ALBERT

Description: Deposition to the sea surface is a major atmospheric loss pathway for many important trace gases, such as sulfur dioxide (SO2). The air–sea transfer of SO2 is controlled entirely on the atmospheric side of the air–sea interface due to high effective solubility and other physical–chemical properties. There have been few direct field measurements of such fluxes due to the challenges associated with making fast-response measurements of highly soluble trace gases at very low ambient levels. In this study, we report direct eddy covariance air–sea flux measurements of SO2, sensible heat, water vapor, and momentum. The measurements were made over shallow coastal waters from the Scripps Pier, La Jolla, CA, using negative ion chemical ionization mass spectrometry as the SO2 sensor. The observed transfer velocities for SO2, sensible heat, water vapor, and momentum and their wind speed dependences indicate that SO2 fluxes can be reliably measured using this approach. As expected, the transfer velocities for SO2, sensible heat, and water vapor are lower than that for momentum, demonstrating the contribution of molecular diffusion to the overall air-side resistance to gas transfer. Furthermore, transfer velocities of SO2 were lower than those of sensible heat and water vapor when observed simultaneously. This result is attributed to diffusive resistance in the interfacial layer of the air–sea interface.

Description: Low concentrations of ice-nucleating particles (INPs) are thought to be important for the properties of mixed-phase clouds, but their detection is challenging. Hence, there is a need for instruments where INP concentrations of less than 0.01 L−1 can be routinely and efficiently determined. The use of larger volumes of suspension in drop assays increases the sensitivity of an experiment to rarer INPs or rarer active sites due to the increase in aerosol or surface area of particulates per droplet. Here we describe and characterise the InfraRed-Nucleation by Immersed Particles Instrument (IR-NIPI), a new immersion freezing assay that makes use of IR emissions to determine the freezing temperature of individual 50 µL droplets each contained in a well of a 96-well plate. Using an IR camera allows the temperature of individual aliquots to be monitored. Freezing temperatures are determined by detecting the sharp rise in well temperature associated with the release of heat caused by freezing. In this paper we first present the calibration of the IR temperature measurement, which makes use of the fact that following ice nucleation aliquots of water warm to the ice–liquid equilibrium temperature (i.e. 0 ∘C when water activity is ∼1), which provides a point of calibration for each individual well in each experiment. We then tested the temperature calibration using ∼100 µm chips of K-feldspar, by immersing these chips in 1 µL droplets on an established cold stage (µL-NIPI) as well as in 50 µL droplets on IR-NIPI; the results were consistent with one another, indicating no bias in the reported freezing temperature. In addition we present measurements of the efficiency of the mineral dust NX-illite and a sample of atmospheric aerosol collected on a filter in the city of Leeds. NX-illite results are consistent with literature data, and the atmospheric INP concentrations were in good agreement with the results from the µL-NIPI instrument. This demonstrates the utility of this approach, which offers a relatively high throughput of sample analysis and access to low INP concentrations.

Description: The European Slope Current provides a shelf-edge conduit for Atlantic Water, a substantial fraction of which is destined for the northern North Sea, with implications for regional hydrography and ecosystems. Drifters drogued at 50 m in the European Slope Current at the Hebridean shelf break follow a wide range of pathways, indicating highly variable Atlantic inflow to the North Sea. Slope Current pathways, timescales and transports over 1988–2007 are further quantified in an eddy-resolving ocean model hindcast. Particle trajectories calculated with model currents indicate that Slope Current water is largely recruited from the eastern subpolar North Atlantic. Observations of absolute dynamic topography and climatological density support theoretical expectations that Slope Current transport is to first order associated with meridional density gradients in the eastern subpolar gyre, which support a geostrophic inflow towards the slope. In the model hindcast, Slope Current transport variability is dominated by abrupt 25–50 % reductions of these density gradients over 1996–1998. Concurrent changes in wind forcing, expressed in terms of density gradients, act in the same sense to reduce Slope Current transport. This indicates that coordinated regional changes of buoyancy and wind forcing acted together to reduce Slope Current transport during the 1990s. Particle trajectories further show that 10–40 % of Slope Current water is destined for the northern North Sea within 6 months of passing to the west of Scotland, with a general decline in this percentage over 1988–2007. Salinities in the Slope Current correspondingly decreased, evidenced in ocean analysis data. Further to the north, in the Atlantic Water conveyed by the Slope Current through the Faroe–Shetland Channel (FSC), salinity is observed to increase over this period while declining in the hindcast. The observed trend may have broadly compensated for a decline in the Atlantic inflow, limiting salinity changes in the northern North Sea during this period. Proxies for both Slope Current transport and Atlantic inflow to the North Sea are sought in sea level height differences across the FSC and between Shetland and the Scottish mainland (Wick). Variability of Slope Current transport on a wide range of timescales, from seasonal to multi-decadal, is implicit in sea level differences between Lerwick (Shetland) and Tórshavn (Faroes), in both tide gauge records from 1957 and a longer model hindcast spanning 1958–2012. Wick–Lerwick sea level differences in tide gauge records from 1965 indicate considerable decadal variability in the Fair Isle Current transport that dominates Atlantic inflow to the northwest North Sea, while sea level differences in the hindcast are dominated by strong seasonal variability. Uncertainties in the Wick tide gauge record limit confidence in this proxy.

