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Assessment was performed of the air quality related risk to the conservation of cultural heritage objects in one urban and one rural indoor location in Romania, with expected different air quality related conservation challenges: the National military museum in Bucharest and the Tismana monastery in Gorj County. The work was performed within and subsequent to the EU-Memori project by applying Memori methodology, Memori®-EWO (Early warning organic) dosimeters and passive pollution badge samplers for acetic and formic acids. The measurements in the National military museum were performed in three rooms with different exposure situations, and inside protective enclosures in the rooms. The rooms had organic and inorganic objects on exhibition and in store. The observed risks were associated with photo-oxidizing impact probably due to traffic pollutants entering from outdoor, and/or light exposure and temperature. The risks were found to be moderate, generally comparable to typical European purpose built museum locations. The highest risk was observed in a more open exhibition room in the main museum building. It was indicated that some observable change might happen to sensitive pigments and paper within 3 years, and to lead, copper and sensitive glass within 30 years in this location. Risk for observable change to sensitive pigments, paper, lead and sensitive glass within 30 years, was indicated in the other locations. The lowest risk was observed in a warehouse. A reduction in photo-oxidizing risk was measured in two of the enclosures, but a slightly higher acidic impact was measured in all the three enclosures, as compared to the respective rooms. In the Tismana monastery, a high level of acetic plus formic acid was observed in the air in the storerooms for icons and textiles, and books. Damage risk within 3 years was indicated for lead objects and sensitive glass, and within 30 years for iron and varnish (Laropal A81, resin mastic and dammar). As organic acid attack increases significantly at higher air humidity (> ~ 60%), this would be especially important to avoid. Risk for photo-oxidizing damage to paper and sensitive pigments within 30 years was indicated.
2018
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 W 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.
2018
A satellite-based estimate of combustion aerosol cloud microphysical effects over the Arctic Ocean
Climate predictions for the rapidly changing Arctic are highly uncertain, largely due to a poor understanding of the processes driving cloud properties. In particular, cloud fraction (CF) and cloud phase (CP) have major impacts on energy budgets, but are poorly represented in most models, often because of uncertainties in aerosol–cloud interactions. Here, we use over 10 million satellite observations coupled with aerosol transport model simulations to quantify large-scale microphysical effects of aerosols on CF and CP over the Arctic Ocean during polar night, when direct and semi-direct aerosol effects are minimal. Combustion aerosols over sea ice are associated with very large (∼ 10Wm−2) differences in longwave cloud radiative effects at the sea ice surface. However, co-varying meteorological changes on factors such as CF likely explain the majority of this signal. For example, combustion aerosols explain at most 40% of the CF differences between the full dataset and the clean-condition subset, compared to between 57% and 91% of the differences that can be predicted by co-varying meteorology. After normalizing for meteorological regime, aerosol microphysical effects have small but significant impacts on CF, CP, and precipitation frequency on an Arctic-wide scale. These effects indicate that dominant aerosol–cloud microphysical mechanisms are related to the relative fraction of liquid-containing clouds, with implications for a warming Arctic.
2018
Methane at Svalbard and over the European Arctic Ocean
Methane (CH<sub>4</sub>) is a powerful greenhouse gas. Its atmospheric mixing ratios have been increasing since 2005. Therefore, quantification of CH<sub>4</sub> sources is essential for effective climate change mitigation. Here we report observations of the CH<sub>4</sub> mixing ratios measured at the Zeppelin Observatory (Svalbard) in the Arctic and aboard the research vessel (RV) Helmer Hanssen over the Arctic Ocean from June 2014 to December 2016, as well as the long-term CH<sub>4</sub> trend measured at the Zeppelin Observatory from 2001 to 2017. We investigated areas over the European Arctic Ocean to identify possible hotspot regions emitting CH<sub>4</sub> from the ocean to the atmosphere, and used state-of-the-art modelling (FLEXPART) combined with updated emission inventories to identify CH<sub>4</sub> sources. Furthermore, we collected air samples in the region as well as samples of gas hydrates, obtained from the sea floor, which we analysed using a new technique whereby