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A 10-year record of oxygen and hydrogen isotopic composition of precipitation is presented here: from 2008 to 2017, 1483 daily precipitation samples were collected year-round on a raised platform at Concordia Station, East Antarctica. Weather data were retrieved from the Italian Antarctic Meteo-Climatological Observatory automatic weather station (AWS), while ERA5 was used to estimate total precipitation. The δ–temperature relationships were moderately high for daily data (r2=0.63 and 0.64 for δ18O and δ2H, respectively) and stronger using monthly data (r2=0.82 for both δ18O and δ2H), with a slope of about 0.5 ‰ °C−1 for δ18O/TAWS (3.5 ‰ °C−1 for δ2H/TAWS), which remains consistent also using annual averages. The isotopic composition of precipitation is the input signal of the snow–ice system, and this dataset will be useful to improve the interpretation of paleoclimate records and promote a better understanding of the post-depositional processes affecting the isotopic signal in ice cores. This dataset represents a benchmark for the evaluation of isotope-enabled general circulation models. Here, the ECHAM6-wiso output was compared to experimental data, showing moderately good relationships for δ18O and δ2H but not for d-excess, nonetheless marking a substantial improvement from the previous release of the model.

The study of aerosols in high mountain regions is essential because particulate matter can play a role in altering the energy balance of high mountain regions, and aerosols can accelerate glacier melting in high mountain areas by darkening the ice surface, reducing its reflectivity (albedo). Studying aerosols in high mountain areas provides insights into long-range transport of pollutants, atmospheric dynamics, and climate change impacts. These regions can serve as valuable observatories for studying atmospheric processes. The main aim of this paper is to define the main sources of aerosols over an entire year of sampling at the Col Margherita Atmospheric Observatory (MRG; 46°22′0.059′′ N, 11°47′30.911′′ E; 2543 m a.s.l.), a high-altitude background site in the eastern Italian Alps. Here, we discuss the potential origins of more than 100 chemical markers (major ions, water-soluble organic compounds, trace elements, and rare earth elements) using different approaches. Some diagnostic ratios were applied, but source apportionment using positive matrix factorization (PMF) was used to define the main inputs of PM10 collected at this high-altitude site, resulting in the identification of four factors: (1) Saharan dust events, (2) long-range marine/anthropogenic influence, (3) biogenic sources, and (4) biomass-burning and anthropogenic emissions. It can be inferred that, despite the distant location of the Col Margherita site, both regional pollution and long-range anthropogenic pollution have discernible effects on this area.

Impurities in polar ice play a critical role in ice flow, deformation, and the integrity of the ice core record. Especially cloudy bands, visible layers with high impurity concentrations, are prominent features in ice from glacial periods. Their physical and chemical properties are poorly understood, highlighting the need to analyse them in more detail. We bridge the gap between decimetre and micrometre scales by combining the visual stratigraphy line scanner, fabric analyser, microstructure mapping, Raman spectroscopy, and laser ablation inductively coupled plasma mass spectrometry 2D impurity imaging. We classified approximately 1300 cloudy bands from glacial ice from the East Greenland Ice-core Project (EGRIP) ice core into seven different types. We determine the localisation and mineralogy of more than 1000 micro-inclusions at 13 depths. The majority of the minerals found are related to terrestrial dust, such as quartz, feldspar, mica, and hematite. We further found carbonaceous particles, dolomite, and gypsum in high abundance. Rutile, anatase, epidote, titanite, and grossular are infrequently observed. The 2D impurity imaging at 20 µm resolution revealed that cloudy bands are clearly distinguishable in the chemical data. Na, Mg, and Sr are mainly present at grain boundaries, whereas dust-related analytes, such as Al, Fe, and Ti, are located in the grain interior, forming clusters of insoluble impurities. We present novel vast micrometre-resolution insights into cloudy bands and describe the differences within and outside these bands. Combining the visual and chemical data results in new insights into the formation of different cloudy band types and could be the starting point for future in-depth studies on impurity signal integrity and internal deformation in deep polar ice cores.

Insoluble particles in ice cores record signatures of past climate parameters like vegetation dynamics, volcanic activity, and aridity. For some of them, the analytical detection relies on intensive bench microscopy investigation and requires dedicated sample preparation steps. Both are laborious, require in-depth knowledge, and often restrict sampling strategies. To help overcome these limitations, we present a framework based on flow imaging microscopy coupled to a deep neural network for autonomous image classification of ice core particles. We train the network to classify seven commonly found classes, namely mineral dust, felsic and mafic (basaltic) volcanic ash grains (tephra), three species of pollen (Corylus avellana, Quercus robur, Quercus suber), and contamination particles that may be introduced onto the ice core surface during core handling operations. The trained network achieves 96.8 % classification accuracy at test time. We present the system's potential and its limitations with respect to the detection of mineral dust, pollen grains, and tephra shards, using both controlled materials and real ice core samples. The methodology requires little sample material, is non-destructive, fully reproducible, and does not require any sample preparation procedures. The presented framework can bolster research in the field by cutting down processing time, supporting human-operated microscopy, and further unlocking the paleoclimate potential of ice core records by providing the opportunity to identify an array of ice core particles. Suggestions for an improved system to be deployed within a continuous flow analysis workflow are also presented.

