We report ground-based atmospheric measurements and emission estimates for the halons H-1211 (CBrClF₂), H-1301 (CBrF₃), and H-2402 (CBrF₂CBrF₂) from the AGAGE (Advanced Global Atmospheric Gases Experiment) and the National Oceanic and Atmospheric Administration global networks. We also include results from archived air samples in canisters and from polar firn in both hemispheres, thereby deriving an atmospheric record of nearly nine decades (1930s to present). All three halons were absent from the atmosphere until ∼1970, when their atmospheric burdens started to increase rapidly. In recent years H-1211 and H-2402 mole fractions have been declining, but H-1301 has continued to grow. High-frequency observations show continuing emissions of H-1211 and H-1301 near most AGAGE sites. For H-2402 the only emissions detected were derived from the region surrounding the Sea of Japan/East Sea. Based on our observations, we derive global emissions using two different inversion approaches. Emissions for H-1211 declined from a peak of 11 kt yr⁻¹ (late 1990s) to 3.9 kt yr⁻¹ at the end of our record (mean of 2013–2015), for H-1301 from 5.4 kt yr⁻¹ (late 1980s) to 1.6 kt yr⁻¹, and for H-2402 from 1.8 kt yr⁻¹ (late 1980s) to 0.38 kt yr⁻¹. Yearly summed halon emissions have decreased substantially; nevertheless, since 2000 they have accounted for ∼30% of the emissions of all major anthropogenic ozone depletion substances, when weighted by ozone depletion potentials.

We present a numerical model of the ocean that couples a three-stream radiative transfer component with a marine biogeochemical–ecosystem component in a dynamic three-dimensional physical framework. The radiative transfer component resolves the penetration of spectral irradiance as it is absorbed and scattered within the water column. We explicitly include the effect of several optically important water constituents (different phytoplankton functional types; detrital particles; and coloured dissolved organic matter, CDOM). The model is evaluated against in situ-observed and satellite-derived products. In particular we compare to concurrently measured biogeochemical, ecosystem, and optical data along a meridional transect of the Atlantic Ocean. The simulation captures the patterns and magnitudes of these data, and estimates surface upwelling irradiance analogous to that observed by ocean colour satellite instruments. We find that incorporating the different optically important constituents explicitly and including spectral irradiance was crucial to capture the variability in the depth of the subsurface chlorophyll a (Chl a) maximum. We conduct a series of sensitivity experiments to demonstrate, globally, the relative importance of each of the water constituents, as well as the crucial feedbacks between the light field, the relative fitness of phytoplankton types, and the biogeochemistry of the ocean. CDOM has proportionally more importance at attenuating light at short wavelengths and in more productive waters, phytoplankton absorption is relatively more important at the subsurface Chl a maximum, and water molecules have the greatest contribution when concentrations of other constituents are low, such as in the oligotrophic gyres. Scattering had less effect on attenuation, but since it is important for the amount and type of upwelling irradiance, it is crucial for setting sea surface reflectance. Strikingly, sensitivity experiments in which absorption by any of the optical constituents was increased led to a decrease in the size of the oligotrophic regions of the subtropical gyres: lateral nutrient supplies were enhanced as a result of decreasing high-latitude productivity. This new model that captures bio-optical feedbacks will be important for improving our understanding of the role of light and optical constituents on ocean biogeochemistry, especially in a changing environment. Further, resolving surface upwelling irradiance will make it easier to connect to satellite-derived products in the future.

© 2015 the authors

Atmosphere–surface exchange of mercury, although a critical component of its global cycle, is currently poorly constrained. Here we use the GEOS-Chem chemical transport model to interpret atmospheric Hg⁰ (gaseous elemental mercury) data collected during the 2013 summer Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks (NOMADSS) aircraft campaign as well as ground- and ship-based observations in terms of their constraints on the atmosphere–surface exchange of Hg⁰ over eastern North America. Model–observation comparison suggests that the Northwest Atlantic may be a net source of Hg⁰, with high evasion fluxes in summer (our best sensitivity simulation shows an average oceanic Hg⁰ flux of 3.3 ng m^-2 h^-1 over the Northwest Atlantic), while the terrestrial ecosystem in the summer of the eastern United States is likely a net sink of Hg⁰ (our best sensitivity simulation shows an average terrestrial Hg⁰ flux of -0.6 ng m^-2 h^-1 over the eastern United States). The inferred high Hg⁰ fluxes from the Northwest Atlantic may result from high wet deposition fluxes of oxidized Hg, which are in turn related to high precipitation rates in this region. We also find that increasing simulated terrestrial fluxes of Hg⁰ in spring compared to other seasons can better reproduce observed seasonal variability of Hg⁰ concentration at ground-based sites in eastern North America.

Long-term response of the climate system to anthropogenic forcing was investigated with the MIT Earth System Model of intermediate complexity version 2.2 (MESM2.2). The MESM2.2 consists of a 2D (zonally averaged) atmospheric model coupled to an anomaly diffusing ocean model. Climate sensitivity of the MESM can be varied using a cloud adjustment technique and rate of oceanic heat uptake can be varied by changing effective diffusion coefficient. An ensemble of four hundred simulations was carried out for the period 1860-2005 using historical forcing. Values of climate sensitivity, rate of ocean heat uptake, and the strength of the aerosol forcing were drawn from the Libardoni and Forest (2013) distribution presented in the IPCC AR5. A 400-member ensemble was carried out for each of four different RCP scenarios from the year 2006 to the year 2500. By the end of the 21st century (2081-2100), the ensemble mean of surface air temperature increases, relative to 1986-2005 period, by 1.2, 1.8, 2.2 and 3.3oC for RCP26, RCP4.5, RCP6.0 and RCP8.5, respectively. Corresponding numbers for the ensemble of the CMPI5 models are 1.0, 1.8, 2.2 and 3.7oC. In spite of the forcing being fixed beyond year 2150 for RCP4.5 and RCP6.0 and beyond 2250 for RCP8.5, surface air temperature keeps rising until the end of 25th century under these scenarios. The upper bound of the 90% probability interval increases significantly more than the mean. For the RCP4.5 scenario, the mean value of possible SAT change increases by 1.6oC from the end of the 21st century to the end of the 25th century, while the value of the 95th percentile increases by 3.2oC. Corresponding numbers for RCP6.0 and RCP8.5 are 3.6 and 10.2oC for the medians and 7.0 and 14.5oC for the 95th percentiles, respectively. Such changes in the shape of probability distributions with time indicate an increase in the probability that surface warming will exceed a given value. For example, the probability of exceeding 3oC warming under the RCP4.5 scenario increases from 2.5% at the end of 21st century to 32% and 50% at the end of 23rd and 25th centuries, respectively. For the RCP2.6 scenario, in which radiative forcing peaks in the year 2070 before decreasing back to the 1990s level by the year 2300, the ensemble mean surface air temperature is still about 0.5oC above present at the end of the simulation. Obtained results show that in spite of large differences in radiative forcing between different RCP scenarios, uncertainties in the climate system characteristics defining climate system response make a significant contribution into overall uncertainty in possible climate change during the next few centuries. Comparison with simulations carried under SRES scenarios also will be presented