Description: Carbon tetrachloride (CCl4) has substantial stratospheric ozone depletion potential and its consumption is controlled under the Montreal Protocol and its amendments. We implement a Kalman filter using atmospheric CCl4 measurements and a 3-dimensional chemical transport model to estimate the interannual regional industrial emissions and seasonal global oceanic uptake of CCl4 for the period of 1996–2004. The Model of Atmospheric Transport and Chemistry (MATCH), driven by offline National Center for Environmental Prediction (NCEP) reanalysis meteorological fields, is used to simulate CCl4 mole fractions and calculate their sensitivities to regional sources and sinks using a finite difference approach. High frequency observations from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the Earth System Research Laboratory (ESRL) of the National Oceanic and Atmospheric Administration (NOAA) and low frequency flask observations are together used to constrain the source and sink magnitudes, estimated as factors that multiply the a priori fluxes. Although industry data imply that the global industrial emissions were substantially declining with large interannual variations, the optimized results show only small interannual variations and a small decreasing trend. The global surface CCl4 mole fractions were declining in this period because the CCl4 oceanic and stratospheric sinks exceeded the industrial emissions. Compared to the a priori values, the inversion results indicate substantial increases in industrial emissions originating from the South Asian/Indian and Southeast Asian regions, and significant decreases in emissions from the European and North American regions.

Description: National parks in the United States are protected areas wherein the natural habitat is to be conserved for future generations. Deposition of anthropogenic nitrogen (N) transported from areas of human activity (fuel combustion, agriculture) may affect these natural habitats if it exceeds an ecosystem-dependent critical load (CL). We quantify and interpret the deposition to Class I US national parks for present-day and future (2050) conditions using the GEOS-Chem global chemical transport model with 1/2° × 2/3° horizontal resolution over North America. We estimate CL values in the range 2.5–5 kg N ha−1 yr−1 for the different parks to protect the most sensitive ecosystem receptors. For present-day conditions, we find 24 out of 45 parks to be in CL exceedance and 14 more to be marginally so. Many of these are in remote areas of the West. Most (40–85%) of the deposition originates from NOx emissions (fuel combustion). We project future changes in N deposition using representative concentration pathway (RCP) anthropogenic emission scenarios for 2050. These feature 52–73% declines in US NOx emissions relative to present but 19–50% increases in US ammonia (NH3) emissions. Nitrogen deposition at US national parks then becomes dominated by domestic NH3 emissions. While deposition decreases in the East relative to present, there is little progress in the West and increases in some regions. We find that 17–25 US national parks will have CL exceedances in 2050 based on the RCP8.5 and RCP2.6 scenarios. Even in total absence of anthropogenic NOx emissions, 14–18 parks would still have a CL exceedance. Returning all parks to N deposition below CL by 2050 would require at least a 50% decrease in US anthropogenic NH3 emissions relative to RCP-projected 2050 levels.