Bromine enrichment (Brenr) has been proposed as an ice core proxy for past sea-ice reconstruction. Understanding the processes that influence bromine preservation in the ice is crucial to achieve a reliable interpretation of ice core signals and to potentially relate them to past sea-ice variability. Here, we present a 210 years bromine record that sheds light on the main processes controlling bromine preservation in the snow and ice at Dome C, East Antarctic plateau. Using observations alongside a modelling approach, we demonstrate that the bromine signal is preserved at Dome C and it is not affected by the strong variations in ultraviolet radiation reaching the Antarctic plateau due to the stratospheric ozone hole. Based on this, we investigate whether the Dome C Brenr record can be used as an effective tracer of past Antarctic sea ice. Due to the limited time window covered by satellite measurements and the low sea-ice variability observed during the last 30 years in East Antarctica, we cannot fully validate Brenr as an effective proxy for past sea-ice reconstructions at Dome C.

This work presents results from an original open-source low-cost sensor (LCS) system developed to measure tropospheric O3 in a remote high altitude alpine site. Our study was conducted at the Col Margherita Observatory (2543 m above sea level), in the Italian Eastern Alps. The sensor system mounts three commercial low-cost O3/NO2 sensors that have been calibrated before field deployment against a laboratory standard (Thermo Scientific; 49i-PS), calibrated against the standard reference photometer no. 15 calibration scale of the World Meteorological Organization (WMO). Intra- and intercomparison between the sensors and a reference instrument (Thermo Scientific; 49c) have been conducted for 7 months from May to December 2018. The sensors required an individual calibration, both in laboratory and in the field. The sensor's dependence on the environmental meteorological variables has been considered and discussed. We showed that it is possible to reduce the bias of one LCS by using the average coefficient values of another LCS working in tandem, suggesting a way forward for the development of remote field calibration techniques. We showed that it is possible reconstruct the environmental ozone concentration during the loss of reference instrument data in situations caused by power outages. The evaluation of the analytical performances of this sensing system provides a limit of detection (LOD) ppb (parts per billion), limit of quantification (LOQ) ppb, linear dynamic range (LDR) up to 250 ppb, intra-Pearson correlation coefficient (PCC) up to 0.96, inter-PCC >0.8, bias >3.5 ppb and ±8.5 at 95 % confidence. This first implementation of a LCS system in an alpine remote location demonstrated how to obtain valuable data from a low-cost instrument in a remote environment, opening new perspectives for the adoption of low-cost sensor networks in atmospheric sciences.

Black carbon (BC) is a significant forcing agent in the Arctic, but substantial uncertainty remains to quantify its climate effects due to the complexity of the different mechanisms involved, in particular related to processes in the snowpack after deposition. In this study, we provide detailed and unique information on the evolution and variability in BC content in the upper surface snow layer during the spring period in Svalbard (Ny-Ålesund). A total of two different snow-sampling strategies were adopted during spring 2014 (from 1 April to 24 June) and during a specific period in 2015 (28 April to 1 May), providing the refractory BC (rBC) mass concentration variability on a seasonal variability with a daily resolution (hereafter seasonal/daily) and daily variability with an hourly sampling resolution (hereafter daily/hourly) timescales. The present work aims to identify which atmospheric variables could interact with and modify the mass concentration of BC in the upper snowpack, which is the snow layer where BC particles affects the snow albedo. Atmospheric, meteorological and snow-related physico-chemical parameters were considered in a multiple linear regression model to identify the factors that could explain the variations in BC mass concentrations during the observation period. Precipitation events were the main drivers of the BC variability during the seasonal experiment; however, in the high-resolution sampling, a negative association has been found. Snow metamorphism and the activation of local sources (Ny-Ålesund was a coal mine settlement) during the snowmelt periods appeared to play a non-negligible role. The statistical analysis suggests that the BC content in the snow is not directly associated to the atmospheric BC load.

Biomass burning influences global atmospheric chemistry by releasing greenhouse gases and climate-forcing aerosols. There is controversy about the magnitude and timing of Holocene changes in biomass burning emissions from millennial to centennial timescales and, in particular, about the possible impact of ancient civilizations. Here we present a 5 kyr record of fire activity proxies levoglucosan, black carbon, and ammonium measured in the RECAP (Renland ice cap) ice core, drilled in coastal eastern Greenland, and therefore affected by processes occurring in the high North Atlantic region. Levoglucosan and ammonium fluxes are high from 5 to 4.5 kyr BP (thousand years before 2000 CE) followed by an abrupt decline, possibly due to monotonic decline in Northern Hemisphere summer insolation. Levoglucosan and black carbon show an abrupt decline at 1.1 kyr BP, suggesting a decline in the wildfire regime in Iceland due to the extensive land clearing caused by Viking colonizers. All fire proxies reach a minimum during the second half of the last century, after which levoglucosan and ammonium fluxes increase again, in particular over the last 200 years. We find that the fire regime reconstructed from RECAP fluxes seems mainly related to climatic changes; however over the last millennium human activities might have influenced wildfire frequency/occurrence substantially.

