Found 10000 publications. Showing page 313 of 400:
2019
Polycyclic Aromatic Hydrocarbons Not Declining in Arctic Air Despite Global Emission Reduction
Two decades of atmospheric measurements of polycyclic aromatic hydrocarbons (PAHs) were conducted at three Arctic sites, i.e., Alert, Canada; Zeppelin, Svalbard; and Pallas, Finland. PAH concentrations decrease with increasing latitude in the order of Pallas > Zeppelin > Alert. Forest fire was identified as an important contributing source. Three representative PAHs, phenanthrene (PHE), pyrene (PYR), and benzo[a]pyrene (BaP) were selected for the assessment of their long-term trends. Significant decline of these PAHs was not observed contradicting the expected decline due to PAH emission reductions. A global 3-D transport model was employed to simulate the concentrations of these three PAHs at the three sites. The model predicted that warming in the Arctic would cause the air concentrations of PHE and PYR to increase in the Arctic atmosphere, while that of BaP, which tends to be particle-bound, is less affected by temperature. The expected decline due to the reduction of global PAH emissions is offset by the increment of volatilization caused by warming. This work shows that this phenomenon may affect the environmental occurrence of other anthropogenic substances, such as more volatile flame retardants and pesticides.
2019
2019
Monitoring Soil Moisture Drought over Northern High Latitudes from Space
Mapping drought from space using, e.g., surface soil moisture (SSM), has become viable in the last decade. However, state of the art SSM retrieval products suffer from very poor coverage over northern latitudes. In this study, we propose an innovative drought indicator with a wider spatial and temporal coverage than that obtained from satellite SSM retrievals. We evaluate passive microwave brightness temperature observations from the Soil Moisture and Ocean Salinity (SMOS) satellite as a surrogate drought metric, and introduce a Standardized Brightness Temperature Index (STBI). We compute the STBI by fitting a Gaussian distribution using monthly brightness temperature data from SMOS; the normal assumption is tested using the Shapior-Wilk test. Our results indicate that the assumption of normally distributed brightness temperature data is valid at the 0.05 significance level. The STBI is validated against drought indices from a land surface data assimilation system (LDAS-Monde), two satellite derived SSM indices, one from SMOS and one from the ESA CCI soil moisture project and a standardized precipitation index based on in situ data from the European Climate Assessment & Dataset (ECA&D) project. When comparing the temporal dynamics of the STBI to the LDAS-Monde drought index we find that it has equal correlation skill to that of the ESA CCI soil moisture product ( 0.71 ). However, in addition the STBI provides improved spatial coverage because no masking has been applied over regions with dense boreal forest. Finally, we evaluate the STBI in a case study of the 2018 Nordic drought. The STBI is found to provide improved spatial and temporal coverage when compared to the drought index created from satellite derived SSM over the Nordic region. Our results indicate that when compared to drought indices from precipitation data and a land data assimilation system, the STBI is qualitatively able to capture the 2018 drought onset, severity and spatial extent. We did see that the STBI was unable to detect the 2018 drought recovery for some areas in the Nordic countries. This false drought detection is likely linked to the recovery of vegetation after the drought, which causes an increase in the passive microwave brightness temperature, hence the STBI shows a dry anomaly instead of normal conditions, as seen for the other drought indices. We argue that the STBI could provide additional information for drought monitoring in regions where the SSM retrieval problem is not well defined. However, it then needs to be accompanied by a vegetation index to account for the recovery of the vegetation which could cause false drought detection.
