Extensive reduction of surface UV radiation since 1750 in world's populated regions

Human activity influences a wide range of components that affect the surface UV radiation levels, among them ozone at high latitudes. We calculate the effect of human-induced changes in the surface erythemally weighted ultra-violet radiation (UV-E) since 1750. We compare results from a radiative transfer model to surface UV-E radiation for year 2000 derived by satellite observations (from Total Ozone Mapping Spectroradiometer) and to ground based measurements at 14 sites. The model correlates well with the observations; the correlation coefficients are 0.97 and 0.98 for satellite and ground based measurements, respectively. In addition to the effect of changes in ozone, we also investigate the effect of changes in SO<sub>2</sub>, NO<sub>2</sub>, the direct and indirect effects of aerosols, albedo changes and aviation-induced contrails and cirrus. The results show an increase of surface UV-E in polar regions, most strongly in the Southern Hemisphere. Furthermore, our study also shows an extensive surface UV-E reduction over most land areas; a reduction up to 20% since 1750 is found in some industrialized regions. This reduction in UV-E over the industrial period is particularly large in highly populated regions

Optical properties in the UV and visible spectral region of organic acids relevant to tropospheric aerosols

International audienceRefractive and absorption indices in the UV and visible region of selected aqueous organic acids relevant to tropospheric aerosols are reported. The acids investigated are the aliphatic dicarboxylic acids oxalic, malonic, tartronic, succinic and glutaric acid. In addition we report data for pyruvic, pinonic, benzoic and phthalic acid. To cover a wide range of conditions we have investigated the aqueous organic acids at different concentrations spanning from highly diluted samples to concentrations close to saturation. The density of the investigated samples is reported and a parameterisation of the absorption and refractive index that allows the calculation of the optical constants of mixed aqueous organic acids at different concentrations is presented. The single scattering albedo is calculated for two size distributions using measured and a synthetic set of optical constants. The results show that tropospheric aerosols consisting of only these organic acids and water have a pure scattering effect

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

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

Quantifying black carbon from biomass burning by means of levoglucosan - A one-year time series at the Arctic observatory Zeppelin

Levoglucosan, a highly specific tracer of particulate matter from biomass burning, has been used to study the influence of residential wood burning, agricultural waste burning and Boreal forest fire emissions on the Arctic atmosphere black carbon (BC) concentration. A one-year time series from March 2008 to March 2009 of levoglucosan has been established at the Zeppelin observatory in the European Arctic. Elevated concentrations of levoglucosan in winter (mean: 1.02 ng/m3) compared to summer (mean: 0.13 ng/m3) were observed, resembling the seasonal variation seen for e.g. sulfate and BC. The mean concentration in the winter period was 2-3 orders of magnitude lower than typical values reported for European urban areas in winter, and 1-2 orders of magnitude lower than European rural background concentrations. Episodes of elevated levoglucosan concentration lasting from 1 to 6 days were more frequent in winter than in summer and peak values were higher, exceeding 10 ng/m3 at the most. Concentrations of elemental carbon from biomass burning (ECbb) were obtained by combining measured concentrations of levoglucosan and emission ratios of levoglucosan and EC for wildfires/agricultural fires and for residential wood burning. Neglecting chemical degradation by OH provides minimum levoglucosan concentrations, corresponding to a mean ECbb concentration of 3.7 +- 1.2 ng/m3 in winter (October-April) and 0.8 +- 0.3 ng/m3 in summer (May-September), or 8.8 +- 4.5% of the measured equivalent black carbon (EBC) concentration in winter and 6.1 +- 3.4% in summer. When accounting for chemical degradation of levoglucosan by OH, an upper estimate of 31-45% of EBC could be attributed to ECbb* (ECbb adjusted for chemical degradation) in winter, whereas no reliable (<100%) upper estimate could be provided for summer for the degradation rates applied. Hence, fossil fuel sources appear to dominate the European Arctic BC concentrations in winter, whereas the very wide range obtained for summer does not allow us to conclude upon this for the warm season. Calculations using the Lagrangian particle dispersion model FLEXPART show that the seasonal variation of the modeled ECbb (ECbb,m) concentration compared relatively well with observationally derived ECbb from agricultural fires/wildfires during summer, and residential wood burning in winter. The model overestimates by a factor of 2.2 in winter and 4.4 in summer when compared to the observationally derived mean ECbb concentration, which provides the minimum estimate, whereas it underestimates by a factor of 2.3-3.3 in winter and a factor of 4.5 in summer when compared to ECbb*, which provides the upper estimate. There are indications of too-low emissions of residential wood burning in northern Russia, a region of great importance with respect to observed concentrations of BC in the European Arctic

Very Strong Atmospheric Methane Growth in the 4 Years 2014–2017:Implications for the Paris Agreement