Due to its micrometer-scale resolution and inherently micro-destructive nature, laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) is particularly suited to exploring the thin and closely spaced layers in the oldest sections of polar ice cores. Recent adaptions to the LA-ICP-MS instrumentation mean we have faster washout times allowing state-of-the-art 2-D imaging of an ice core. This new method has great potential especially when applied to the localization of impurities on the ice sample, something that is crucial, to avoiding misinterpretation of the ultra-fine-resolution signals. Here we present the first results of the application of LA-ICP-MS elemental imaging to the analysis of selected glacial and interglacial samples from the Talos Dome and EPICA Dome C ice cores from central Antarctica. The localization of impurities from both marine and terrestrial sources is discussed, with special emphasis on observing a connection with the network of grain boundaries and differences between different climatic periods. Scale-dependent image analysis shows that the spatial significance of a single line profile along the main core axis increases systematically as the imprint of the grain boundaries weakens. It is demonstrated how instrumental settings can be adapted to suit the purpose of the analysis, i.e., by either employing LA-ICP-MS to study the interplay between impurities and the ice microstructure or to investigate the extremely thin climate proxy signals in deep polar ice.

Iron (Fe) is a key element in the Earth climate system, as it can enhance marine primary productivity in the high-nutrient low-chlorophyll (HNLC) regions where, despite a high concentration of major nutrients, chlorophyll production is low due to iron limitation. Eolian mineral dust represents one of the main Fe sources to the oceans; thus, quantifying its variability over the last glacial cycle is crucial to evaluate its role in strengthening the biological carbon pump. Polar ice cores, which preserve detailed climate records in their stratigraphy, provide a sensitive and continuous archive for reconstructing past eolian Fe fluxes. Here, we show the Northern Hemisphere Fe record retrieved from the NEEM ice core (Greenland), which offers a unique opportunity to reconstruct the past Fe fluxes in a portion of the Arctic over the last 108 kyr. Holocene Fe fluxes (0.042–11.7 ka, 0.5 mg m−2 yr−1) at the NEEM site were 4 times lower than the average recorded over the last glacial period (11.7–108 ka, 2.0 mg m−2 yr−1), whereas they were greater during the Last Glacial Maximum (LGM; 14.5–26.5 ka, 3.6 mg m−2 yr−1) and Marine Isotope Stage 4 (MIS 4; 60–71 ka, 5.8 mg m−2 yr−1). Comparing the NEEM Fe record with paleoceanographic records retrieved from the HNLC North Pacific, we found that the coldest periods, characterized by the highest Fe fluxes, were distinguished by low marine primary productivity in the subarctic Pacific Ocean, likely due to the greater sea ice extent and the absence of major nutrients upwelling. This supports the hypothesis that Fe fertilization during colder and dustier periods (i.e., LGM and MIS 4) was more effective in other regions, such as the midlatitude North Pacific, where a closer relationship between marine productivity and the NEEM Fe fluxes was observed.

The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. We set up the ERA-PLANET Strand 4 project “iCUPE – integrative and Comprehensive Understanding on Polar Environments” to provide novel insights and observational data on global grand challenges with an Arctic focus. We utilize an integrated approach combining in situ observations, satellite remote sensing Earth observations (EOs), and multi-scale modeling to synthesize data from comprehensive long-term measurements, intensive campaigns, and satellites to deliver data products, metrics, and indicators to stakeholders concerning the environmental status, availability, and extraction of natural resources in the polar areas. The iCUPE work consists of thematic state-of-the-art research and the provision of novel data in atmospheric pollution, local sources and transboundary transport, the characterization of arctic surfaces and their changes, an assessment of the concentrations and impacts of heavy metals and persistent organic pollutants and their cycling, the quantification of emissions from natural resource extraction, and the validation and optimization of satellite Earth observation (EO) data streams. In this paper we introduce the iCUPE project and summarize initial results arising out of the integration of comprehensive in situ observations, satellite remote sensing, and multi-scale modeling in the Arctic context.

Atmospheric iodine chemistry has a large influence on the oxidizing capacity and associated radiative impacts in the troposphere. However, information on the evolution of past atmospheric iodine levels is restricted to the industrial period while its long-term natural variability remains unknown. The current levels of iodine in the atmosphere are controlled by anthropogenic ozone deposition to the ocean surface. Here, using high-resolution geochemical measurements from coastal eastern Greenland ReCAP (REnland ice CAP project) ice core, we report the first record of atmospheric iodine variability in the North Atlantic during the Holocene (i.e., the last 11 700 years). Surprisingly, our results reveal that the highest iodine concentrations in the record were found during the Holocene Thermal Maximum (HTM; ∼ 11 500–5500 years before-present). These high iodine levels could be driven by marine primary productivity resulting in an Early Holocene “biological iodine explosion”. The high and stable iodine levels during this past warm period are a useful observational constraint on projections of future changes in Arctic atmospheric composition and climate resulting from global warming.