2019
2019
Two years of continuous in situ measurements of Arctic low‐level clouds have been made at the Mount Zeppelin Observatory (78°56′N, 11°53′E), in Ny‐Ålesund, Spitsbergen. The monthly median value of the cloud particle number concentration (Nc) showed a clear seasonal variation: Its maximum appeared in May–July (65 ± 8 cm−3), and it remained low between October and March (8 ± 7 cm−3). At temperatures warmer than 0 °C, a clear correlation was found between the hourly Nc values and the number concentrations of aerosols with dry diameters larger than 70 nm (N70), which are proxies for cloud condensation nuclei (CCN). When clouds were detected at temperatures colder than 0 °C, some of the data followed the summertime Nc to N70 relationship, while other data showed systematically lower Nc values. The lidar‐derived depolarization ratios suggested that the former (CCN‐controlled) and latter (CCN‐uncontrolled) data generally corresponded to clouds consisting of supercooled water droplets and those containing ice particles, respectively. The CCN‐controlled data persistently appeared throughout the year at Zeppelin. The aerosol‐cloud interaction index (ACI = dlnNc/(3dlnN70)) for the CCN‐controlled data showed high sensitivities to aerosols both in the summer (clean air) and winter–spring (Arctic haze) seasons (0.22 ± 0.03 and 0.25 ± 0.02, respectively). The air parcel model calculations generally reproduced these values. The threshold diameters of aerosol activation (Dact), which account for the Nc of the CCN‐controlled data, were as low as 30–50 nm when N70 was less than 30 cm−3, suggesting that new particle formation can affect Arctic cloud microphysics.
2019
The comet assay applied to HepG2 liver spheroids
In accordance with the 3 Rs to reduce in vivo testing, more advanced in vitro models, moving from 2D monolayer to 3D cultures, should be developed for prediction of human toxicity of industrial chemicals and environmental pollutants. In this study we compared cytotoxic and genotoxic responses induced by chemicals in 2D and 3D spheroidal cultures of the human liver cancer cell line HepG2.
HepG2 spheroids were prepared by hanging drop technology. Both 3D spheroids and 2D monolayer cultures were exposed to different chemicals (colchicine, chlorpromazine hydrochloride or methyl methanesulfonate) for geno- and cytotoxicity studies. Cytotoxicity was investigated by alamarBlue assay, flow cytometry and confocal imaging. DNA damage was investigated by the comet assay with and without Fpg enzyme for detection of DNA strand breaks and oxidized or alkylated base lesions.
The results from the cyto- and genotoxicity tests showed differences in sensitivity comparing the 2D and 3D HepG2 models. This study shows that human 3D spheroidal hepatocellular cultures can be successfully applied for genotoxicity testing by the comet assay and represent a promising advanced in vitro model for toxicity testing.
2019
This paper reports estimated maintenance-cleaning costs, cost savings and cleaning interval increases for structural surfaces and windows in Europe obtainable by reducing the air pollution. Methodology and data from the ICP-materials project were used. The average present (2018) cleaning costs for sheltered white painted steel surfaces and modern glass due to air pollution over background, was estimated to be ~2.5 Euro/m2∙year. Hypothetical 50% reduction in the air pollution was found to give savings in these cleaning costs of ~1.5 Euro/m2∙year. Observed reduction in the air pollution, from 2002–2005 until 2011–2014, have probably increased the cleaning interval for white painted steel with ~100% (from 12 to 24 years), representing reductions in the single intervention cleaning costs from 7 to 4%/year (= % of one cleaning investment, per year during the cleaning interval) and for the modern glass with ~65% (from 0.85 to 1.3 years), representing reductions in the cleaning cost from 124 to 95%/year. The cleaning cost reductions, obtainable by 50% reduction in air pollution, would have been ~3 %/year for white painted steel and ~60%/year for the modern glass, representing ~100 and 50% additional cleaning interval increases. These potential cleaning cost savings are significantly higher than previously reported for the weathering of Portland limestone ornament and zinc monuments.
2019
There is little information to decision support in air traffic management in case of nuclear releases into the atmosphere. In this paper, the dose estimation due to both, external exposure (i.e. cloud immersion, deposition inside and outside the aircraft), and due to internal exposure (i.e, inhalation of radionuclides inside the aircraft) to passengers and crew is calculated for a worst-case emergency scenario. The doses are calculated for different radionuclides and activities. Calculations are mainly considered according to International Commission on Radiological Protection (ICRP) recommendations and Monte Carlo simulations. In addition, a discussion on potential detectors installed inside the aircraft for monitoring the aerosol concentration and the ambient dose equivalent rate, H*(10), for during-flight monitoring and early warning is provided together with the evaluation of a response of a generic detector. The results show that the probability that a catastrophic nuclear accident would produce significant radiological doses to the passengers and crew of an aircraft is very low. In the worst-case scenarios studied, the maximum estimated effective dose was about 1 mSv during take-off or landing operations, which is the recommended yearly threshold for the public. However, in order to follow the ALARA (As Low As Reasonably Achievable) criteria and to avoid aircraft contamination, the installation of radiological detectors is considered. This would, on one hand help the pilot or corresponding decision maker to decide about the potential change of the route and, on the other, allow for gathering of 4D data for future studies.