Description: Surface ozone (O3) pollution levels are strongly correlated with daytime surface temperatures, especially in highly polluted regions. This correlation is nonlinear and occurs through a variety of temperature-dependent mechanisms related to O3 precursor emissions, lifetimes, and reaction rates, making the reproduction of temperature sensitivities – and the projection of associated human health risks – a complex problem. Here we explore the summertime O3–temperature relationship in the United States and Europe using the chemical transport model GEOS-Chem. We remove the temperature dependence of several mechanisms most frequently cited as causes of the O3–temperature “climate penalty”, including PAN decomposition, soil NOx emissions, biogenic volatile organic compound (VOC) emissions, and dry deposition. We quantify the contribution of each mechanism to the overall correlation between O3 and temperature both individually and collectively. Through this analysis we find that the thermal decomposition of PAN can explain, on average, 20 % of the overall O3–temperature correlation in the United States. The effect is weaker in Europe, explaining 9 % of the overall O3–temperature relationship. The temperature dependence of biogenic emissions contributes 3 % and 9 % of the total O3–temperature correlation in the United States and Europe on average, while temperature-dependent deposition (6 % and 1 %) and soil NOx emissions (10 % and 7 %) also contribute. Even considered collectively these mechanisms explain less than 46 % of the modeled O3–temperature correlation in the United States and 36 % in Europe. We use commonality analysis to demonstrate that covariance with other meteorological phenomena such as stagnancy and humidity can explain the bulk of the remainder of the O3–temperature correlation. Thus, we demonstrate that the statistical correlation between O3 and temperature alone may greatly overestimate the direct impacts of temperature on O3, with implications for the interpretation of policy-relevant metrics such as climate penalty.

Description: We report on the appearance of a 2 km wide, 70 m deep circular depression located 50 km inland of the southwestern margin of the Greenland Ice Sheet that provides the first direct evidence for concentrated, long-term storage, and sudden release, of meltwater at the bed. Drainage of the lake may have been triggered by the recent increase in meltwater runoff. The abundance of such lakes and their potential importance to the ice sheet's hydrologic system and flow regime remain unknown.

Description: We report on the appearance of a 2 km wide, 70 m deep circular depression located 50 km inland of the southwestern margin of the Greenland Ice Sheet that provides the first direct evidence for concentrated, long-term storage, and sudden release, of meltwater at the bed. Drainage of the lake may have been triggered by the recent increase in meltwater runoff. The abundance of such lakes and their potential importance to the ice sheet's hydrologic system and flow regime remain unknown.

Description: The Antarctic outer coastal margin (i.e., the coastline itself, or the terminus/front of ice shelves, whichever is adjacent to the ocean) is a key interface between the ice-sheet and terrestrial environments and the Southern Ocean. Its physical configuration (including both length scale of variation and orientation/aspect) has direct bearing on several closely associated cryospheric, biological, oceanographical and ecological processes, yet no study has quantified the coastal complexity or orientation of Antarctica’s coastal margin. This first-of-a-kind characterisation of Antarctic coastal complexity aims to address this knowledge gap. We quantify and investigate the physical configuration and complexity of Antarctica’s circumpolar outer coastal margin using a novel, technique based on ∼ 40,000 random points selected along a vector coastline derived from the MODIS Mosaic of Antarctica dataset. At each point, a complexity metric is calculated at length scales from 1 to 256 km, giving a multiscale estimate of the magnitude and direction of undulation or complexity at each point location along the entire coastline. Using a cluster analysis to determine characteristic complexity ‘signatures’ for random nodes, the coastline is found to comprise three basic groups or classes: (i) low complexity at all scales; (ii) most complexity at shorter scales; and (iii) most complexity at longer scales. These classes are somewhat heterogeneously distributed throughout the continent. We also consider bays and peninsulas separately and characterise their multi-scale orientation. This unique dataset and its summary analysis have numerous applications for both geophysical and biological studies and will contribute to Antarctic research requiring quantitative information on, and related to, coastal complexity and configuration. All these data are referenced by https://doi.org/10.26179/5d1af0ba45c03 and are available free of charge at https://data.antarctica.gov.au.

Description: A unique stratigraphic sequence of fossil leaves of Eotrigonobalanus furcinervis (extinct trees of the beech family, Fagaceae) from central Germany has been used to derive an atmospheric pCO2 record with multiple data points spanning the late middle to late Eocene, two sampling levels which may be earliest Oligocene, and two samples from later in the Oligocene. Using the inverse relationship between the density of stomata and pCO2, we show that pCO2 decreased continuously from the late middle to late Eocene, reaching a relatively stable low value before the end of the Eocene. Based on the subsequent records, pCO2 in parts of the Oligocene was similar to latest Eocene values. These results suggest that a decrease in pCO2 preceded the large shift in marine oxygen isotope records that characterizes the Eocene–Oligocene transition and that when a certain threshold of pCO2 change was crossed, the cumulative effects of this and other factors resulted in rapid temperature decline, ice build up on Antarctica and hence a change of climate mode.