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The mid-Pliocene is a valuable time interval for investigating equilibrium climate at current atmospheric CO2 concentrations because atmospheric CO2 concentrations are thought to have been comparable to the current day and yet the climate and distribution of ecosystems were quite different. One intriguing, but not fully understood, feature of the early to mid-Pliocene climate is the amplified Arctic temperature response and its impact on Arctic ecosystems. Only the most recent models appear to correctly estimate the degree of warming in the Pliocene Arctic and validation of the currently proposed feedbacks is limited by scarce terrestrial records of climate and environment. Here we reconstruct the summer temperature and fire regime from a subfossil fen-peat deposit on west–central Ellesmere Island, Canada, that has been chronologically constrained using cosmogenic nuclide burial dating to 3.9+1.5/-0.5 Ma. The estimate for average mean summer temperature is 15.4±0.8 ∘C using specific bacterial membrane lipids, i.e., branched glycerol dialkyl glycerol tetraethers. This is above the proposed threshold that predicts a substantial increase in wildfire in the modern high latitudes. Macro-charcoal was present in all samples from this Pliocene section with notably higher charcoal concentration in the upper part of the sequence. This change in charcoal was synchronous with a change in vegetation that included an increase in abundance of fire-promoting Pinus and Picea. Paleo-vegetation reconstructions are consistent with warm summer temperatures, relatively low summer precipitation and an incidence of fire comparable to fire-adapted boreal forests of North America and central Siberia. To our knowledge, this site provides the northernmost evidence of fire during the Pliocene. It suggests that ecosystem productivity was greater than in the present day, providing fuel for wildfires, and that the climate was conducive to the ignition of fire during this period. The results reveal that interactions between paleo-vegetation and paleoclimate were mediated by fire in the High Arctic during the Pliocene, even though CO2 concentrations were similar to modern values.

Enhanced release of alkalinity from the seafloor, principally driven by anaerobic degradation of organic matter under low-oxygen conditions and associated secondary redox reactions, can increase the carbon dioxide (CO2) buffering capacity of seawater and therefore oceanic CO2 uptake. The Baltic Sea has undergone severe changes in oxygenation state and total alkalinity (TA) over the past decades. The link between these concurrent changes has not yet been investigated in detail. A recent system-wide TA budget constructed for the past 50 years using BALTSEM, a coupled physical–biogeochemical model for the whole Baltic Sea area revealed an unknown TA source. Here we use BALTSEM in combination with observational data and one-dimensional reactive-transport modeling of sedimentary processes in the Fårö Deep, a deep Baltic Sea basin, to test whether sulfate (SO42-) reduction coupled to iron (Fe) sulfide burial can explain the missing TA source in the Baltic Proper. We calculated that this burial can account for up to 26 % of the missing source in this basin, with the remaining TA possibly originating from unknown river inputs or submarine groundwater discharge. We also show that temporal variability in the input of Fe to the sediments since the 1970s drives changes in sulfur (S) burial in the Fårö Deep, suggesting that Fe availability is the ultimate limiting factor for TA generation under anoxic conditions. The implementation of projected climate change and two nutrient load scenarios for the 21st century in BALTSEM shows that reducing nutrient loads will improve deep water oxygen conditions, but at the expense of lower surface water TA concentrations, CO2 buffering capacities and faster acidification. When these changes additionally lead to a decrease in Fe inputs to the sediment of the deep basins, anaerobic TA generation will be reduced even further, thus exacerbating acidification. This work highlights that Fe dynamics plays a key role in the release of TA from sediments where Fe sulfide formation is limited by Fe availability, as exemplified by the Baltic Sea. Moreover, it demonstrates that burial of Fe sulfides should be included in TA budgets of low-oxygen basins.

