Aircraft and satellite derived arctic BrO profiles of the tropospheric column

We derive tropospheric column BrO during the ARCTAS and ARCPAC field campaigns in spring 2008 using retrievals of total column BrO from the satellite UV nadir sensors OMI and GOME-2 using a radiative transfer model and stratospheric column BrO from a photochemical simulation. We conduct a comprehensive comparison of satellite-derived tropospheric BrO column to aircraft in-situ observations of BrO and related species. The aircraft profiles reveal that tropospheric BrO, when present during April 2008, was distributed over a broad range of altitudes rather than being confined to the planetary boundary layer (PBL). Perturbations to the total column resulting from tropospheric BrO are the same magnitude as perturbations due to longitudinal variations in the stratospheric component, so proper accounting of the stratospheric signal is essential for accurate determination of satellite-derived tropospheric BrO. We find reasonably good agreement between satellite-derived tropospheric BrO and columns found using aircraft in-situ BrO profiles, particularly when satellite radiances were obtained over bright surfaces (albedo >0.7), for solar zenith angle <80° and clear sky conditions. The rapid activation of BrO due to surface processes (the bromine explosion) is apparent in both the OMI and GOME-2 based tropospheric columns. The wide orbital swath of OMI allows examination of the evolution of tropospheric BrO on about hourly time intervals near the pole. Low surface pressure, strong wind, and high PBL height are associated with an observed BrO activation event, supporting the notion of bromine activation by high winds over snow.

(Appendix A) Geochemical composition of snow and eolian mineral dust from Berkner Island ice sheet, Antarctica

The Sr and Nd isotopic composition of dust extracted from recent snow layers at the top of Berkner Island ice sheet (located within the Filchner-Ronne Ice Shelf at the southern end of the Weddell Sea) enables us, for the first time, to document dust provenance in Antarctica outside the East Antarctic Plateau (EAP) where all previous studies based on isotopic fingerprinting were carried out. Berkner dust displays an overall crust-like isotopic signature, characterized by more radiogenic 87Sr/86Sr and much less radiogenic 143Nd/144Nd compared to dust deposited on the EAP during glacial periods. Differences with EAP interglacial dust are not as marked but still significant, indicating that present-day Berkner dust provenance is distinct, at least to some extent, from that of the dust reaching the EAP. The fourteen snow-pit sub-seasonal samples that were obtained span a two-year period (2002-2003) and their dust Sr and Nd isotopic composition reveals that multiple sources are at play over a yearly time period. Southern South America, Patagonia in particular, likely accounts for part of the observed spring/summer dust deposition maxima, when isotopic composition is shifted towards 'younger' isotopic signatures. In the spring, possible additional inputs from Australian sources would also be supported by the data. Most of the year, however, the measured isotopic signatures would be best explained by a sustained background supply from putative local sources in East Antarctica, which carry old-crust-like isotopic fingerprints. Whether the restricted East Antarctic ice-free areas produce sufficient eolian material has yet to be substantiated however. The fact that large (> 5 µm) particles represent a significant fraction of the samples throughout the entire time-series supports scenarios that involve contributions from proximal sources, either in Patagonia and/or Antarctica (possibly including snow-free areas in the Antarctic Peninsula and other areas as well). This also indicates that additional dust transport, which does not reach the EAP, must occur at low-tropospheric levels to this coastal sector of Antarctica.

Larcform 1 - single column model intercomparison of Arctic air formation, link to model results in NetCDF format

Weather and climate models struggle to represent lower tropospheric temperature and moisture profiles and surface fluxes in Arctic winter, not least because they lack or misrepresent physical processes that are specific to high latitudes. The Arctic boundary layer in winter has been observed to be in either a radiatively clear or cloudy state: The radiatively clear state is characterized by strong surface radiative cooling leading to the build-up of surface-based temperature inversions, whereas the cloudy state occurs when cloud liquid water is present in the atmospheric column, allowing little or no surface radiative cooling and leading to weaker and typically elevated temperature inversions. Many large-scale models have been shown to lack the cloudy state, and some do substantially underestimate stability in the clear state. We here present results from the first Lagrangian ARCtic air FORMation experiment (Larcform 1), a GASS (Global atmospheric system studies) single-column model intercomparison which reproduces these biases of large-scale models in an idealised setup.

