Irene Stemmler

On the contribution of biomass burning to POPs (PAHs and PCDDs) in air in Africa.

Forest, savannah, and agricultural fires in the tropics and subtropics are sources for widespread pollution and release many organic substances into the air and soil, including persistent organic pollutants, i.e., polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polycyclic aromatic hydrocarbons (PAHs). The significance of this source for the exposure of humans and the environment in Africa toward phenanthrene, fluoranthene, pyrene, benzo(a)pyrene, 2,3,7,8-tetrachlorodibenzo-p-dioxin, 1,2,3,4,6,7,8-heptachlorodibenzo-p-dioxin, and octachlorodibenzo-p-dioxin is studied using daily global emissions from vegetation fires observed by satellite and a global multicompartment chemistry-transport model. Near-ground atmospheric concentrations of model-predicted vegetation fire related concentrations of PAHs and PCDDs were in the 10-1000 and 10(-5)-10(-3) pg m(-3) ranges, respectively. Vegetation fires in Africa are found to emit 180 ± 25 kg yr(-1) of PCDD/Fs. By comparison with observations, it is found that fires explain 1-10% of the PCDD (5% of 2,3,7,8- tetrachlorodibenzo-p-dioxin) concentrations in the rural and background atmosphere of sub-Saharan Africa. The contribution of vegetation fires to exposure to PAH is probably >10%, but cannot be quantified due to lack of knowledge with regard to both emission factors and photochemistry. A sensitivity analysis suggests that the heterogeneous reaction of PAHs with ozone is effectively limiting atmospheric lifetime and long-range transport.

The impact of organochlorines cycling in the cryosphere on global distributions and fate-2. Land ice and temporary snow cover

Global fate and transport of γ-HCH and DDT was studied using a global multicompartment chemistry-transport model, MPI-MCTM, with and without inclusion of land ice (in Antarctica and Greenland) or snow cover (dynamic). MPI-MCTM is based on coupled ocean and atmosphere general circulation models. After a decade of simulation 4.2% γ-HCH and 2.3% DDT are stored in land ice and snow. Neglection of land ice and snow in modelling would underestimate the total environmental residence time, τ(ov), of γ-HCH and overestimate τ(ov) for DDT, both on the order of 1% and depending on actual compartmental distribution. Volatilisation of DDT from boreal, seasonally snow covered land is enhanced throughout the year, while volatilisation of γ-HCH is only enhanced during the snow-free season. Including land ice and snow cover in modelling matters in particular for the Arctic, where higher burdens are predicted to be stored.

The impact of organochlorines cycling in the cryosphere on their global distribution and fate - 1. Sea ice

Global fate and transport of γ-HCH and DDT was studied using a global multicompartment chemistry-transport model, MPI-MCTM, with and without a dynamic sea ice compartment. The MPI-MCTM is based on coupled ocean and atmosphere general circulation models. Sea ice hosts 7-9% of the burden of the surface ocean. Without cycling in sea ice the geographic distributions are shifted from land to sea. This shift of burdens exceeds the sea ice burden by a factor of ≈8 for γ-HCH and by a factor of ≈15 for DDT. As regional scale seasonal sea ice melting may double surface ocean contamination, a neglect of cycling in sea ice (in an otherwise unchanged model climate) would underestimate ocean exposure in high latitudes. Furthermore, it would lead to overestimates of the residence times in ocean by 40% and 33% and of the total environmental residence times, τ(overall), of γ-HCH and DDT by 1.6% and 0.6%, respectively.

Strengthening seasonal marine CO2 variations due to increasing atmospheric CO2

The increase of atmospheric CO2 (ref. 1) has been predicted to impact the seasonal cycle of inorganic carbon in the global ocean2,3, yet the observational evidence to verify this prediction has been missing. Here, using an observation-based product of the oceanic partial pressure of CO2 (pCO2) covering the past 34 years, we find that the winter-to-summer difference of the pCO2 has increased on average by 2.2 ± 0.4 μatm per decade from 1982 to 2015 poleward of 10° latitude. This is largely in agreement with the trend expected from thermodynamic considerations. Most of the increase stems from the seasonality of the drivers acting on an increasing oceanic pCO2 caused by the uptake of anthropogenic CO2 from the atmosphere. In the high latitudes, the concurrent ocean-acidification-induced changes in the buffer capacity of the ocean enhance this effect. This strengthening of the seasonal winter-to-summer difference pushes the global ocean towards critical thresholds earlier, inducing stress to ocean ecosystems and fisheries4. Our study provides observational evidence for this strengthening seasonal difference in the oceanic carbon cycle on a global scale, illustrating the inevitable consequences of anthropogenic CO2 emissions.Uptake of anthropogenic CO2 changes the surface ocean inorganic carbon system. Analysis of observations shows an increase in the seasonal oceanic carbon cycle, amplifying the ocean acidification signal with implications for marine biota.