During the last decade, several limb sounding satellites have measured the global sodium (Na) number densities in the mesosphere and lower thermosphere (MLT). Datasets are now available from Global Ozone Monitoring by Occultation of Stars (GOMOS), the SCanning Imaging Absorption spectroMeter for Atmospheric CHartography (SCIAMACHY) (both on Envisat) and the Optical Spectrograph and InfraRed Imager System (OSIRIS) (on Odin). Furthermore, global model simulations of the Na layer in the MLT simulated by the Whole Atmosphere Community Climate Model, including the Na species (WACCM-Na), are available. In this paper, we compare these global datasets.The observed and simulated monthly averages of Na vertical column densities agree reasonably well with each other. They show a clear seasonal cycle with a summer minimum most pronounced at the poles. They also show signs of a semi-annual oscillation in the equatorial region. The vertical column densities vary from 0. 5 × 109 to 7 × 109 cm−2 near the poles and from 3 × 109 to 4 × 109 cm−2 at the Equator. The phase of the seasonal cycle and semi-annual oscillation shows small differences between the Na amounts retrieved from different instruments. The full width at half maximum of the profiles is 10 to 16 km for most latitudes, but significantly smaller in the polar summer. The centroid altitudes of the measured sodium profiles range from 89 to 95 km, whereas the model shows on average 2 to 4 km lower centroid altitudes. This may be explained by the mesopause being 3 km lower in the WACCM simulations than in measurements. Despite this global 2–4 km shift, the model captures well the latitudinal and temporal variations. The variation of the WACCM dataset during the year at different latitudes is similar to the one of the measurements. Furthermore, the differences between the measured profiles with different instruments and therefore different local times (LTs) are also present in the model-simulated profiles. This capturing of latitudinal and temporal variations is also found for the vertical column densities and profile widths.

Improving measurements of water vapour in the upper troposphere and lower stratosphere (UTLS) is a priority for the atmospheric science community. In this work, UTLS water vapour profiles derived from Atmospheric Chemistry Experiment (ACE) satellite measurements are assessed with coincident ground-based measurements taken at a high Arctic observatory at Eureka, Nunavut, Canada. Additional comparisons to satellite measurements taken by the Atmospheric Infrared Sounder (AIRS), Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), Microwave Limb Sounder (MLS), Scanning Imaging Absorption Spectrometer for Atmospheric CHartography (SCIAMACHY), and Tropospheric Emission Spectrometer (TES) are included to put the ACE Fourier transform spectrometer (ACE-FTS) and ACE Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) results in context. Measurements of water vapour profiles at Eureka are made using a Bruker 125HR solar absorption Fourier transform infrared spectrometer at the Polar Environment Atmospheric Research Laboratory (PEARL) and radiosondes launched from the Eureka Weather Station. Radiosonde measurements used in this study were processed with software developed by the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) to account for known biases and calculate uncertainties in a well-documented and consistent manner. ACE-FTS measurements were within 11 ppmv (parts per million by volume; 13 %) of 125HR measurements between 6 and 14 km. Between 8 and 14 km ACE-FTS profiles showed a small wet bias of approximately 8 % relative to the 125HR. ACE-FTS water vapour profiles had mean differences of 13 ppmv (32 %) or better when compared to coincident radiosonde profiles at altitudes between 6 and 14 km; mean differences were within 6 ppmv (12 %) between 7 and 11 km. ACE-MAESTRO profiles showed a small dry bias relative to the 125HR of approximately 7 % between 6 and 9 km and 10 % between 10 and 14 km. ACE-MAESTRO profiles agreed within 30 ppmv (36 %) of the radiosondes between 7 and 14 km. ACE-FTS and ACE-MAESTRO comparison results show closer agreement with the radiosondes and PEARL 125HR overall than other satellite datasets – except for AIRS. Close agreement was observed between AIRS and the 125HR and radiosonde measurements, with mean differences within 5 % and correlation coefficients above 0.83 in the troposphere between 1 and 7 km. Comparisons to MLS at altitudes around 10 km showed a dry bias, e.g. mean differences between MLS and radiosondes were −25.6 %. SCIAMACHY comparisons were very limited due to minimal overlap between the vertical extent of the measurements. TES had no temporal overlap with the radiosonde dataset used in this study. Comparisons between TES and the 125HR showed a wet bias of approximately 25 % in the UTLS and mean differences within 14 % below 5 km.