2019
2019
2019
Frequency of extreme precipitation increases extensively with event rareness under global warming
The intensity of the heaviest extreme precipitation events is known to increase with global warming. How often such events occur in a warmer world is however less well established, and the combined effect of changes in frequency and intensity on the total amount of rain falling as extreme precipitation is much less explored, in spite of potentially large societal impacts. Here, we employ observations and climate model simulations to document strong increases in the frequencies of extreme precipitation events occurring on decadal timescales. Based on observations we find that the total precipitation from these intense events almost doubles per degree of warming, mainly due to changes in frequency, while the intensity changes are relatively weak, in accordance to previous studies. This shift towards stronger total precipitation from extreme events is seen in observations and climate models, and increases with the strength – and hence the rareness – of the event. Based on these results, we project that if historical trends continue, the most intense precipitation events observed today are likely to almost double in occurrence for each degree of further global warming. Changes to extreme precipitation of this magnitude are dramatically stronger than the more widely communicated changes to global mean precipitation.
2019
Diurnal cycle of iodine, bromine, and mercury concentrations in Svalbard surface snow
Sunlit snow is highly photochemically active and plays a key role in the exchange of gas phase species between the cryosphere and the atmosphere. Here, we investigate the behaviour of two selected species in surface snow: mercury (Hg) and iodine (I). Hg can deposit year-round and accumulate in the snowpack. However, photo-induced re-emission of gas phase Hg from the surface has been widely reported. Iodine is active in atmospheric new particle formation, especially in the marine boundary layer, and in the destruction of atmospheric ozone. It can also undergo photochemical re-emission. Although previous studies indicate possible post-depositional processes, little is known about the diurnal behaviour of these two species and their interaction in surface snow. The mechanisms are still poorly constrained, and no field experiments have been performed in different seasons to investigate the magnitude of re-emission processes Three sampling campaigns conducted at an hourly resolution for 3 d each were carried out near Ny-Ålesund (Svalbard) to study the behaviour of mercury and iodine in surface snow under different sunlight and environmental conditions (24 h darkness, 24 h sunlight and day–night cycles). Our results indicate a different behaviour of mercury and iodine in surface snow during the different campaigns. The day–night experiments demonstrate the existence of a diurnal cycle in surface snow for Hg and iodine, indicating that these species are indeed influenced by the daily solar radiation cycle. Differently, bromine did not show any diurnal cycle. The diurnal cycle also disappeared for Hg and iodine during the 24 h sunlight period and during 24 h darkness experiments supporting the idea of the occurrence (absence) of a continuous recycling or exchange at the snow–air interface. These results demonstrate that this surface snow recycling is seasonally dependent, through sunlight. They also highlight the non-negligible role that snowpack emissions have on ambient air concentrations and potentially on iodine-induced atmospheric nucleation processes.
2019
2019
Physical controls of dynamics of methane venting from a shallow seep area west of Svalbard
We investigate methane seepage on the shallow shelf west of Svalbard during three consecutive years, using discrete sampling of the water column, echosounder-based gas flux estimates, water mass properties, and numerical dispersion modelling. The results reveal three distinct hydrographic conditions in spring and summer, showing that the methane content in the water column is controlled by a combination of free gas seepage intensity and lateral water mass movements, which disperse and displace dissolved methane horizontally away from the seeps. Horizontal dispersion and displacement of dissolved methane are promoted by eddies originating from the West Spitsbergen Current and passing over the shallow shelf, a process that is more intense in winter and spring than in the summer season. Most of the methane injected from seafloor seeps resides in the bottom layer even when the water column is well mixed, implying that the controlling effect of water column stratification on vertical methane transport is small. Only small concentrations of methane are found in surface waters, and thus the escape of methane into the atmosphere above the site of seepage is also small. The magnitude of the sea to air methane flux is controlled by wind speed, rather than by the concentration of dissolved methane in the surface ocean.
