Description: The formation and recycling of reactive nitrogen (NO, NO2, HONO) at the air–snow interface has implications for air quality and the oxidation capacity of the atmosphere in snow-covered regions. Nitrate (NO3−) photolysis in snow provides a source of oxidants (e.g., hydroxyl radical) and oxidant precursors (e.g., nitrogen oxides) to the overlying boundary layer, and alters the concentration and isotopic (e.g., δ15N) signature of NO3− preserved in ice cores. We have incorporated an idealized snowpack with a NO3− photolysis parameterization into a global chemical transport model (Goddard Earth Observing System (GEOS) Chemistry model, GEOS-Chem) to examine the implications of snow NO3− photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core NO3− in ice cores across Antarctica and Greenland, where observations of these parameters over large spatial scales are difficult to obtain. A major goal of this study is to examine the influence of meteorological parameters and chemical, optical, and physical snow properties on the magnitudes and spatial patterns of snow-sourced NOx fluxes and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland. Snow-sourced NOx fluxes are most influenced by temperature-dependent quantum yields of NO3− photolysis, photolabile NO3− concentrations in snow, and concentrations of light-absorbing impurities (LAIs) in snow. Despite very different assumptions about snowpack properties, the range of model-calculated snow-sourced NOx fluxes are similar in Greenland (0.5–11 × 108 molec cm−2 s−1) and Antarctica (0.01–6.4 × 108 molec cm−2 s−1) due to the opposing effects of higher concentrations of both photolabile NO3− and LAIs in Greenland compared to Antarctica. Despite the similarity in snow-sourced NOx fluxes, these fluxes lead to smaller factor increases in mean austral summer boundary layer mixing ratios of total nitrate (HNO3+ NO3−), NOx, OH, and O3 in Greenland compared to Antarctica because of Greenland's proximity to pollution sources. The degree of nitrogen recycling in the snow is dependent on the relative magnitudes of snow-sourced NOx fluxes versus primary NO3− deposition. Recycling of snow NO3− in Greenland is much less than in Antarctica Photolysis-driven loss of snow NO3− is largely dependent on the time that NO3− remains in the snow photic zone (up to 6.5 years in Antarctica and 7 months in Greenland), and wind patterns that redistribute snow-sourced reactive nitrogen across Antarctica and Greenland. The loss of snow NO3− is higher in Antarctica (up to 99 %) than in Greenland (up to 83 %) due to deeper snow photic zones and lower snow accumulation rates in Antarctica. Modeled enrichments in ice-core δ15N(NO3−) due to photolysis-driven loss of snow NO3− ranges from 0 to 363 ‰ in Antarctica and 0 to 90 ‰ in Greenland, with the highest fraction of NO3− loss and largest enrichments in ice-core δ15N(NO3−) at high elevations where snow accumulation rates are lowest. There is a strong relationship between the degree of photolysis-driven loss of snow NO3− and the degree of nitrogen recycling between the air and snow throughout all of Greenland and in Antarctica where snow accumulation rates are greater than 130 kg m−2 a−1 in the present day.

Description: The Surface Ocean – Lower Atmosphere Study (SOLAS) (http://www.solas-int.org/) is an international research initiative focused on understanding the key biogeochemical-physical interactions and feedbacks between the ocean and atmosphere that are critical elements of climate and global biogeochemical cycles. Following the release of the SOLAS Decadal Science Plan (2015-2025) (Brévière et al., 2016), the Ocean-Atmosphere Interaction Committee (OAIC) was formed as a subcommittee of the Ocean Carbon and Biogeochemistry (OCB) Scientific Steering Committee to coordinate US SOLAS efforts and activities, facilitate interactions among atmospheric and ocean scientists, and strengthen US contributions to international SOLAS. In October 2019, with support from OCB, the OAIC convened an open community workshop, Ocean-Atmosphere Interactions: Scoping directions for new research with the goal of fostering new collaborations and identifying knowledge gaps and high-priority science questions to formulate a US SOLAS Science Plan. Based on presentations and discussions at the workshop, the OAIC and workshop participants have developed this US SOLAS Science Plan. The first part of the workshop and this Science Plan were purposefully designed around the five themes of the SOLAS Decadal Science Plan (2015-2025) (Brévière et al., 2016) to provide a common set of research priorities and ensure a more cohesive US contribution to international SOLAS.

Description: This report was developed with federal support of NSF (OCE-1558412) and NASA (NNX17AB17G).

Description: Tropospheric reactive bromine (Bry) influences the oxidation capacity of the atmosphere by acting as a sink for ozone and nitrogen oxides. Aerosol acidity plays a crucial role in Bry abundances through acid-catalyzed debromination from sea-salt-aerosol, the largest global source. Bromine concentrations in a Russian Arctic ice-core, Akademii Nauk, show a 3.5-fold increase from pre-industrial (PI) to the 1970s (peak acidity, PA), and decreased by half to 1999 (present day, PD). Ice-core acidity mirrors this trend, showing robust correlation with bromine, especially after 1940 (r = 0.9). Model simulations considering anthropogenic emission changes alone show that atmospheric acidity is the main driver of Bry changes, consistent with the observed relationship between acidity and bromine. The influence of atmospheric acidity on Bry should be considered in interpretation of ice-core bromine trends.

Description: Snowpack emissions are recognized as an important source of gas-phase reactive bromine in the Arctic and are necessary to explain ozone depletion events in spring caused by the catalytic destruction of ozone by halogen radicals. Quantifying bromine emissions from snowpack is essential for interpretation of ice-core bromine. We present ice-core bromine records since the pre-industrial (1750 CE) from six Arctic locations and examine potential post-depositional loss of snowpack bromine using a global chemical transport model. Trend analysis of the ice-core records shows that only the high-latitude coastal Akademii Nauk (AN) ice core from the Russian Arctic preserves significant trends since pre-industrial times that are consistent with trends in sea ice extent and anthropogenic emissions from source regions. Model simulations suggest that recycling of reactive bromine on the snow skin layer (top 1 mm) results in 9–17% loss of deposited bromine across all six ice-core locations. Reactive bromine production from below the snow skin layer and within the snow photic zone is potentially more important, but the magnitude of this source is uncertain. Model simulations suggest that the AN core is most likely to preserve an atmospheric signal compared to five Greenland ice cores due to its high latitude location combined with a relatively high snow accumulation rate. Understanding the sources and amount of photochemically reactive snow bromide in the snow photic zone throughout the sunlit period in the high Arctic is essential for interpreting ice-core bromine, and warrants further lab studies and field observations at inland locations.