Although it has been demonstrated that the speed and magnitude of the recent Arctic sea ice decline is unprecedented for the past 1450 years, few records are available to provide a paleoclimate context for Arctic sea ice extent. Bromine enrichment in ice cores has been suggested to indicate the extent of newly formed sea ice areas. Despite the similarities among sea ice indicators and ice core bromine enrichment records, uncertainties still exist regarding the quantitative linkages between bromine reactive chemistry and the first-year sea ice surfaces. Here we present a 120 000-year record of bromine enrichment from the RECAP (REnland ice CAP) ice core, coastal east Greenland, and interpret it as a record of first-year sea ice. We compare it to existing sea ice records from marine cores and tentatively reconstruct past sea ice conditions in the North Atlantic as far north as the Fram Strait (50–85∘ N). Our interpretation implies that during the last deglaciation, the transition from multi-year to first-year sea ice started at ∼17.5 ka, synchronously with sea ice reductions observed in the eastern Nordic Seas and with the increase in North Atlantic ocean temperature. First-year sea ice reached its maximum at 12.4–11.8 ka during the Younger Dryas, after which open-water conditions started to dominate, consistent with sea ice records from the eastern Nordic Seas and the North Icelandic shelf. Our results show that over the last 120 000 years, multi-year sea ice extent was greatest during Marine Isotope Stage (MIS) 2 and possibly during MIS 4, with more extended first-year sea ice during MIS 3 and MIS 5. Sea ice extent during the Holocene (MIS 1) has been less than at any time in the last 120 000 years.

Sunlit snow is highly photochemically active and plays a key role in the exchange of gas phase species between the cryosphere and the atmosphere. Here, we investigate the behaviour of two selected species in surface snow: mercury (Hg) and iodine (I). Hg can deposit year-round and accumulate in the snowpack. However, photo-induced re-emission of gas phase Hg from the surface has been widely reported. Iodine is active in atmospheric new particle formation, especially in the marine boundary layer, and in the destruction of atmospheric ozone. It can also undergo photochemical re-emission. Although previous studies indicate possible post-depositional processes, little is known about the diurnal behaviour of these two species and their interaction in surface snow. The mechanisms are still poorly constrained, and no field experiments have been performed in different seasons to investigate the magnitude of re-emission processes Three sampling campaigns conducted at an hourly resolution for 3 d each were carried out near Ny-Ålesund (Svalbard) to study the behaviour of mercury and iodine in surface snow under different sunlight and environmental conditions (24 h darkness, 24 h sunlight and day–night cycles). Our results indicate a different behaviour of mercury and iodine in surface snow during the different campaigns. The day–night experiments demonstrate the existence of a diurnal cycle in surface snow for Hg and iodine, indicating that these species are indeed influenced by the daily solar radiation cycle. Differently, bromine did not show any diurnal cycle. The diurnal cycle also disappeared for Hg and iodine during the 24 h sunlight period and during 24 h darkness experiments supporting the idea of the occurrence (absence) of a continuous recycling or exchange at the snow–air interface. These results demonstrate that this surface snow recycling is seasonally dependent, through sunlight. They also highlight the non-negligible role that snowpack emissions have on ambient air concentrations and potentially on iodine-induced atmospheric nucleation processes.

The fire history of the Tibetan Plateau over centennial to millennial timescales is not well known. Recent ice core studies reconstruct fire history over the past few decades but do not extend through the Holocene. Lacustrine sedimentary cores, however, can provide continuous records of local environmental change on millennial scales during the Holocene through the accumulation and preservation of specific organic molecular biomarkers. To reconstruct Holocene fire events and vegetation changes occurring on the southeastern Tibetan Plateau and the surrounding areas, we used a multi-proxy approach, investigating multiple biomarkers preserved in core sediment samples retrieved from Paru Co, a small lake located in the Nyainqentanglha Mountains (29°47′45.6′′ N, 92°21′07.2′′ E; 4845 m a.s.l.). Biomarkers include n-alkanes as indicators of vegetation, polycyclic aromatic hydrocarbons (PAHs) as combustion proxies, fecal sterols and stanols (FeSts) as indicators of the presence of humans or grazing animals, and finally monosaccharide anhydrides (MAs) as specific markers of vegetation burning processes. Insolation changes and the associated influence on the Indian summer monsoon (ISM) affect the vegetation distribution and fire types recorded in Paru Co throughout the Holocene. The early Holocene (10.7–7.5 cal kyr BP) n-alkane ratios demonstrate oscillations between grass and conifer communities, resulting in respective smouldering fires represented by levoglucosan peaks, and high-temperature fires represented by high-molecular-weight PAHs. Forest cover increases with a strengthened ISM, where coincident high levoglucosan to mannosan (L ∕ M) ratios are consistent with conifer burning. The decrease in the ISM at 4.2 cal kyr BP corresponds with the expansion of regional civilizations, although the lack of human FeSts above the method detection limits excludes local anthropogenic influence on fire and vegetation changes. The late Holocene is characterized by a relatively shallow lake surrounded by grassland, where all biomarkers other than PAHs display only minor variations. The sum of PAHs steadily increases throughout the late Holocene, suggesting a net increase in local to regional combustion that is separate from vegetation and climate change.