Atmospheric methane grew very rapidly in 2014 (12.7 ± 0.5 ppb/year), 2015 (10.1 ± 0.7 ppb/year), 2016 (7.0 ± 0.7 ppb/year), and 2017 (7.7 ± 0.7 ppb/year), at rates not observed since the 1980s. The increase in the methane burden began in 2007, with the mean global mole fraction in remote surface background air rising from about 1,775 ppb in 2006 to 1,850 ppb in 2017. Simultaneously the 13 C/ 12 C isotopic ratio (expressed as δ 13 C CH4 ) has shifted, has shifted, now trending negative for more than a decade. The causes of methane's recent mole fraction increase are therefore either a change in the relative proportions (and totals) of emissions from biogenic and thermogenic and pyrogenic sources, especially in the tropics and subtropics, or a decline in the atmospheric sink of methane, or both. Unfortunately, with limited measurement data sets, it is not currently possible to be more definitive. The climate warming impact of the observed methane increase over the past decade, if continued at >5 ppb/year in the coming decades, is sufficient to challenge the Paris Agreement, which requires sharp cuts in the atmospheric methane burden. However, anthropogenic methane emissions are relatively very large and thus offer attractive targets for rapid reduction, which are essential if the Paris Agreement aims are to be attained

Discrepancy between simulated and observed ethane and propane levels explained by underestimated fossil emissions

Ethane and propane are the most abundant non-methane hydrocarbons in the atmosphere. However, their emissions, atmospheric distribution, and trends in their atmospheric concentrations are insufficiently understood. Atmospheric model simulations using standard community emission inventories do not reproduce available measurements in the Northern Hemisphere. Here, we show that observations of pre-industrial and present-day ethane and propane can be reproduced in simulations with a detailed atmospheric chemistry transport model, provided that natural geologic emissions are taken into account and anthropogenic fossil fuel emissions are assumed to be two to three times higher than is indicated in current inventories. Accounting for these enhanced ethane and propane emissions results in simulated surface ozone concentrations that are 5–13% higher than previously assumed in some polluted regions in Asia. The improved correspondence with observed ethane and propane in model simulations with greater emissions suggests that the level of fossil (geologic + fossil fuel) methane emissions in current inventories may need re-evaluation

Historical total ozone radiative forcing derived from CMIP6 simulations

Radiative forcing (RF) time series for total ozone from 1850 up to the present day are calculated based on historical simulations of ozone from 10 climate models contributing to the Coupled Model Intercomparison Project Phase 6 (CMIP6). In addition, RF is calculated for ozone fields prepared as an input for CMIP6 models without chemistry schemes and from a chemical transport model simulation. A radiative kernel for ozone is constructed and used to derive the RF. The ozone RF in 2010 (2005–2014) relative to 1850 is 0.35 W m−2 [0.08–0.61] (5–95% uncertainty range) based on models with both tropospheric and stratospheric chemistry. One of these models has a negative present-day total ozone RF. Excluding this model, the present-day ozone RF increases to 0.39 W m−2 [0.27–0.51] (5–95% uncertainty range). The rest of the models have RF close to or stronger than the RF time series assessed by the Intergovernmental Panel on Climate Change in the fifth assessment report with the primary driver likely being the new precursor emissions used in CMIP6. The rapid adjustments beyond stratospheric temperature are estimated to be weak and thus the RF is a good measure of effective radiative forcing

Extensive release of methane from Arctic seabed west of Svalbard during summer 2014 does not influence the atmosphere

© 2016. American Geophysical Union. All Rights Reserved. We find that summer methane (CH4) release from seabed sediments west of Svalbard substantially increases CH4 concentrations in the ocean but has limited influence on the atmospheric CH4 levels. Our conclusion stems from complementary measurements at the seafloor, in the ocean, and in the atmosphere from land-based, ship and aircraft platforms during a summer campaign in 2014. We detected high concentrations of dissolved CH4 in the ocean above the seafloor with a sharp decrease above the pycnocline. Model approaches taking potential CH4 emissions from both dissolved and bubble-released CH4 from a larger region into account reveal a maximum flux compatible with the observed atmospheric CH4 mixing ratios of 2.4-3.8 nmol m-2 s-1. This is too low to have an impact on the atmospheric summer CH4 budget in the year 2014. Long-term ocean observatories may shed light on the complex variations of Arctic CH4 cycles throughout the year.The project MOCA- Methane Emissions from the Arctic OCean to the Atmosphere: Present and Future Climate Effects is funded by the Research Council of Norway, grant no.225814 CAGE – Centre for Arctic Gas Hydrate, Environment and Climate research work was supported by the Research Council of Norway through its Centres of Excellence funding scheme grant no. 223259. Nordic Center of Excellence eSTICC (eScience Tool for Investigating Climate Change in northern high latitudes) funded by Nordforsk, grant no. 57001