2019
The Lagrangian particle dispersion model FLEXPART version 10.4
The Lagrangian particle dispersion model FLEXPART in its original version in the mid-1990s was designed for calculating the long-range and mesoscale dispersion of hazardous substances from point sources, such as those released after an accident in a nuclear power plant. Over the past decades, the model has evolved into a comprehensive tool for multi-scale atmospheric transport modeling and analysis and has attracted a global user community. Its application fields have been extended to a large range of atmospheric gases and aerosols, e.g., greenhouse gases, short-lived climate forcers like black carbon and volcanic ash, and it has also been used to study the atmospheric branch of the water cycle. Given suitable meteorological input data, it can be used for scales from dozens of meters to global. In particular, inverse modeling based on source–receptor relationships from FLEXPART has become widely used. In this paper, we present FLEXPART version 10.4, which works with meteorological input data from the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS) and data from the United States National Centers of Environmental Prediction (NCEP) Global Forecast System (GFS). Since the last publication of a detailed FLEXPART description (version 6.2), the model has been improved in different aspects such as performance, physicochemical parameterizations, input/output formats, and available preprocessing and post-processing software. The model code has also been parallelized using the Message Passing Interface (MPI). We demonstrate that the model scales well up to using 256 processors, with a parallel efficiency greater than 75 % for up to 64 processes on multiple nodes in runs with very large numbers of particles. The deviation from 100 % efficiency is almost entirely due to the remaining nonparallelized parts of the code, suggesting large potential for further speedup. A new turbulence scheme for the convective boundary layer has been developed that considers the skewness in the vertical velocity distribution (updrafts and downdrafts) and vertical gradients in air density. FLEXPART is the only model available considering both effects, making it highly accurate for small-scale applications, e.g., to quantify dispersion in the vicinity of a point source. The wet deposition scheme for aerosols has been completely rewritten and a new, more detailed gravitational settling parameterization for aerosols has also been implemented. FLEXPART has had the option of running backward in time from atmospheric concentrations at receptor locations for many years, but this has now been extended to also work for deposition values and may become useful, for instance, for the interpretation of ice core measurements. To our knowledge, to date FLEXPART is the only model with that capability. Furthermore, the temporal variation and temperature dependence of chemical reactions with the OH radical have been included, allowing for more accurate simulations for species with intermediate lifetimes against the reaction with OH, such as ethane. Finally, user settings can now be specified in a more flexible namelist format, and output files can be produced in NetCDF format instead of FLEXPART's customary binary format. In this paper, we describe these new developments. Moreover, we present some tools for the preparation of the meteorological input data and for processing FLEXPART output data, and we briefly report on alternative FLEXPART versions.
2019
2019
We present here emissions estimated from a newly developed emission model for residential wood combustion (RWC) at high spatial and temporal resolution, which we name the MetVed model. The model estimates hourly emissions resolved on a 250 m grid resolution for several compounds, including particulate matter (PM), black carbon (BC) and polycyclic aromatic hydrocarbons (PAHs) in Norway for a 12-year period. The model uses novel input data and calculation methods that combine databases built with an unprecedented high level of detail and near-national coverage. The model establishes wood burning potential at the grid based on the dependencies between variables that influence emissions: i.e. outdoor temperature, number of and type and size of dwellings, type of available heating technologies, distribution of wood-based heating installations and their associated emission factors. RWC activity with a 1 h temporal profile was produced by combining heating degree day and hourly and weekday activity profiles reported by wood consumers in official statistics. This approach results in an improved characterisation of the spatio-temporal distribution of wood use, and subsequently of emissions, required for urban air quality assessments. Whereas most variables are calculated based on bottom-up approaches on a 250 m spatial grid, the MetVed model is set up to use official wood consumption at the county level and then distributes consumption to individual grids proportional to the physical traits of the residences within it. MetVed combines consumption with official emission factors that makes the emissions also upward scalable from the 250 m grid to the national level.