We present the first search for galaxy counterparts of intervening high-z (2 < z < 3.6) sub-damped Lyα absorbers (sub-DLAs) and DLAs towards gamma-ray bursts (GRBs). Our final sample comprises five intervening sub-DLAs and DLAs in four GRB fields. To identify candidate galaxy counterparts of the absorbers we used deep optical- and near-infrared imaging, and low-, mid- and high-resolution spectroscopy acquired with 6-m to 10-m class telescopes, the Hubble and the Spitzer Space Telescopes. Furthermore, we used the spectroscopic information and spectral-energy-distribution fitting techniques to study them in detail. Our main result is the detection and spectroscopic confirmation of the galaxy counterpart of the intervening DLA at z = 3.096 in the field of GRB 070721B (zGRB = 3.6298) as proposed by other authors. We also identify good candidates for the galaxy counterparts of the two strong Mg ii absorbers at z = 0.6915 and 1.4288 towards GRB 050820A (zGRB = 2.615). The properties of the detected DLA galaxy are typical for Lyman-break galaxies (LBGs) at similar redshifts; a young, highly star-forming galaxy that shows evidence for a galactic outflow. This supports thehypothesis that a DLA can be the gaseous halo of an LBG. In addition, we report a redshift coincidence of different objects associated with metal lines in the same field, separated by 130–161 kpc. The high detection rate of three correlated structures on a length scale as short as ~150 kpc in two pairs of lines of sight is intriguing. The absorbers in each of these are most likely not part of the same gravitationally bound structure. They more likely represent groups of galaxies.

Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased diameter and hygroscopicity, facilitating droplet activation. This affects BC radiative forcing through aerosol–cloud interactions (ACIs) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015–2016 in a residential area of Zurich which aimed at establishing relations between the size and mixing state of BC particles and their activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single-particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that in the morning hours of weekdays, the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles, which do not act as CCN within the CCNC. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 % and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 % to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have very similar activation behaviour to BC-free particles. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core–shell particle geometry constrained with single-particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size- and mixing-state-resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.

Liquid clouds form by condensation of water vapour on aerosol particles in the atmosphere. Even black carbon (BC) particles, which are known to be slightly hygroscopic, have been shown to readily form cloud droplets once they have acquired water-soluble coatings by atmospheric aging processes. Accurately simulating the life cycle of BC in the atmosphere, which strongly depends on the wet removal following droplet activation, has recently been identified as a key element for accurate prediction of the climate forcing of BC. Here, to assess BC activation in detail, we performed in situ measurements during cloud events at the Jungfraujoch high-altitude station in Switzerland in summer 2010 and 2016. Cloud droplet residual and interstitial (unactivated) particles as well as the total aerosol were selectively sampled using different inlets, followed by their physical characterization using scanning mobility particle sizers (SMPSs), multi-angle absorption photometers (MAAPs) and a single-particle soot photometer (SP2). By calculating cloud droplet activated fractions with these measurements, we determined the roles of various parameters on the droplet activation of BC. The half-rise threshold diameter for droplet activation (Dhalfcloud), i.e. the size above which aerosol particles formed cloud droplets, was inferred from the aerosol size distributions measured behind the different inlets. The effective peak supersaturation (SSpeak) of a cloud was derived from Dhalfcloud by comparing it to the supersaturation dependence of the threshold diameter for cloud condensation nuclei (CCN) activation measured by a CCN counter (CCNC). In this way, we showed that the mass-based scavenged fraction of BC strongly correlates with that of the entire aerosol population because SSpeak modulates the critical size for activation of either particle type. A total of 50 % of the BC-containing particles with a BC mass equivalent core diameter of 90 nm was activated in clouds with SSpeak≈0.21 %, increasing up to ∼80 % activated fraction at SSpeak≈0.50 %. On a single-particle basis, BC activation at a certain SSpeak is controlled by the BC core size and internally mixed coating, which increases overall particle size and hygroscopicity. However, the resulting effect on the population averaged and on the size-integrated BC scavenged fraction by mass is small for two reasons: first, acquisition of coatings only matters for small cores in clouds with low SSpeak; and, second, variations in BC core size distribution and mean coating thickness are limited in the lower free troposphere in summer. Finally, we tested the ability of a simplified theoretical model, which combines the κ-Köhler theory with the Zdanovskii–Stokes–Robinson (ZSR) mixing rule under the assumptions of spherical core–shell particle geometry and surface tension of pure water, to predict the droplet activation behaviour of BC-containing particles in real clouds. Predictions of BC activation constrained with SSpeak and measured BC-containing particle size and mixing state were compared with direct cloud observations. These predictions achieved closure with the measurements for the particle size ranges accessible to our instrumentation, that is, BC core diameters and total particle diameters of approximately 50 and 180 nm, respectively. This clearly indicates that such simplified theoretical models provide a sufficient description of BC activation in clouds, as previously shown for activation occurring in fog at lower supersaturation and also shown in laboratory experiments under controlled conditions. This further justifies application of such simplified theoretical approaches in regional and global simulations of BC activation in clouds, which include aerosol modules that explicitly simulate BC-containing particle size and mixing state.