hydrate gases are sampled directly into evacuated canisters. Using this new methodology, we evaluated the suitability of ethane and isotopic signatures (δ<sup>13</sup>C in CH<sub>4</sub>) as tracers for ocean-to-atmosphere CH<sub>4</sub> emission. We found that the average methane / light hydrocarbon (ethane and propane) ratio is an order of magnitude higher for the same sediment samples using our new methodology compared to previously reported values, 2379.95 vs. 460.06, respectively. Meanwhile, we show that the mean atmospheric CH<sub>4</sub> mixing ratio in the Arctic increased by 5.9±0.38 parts per billion by volume (ppb) per year (yr<sup>−1</sup>) from 2001 to 2017 and ∼8 pbb yr<sup>−1</sup> since 2008, similar to the global trend of ∼ 7–8 ppb yr<sup>−1</sup>. Most large excursions from the baseline CH<sub>4</sub> mixing ratio over the European Arctic Ocean are due to long-range transport from land-based sources, lending confidence to the present inventories for high-latitude CH<sub>4</sub> emissions. However, we also identify a potential hotspot region with ocean–atmosphere CH<sub>4</sub> flux north of Svalbard (80.4∘ N, 12.8∘ E) of up to 26 nmol m<sup>−2</sup>s<sup>−1</sup> from a large mixing ratio increase at the location of 30 ppb. Since this flux is consistent with previous constraints (both spatially and temporally), there is no evidence that the area of interest north of Svalbard is unique in the context of the wider Arctic. Rather, because the meteorology at the time of the observation was unique in the context of the measurement time series, we obtained over the short course of the episode measurements highly sensitive to emissions over an active seep site, without sensitivity to land-based emissions.
2018
Observation of turbulent dispersion of artificially released SO2 puffs with UV cameras
In atmospheric tracer experiments, a substance is released into the turbulent atmospheric flow to study the dispersion parameters of the atmosphere. That can be done by observing the substance's concentration distribution downwind of the source. Past experiments have suffered from the fact that observations were only made at a few discrete locations and/or at low time resolution. The Comtessa project (Camera Observation and Modelling of 4-D Tracer Dispersion in the Atmosphere) is the first attempt at using ultraviolet (UV) camera observations to sample the three-dimensional (3-D) concentration distribution in the atmospheric boundary layer at high spatial and temporal resolution. For this, during a three-week campaign in Norway in July 2017, sulfur dioxide (SO2), a nearly passive tracer, was artificially released in continuous plumes and nearly instantaneous puffs from a 9m high tower. Column-integrated SO2 concentrations were observed with six UV SO2 cameras with sampling rates of several hertz and a spatial resolution of a few centimetres. The atmospheric flow was characterised by eddy covariance measurements of heat and momentum fluxes at the release mast and two additional towers. By measuring simultaneously with six UV cameras positioned in a half circle around the release point, we could collect a data set of spatially and temporally resolved tracer column densities from six different directions, allowing a tomographic reconstruction of the 3-D concentration field. However, due to unfavourable cloudy conditions on all measurement days and their restrictive effect on the SO2 camera technique, the presented data set is limited to case studies. In this paper, we present a feasibility study demonstrating that the turbulent dispersion parameters can be retrieved from images of artificially released puffs, although the presented data set does not allow for an in-depth analysis of the obtained parameters. The 3-D trajectories of the centre of mass of the puffs were reconstructed enabling both a direct determination of the centre of mass meandering and a scaling of the image pixel dimension to the position of the puff. The latter made it possible to retrieve the temporal evolution of the puff spread projected to the image plane. The puff spread is a direct measure of the relative dispersion process. Combining meandering and relative dispersion, the absolute dispersion could be retrieved. The turbulent dispersion in the vertical is then used to estimate the effective source size, source timescale and the Lagrangian integral time. In principle, the Richardson–Obukhov constant of relative dispersion in the inertial subrange could be also obtained, but the observation time was not sufficiently long in comparison to the source timescale to allow an observation of this dispersion range. While the feasibility of the methodology to measure turbulent dispersion could be demonstrated, a larger data set with a larger number of cloud-free puff releases and longer observation times of each puff will be recorded in future studies to give a solid estimate for the turbulent dispersion under a variety of stability conditions.
