Emerging Asian aerosol patterns

Anthropogenic aerosol emissions over Asia are changing rapidly, both in composition and spatial distribution1. The Shared Socioeconomic Pathways (SSPs), potential narratives of development used by the Intergovernmental Panel for Climate Change in future projections, span a range of influences of aerosols on climate over the next decades. Several of these narratives project the continuation of a trend manifested in observations since 2010, with a clear dipole between South and East Asia. The patterns of radiative forcing that result from these distributions of aerosols will differ from those of the late 20th century. They may instigate large-scale atmospheric responses that could have wide ranging impacts on climate and society well beyond the aerosol source regions. South and East Asia are particularly vulnerable to climate change because of strong seasonal variations in precipitation, high average temperature, and very high population density. Therefore, any aerosol impacts on the strength or seasonal variations in monsoon rainfall, freshwater availability, or climate extremes, will incur large societal costs. We urge the scientific community to make definite progress towards understanding and quantifying the impacts of Asian aerosols and to tackle the potentially large regional and hemispheric implications of these emerging trends

Regional Aerosol Optical Properties and Radiative Impact of the Extreme Smoke Event in the European Arctic in Spring 2006

In spring 2006 a special meteorological situation occurred in the European Arctic region giving record high levels of air pollution. The synoptic situation resulted in extensive transport of pollution predominantly from agricultural fires in Eastern Europe into the Arctic region and record high air-pollution levels were measured at the Zeppelin observatory at Ni-Alesun(78deg 54'N, 11deg 53'E) in the period from 25 April to 12 May. In the present study we investigate the optical properties of the aerosols from this extreme event and we estimate the radiative forcing of this episode. We examine the aerosol optical properties from the source region and into the European Arctic and explore the evolution of the episode and the changes in the optical properties. A number of sites in Eastern Europe, Northern Scandinavia and Svalbard are included in the study. In addition to AOD measurements, we explored lidar measurements from Minsk, ALOMAR (Arctic Lidar Observatory for Middle Atmosphere Research at Andenes) and Ny-Alesund. For the AERONET sites included (Minsk, Toravere, Hornsund) we have further studied the evolution of the aerosol size. Importantly, at Svalbard it is consistency between the AERONET measurements and calculations of single scattering albedo based on aerosol chemical composition. We have found strong agreement between the satellite dally MODIS AOD and the ground-based AOD observations. This agreement is crucial for the radiative forcing calculations. We calculate a strong negative radiative forcing for the most polluted days employing the analysed ground based data, MODIS AOD and a multi-stream model for radiative transfer of solar radiation

Observation of ultrafast intersystem crossing in thymine by extreme ultraviolet time-resolved photoelectron spectroscopy

We studied the photoinduced ultrafast relaxation dynamics of the nucleobase thymine using gas-phase time-resolved photoelectron spectroscopy. By employing extreme ultraviolet pulses from high harmonic generation for photoionization, we substantially extend our spectral observation window with respect to previous studies. This enables us to follow relaxation of the excited state population all the way to low-lying electronic states including the ground state. In thymine, we observe relaxation from the optically bright1IIII* state of thymine to a dark1nII* state within 80 ± 30 fs. The1nII* state relaxes further within 3.5 ± 0.3 ps to a low-lying electronic state. By comparison with quantum chemical simulations, we can unambiguously assign its spectroscopic signature to the3IIII* state. Hence, our study draws a comprehensive picture of the relaxation mechanism of thymine including ultrafast intersystem crossing to the triplet manifold

An investigation into linearity with cumulative emissions of the climate and carbon cycle response in HadCM3LC