The MetVed spatial distribution obtained was compared at the urban scale to other existing emissions at the same scale. The annual urban emissions, developed according to different spatial proxies, were found to have differences up to an order of magnitude. The MetVed total annual PM2.5 emissions in the urban domains compare well to emissions adjusted based on concentration measurements. In addition, hourly PM2.5 concentrations estimated by an Eulerian dispersion model using MetVed emissions were compared to measurements at air quality stations. Both hourly daily profiles and the seasonality of PM2.5 show a slight overestimation of PM2.5 levels. However, a comparison with black carbon from biomass burning and benzo(a)pyrene measurements indicates higher emissions during winter than that obtained by MetVed. The accuracy of urban emissions from RWC relies on the accuracy of the wood consumption (activity data), emission factors and the spatio-temporal distribution. While there are still knowledge gaps regarding emissions, MetVed represents a vast improvement in the spatial and temporal distribution of RWC.
2019
2019
The aim of this work was to assess how improvements to the indoor environment could affect the future condition, frequency and costs of major conservation-cleaning campaigns on the monumental paintings (1909–1916) by Edvard Munch, centrally located in the Aula assembly hall of the University of Oslo. A lower soiling rate is expected to reduce the need for frequent and major cleaning campaigns. Estimations were performed using the freely available NILU-EnvCul web-model. The conservation of these large, mostly unvarnished, oil paintings is challenging, and it is important to understand the potential benefits of preventive conservation measures. The results from the model suggested benefits from preventive conservation in protecting the paintings, and as a cost-efficient strategy to reduce the soiling and cleaning frequency. The model results indicated that an improvement in the indoor air quality in the Aula, of 50–80% as compared to the 1916–2009 average, would increase the time until the next similar major conservation cleaning campaign from approximately 45 years to between about 85 and 165 years. This should give a 45–70% reduction in the respective conservation costs. This saving was probably initiated by improvements in the recent past, before the last Aula campaign in 2009–11.
2019
This paper describes the CityChem extension of the Eulerian urban dispersion model EPISODE. The development of the CityChem extension was driven by the need to apply the model in largely populated urban areas with highly complex pollution sources of particulate matter and various gaseous pollutants. The CityChem extension offers a more advanced treatment of the photochemistry in urban areas and entails specific developments within the sub-grid components for a more accurate representation of dispersion in proximity to urban emission sources. Photochemistry on the Eulerian grid is computed using a numerical chemistry solver. Photochemistry in the sub-grid components is solved with a compact reaction scheme, replacing the photo-stationary-state assumption. The simplified street canyon model (SSCM) is used in the line source sub-grid model to calculate pollutant dispersion in street canyons. The WMPP (WORM Meteorological Pre-Processor) is used in the point source sub-grid model to calculate the wind speed at plume height. The EPISODE–CityChem model integrates the CityChem extension in EPISODE, with the capability of simulating the photochemistry and dispersion of multiple reactive pollutants within urban areas. The main focus of the model is the simulation of the complex atmospheric chemistry involved in the photochemical production of ozone in urban areas. The ability of EPISODE–CityChem to reproduce the temporal variation of major regulated pollutants at air quality monitoring stations in Hamburg, Germany, was compared to that of the standard EPISODE model and the TAPM (The Air Pollution Model) air quality model using identical meteorological fields and emissions. EPISODE–CityChem performs better than EPISODE and TAPM for the prediction of hourly NO2 concentrations at the traffic stations, which is attributable to the street canyon model. Observed levels of annual mean ozone at the five urban background stations in Hamburg are captured by the model within ±15 %. A performance analysis with the FAIRMODE DELTA tool for air quality in Hamburg showed that EPISODE–CityChem fulfils the model performance objectives for NO2 (hourly), O3 (daily max. of the 8 h running mean) and PM10 (daily mean) set forth in the Air Quality Directive, qualifying the model for use in policy applications. Envisaged applications of the EPISODE–CityChem model are urban air quality studies, emission control scenarios in relation to traffic restrictions and the source attribution of sector-specific emissions to observed levels of air pollutants at urban monitoring stations.