2018
Atmospheric measurements show an increase in CH4 from the 1980s to 1998 followed by a period of near‐zero growth until 2007. However, from 2007, CH4 has increased again. Understanding the variability in CH4 is critical for climate prediction and climate change mitigation. We examine the role of CH4 sources and the dominant CH4 sink, oxidation by the hydroxyl radical (OH), in atmospheric CH4 variability over the past three decades using observations of CH4, C2H6, and δ13CCH4 in an inversion. From 2006 to 2014, microbial and fossil fuel emissions increased by 36 ± 12 and 15 ± 8 Tg y−1, respectively. Emission increases were partially offset by a decrease in biomass burning of 3 ± 2 Tg y−1 and increase in soil oxidation of 5 ± 6 Tg y−1. A change in the atmospheric sink did not appear to be a significant factor in the recent growth of CH4.
2018
The chlorinated polyfluoroalkyl ether sulfonate F-53B is used as a mist suppressant in the Chinese electroplating industry. Because of the regulations on perfluorooctanesulfonate (PFOS), its use is expected to increase. Until now, F-53B toxicity data have been scarce and are, to our knowledge, lacking for birds. This study therefore investigated the effects of PFOS and F-53B, separately and as mixtures, on the development of the chicken (Gallus gallus domesticus). Compounds were injected in ovo, before incubation, at 150 and 1500 ng/g egg. At embryonic day 20, a significantly lower heart rate was observed in all treated groups compared to the control group and hatchlings exposed to the high dose of F-53B had a significantly enlarged liver (8%). Embryonic survival was not affected and no significant effects on hatchling body mass or oxidative stress parameters were found. Our results suggest that these compounds likely have different toxicity thresholds for the investigated endpoints, and/or different modes of action. This study thereby underlines the potential developmental toxicity of PFOS and F-53B at environmentally relevant concentrations. Assessment of PFOS alternatives should therefore continue, preferably prior to their large scale use, as they should be ensured to be less harmful than PFOS itself.
2018
Recent Arctic ozone depletion: Is there an impact of climate change?
After the well-reported record loss of Arctic stratospheric ozone of up to 38% in the winter 2010–2011, further large depletion of 27% occurred in the winter 2015–2016. Record low winter polar vortex temperatures, below the threshold for ice polar stratospheric cloud (PSC) formation, persisted for one month in January 2016. This is the first observation of such an event and resulted in unprecedented dehydration/denitrification of the polar vortex. Although chemistry–climate models (CCMs) generally predict further cooling of the lower stratosphere with the increasing atmospheric concentrations of greenhouse gases (GHGs), significant differences are found between model results indicating relatively large uncertainties in the predictions. The link between stratospheric temperature and ozone loss is well understood and the observed relationship is well captured by chemical transport models (CTMs). However, the strong dynamical variability in the Arctic means that large ozone depletion events like those of 2010–2011 and 2015–2016 may still occur until the concentrations of ozone-depleting substances return to their 1960 values. It is thus likely that the stratospheric ozone recovery, currently anticipated for the mid-2030s, might be significantly delayed. Most important in order to predict the future evolution of Arctic ozone and to reduce the uncertainty of the timing for its recovery is to ensure continuation of high-quality ground-based and satellite ozone observations with special focus on monitoring the annual ozone loss during the Arctic winter.
2018
Water column distribution of mercury species in permanently stratified aqueous environments
Biogeochemical structures of three permanently stratified waterbodies were studied: a sea water basin (the Black Sea), an estuary (Hunnbunn fjord), and a freshwater lake (Nordbytjernet), with focus on the distributions of methylmercury (MeHg) and total mercury (THg). THg concentrations were similar in the sea water basin (0.2–1.8 ng/L) and the freshwater lake (0.8–1.2 ng/L), but significantly higher in the estuary (0.6–9.4 ng/L). An increase in the MeHg concentration and MeHg/THg ratio were found in the redox zone in all three basins, indicating bacterial production of MeHg in the aqueous phase. In the lake and estuary, the maximum MeHg concentration and MeHg/THg ratio were found in samples located closest to the bottom sediments, likely due to the formation of MeHg in surface sediments and subsequent diffusion to the overlying waters.
2018
Assessing, quantifying and valuing the ecosystem services of coastal lagoons
The natural conservation of coastal lagoons is important not only for their ecological importance, but also because of the valuable ecosystem services they provide for human welfare and wellbeing. Coastal lagoons are shallow semi-enclosed systems that support important habitats such as wetlands, mangroves, salt-marshes and seagrass meadows, as well as a rich biodiversity. Coastal lagoons are also complex social-ecological systems and the ecosystem services that lagoons deliver provide livelihoods, benefits wellbeing and welfare to humans. This study assessed, quantified and valued the ecosystem services of 32 coastal lagoons. The main findings of the study were: (i) the definitions of ecosystem services are still not generally accepted; (ii) the quantification of ecosystem services is made in many different ways, using different units; (iii) the evaluation in monetary terms of some ecosystem service is problematic, often relying on non-monetary evaluation methods; (iv) when ecosystem services are valued in monetary terms, this may represent very different human benefits; and, (v) different aspects of climate change, including increasing temperature (SST), sea-level rise (SLR) and changes in rainfall patterns threaten the valuable ecosystem services of coastal lagoons.