We investigate the extent to which global mean temperature, precipitation, and the carbon cycle are constrained by cumulative carbon emissions throughout four experiments with a fully coupled climate-carbon cycle model. The two paired experiments adopt contrasting, idealised approaches to climate change mitigation at different action points this century, with total emissions exceeding two trillion tonnes of carbon in the later pair. Their initially diverging cumulative emissions trajectories cross after several decades, before diverging again. We find that their global mean temperatures are, to first order, linear with cumulative emissions, though regional differences in temperature of up to 1.5K exist when cumulative emissions of each pair coincide. Interestingly, although the oceanic precipitation response scales with cumulative emissions, the global precipitation response does not, due to a decrease in precipitation over land above cumulative emissions of around one trillion tonnes of carbon (TtC). Most carbon fluxes and stores are less well constrained by cumulative emissions as they reach two trillion tonnes. The opposing mitigation approaches have different consequences for the Amazon rainforest, which affects the linearity with which the carbon cycle responds to cumulative emissions. Averaged over the two fixed-emissions experiments, the transient response to cumulative carbon emissions (TCRE) is 1.95 K TtC-1, at the upper end of the IPCC’s range of 0.8-2.5 K TtC-1

Biomarkers in monitoring - a review

Årsliste 2006Biological effects are increasingly used to monitor impacts of contaminants in marine ecosystems. Biomarkers have been defined as ”biochemical, cellular, physiological or behavioural variations in the tissue or body fluids or at the level of whole organism that provide evidence of exposure to chemical pollutants, and may also indicate a toxic effect”. The biomarkers reviewed here were PAH bile metabolites, cytochrome P4501A, glutathione S-transferase, markers for DNA damage (adducts, alkaline unwinding, Comet assay), micronucleus formation, peroxisomal proliferation, acetyl cholinesterase inhibition, metallothionein, vitellogenin and delta-aminolevulinic acid dehydratase. Focus for the review was dose-response relationships, confounding factors, links to population effects, baseline values, assessment criteria and quality assurance for the relevant biomarker. Whereas correlative links to population-relevant effects have been found for some biomarkers, e.g. biomarkers for DNA damage, most biomarkers are generally more useful as markers for possible impacts elsewhere in ecosystems.OL

TRADEOFFs in climate effects through aircraft routing: forcing due to radiatively active gases

We have estimated impacts of alternative aviation routings on the radiative forcing. Changes in ozone and OH have been estimated in four Chemistry Transport Models (CTMs) participating in the TRADEOFF project. Radiative forcings due to ozone and methane have been calculated accordingly. In addition radiative forcing due to CO2 is estimated based on fuel consumption. Three alternative routing cases are investigated; one scenario assuming additional polar routes and two scenarios assuming aircraft cruising at higher (+2000 ft) and lower (−6000 ft) altitudes. Results from the base case in year 2000 are included as a reference. Taking first a steady state backward looking approach, adding the changes in the forcing from ozone, CO2 and CH4, the ranges of the models used in this work are −0.8 to −1.8 and 0.3 to 0.6 m Wm−2 in the lower (−6000 ft) and higher (+2000 ft) cruise levels, respectively. In relative terms, flying 6000ft lower reduces the forcing by 5–10% compared to the current flight pattern, whereas flying higher, while saving fuel and presumably flying time, increases the forcing by about 2–3%. Taking next a forward looking approach we have estimated the integrated forcing (m Wm−2 yr) over 20 and 100 years time horizons. The relative contributions from each of the three climate gases are somewhat different from the backward looking approach. The differences are moderate adopting 100 year time horizon, whereas under the 20 year horizon CO2 naturally becomes less important relatively. Thus the forcing agents impact climate differently on various time scales. Also, we have found significant differences between the models for ozone and methane. We conclude that we are not yet at a point where we can include non-CO2 effects of aviation in emission trading schemes. Nevertheless, the rerouting cases that have been studied here yield relatively small changes in the radiative forcing due to the radiatively active gases

Radiative forcing in the 21st century due to ozone changes in the troposphere and the lower stratosphere

