Earth Systems

Role of the ocean’s AMOC in setting the uptake efficiency of transient tracers

The central role played by the ocean's Atlantic Meridional Overturning Circulation (AMOC) in the uptake and sequestration of transient tracers is studied in a series of experiments with the Goddard Institute for Space Studies and Massachusetts Institute of Technology ocean circulation models. Forced by observed atmospheric time series of CFC-11, both models exhibit realistic distributions in the ocean, with similar surface biases but different response over time. To better understand what controls uptake, we ran idealized forcing experiments in which the AMOC strength varied over a wide range, bracketing the observations. We found that differences in the strength and vertical scale of the AMOC largely accounted for the different rates of CFC-11 uptake and vertical distribution thereof. A two-box model enables us to quantify and relate uptake efficiency of passive tracers to AMOC strength and how uptake efficiency decreases in time. We also discuss the relationship between passive tracer and heat uptake efficiency, of which the latter controls the transient climate response to anthropogenic forcing in the North Atlantic. We find that heat uptake efficiency is substantially less (by about a factor of 5) than that for a passive tracer.

Phytoplankton functional diversity increases ecosystem productivity and stability

The effect of biodiversity on ecosystem functioning is one of the major questions of ecology. However, the role of phytoplankton functional diversity in ecosystem productivity and stability under fluctuating (i.e. non-equilibrium) environments remains largely unknown. Here we use a marine ecosystem model to study the effect of phytoplankton functional diversity on both ecosystem productivity and its stability for seasonally variable nutrient supply and temperature. Functional diversity ranges from low to high along these two environmental axes independently. Changes in diversity are obtained by varying the range of uptake strategies and thermal preferences of the species present in the community. Species can range from resource gleaners to opportunists, and from cold to warm thermal preferences. The phytoplankton communities self-assemble as a result of species selection by resource competition (nutrients) and environmental filtering (temperature). Both processes lead to species asynchrony but their effect on productivity and stability differ. We find that the diversity of temperature niches has a strong and direct positive effect on productivity and stability due to species complementarity, while the diversity of uptake strategies has a weak and indirect positive effect due to sampling probability. These results show that more functionally diverse phytoplankton communities lead to higher and more stable ecosystem productivity but the positive effect of biodiversity on ecosystem functioning depends critically on the type of environmental gradient.

How might climate change affect the acidification of the world’s oceans or air quality in China and india in the coming decades, and what climate policies could be effective in minimizing such impacts? To answer such questions, decision-makers routinely rely on science-based projections of physical and economic impacts of climate change on selected regions and economic sectors. But the projections they obtain may not be as reliable or useful as they appear: today’s gold standard for climate impact assessments—model intercomparison projects (MIPs)—fall short in many ways.

Projecting the impacts of climate change
Top-down constraints on global N2O emissions at optimal resolution: application of a new dimension reduction technique

We present top-down constraints on global monthly N2O emissions for 2011 from a multi-inversion approach and an ensemble of surface observations. The inversions employ the GEOS-Chem adjoint and an array of aggregation strategies to test how well current observations can constrain the spatial distribution of global N2O emissions. The strategies include (1) a standard 4D-Var inversion at native model resolution (4° × 5°), (2) an inversion for six continental and three ocean regions, and (3) a fast 4D-Var inversion based on a novel dimension reduction technique employing randomized singular value decomposition (SVD). The optimized global flux ranges from 15.9 Tg N yr−1 (SVD-based inversion) to 17.5–17.7 Tg N yr−1 (continental-scale, standard 4D-Var inversions), with the former better capturing the extratropical N2O background measured during the HIAPER Pole-to-Pole Observations (HIPPO) airborne campaigns. We find that the tropics provide a greater contribution to the global N2O flux than is predicted by the prior bottom-up inventories, likely due to underestimated agricultural and oceanic emissions. We infer an overestimate of natural soil emissions in the extratropics and find that predicted emissions are seasonally biased in northern midlatitudes. Here, optimized fluxes exhibit a springtime peak consistent with the timing of spring fertilizer and manure application, soil thawing, and elevated soil moisture. Finally, the inversions reveal a major emission underestimate in the US Corn Belt in the bottom-up inventory used here. We extensively test the impact of initial conditions on the analysis and recommend formally optimizing the initial N2O distribution to avoid biasing the inferred fluxes. We find that the SVD-based approach provides a powerful framework for deriving emission information from N2O observations: by defining the optimal resolution of the solution based on the information content of the inversion, it provides spatial information that is lost when aggregating to political or geographic regions, while also providing more temporal information than a standard 4D-Var inversion.

Atmospheric histories and emissions of chlorofluorocarbons CFC-13 (CClF3), ΣCFC-114 (C2Cl2F4), and CFC-115 (C2ClF5)

Based on observations of the chlorofluorocarbons CFC-13 (chlorotrifluoromethane), ΣCFC-114 (combined measurement of both isomers of dichlorotetrafluoroethane), and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly 8 decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry-air mole fraction in parts per trillion, pmol mol−1) in 2016. Its growth rate has decreased since the mid-1980s but has remained at a surprisingly high mean level of 0.02 ppt yr−1 since 2000, resulting in a continuing growth of CFC-13 in the atmosphere. ΣCFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.49 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unchanging lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr−1 (> 15 % of past peak emissions), of ΣCFC-114 at 1.90 ± 0.84 kt yr−1 (∼ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr−1 (> 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2015–2016 are 1.14 ± 0.50 kt yr−1 and have doubled compared to the 2007–2010 minimum. We find CFC-13 emissions from aluminum smelters but if extrapolated to global emissions, they cannot account for the lingering global emissions determined from the atmospheric observations. We find impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions, they can neither account for the lingering global CFC-115 emissions determined from the atmospheric observations nor for their recent increases. We also conduct regional inversions for the years 2012–2016 for the northeastern Asian area using observations from the Korean AGAGE site at Gosan and find significant emissions for ΣCFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in northeastern Asia and more specifically on the Chinese mainland.