Diatoms account for a large proportion of primary productivity in Antarctic coastal and continental shelf zones. Diatoms, which have been used for a long time to infer past sea surface conditions in the Southern Ocean, have recently been associated with diatom-specific biomarkers (highly branched isoprenoids, HBI). Our study is one of the few sedimentary research projects on diatom ecology and associated biomarkers in the Antarctic seasonal sea ice zone. To date, the Adélie Land region has received little attention, despite evidence for the presence of high accumulation of laminated sediment, allowing for finer climate reconstructions and sedimentary process studies. Here we provide a sequence of seasonally to annually laminated diatomaceous sediment from a 72.5 cm interface core retrieved on the continental shelf off Adélie Land, covering the 1970–2010 CE period. Investigations through statistical analyses of diatom communities, diatom-specific biomarkers and major element abundances document the relationships between these proxies at an unprecedented resolution. Additionally, comparison of sedimentary records to meteorological data monitored by automatic weather station and satellite derived sea ice concentrations help to refine the relationships between our proxies and environmental conditions over the last decades. Our results suggest a coupled interaction of the atmospheric and sea surface variability on sea ice seasonality, which acts as the proximal forcing of siliceous productivity at that scale.

Within the NDACC (Network for the Detection of Atmospheric Composition Change), more than 20 FTIR (Fourier-transform infrared) spectrometers, spread worldwide, provide long-term data records of many atmospheric trace gases. We present a method that uses measured and modelled XCO2 for assessing the consistency of these NDACC data records. Our XCO2 retrieval setup is kept simple so that it can easily be adopted for any NDACC/FTIR-like measurement made since the late 1950s. By a comparison to coincident TCCON (Total Carbon Column Observing Network) measurements, we empirically demonstrate the useful quality of this suggested NDACC XCO2 product (empirically obtained scatter between TCCON and NDACC is about 4‰ for daily mean as well as monthly mean comparisons, and the bias is 25‰). Our XCO2 model is a simple regression model fitted to CarbonTracker results and the Mauna Loa CO2 in situ records. A comparison to TCCON data suggests an uncertainty of the model for monthly mean data of below 3‰. We apply the method to the NDACC/FTIR spectra that are used within the project MUSICA (multi-platform remote sensing of isotopologues for investigating the cycle of atmospheric water) and demonstrate that there is a good consistency for these globally representative set of spectra measured since 1996: the scatter between the modelled and measured XCO2 on a yearly time scale is only 3‰.

Thermokarst lakes and ponds are major elements of permafrost landscapes, occupying up to 40% of the land area in some Arctic regions. Shallow lakes freeze to the bed, thus preventing permafrost thaw underneath them and limiting the length of the period with greenhouse gas production in the unfrozen lake sediments. Radar remote sensing permits to distinguish lakes with bedfast ice due to the difference in backscatter intensities from bedfast and floating ice. This study investigates the potential of a unique time series of three-year repeat-pass TerraSAR-X (TSX) imagery with high temporal (11 days) and spatial (10 m) resolution for monitoring bedfast ice as well as ice phenology of lakes in the zone of continuous permafrost in the Lena River Delta, Siberia. TSX backscatter intensity is shown to be an excellent tool for monitoring floating versus bedfast lake ice as well as ice phenology. TSX-derived timing of ice grounding and the ice growth model CLIMo are used to retrieve the ice thicknesses of the bedfast ice at points where in situ ice thickness measurements were available. Comparison shows good agreement in the year of field measurements. Additionally, for the first time, an 11-day sequential interferometric coherence time series is analyzed as a supplementary approach for the bedfast ice monitoring. The coherence time series detects most of the ice grounding as well as spring snow/ice melt onset. Overall, the results show the great value of TSX time series for monitoring Arctic lake ice and provide a basis for various applications: for instance, derivation of shallow lakes bathymetry, evaluation of winter water resources and locating fish winter habitat as well as estimation of taliks extent in permafrost.