Radiative forcing due to changes in ozone is expected for the 21st century. An assessment on changes in the tropospheric oxidative state through a model intercomparison ("OxComp'') was conducted for the IPCC Third Assessment Report (IPCC-TAR). OxComp estimated tropospheric changes in ozone and other oxidants during the 21st century based on the "SRES'' A2p emission scenario. In this study we analyze the results of 11 chemical transport models (CTMs) that participated in OxComp and use them as input for detailed radiative forcing calculations. We also address future ozone recovery in the lower stratosphere and its impact on radiative forcing by applying two models that calculate both tropospheric and stratospheric changes. The results of OxComp suggest an increase in global-mean tropospheric ozone between 11.4 and 20.5 DU for the 21st century, representing the model uncertainty range for the A2p scenario. As the A2p scenario constitutes the worst case proposed in IPCC-TAR we consider these results as an upper estimate. The radiative transfer model yields a positive radiative forcing ranging from 0.40 to 0.78 W m(-2) on a global and annual average. The lower stratosphere contributes an additional 7.5-9.3 DU to the calculated increase in the ozone column, increasing radiative forcing by 0.15-0.17 W m(-2). The modeled radiative forcing depends on the height distribution and geographical pattern of predicted ozone changes and shows a distinct seasonal variation. Despite the large variations between the 11 participating models, the calculated range for normalized radiative forcing is within 25%, indicating the ability to scale radiative forcing to global-mean ozone column change

Concentrations and radiative forcing of anthropogenic aerosols from 1750 to 2014 simulated with the Oslo CTM3 and CEDS emission inventory

We document the ability of the new-generation Oslo chemistry-transport model, Oslo CTM3, to accurately simulate present-day aerosol distributions. The model is then used with the new Community Emission Data System (CEDS) historical emission inventory to provide updated time series of anthropogenic aerosol concentrations and consequent direct radiative forcing (RFari) from 1750 to 2014.Overall, Oslo CTM3 performs well compared with measurements of surface concentrations and remotely sensed aerosol optical depth. Concentrations are underestimated in Asia, but the higher emissions in CEDS than previous inventories result in improvements compared to observations. The treatment of black carbon (BC) scavenging in Oslo CTM3 gives better agreement with observed vertical BC profiles relative to the predecessor Oslo CTM2. However, Arctic wintertime BC concentrations remain underestimated, and a range of sensitivity tests indicate that better physical understanding of processes associated with atmospheric BC processing is required to simultaneously reproduce both the observed features. Uncertainties in model input data, resolution, and scavenging affect the distribution of all aerosols species, especially at high latitudes and altitudes. However, we find no evidence of consistently better model performance across all observables and regions in the sensitivity tests than in the baseline configuration.Using CEDS, we estimate a net RFari in 2014 relative to 1750 of −0.17&thinsp;W&thinsp;m−2, significantly weaker than the IPCC AR5 2011–1750 estimate. Differences are attributable to several factors, including stronger absorption by organic aerosol, updated parameterization of BC absorption, and reduced sulfate cooling. The trend towards a weaker RFari over recent years is more pronounced than in the IPCC AR5, illustrating the importance of capturing recent regional emission changes.</p

Organic aerosol and global climate modelling: a review

The present paper reviews existing knowledge with regard to Organic Aerosol (OA) of importance for global climate modelling and defines critical gaps needed to reduce the involved uncertainties. All pieces required for the representation of OA in a global climate model are sketched out with special attention to Secondary Organic Aerosol (SOA): The emission estimates of primary carbonaceous particles and SOA precursor gases are summarized. The up-to-date understanding of the chemical formation and transformation of condensable organic material is outlined. Knowledge on the hygroscopicity of OA and measurements of optical properties of the organic aerosol constituents are summarized. The mechanisms of interactions of OA with clouds and dry and wet removal processes parameterisations in global models are outlined. This information is synthesized to provide a continuous analysis of the flow from the emitted material to the atmosphere up to the point of the climate impact of the produced organic aerosol. The sources of uncertainties at each step of this process are highlighted as areas that require further studies