We determined the specific biomass burning biomarker levoglucosan in an ice core from the TALos Dome Ice CorE drilling project (TALDICE) during the mid- to late Holocene (6000–750 BP). The levoglucosan record is characterized by a long-term increase with higher rates starting at ∼ 4000 BP and peaks between 2500 and 1500 BP. The anomalous increase in levoglucosan centered at ∼ 2000 BP is consistent with other Antarctic biomass burning records. Multiple atmospheric phenomena affect the coastal Antarctic Talos Dome drilling site, where the Southern Annular Mode (SAM) is the most prominent as the Southern Annular Mode Index (SAMA) correlates with stable isotopes in precipitation throughout the most recent 1000 years of the ice core. If this connection remains throughout the mid- to late Holocene, then our results demonstrate that changes in biomass burning, rather than changes in atmospheric transport, are the major influence on the TALDICE levoglucosan record. Comparisons with charcoal syntheses help evaluate fire sources, showing a greater contribution from southern South American fires than from Australian biomass burning. The levoglucosan peak centered at ∼ 2000 BP occurs during a cool period throughout the Southern Hemisphere, yet during a time of increased fire activity in both northern and southern Patagonia. This peak in biomass burning is influenced by increased vegetation in southern South America from a preceding humid period, in which the vegetation desiccated during the following cool, dry period. The Talos Dome ice core record from 6000 to ∼ 750 BP currently does not provide clear evidence that the fire record may be strongly affected by anthropogenic activities during the mid- to late Holocene, although we cannot exclude at least a partial influence.

Past climate changes in Greenland ice were accompanied by large aerosol concentration changes. Here, the authors show that by correcting for transport effects, reliable source changes for biogenic aerosol from North America, sea salt aerosol from the North Atlantic, and dust from East Asian deserts can be derived.

Halogen chemistry in the polar regions occurs through the release of halogen elements from different sources. Bromine is primarily emitted from sea salt aerosols and other saline condensed phases associated with sea ice surfaces, while iodine is affected by the release of organic compounds from algae colonies living within the sea ice environment. Measurements of halogen species in polar snow samples are limited to a few sites although there is some evidence that they are related to sea ice extent. We examine here total bromine, iodine and sodium concentrations in a series of 2 m cores collected during a traverse from Talos Dome (72°48' S, 159°06' E) to GV7 (70°41' S, 158°51' E) analyzed by inductively coupled plasma-sector field mass spectrometry (ICP-SFMS) at a resolution of 5 cm. We find a distinct seasonality of the bromine enrichment signal in most of the cores, with maxima during the austral spring. Iodine shows average concentrations of 0.04 ppb with little variability. No distinct seasonality is found for iodine and sodium. The transect reveals homogeneous air-to-snow fluxes for the three chemical species along the transect due to competing effects of air masses originating from the Ross Sea and the Southern Ocean.

The atmospheric deposition of mercury (Hg) occurs via several mechanisms, including dry and wet scavenging by precipitation events. In an effort to understand the atmospheric cycling and seasonal depositional characteristics of Hg, wet deposition samples were collected for approximately 5 years at 17 selected GMOS monitoring sites located in the Northern and Southern hemispheres in the framework of the Global Mercury Observation System (GMOS) project. Total mercury (THg) exhibited annual and seasonal patterns in Hg wet deposition samples. Interannual differences in total wet deposition are mostly linked with precipitation volume, with the greatest deposition flux occurring in the wettest years. This data set provides a new insight into baseline concentrations of THg concentrations in precipitation worldwide, particularly in regions such as the Southern Hemisphere and tropical areas where wet deposition as well as atmospheric Hg species were not investigated before, opening the way for future and additional simultaneous measurements across the GMOS network as well as new findings in future modeling studies.

In 2011 four ice cores were extracted from the summit of Alto dell'Ortles (3859 m), the highest glacier of South Tyrol in the Italian Alps. This drilling site is located only 37 km southwest from where the Tyrolean Iceman, ∼ 5.3 kyrs old, was discovered emerging from the ablating ice field of Tisenjoch (3210 m, near the Italian–Austrian border) in 1991. The excellent preservation of this mummy suggested that the Tyrolean Iceman was continuously embedded in prehistoric ice and that additional ancient ice was likely preserved elsewhere in South Tyrol. Dating of the ice cores from Alto dell'Ortles based on 210Pb, tritium, beta activity and 14C determinations, combined with an empirical model (COPRA), provides evidence for a chronologically ordered ice stratigraphy from the modern glacier surface down to the bottom ice layers with an age of ∼ 7 kyrs, which confirms the hypothesis. Our results indicate that the drilling site has continuously been glaciated on frozen bedrock since ∼ 7 kyrs BP. Absence of older ice on the highest glacier of South Tyrol is consistent with the removal of basal ice from bedrock during the Northern Hemisphere Climatic Optimum (6–9 kyrs BP), the warmest interval in the European Alps during the Holocene. Borehole inclinometric measurements of the current glacier flow combined with surface ground penetration radar (GPR) measurements indicate that, due to the sustained atmospheric warming since the 1980s, an acceleration of the glacier Alto dell'Ortles flow has just recently begun. Given the stratigraphic–chronological continuity of the Mt. Ortles cores over millennia, it can be argued that this behaviour has been unprecedented at this location since the Northern Hemisphere Climatic Optimum.

Long-term monitoring of data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (http://www.gmos.eu) and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere as well as in the lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010–2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both.

