optimized by maximizing the signal-to-noise ratio (frequency 150Hz, amplitude 20mV). The limits of detection (e.g. for atmospheric concentration 0.1–0.3pgm−3 for Cd and 1–5pgm−3 for Pb and Cu) and the repeatabilities (Cd 21–26%, Pb 16–20%, Cu 11–14% as atmospheric concentration) compared favourably with literature reports. Significant aliquots of metals were present in all the three fractions determined and the inert fraction represented 20–74% for Cd, 10–63% for Pb, and 7–33% for Cu, against total contents of Cd 1–19pgm−3, Pb 17–36pgm−3, and Cu 177–429pgm−3. Possibly significant metal fractions could be associated to the crustal origin.