Incorporating a prognostic representation of marine nitrogen fixers into the global ocean biogeochemical model HAMOCC

Nitrogen (N2) fixation is a major source of bioavailable nitrogen to the euphotic zone, thereby exerting an important control on ocean biogeochemical cycling. This paper presents the incorporation of prognostic N2 fixers into the Hamburg Ocean Carbon Cycle model (HAMOCC), a component of the Max Planck Institute Earth System Model (MPI-ESM). Growth dynamics of N2 fixers in the model are based on physiological characteristics of the cyanobacterium Trichodesmium. The applied temperature dependency confines diazotrophic growth and N2 fixation to the tropical and subtropical ocean roughly between 40°S and 40°N. Simulated large scale spatial patterns compare well with observations, and the global N2 fixation rate of 135.6 Tg N yr−1 is within the range of current estimates. Also the vertical distribution of N2 fixation matches well the observations, with a major fraction of about 85% occurring in the upper 20 m. The observed seasonal variability at the stations BATS and ALOHA is reasonably reproduced, with highest fixation rates in northern summer/fall. Iron limitation was found to be an important factor in controlling the simulated distribution of N2 fixation, especially in the Pacific Ocean. The new model component considerably improves the representation of present-day N2 fixation in HAMOCC. It provides the basis for further studies on the role of diazotrophs in global biogeochemical cycles, as well as on the response of N2 fixation to changing environmental conditions. This article is protected by copyright. All rights reserved.

A Higher‐resolution Version of the Max Planck Institute Earth System Model (MPI‐ESM1.2‐HR)

The MPI‐ESM1.2 is the latest version of the Max Planck Institute Earth System Model and is the baseline for the Coupled Model Intercomparison Project Phase 6 and current seasonal and decadal climate predictions. This paper evaluates a coupled higher‐resolution version (MPI‐ESM1.2‐HR) in comparison with its lower‐resolved version (MPI‐ESM1.2‐LR). We focus on basic oceanic and atmospheric mean states and selected modes of variability, the El Nino/Southern Oscillation and the North Atlantic Oscillation. The increase in atmospheric resolution in MPI‐ESM1.2‐HR reduces the biases of upper‐level zonal wind and atmospheric jet stream position in the northern extratropics. This results in a decrease of the storm track bias over the northern North Atlantic, for both winter and summer season. The blocking frequency over the European region is improved in summer, and North Atlantic Oscillation and related storm track variations improve in winter. Stable Atlantic meridional overturning circulations are found with magnitudes of ~16 Sv for MPI‐ESM1.2‐HR and ~20 Sv for MPI‐ESM1.2‐LR at 26°N. A strong sea surface temperature bias of ~5°C along with a too zonal North Atlantic current is present in both versions. The sea surface temperature bias in the eastern tropical Atlantic is reduced by ~1°C due to higher‐resolved orography in MPI‐ESM‐HR, and the region of the cold‐tongue bias is reduced in the tropical Pacific. MPI‐ESM1.2‐HR has a well‐balanced radiation budget and its climate sensitivity is explicitly tuned to 3 K. Although the obtained reductions in long‐standing biases are modest, the improvements in atmospheric dynamics make this model well suited for prediction and impact studies.

Polychlorinated biphenyls (PCBs) as sentinels for the elucidation of Arctic environmental change processes: a comprehensive review combined with ArcRisk project results

Polychlorinated biphenyls (PCBs) can be used as chemical sentinels for the assessment of anthropogenic influences on Arctic environmental change. We present an overview of studies on PCBs in the Arctic and combine these with the findings from ArcRisk—a major European Union-funded project aimed at examining the effects of climate change on the transport of contaminants to and their behaviour of in the Arctic—to provide a case study on the behaviour and impact of PCBs over time in the Arctic. PCBs in the Arctic have shown declining trends in the environment over the last few decades. Atmospheric long-range transport from secondary and primary sources is the major input of PCBs to the Arctic region. Modelling of the atmospheric PCB composition and behaviour showed some increases in environmental concentrations in a warmer Arctic, but the general decline in PCB levels is still the most prominent feature. ‘Within-Arctic’ processing of PCBs will be affected by climate change-related processes such as changing wet deposition. These in turn will influence biological exposure and uptake of PCBs. The pan-Arctic rivers draining large Arctic/sub-Arctic catchments provide a significant source of PCBs to the Arctic Ocean, although changes in hydrology/sediment transport combined with a changing marine environment remain areas of uncertainty with regard to PCB fate. Indirect effects of climate change on human exposure, such as a changing diet will influence and possibly reduce PCB exposure for indigenous peoples. Body burdens of PCBs have declined since the 1980s and are predicted to decline further.