2019
In the present study, concentrations of legacy and emerging contaminants were determined in three non-destructive matrices (plasma, preen oil and body feathers) of northern goshawk (Accipiter gentilis) nestlings. Persistent organic pollutants (POPs), including polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs) and polybrominated diphenyl ethers (PBDEs), together with emerging pollutants, including per- and polyfluorinated alkyl substances (PFASs), novel brominated flame retardants (NBFRs), phosphorus flame retardants (PFRs) and Dechlorane Plus isomers (DPs) were targeted. Plasma, preen oil and feather samples were collected from 61 goshawk nestlings in Norway (Trøndelag and Troms) in 2015 and 2016, and pollutant concentrations were compared between the three matrices. In plasma, PFASs were detected in the highest concentrations, ranging between 1.37 and 36.0 ng/mL, which suggests that the nestlings were recently and continuously exposed to these emerging contaminants, likely through dietary input. In preen oil, OCPs (169–3560 ng/g) showed the highest concentrations among the investigated compounds, consistent with their high lipophilicity. PFRs (2.60–314 ng/g) were the dominant compounds in feathers and are thought to originate mainly from external deposition, as they were not detected in the other two matrices. NBFRs and DPs were generally not detected in the nestlings, suggesting low presence of these emerging contaminants in their environment and/or low absorption. Strong and significant correlations between matrices were found for all POPs (rs = 0.46–0.95, p < 0.001), except for hexachlorobenzene (HCB, rs = 0.20, p = 0.13). Correlations for PFASs were less conclusive: linear perfluorooctane sulfonate (PFOS), perfluoroundecanoate (PFUnA), perfluorododecanoate (PFDoA) and perfluorotetradecanoate (PFTeA) showed strong and significant correlations between plasma and feathers (rs = 0.42–0.72, p < 0.02), however no correlation was found for perfluorohexane sulfonate (PFHxS), perfluorononanoate (PFNA) and perfluorotridecanoate (PFTriA) (rs = 0.05–0.33, p = 0.09–0.85). A lack of consistency between the PFAS compounds (contrary to POPs), and between studies, prevents concluding on the suitability of the investigated matrices for PFAS biomonitoring.
2019
Perfluorocyclobutane (PFC-318, c-C4F8) in the global atmosphere
We reconstruct atmospheric abundances of the potent greenhouse gas c-C4F8 (perfluorocyclobutane, perfluorocarbon PFC-318) from measurements of in situ, archived, firn, and aircraft air samples with precisions of ∼1 %–2 % reported on the SIO-14 gravimetric calibration scale. Combined with inverse methods, we found near-zero atmospheric abundances from the early 1900s to the early 1960s, after which they rose sharply, reaching 1.66 ppt (parts per trillion dry-air mole fraction) in 2017. Global c-C4F8 emissions rose from near zero in the 1960s to 1.2±0.1 (1σ) Gg yr−1 in the late 1970s to late 1980s, then declined to 0.77±0.03 Gg yr−1 in the mid-1990s to early 2000s, followed by a rise since the early 2000s to 2.20±0.05 Gg yr−1 in 2017. These emissions are significantly larger than inventory-based emission estimates. Estimated emissions from eastern Asia rose from 0.36 Gg yr−1 in 2010 to 0.73 Gg yr−1 in 2016 and 2017, 31 % of global emissions, mostly from eastern China. We estimate emissions of 0.14 Gg yr−1 from northern and central India in 2016 and find evidence for significant emissions from Russia. In contrast, recent emissions from northwestern Europe and Australia are estimated to be small (≤1 % each). We suggest that emissions from China, India, and Russia are likely related to production of polytetrafluoroethylene (PTFE, “Teflon”) and other fluoropolymers and fluorochemicals that are based on the pyrolysis of hydrochlorofluorocarbon HCFC-22 (CHClF2) in which c-C4F8 is a known by-product. The semiconductor sector, where c-C4F8 is used, is estimated to be a small source, at least in South Korea, Japan, Taiwan, and Europe. Without an obvious correlation with population density, incineration of waste-containing fluoropolymers is probably a minor source, and we find no evidence of emissions from electrolytic production of aluminum in Australia. While many possible emissive uses of c-C4F8 are known and though we cannot categorically exclude unknown sources, the start of significant emissions may well be related to the advent of commercial PTFE production in 1947. Process controls or abatement to reduce the c-C4F8 by-product were probably not in place in the early decades, explaining the increase in emissions in the 1960s and 1970s. With the advent of by-product reporting requirements to the United Nations Framework Convention on Climate Change (UNFCCC) in the 1990s, concern about climate change and product stewardship, abatement, and perhaps the collection of c-C4F8 by-product for use in the semiconductor industry where it can be easily abated, it is conceivable that emissions in developed countries were stabilized and then reduced, explaining the observed emission reduction in the 1980s and 1990s. Concurrently, production of PTFE in China began to increase rapidly. Without emission reduction requirements, it is plausible that global emissions today are dominated by China and other developing countries. We predict that c-C4F8 emissions will continue to rise and that c-C4F8 will become the second most important emitted PFC in terms of CO2-equivalent emissions within a year or two. The 2017 radiative forcing of c-C4F8 (0.52 mW m−2) is small but emissions of c-C4F8 and other PFCs, due to their very long atmospheric lifetimes, essentially permanently alter Earth's radiative budget and should be reduced. Significant emissions inferred outside of the investigated regions clearly show that observational capabilities and reporting requirements need to be improved to understand global and country-scale emissions of PFCs and other synthetic greenhouse gases and ozone-depleting substances.