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This study quantifies the present-day global and regional distributions (2010–2014) and trends (2000–2014) for five ozone metrics relevant for short-term and long-term human exposure. These metrics, calculated by the Tropospheric Ozone Assessment Report, are: 4th highest daily maximum 8-hour ozone (4MDA8); number of days with MDA8 > 70 ppb (NDGT70), SOMO35 (annual Sum of Ozone Means Over 35 ppb) and two seasonally averaged metrics (3MMDA1; AVGMDA8). These metrics were explored at ozone monitoring sites worldwide, which were classified as urban or non-urban based on population and nighttime lights data.
Present-day distributions of 4MDA8 and NDGT70, determined predominantly by peak values, are similar with highest levels in western North America, southern Europe and East Asia. For the other three metrics, distributions are similar with North–South gradients more prominent across Europe and Japan. Between 2000 and 2014, significant negative trends in 4MDA8 and NDGT70 occur at most US and some European sites. In contrast, significant positive trends are found at many sites in South Korea and Hong Kong, with mixed trends across Japan. The other three metrics have similar, negative trends for many non-urban North American and some European and Japanese sites, and positive trends across much of East Asia. Globally, metrics at many sites exhibit non-significant trends. At 59% of all sites there is a common direction and significance in the trend across all five metrics, whilst 4MDA8 and NDGT70 have a common trend at ~80% of all sites. Sensitivity analysis shows AVGMDA8 trends differ with averaging period (warm season or annual). Trends are unchanged at many sites when a 1995–2014 period is used; although fewer sites exhibit non-significant trends. Over the longer period 1970–2014, most Japanese sites exhibit positive 4MDA8/SOMO35 trends. Insufficient data exist to characterize ozone trends for the rest of Asia and other world regions.
2018
Warm Arctic–cold Siberia: comparing the recent and the early 20th century Arctic warmings
The Warm Arctic–cold Siberia surface temperature pattern during recent boreal winter is suggested to be triggered by the ongoing decrease of Arctic autumn sea ice concentration and has been observed together with an increase in mid-latitude extreme events and a meridionalization of tropospheric circulation. However, the exact mechanism behind this dipole temperature pattern is still under debate, since model experiments with reduced sea ice show conflicting results. We use the early twentieth-century Arctic warming (ETCAW) as a case study to investigate the link between September sea ice in the Barents–Kara Sea (BKS) and the Siberian temperature evolution. Analyzing a variety of long-term climate reanalyses, we find that the overall winter temperature and heat flux trend occurs with the reduction of September BKS sea ice. Tropospheric conditions show a strengthened atmospheric blocking over the BKS, strengthening the advection of cold air from the Arctic to central Siberia on its eastern flank, together with a reduction of warm air advection by the westerlies. This setup is valid for both the ETCAW and the current Arctic warming period.
2018
Comparison of dust-layer heights from active and passive satellite sensors
Aerosol-layer height is essential for understanding the impact of aerosols on the climate system. As part of the European Space Agency Aerosol_cci project, aerosol-layer height as derived from passive thermal and solar satellite sensors measurements have been compared with aerosol-layer heights estimated from CALIOP measurements. The Aerosol_cci project targeted dust-type aerosol for this study. This ensures relatively unambiguous aerosol identification by the CALIOP processing chain. Dust-layer height was estimated from thermal IASI measurements using four different algorithms (from BIRA-IASB, DLR, LMD, LISA) and from solar GOME-2 (KNMI) and SCIAMACHY (IUP) measurements. Due to differences in overpass time of the various satellites, a trajectory model was used to move the CALIOP-derived dust heights in space and time to the IASI, GOME-2 and SCIAMACHY dust height pixels. It is not possible to construct a unique dust-layer height from the CALIOP data. Thus two CALIOP-derived layer heights were used: the cumulative extinction height defined as the height where the CALIOP extinction column is half of the total extinction column, and the geometric mean height, which is defined as the geometrical mean of the top and bottom heights of the dust layer. In statistical average over all IASI data there is a general tendency to a positive bias of 0.5–0.8 km against CALIOP extinction-weighted height for three of the four algorithms assessed, while the fourth algorithm has almost no bias. When comparing geometric mean height there is a shift of −0.5 km for all algorithms (getting close to zero for the three algorithms and turning negative for the fourth). The standard deviation of all algorithms is quite similar and ranges between 1.0 and 1.3 km. When looking at different conditions (day, night, land, ocean), there is more detail in variabilities (e.g. all algorithms overestimate more at night than during the day). For the solar sensors it is found that on average SCIAMACHY data are lower by −1.097 km (−0.961 km) compared to the CALIOP geometric mean (cumulative extinction) height, and GOME-2 data are lower by −1.393 km (−0.818 km).