To investigate the impact of marine aerosols on global climate change it is important to study their chemical composition and size distribution. Amino acids are a component of the organic nitrogen in aerosols and particles containing amino acids have been found to be efficient ice nuclei. The main aim of this study was to investigate the L- and D-free amino acid composition as possible tracers of primary biological production in Antarctic aerosols from three different areas: two continental bases, Mario Zucchelli Station (MZS) on the coast of the Ross Sea, Concordia Station at Dome C on the Antarctic Plateau, and the Southern Ocean near the Antarctic continent. Studying the size distribution of amino acids in aerosols allowed us to characterize this component of the water-soluble organic carbon (WSOC) in marine aerosols near their source and after long-range transport. The presence of only free L-amino acids in our samples is indicative of the prevalence of phytoplanktonic material. Sampling at these three points allowed us to study the reactivity of these compounds during long-range transport. The mean total amino acid concentration detected at MZS was 11 pmol m−3, a higher percentage of amino acids were found in the fine fraction. The aerosol samples collected at Dome C had the lowest amino acid values (0.7 and 0.8 pmol m−3), and the coarse particles were found to have higher concentrations of amino acids compared to the coastal site. The amino acid composition in the aerosol collected at Dome C had also changed compared to the coastal site, suggesting that physical and chemical transformations had occurred during long range transport. During the sampling cruise on the R/V Italica on the Southern Ocean, high concentrations of amino acids were found in the total suspended particles, this we attribute to the presence of intact biological material (as microorganisms or plant material) in the sample.

Biomass burning is a major source of greenhouse gases and influences regional to global climate. Pre-industrial fire-history records from black carbon, charcoal and other proxies provide baseline estimates of biomass burning at local to global scales spanning millennia, and are thus useful to examine the role of fire in the carbon cycle and climate system. Here we use the specific biomarker levoglucosan together with black carbon and ammonium concentrations from the North Greenland Eemian (NEEM) ice cores (77.49° N, 51.2° W; 2480 m a.s.l) over the past 2000 years to infer changes in boreal fire activity. Increases in boreal fire activity over the periods 1000–1300 CE and decreases during 700–900 CE coincide with high-latitude NH temperature changes. Levoglucosan concentrations in the NEEM ice cores peak between 1500 and 1700 CE, and most levoglucosan spikes coincide with the most extensive central and northern Asian droughts of the past millennium. Many of these multi-annual droughts are caused by Asian monsoon failures, thus suggesting a connection between low- and high-latitude climate processes. North America is a primary source of biomass burning aerosols due to its relative proximity to the Greenland Ice Cap. During major fire events, however, isotopic analyses of dust, back trajectories and links with levoglucosan peaks and regional drought reconstructions suggest that Siberia is also an important source of pyrogenic aerosols to Greenland.

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 emission is attributed to biological communities in the open ocean and 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 and iodine concentrations and Br enrichment (relative to sea salt content) in polar ice do vary seasonally in Arctic snow and Antarctic ice. Although seasonal variability in halogen emission sources is recorded by satellite-based observations of tropospheric halogen concentrations, seasonal patterns observed in snowpack are likely also influenced by photolysis-driven processes. Peaks of bromine concentration and Br enrichment in Arctic snow and Antarctic ice occur in spring and summer, when sunlight is present. A secondary bromine peak, observed at the end of summer, is attributed to bromine deposition at the end of the polar day. Iodine concentrations are largest in winter Antarctic ice strata, contrary to contemporary observations of summer maxima in iodine emissions. These findings support previous observations of iodine peaks in winter snow strata attributed to the absence of sunlight-driven photolytic re-mobilisation of iodine from surface snow. Further investigation is required to confirm these proposed mechanisms explaining observations of halogens in polar snow and ice, and to evaluate the extent to which halogens may be applied as sea ice proxies.

In this study we report on new non-sea salt calcium (nssCa2+, mineral dust proxy) and sea salt sodium (ssNa+, sea ice proxy) records along the East Antarctic Talos Dome deep ice core in centennial resolution reaching back 150 thousand years (ka) before present. During glacial conditions nssCa2+ fluxes in Talos Dome are strongly related to temperature as has been observed before in other deep Antarctic ice core records, and has been associated with synchronous changes in the main source region (southern South America) during climate variations in the last glacial. However, during warmer climate conditions Talos Dome mineral dust input is clearly elevated compared to other records mainly due to the contribution of additional local dust sources in the Ross Sea area. Based on a simple transport model, we compare nssCa2+ fluxes of different East Antarctic ice cores. From this multi-site comparison we conclude that changes in transport efficiency or atmospheric lifetime of dust particles do have a minor effect compared to source strength changes on the large-scale concentration changes observed in Antarctic ice cores during climate variations of the past 150 ka. Our transport model applied on ice core data is further validated by climate model data. The availability of multiple East Antarctic nssCa2+ records also allows for a revision of a former estimate on the atmospheric CO2 sensitivity to reduced dust induced iron fertilisation in the Southern Ocean during the transition from the Last Glacial Maximum to the Holocene (T1). While a former estimate based on the EPICA Dome C (EDC) record only suggested 20 ppm, we find that reduced dust induced iron fertilisation in the Southern Ocean may be responsible for up to 40 ppm of the total atmospheric CO2 increase during T1. During the last interglacial, ssNa+ levels of EDC and EPICA Dronning Maud Land (EDML) are only half of the Holocene levels, in line with higher temperatures during that period, indicating much reduced sea ice extent in the Atlantic as well as the Indian Ocean sector of the Southern Ocean. In contrast, Holocene ssNa+ flux in Talos Dome is about the same as during the last interglacial, indicating that there was similar ice cover present in the Ross Sea area during MIS 5.5 as during the Holocene.