Pollen analyses of sediment core GeoB9508-5

Millennial-scale dry events in the Northern Hemisphere monsoon regions during the last Glacial period are commonly attributed to southward shifts of the Intertropical Convergence Zone (ITCZ) associated with an intensification of the northeasterly (NE) trade wind system during intervals of reduced Atlantic meridional overturning circulation (AMOC). Through the use of high-resolution last deglaciation pollen records from the continental slope off Senegal, our data show that one of the longest and most extreme droughts in the western Sahel history, which occurred during the North Atlantic Heinrich Stadial 1 (HS1), displayed a succession of three major phases. These phases progressed from an interval of maximum pollen representation of Saharan elements between ~19 and 17.4 kyr BP indicating the onset of aridity and intensified NE trade winds, followed by a millennial interlude of reduced input of Saharan pollen and increased input of Sahelian pollen, to a final phase between ~16.2 and 15 kyr BP that was characterized by a second maximum of Saharan pollen abundances. This change in the pollen assemblage indicates a mid-HS1 interlude of NE trade wind relaxation, occurring between two distinct trade wind maxima, along with an intensified mid-tropospheric African Easterly Jet (AEJ) indicating a substantial change in West African atmospheric processes. The pollen data thus suggest that although the NE trades have weakened, the Sahel drought remained severe during this time interval. Therefore, a simple strengthening of trade winds and a southward shift of the West African monsoon trough alone cannot fully explain millennial-scale Sahel droughts during periods of AMOC weakening. Instead, we suggest that an intensification of the AEJ is needed to explain the persistence of the drought during HS1. Simulations with the Community Climate System Model indicate that an intensified AEJ during periods of reduced AMOC affected the North African climate by enhancing moisture divergence over the West African realm, thereby extending the Sahel drought for about 4000 years.

Model results in NetCDF format of North African vegetation-precipitation in early and mid-Holocene climate simulated by CCSM3-DGVM//

The present study analyses the sign, strength, and working mechanism of the vegetation-precipitation feedback over North Africa in middle (6 ka BP) and early Holocene (9 ka BP) simulations using the comprehensive coupled climate-vegetation model CCSM3-DGVM (Community Climate System Model version 3 and a dynamic global vegetation model). The coupled model simulates enhanced summer rainfall and a northward migration of the West African monsoon trough along with an expansion of the vegetation cover for the early and middle Holocene compared to the pre-industrial period. It is shown that dynamic vegetation enhances the orbitally triggered summer precipitation anomaly by approximately 20% in the Sahara-Sahel region (10-25° N, 20° W-30° E) in both the early and mid-Holocene experiments compared to their fixed-vegetation counterparts. The primary vegetation-rainfall feedback identified here operates through surface latent heat flux anomalies by canopy evaporation and transpiration and their effect on the mid-tropospheric African easterly jet, whereas the effects of vegetation changes on surface albedo and local water recycling play a negligible role. Even though CCSM3-DGVM simulates a positive vegetation-precipitation feedback in the North African region, this feedback is not strong enough to produce multiple equilibrium climate-ecosystem states on a regional scale.

Homogenized radiosonde record at station Ny-Ålesund, Spitsbergen, 1993-2014

Radiosonde measurements obtained at the Arctic site Ny-Ålesund (78.9° N, 11.9° E), Svalbard, from 1993 to 2014 have been homogenized accounting for instrumentation discontinuities by correcting known errors in the manufacturer provided profiles. From the homogenized data record, the first Ny-Ålesund upper-air climatology of wind, temperature and humidity is presented, forming the background for the analysis of changes during the 22-year period. Particularly during the winter season, a strong increase in atmospheric temperature and humidity is observed, with a significant warming of the free troposphere in January and February up to 3 K per decade. This winter warming is even more pronounced in the boundary layer below 1 km, presumably amplified by mesoscale processes including e.g. orographic effects or the boundary layer capping inversion. Though the largest contribution to the increasing atmospheric water vapour column in winter originates from the lowermost 2 km, no increase in the contribution by specific humidity inversions is detected. Instead, we find an increase in the humidity content of the large scale background humidity profiles. At the same time, the tropospheric flow in winter is found to occur less frequent from northerly directions and to the same amount more frequent from the South. We conclude that changes in the atmospheric circulation lead to an enhanced advection of warm and moist air from lower latitudes to the Svalbard region in the winter season, causing the warming and moistening of the atmospheric column above Ny-Ålesund.

Halogen deposition in polar snow and ice

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

Geochemistry, isotopic ratios and aldehyde concentrations of frost flowers, snow and ice near Barrow, Alaska

Frost flowers, intricate featherlike crystals that grow on refreezing sea ice leads, have been implicated in lower atmospheric chemical reactions. Few studies have presented chemical composition information for frost flowers over time and many of the chemical species commonly associated with Polar tropospheric reactions have never been reported for frost flowers. We undertook this study on the sea ice north of Barrow, Alaska to quantify the major ion, stable oxygen and hydrogen isotope, alkalinity, light absorbance by soluble species, organochlorine, and aldehyde composition of seawater, brine, and frost flowers. For many of these chemical species we present the first measurements from brine or frost flowers. Results show that major ion and alkalinity concentrations, stable isotope values, and major chromophore (NO3- and H2O2) concentrations are controlled by fractionation from seawater and brine. The presence of these chemical species in present and future sea ice scenarios is somewhat predictable. However, aldehydes, organochlorine compounds, light absorbing species, and mercury (part 2 of this research and Sherman et al. (2012, doi:10.1029/2011JD016186)) are deposited to frost flowers through less predictable processes that probably involve the atmosphere as a source. The present and future concentrations of these constituents in frost flowers may not be easily incorporated into future sea ice or lower atmospheric chemistry scenarios. Thinning of Arctic sea ice will likely present more open sea ice leads where young ice, brine, and frost flowers form. How these changing ice conditions will affect the interactions between ice, brine, frost flowers and the lower atmosphere is unknown.