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Understanding the bioaccumulation mechanisms of per- and polyfluoroalkyl substances (PFASs) across different chain-lengths, isomers and functional groups represents a monumental scientific challenge with implications for chemical regulation. Here, we investigate how the differential tissue distribution and bioaccumulation behavior of 25 PFASs in crucian carp from two field sites impacted by point sources can provide information about the processes governing uptake, distribution and elimination of PFASs. Median tissue/blood ratios (TBRs) were consistently <1 for all PFASs and tissues except bile which displayed a distinct distribution pattern and enrichment of several perfluoroalkyl sulfonic acids. Transformation of concentration data into relative body burdens (RBBs) demonstrated that blood, gonads, and muscle together accounted for >90% of the amount of PFASs in the organism. Principal component analyses of TBRs and RBBs showed that the functional group was a relatively more important predictor of internal distribution than chain-length for PFASs. Whole body bioaccumulation factors (BAFs) for short-chain PFASs deviated from the positive relationship with hydrophobicity observed for longer-chain homologues. Overall, our results suggest that TBR, RBB, and BAF patterns were most consistent with protein binding mechanisms although partitioning to phospholipids may contribute to the accumulation of long-chain PFASs in specific tissues.
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A combination of local (i.e. firefighting training facilities) and remote sources (i.e., long-range transport) are assumed to be responsible for the occurrence of per- and polyfluoroalkyl substances (PFASs) in Svalbard (Norwegian Arctic). However, no systematic elucidation of local PFASs sources have been conducted yet. Therefore, a survey was performed aiming at identifying local PFASs pollution sources on the island of Spitsbergen (Svalbard, Norway). Soil, fresh water (lake, draining rivers), sea water, melt-water run-off, surface snow and coastal sediment samples were collected from Longyearbyen (Norwegian mining town), Ny-Ålesund (research facility) and the Lake Linnévatnet area (background site) during several campaigns (2014-2016) and analysed for 14 individual target PFASs. For background site (Linnévatnet area, sampling during April to June 2015), ∑PFAS levels ranged from 0.4 – 4 ng/L in surface lake water (n = 20). PFAS in melt water from the contributing glaciers showed similar concentrations (~4 ng/L, n = 2). The short chain perfluorobutanoate (PFBA) was predominant in lake water (60-80% of the ∑PFASs), meltwater (20-30 %) and run-off water (40 %). Long range transport is assumed to be the major PFAS source. In Longyearbyen, 5 water samples (i.e. 2 seawater, 3 run-off) were collected near the local firefighting training site (FFTS) in November 2014 and June 2015, respectively. The highest PFAS levels were found in FFTS melt water run-off (118 ng/L). PFOS was the most abundant compound in the FFTS meltwater run-off (53 – 58 % PFASs). At the research station Ny-Ålesund, sea water (n = 6), soil (n = 9) and fresh water (n = 10) were collected in June 2016. Low ∑PFAS concentrations were determined for sea water (5 - 6 ng/L), whereas high ∑PFAS concentrations were found in run-off water (113 – 119 ng/L) and soil (211 – 800 ng/g dry weight (dw)) collected close to the local FFTS. In addition, high ∑PFAS levels (127 ng/L) were also found in fresh water from lake Solvatnet close to former sewage treatment facility. Overall, at both FFTS affected sites (soil, water), PFOS was the most abundant compound (60 – 69% of ∑PFASs). FFTS and landfill locations were identified as major PFASs sources for Svalbard settlements.
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