Sea ice is an important parameter in the climate system and its changes impact upon the polar albedo and atmospheric and oceanic circulation. Iodine (I) and bromine (Br) have been measured in a shallow firn core drilled at the summit of the Holtedahlfonna glacier (Northwest Spitsbergen, Svalbard). Changing I concentrations can be linked to the March–May maximum sea ice extension. Bromine enrichment, indexed to the Br / Na sea water mass ratio, appears to be influenced by changes in the seasonal sea ice area. I is emitted from marine biota and so the retreat of March–May sea ice coincides with enlargement of the open-ocean surface which enhances marine primary production and consequent I emission. The observed Br enrichment could be explained by greater Br emissions during the Br explosions that have been observed to occur mainly above first year sea ice during the early springtime. In this work we present the first comparison between halogens in surface snow and Arctic sea ice extension. Although further investigation is required to characterize potential depositional and post-depositional processes, these preliminary findings suggest that I and Br can be linked to variability in the spring maximum sea ice extension and seasonal sea ice surface area.

Sea ice is an integral part of the earth's climate system because it affects planetary albedo, sea-surface salinity, and the atmosphere–ocean exchange of reactive gases and aerosols. Bromine and iodine chemistry is active at polar sea ice margins with the occurrence of bromine explosions and the biological production of organoiodine from sea ice algae. Satellite measurements demonstrate that concentrations of bromine oxide (BrO) and iodine oxide (IO) decrease over sea ice toward the Antarctic interior. Here we present speciation measurements of bromine and iodine in the TALDICE (TALos Dome Ice CorE) ice core (159°11' E, 72°49' S; 2315 m a.s.l.) spanning the last 215 ky. The Talos Dome ice core is located 250 km inland and is sensitive to marine air masses intruding onto the Antarctic Plateau. Talos Dome bromide (Br−) is positively correlated with temperature and negatively correlated with sodium (Na). Based on the Br−/Na seawater ratio, bromide is depleted in the ice during glacial periods and enriched during interglacial periods. Total iodine, consisting of iodide (I−) and iodate (IO3−), peaks during glacials with lower values during interglacial periods. Although IO3− is considered the most stable iodine species in the atmosphere it was only observed in the TALDICE record during glacial maxima. Sea ice dynamics are arguably the primary driver of halogen fluxes over glacial–interglacial timescales, by altering the distance between the sea ice edge and the Antarctic plateau and by altering the surface area of sea ice available to algal colonization. Based on our results we propose the use of both halogens for examining Antarctic variability of past sea ice extent.

Volcanic tephra are independent age horizons and can synchronize strata of various paleoclimate records including ice and sediment cores. The Holocene section of the Greenland Ice Core Project (GRIP) ice core is dated by multi-parameter annual layer counting, and contains peaks in acidity, SO42− and microparticle concentrations at a depth of 429.1 to 429.3 m, which have not previously been definitively ascribed to a volcanic eruption. Here, we identify tephra particles and determine that volcanic shards extracted from a depth of 429.3 m in the GRIP ice core are likely due to the 79 AD Vesuvius eruption. The chemical composition of the tephra particles is consistent with the K-phonolitic composition of the Vesuvius juvenile ejecta and differs from the chemical composition of other major eruptions (≥ VEI 4) between 50–100 AD.

Atmospheric fluxes of iron (Fe) over the past 200 kyr are reported for the coastal Antarctic Talos Dome ice core, based on acid leachable Fe concentrations. Fluxes of Fe to Talos Dome were consistently greater than those at Dome C, with the greatest difference observed during interglacial climates. We observe different Fe flux trends at Dome C and Talos Dome during the deglaciation and early Holocene, attributed to a combination of deglacial activation of dust sources local to Talos Dome and the reorganisation of atmospheric transport pathways with the retreat of the Ross Sea ice shelf. This supports similar findings based on dust particle sizes and fluxes and Rare Earth Element fluxes. We show that Ca and Fe should not be used as quantitative proxies for mineral dust, as they all demonstrate different deglacial trends at Talos Dome and Dome C. Considering that a 20 ppmv decrease in atmospheric CO2 at the coldest part of the last glacial maximum occurs contemporaneously with the period of greatest Fe and dust flux to Antarctica, we confirm that the maximum contribution of aeolian dust deposition to Southern Ocean sequestration of atmospheric CO2 is approximately 20 ppmv.