Multi-model study of mercury dispersion in the atmosphere: Vertical distribution of mercury species

Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model intercomparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground-based observations of mercury concentration and deposition, here we investigate the vertical and interhemispheric distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on intercontinental flights.

The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including interhemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury patterns depending on altitude. High concentrations of oxidized mercury in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parameterizations in the chemistry transport models also proved to have a substantial impact on model results.

Multi-model study of mercury dispersion in the atmosphere: Atmospheric processes and model evaluation

Current understanding of mercury (Hg) behavior in the atmosphere contains significant gaps. Some key characteristics of Hg processes, including anthropogenic and geogenic emissions, atmospheric chemistry, and air–surface exchange, are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measured data from ground-based sites and simulation results from chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux have been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were used, both in their state-of-the-art configurations and for a number of numerical experiments to evaluate particular processes. Results of the model simulations were evaluated against measurements. As follows from the analysis, the interhemispheric GEM gradient is largely formed by the prevailing spatial distribution of anthropogenic emissions in the Northern Hemisphere. The contributions of natural and secondary emissions enhance the south-to-north gradient, but their effect is less significant. Atmospheric chemistry has a limited effect on the spatial distribution and temporal variation of GEM concentration in surface air. In contrast, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism can reproduce successfully the observed seasonal variation of the RM ∕ GEM ratio in the near-surface layer, but it predicts a wet deposition maximum in spring instead of in summer as observed at monitoring sites in North America and Europe. Model runs with OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but shift the maximum RM ∕ GEM ratios from spring to summer. O3 chemistry does not predict significant seasonal variation of Hg oxidation. Hence, the performance of the Hg oxidation mechanisms under study differs in the extent to which they can reproduce the various observed parameters. This variation implies possibility of more complex chemistry and multiple Hg oxidation pathways occurring concurrently in various parts of the atmosphere.

Uncertainty and variability in atmospheric formation of PFCAs from fluorotelomer precursors

Perfluoroalkyl carboxylic acids (PFCAs) are environmental contaminants that are highly persistent, bio-accumulative, and have been detected along with their atmospheric precursors far from emissions sources. The importance of precursor emissions as an indirect source of PFCAs to the environment is uncertain. Modeling studies have used degradation mechanisms of differing complexities to estimate the atmospheric production of PFCAs, and these differing mechanisms lead to quantitatively different yields of PFCAs under differing atmospheric conditions. We evaluate PFCA formation with the most complete degradation mechanism to date, to our knowledge, using a box model analysis to simulate the atmospheric chemical fate of fluorotelomer precursors to long-chain PFCAs. In particular, we examine the variability in PFCA formation in different chemical environments, and estimate the uncertainty in PFCA formation due to reaction rate constants.

We calculate long-chain PFCA formation theoretical maximum yields for the degradation of fluorotelomer precursor species at a representative sample of atmospheric conditions from a three-dimensional chemical transport model, and estimate uncertainties in such calculations for urban, ocean, and Arctic conditions using polynomial chaos methods. We find that atmospheric conditions farther from pollution sources have both higher capacities to form long-chain PFCAs and higher uncertainties in those capacities.

Our calculations of theoretical maximum yields indicate that under typical Northern Hemisphere conditions, less than 10 % of emitted precursor may reach long-chain PFCA end products. This results in a possible upper bound of 2–50 t year−1 of long-chain PFCA (depending on quantity of emitted precursor) produced in the atmosphere via degradation of fluorotelomer products. However, transport to high-yield areas could result in higher yields. While the atmosphere is a potentially growing source of long-chain PFCAs in the Arctic, oceanic transport and interactions between the atmosphere and ocean may be relatively more important pathways to the Arctic for long-chain PFCAs.

Developing a Consistent Database for Regional Geologic CO2 Storage Capacity Worldwide

Assessments of the geologic storage capacity of carbon dioxide in the current literature are incomplete and inconsistent, complicating efforts to assess the worldwide potential for carbon dioxide capture and storage (CCS). We developed a method for generating first-order estimates of storage capacity requiring minimal data to characterize a geologic formation. We show this simplified method accounts for the majority of the variance in storage capacity found in more detailed studies conducted in the United States. We apply our method to create a worldwide database of storage capacity, disaggregated into 18 regions, and compare this storage capacity to CCS deployment in the MIT Economic Prediction and Policy Analysis (EPPA) model. Globally, we estimate there are between 8,000 and 55,000 gigatonnes (Gt) of practically accessible geologic storage capacity for carbon dioxide. For most of the regions, our results indicate storage capacity is not a limiting factor for CCS deployment through the rest of this century even if stringent emissions reductions are required.

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