2019
Snow initialization has been previously investigated as a potential source of predictability atthe subseasonal‐to‐seasonal (S2S) timescale in winter and spring, through its local radiative,thermodynamical, and hydrological feedbacks. However, previous studies were conducted with low‐topmodels over short periods only. Furthermore, the potential role of the land surface‐stratosphere connectionupon the S2S predictability had remained unclear. To this end, we have carried out twin 30‐memberensembles of 2‐month (November and December) retrospective forecasts over the period 1985–2016, witheither realistic or degraded snow initialization. A high‐top version of the Norwegian Climate PredictionModel is used, based on the Whole Atmosphere Community Climate Model, to insure improved couplingwith the stratosphere. In a composite difference of high versus low initial Eurasian snow, the surfacetemperature is strongly impacted by the presence of snow, and wave activityfluxes into the stratosphere areenhanced at a 1‐month lag, leading to a weakened polar vortex. Focusing further on 7 years characterized bya strongly negative phase of the Arctic Oscillation, wefind a weak snow feedback contributing to themaintenance of the negative Arctic Oscillation. By comparing the twin forecasts, we extracted the predictiveskill increment due to realistic snow initialization. The prediction of snow itself is greatly improved, andthere is increased skill in surface temperature over snow‐covered land in thefirst 10 days, and localized skillincrements in the mid‐latitude transition regions on the southernflanks of the snow‐covered land areas, atlead times longer than 30 days.
2019
Carbonaceous aerosol (total carbon, TCp) was source apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme (EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five predefined fractions were apportioned based on ambient measurements: elemental and organic carbon, from combustion of biomass (ECbb and OCbb) and from fossil-fuel (ECff and OCff) sources, and remaining non-fossil organic carbon (OCrnf), dominated by natural sources.
OCrnf made a larger contribution to TCp than anthropogenic sources (ECbb, OCbb, ECff, and OCff) at four out of nine sites in fall, reflecting the vegetative season, whereas anthropogenic sources dominated at all but one site in winter/spring. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the central European sites in fall, whereas fossil-fuel (OCff + ECff) sources dominated at the southernmost and the two northernmost sites. Residential wood burning emissions explained 30 %–50 % of TCp at most sites in the first week of sampling in fall, showing that this source can be the dominant one, even outside the heating season. In winter/spring, biomass burning was the major anthropogenic source at all but two sites, reflecting increased residential wood burning emissions in the heating season. Fossil-fuel sources dominated EC at all sites in fall, whereas there was a shift towards biomass burning for the southernmost sites in winter/spring.
Model calculations based on base-case emissions (mainly officially reported national emissions) strongly underpredicted observational derived levels of OCbb and ECbb outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential wood burning (and including intermediate volatility compounds, IVOCs) improved model results compared to the base-case emissions, but modeled levels were still substantially underestimated compared to observational derived OCbb and ECbb levels at the southernmost sites.
Our study shows that natural sources are a major contributor to carbonaceous aerosol in Europe, even in fall and in winter/spring, and that residential wood burning emissions are equally as large as or larger than that of fossil-fuel sources, depending on season and region. The poorly constrained residential wood burning emissions for large parts of Europe show the obvious need to improve emission inventories, with harmonization of emission factors between countries likely being the most important step to improve model calculations for biomass burning emissions, and European PM2.5 concentrations in general.
2019