Amino acids are significant components of atmospheric aerosols, affecting organic nitrogen input to marine ecosystems, atmospheric radiation balance, and the global water cycle. The wide range of amino acid reactivities suggest that amino acids may serve as markers of atmospheric transport and deposition of particles. Despite this potential, few measurements have been conducted in remote areas to assess amino acid concentrations and potential sources. Polar regions offer a unique opportunity to investigate atmospheric processes and to conduct source apportionment studies of such compounds. In order to better understand the importance of amino acid compounds in the global atmosphere, we determined free amino acids (FAAs) in seventeen size-segregated aerosol samples collected in a polar station in the Svalbard Islands from 19 April until 14 September 2010. We used an HPLC coupled with a tandem mass spectrometer (ESI-MS/MS) to analyze 20 amino acids and quantify compounds at fmol m−3 levels. Mean total FAA concentration was 1070 fmol m−3 where serine and glycine were the most abundant compounds in almost all samples and accounted for 45–60% of the total amino acid relative abundance. The other eighteen compounds had average concentrations between 0.3 and 98 fmol m−3. The higher amino acid concentrations were present in the ultrafine aerosol fraction (< 0.49 μm) and accounted for the majority of the total amino acid content. Local marine sources dominate the boreal summer amino acid concentrations, with the exception of the regional input from Icelandic volcanic emissions.

We present a Rare Earth Elements (REE) record determined on the EPICA ice core drilled at Dronning Maud Land (EDML) in the Atlantic sector of the East Antarctic Plateau. The record covers the transition from the last glacial stage (LGS) to the early Holocene (26 600–7500 yr BP) at decadal to centennial resolution. Additionally, samples from potential source areas (PSAs) for Antarctic dust were analyzed for their REE characteristics. The dust provenance is discussed by comparing the REE fingerprints in the ice core and the PSA samples. We find a shift in variability in REE composition at ~15 000 yr BP in the ice core samples. Before 15 000 yr BP, the dust composition is very uniform and its provenance was most certainly dominated by a South American source. After 15 000 yr BP, multiple sources such as Australia and New Zealand become relatively more important, although South America remains the major dust source. A similar change in the dust characteristics was observed in the EPICA Dome C ice core at around ~15 000 yr BP, accompanied by a shift in the REE composition, thus suggesting a change of atmospheric circulation in the Southern Hemisphere.

In June 2009, we conducted the first extensive glaciological survey of Alto dell'Ortles, the uppermost glacier of Mt. Ortles (3905 m a.s.l.), the highest summit of the Eastern European Alps. This section of the Alps is located in a rain shadow and is characterized by the lowest precipitation rate in the entire Alpine arc. Mt. Ortles offers a unique opportunity to test deposition mechanisms of chemical species that until now were studied only in the climatically-different western sector. We analyzed snow samples collected on Alto dell'Ortles from a 4.5 m snow-pit at 3830 m a.s.l., and we determined a large suite of trace elements and ionic compounds that comprise the atmospheric deposition over the past two years. Trace element concentrations measured in snow samples are extremely low with mean concentrations at pg g−1 levels. Only Al and Fe present median values of 1.8 and 3.3 ng g−1, with maximum concentrations of 21 and 25 ng g−1. The median crustal enrichment factor (EFc) values for Be, Rb, Sr, Ba, U, Li, Al, Ca, Cr, Mn, Fe, Co, Ga and V are lower than 10 suggesting that these elements originated mainly from soil and mineral aerosol. EFc higher than 100 are reported for Zn (118), Ag (135), Bi (185), Sb (401) and Cd (514), demonstrating the predominance of non-crustal depositions and suggesting an anthropogenic origin. Our data show that the physical stratigraphy and the chemical signals of several species were well preserved in the uppermost snow of the Alto dell'Ortles glacier. A clear seasonality emerges from the data as the summer snow is more affected by anthropogenic and marine contributions while the winter aerosol flux is dominated by crustal sources. For trace elements, the largest mean EFc seasonal variations are displayed by V (with a factor of 3.8), Sb (3.3), Cu (3.3), Pb (2.9), Bi (2.8), Cd (2.1), Zn (1.9), Ni (1.8), Ag (1.8), As (1.7) and Co (1.6). When trace species ratios in local and Po Valley emissions are compared with those in Alto dell'Ortles snow, the deposition on Mt. Ortles is clearly linked with Po Valley summer emissions. Despite climatic differences between the Eastern and Western Alps, trace element ratios from Alto dell'Ortles are comparable with those obtained from high-altitude glaciers in the Western Alps, suggesting similar sources and transport processes at seasonal time scales in these two distinct areas. In particular, the large changes in trace element concentrations both in the Eastern and Western Alps appear to be more related to the regional vertical structure of the troposphere rather than the synoptic weather patterns.

Gaseous Elemental Mercury (Hg° or GEM) was investigated at Summit Station, Greenland, in the interstitial air extracted from the perennial snowpack (firn) at depths ranging from the surface to 30 m, during summer 2005 and spring 2006. Photolytic production and destruction of Hg° were observed close to the snow surface during summer 2005 and spring 2006, and we observed dark oxidation of GEM up to 270 cm depth in June 2006. Photochemical transformation of gaseous elemental mercury resulted in diel variations in the concentrations of this gas in the near-surface interstitial air, but destruction of Hg° was predominant in June, and production was the main process in July. This seasonal evolution of the chemical mechanisms involving gaseous elemental mercury produces a signal that propagates downward through the firn air, but is unobservably small below 15 m in depth. As a consequence, multi-annual averaged records of GEM concentration should be well preserved in deep firn air at depths below 15 m, and available for the reconstruction of the past atmospheric history of GEM over the last decades.