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Technical note: Reanalysis of Aura MLS chemical observations
This paper presents a reanalysis of the atmospheric chemical composition from the upper troposphere to the lower mesosphere from August 2004 to December 2017. This reanalysis is produced by the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by the chemical observations from the Microwave Limb Sounder (MLS) on board the Aura satellite. BASCOE is based on the ensemble Kalman filter (EnKF) method and includes a chemical transport model driven by the winds and temperature from the ERA-Interim meteorological reanalysis. The model resolution is 3.75∘ in longitude, 2.5∘ in latitude and 37 vertical levels from the surface to 0.1 hPa with 25 levels above 100 hPa. The outputs are provided every 6 h. This reanalysis is called BRAM2 for BASCOE Reanalysis of Aura MLS, version 2.
Vertical profiles of eight species from MLS version 4 are assimilated and are evaluated in this paper: ozone (O3), water vapour (H2O), nitrous oxide (N2O), nitric acid (HNO3), hydrogen chloride (HCl), chlorine oxide (ClO), methyl chloride (CH3Cl) and carbon monoxide (CO). They are evaluated using independent observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) and N2O observations from a different MLS radiometer than the one used to deliver the standard product and ozonesondes. The evaluation is carried out in four regions of interest where only selected species are evaluated. These regions are (1) the lower-stratospheric polar vortex where O3, H2O, N2O, HNO3, HCl and ClO are evaluated; (2) the upper-stratospheric–lower-mesospheric polar vortex where H2O, N2O, HNO3 and CO are evaluated; (3) the upper troposphere–lower stratosphere (UTLS) where O3, H2O, CO and CH3Cl are evaluated; and (4) the middle stratosphere where O3, H2O, N2O, HNO3, HCl, ClO and CH3Cl are evaluated.
In general BRAM2 reproduces MLS observations within their uncertainties and agrees well with independent observations, with several limitations discussed in this paper (see the summary in Sect. 5.5). In particular, ozone is not assimilated at altitudes above (i.e. pressures lower than) 4 hPa due to a model bias that cannot be corrected by the assimilation. MLS ozone profiles display unphysical oscillations in the tropical UTLS, which are corrected by the assimilation, allowing a good agreement with ozonesondes. Moreover, in the upper troposphere, comparison of BRAM2 with MLS and independent observations suggests a positive bias in MLS O3 and a negative bias in MLS H2O. The reanalysis also reveals a drift in MLS N2O against independent observations, which highlights the potential use of BRAM2 to estimate biases between instruments. BRAM2 is publicly available and will be extended to assimilate MLS observations after 2017.
2019
Plastic litter in the European Arctic: What do we know?
Despite an exponential increase in available data on marine plastic debris globally, information on levels and trends of plastic pollution and especially microplastics in the Arctic remains scarce. The few available peer-reviewed scientific works, however, point to a ubiquitous distribution of plastic particles in all environmental compartments, including sea ice. Here, we review the current state of knowledge on the sources, distribution, transport pathways and fate of meso- and microplastics with a focus on the European Arctic and discuss observed and projected impacts on biota and ecosystems.
2019
2019
2019
This modeling study presents the sectoral contributions of anthropogenic emissions in the four Nordic countries (Denmark, Finland, Norway and Sweden) on air pollution levels and the associated health impacts and costs over the Nordic and the Arctic regions for the year 2015. The Danish Eulerian Hemispheric Model (DEHM) has been used on a 50 km resolution over Europe in tagged mode in order to calculate the response of a 30 % reduction of each emission sector in each Nordic country individually. The emission sectors considered in the study were energy production, non-industrial/commercial heating, industry, traffic, off-road mobile sources and waste management/agriculture. In total, 28 simulations were carried out. Following the air pollution modeling, the Economic Valuation of Air Pollution (EVA) model has been used to calculate the associated premature mortality and their costs. Results showed that more than 80 % of the PM2.5 concentration was attributed to transport from outside these four countries, implying an effort outside the Nordic region in order to decrease the pollutant levels over the area. The leading emission sector in each country was found to be non-industrial combustion (contributing by more than 60 % to the total PM2.5 mass coming from the country itself), except for Sweden, where industry contributed to PM2.5 with a comparable amount to non-industrial combustion. In addition to non-industrial combustion, the next most important source categories were industry, agriculture and traffic. The main chemical constituent of PM2.5 concentrations that comes from the country itself is calculated to be organic carbon in all countries, which suggested that non-industrial wood burning was the dominant national source of pollution in the Nordic countries. We have estimated the total number of premature mortality cases due to air pollution to be around 4000 in Denmark and Sweden and around 2000 in Finland and Norway. These premature mortality cases led to a total cost of EUR 7 billion in the selected Nordic countries. The assessment of the related premature mortality and associated cost estimates suggested that non-industrial combustion, together with industry and traffic, will be the main sectors to be targeted in emission mitigation strategies in the future.
2019
2019
2019
The carbonaceous aerosol accounts for an important part of total aerosol mass, affects human health and climate through its effects on physical and chemical properties of the aerosol, yet the understanding of its atmospheric sources and sinks is still incomplete. This study shows the state-of-the-art in modelling carbonaceous aerosol over Europe by comparing simulations performed with seven chemical transport models (CTMs) currently in air quality assessments in Europe: CAMx, CHIMERE, CMAQ, EMEP/MSC-W, LOTOS-EUROS, MINNI and RCGC. The simulations were carried out in the framework of the EURODELTA III modelling exercise and were evaluated against field measurements from intensive campaigns of European Monitoring and Evaluation Programme (EMEP) and the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI). Model simulations were performed over the same domain, using as much as possible the same input data and covering four seasons: summer (1–30 June 2006), winter (8 January – 4 February 2007), autumn (17 September- 15 October 2008) and spring (25 February - 26 March 2009). The analyses of models’ performances in prediction of elemental carbon (EC) for the four seasons and organic aerosol components (OA) for the last two seasons show that all models generally underestimate the measured concentrations. The maximum underestimation of EC is about 60% and up to about 80% for total organic matter (TOM). The underestimation of TOM outside of highly polluted area is a consequence of an underestimation of secondary organic aerosol (SOA), in particular of its main contributor: biogenic secondary aerosol (BSOA). This result is independent on the SOA modelling approach used and season. The concentrations and daily cycles of total primary organic matter (TPOM) are generally better reproduced by the models since they used the same anthropogenic emissions. However, the combination of emissions and model formulation leads to overestimate TPOM concentrations in 2009 for most of the models. All models capture relatively well the SOA daily cycles at rural stations mainly due to the spatial resolution used in the simulations. For the investigated carbonaceous aerosol compounds, the differences between the concentrations simulated by different models are lower than the differences between the concentrations simulated with a model for different seasons.
2019
2019
Estimating tropospheric and stratospheric winds using infrasound from explosions
The receiver-to-source backazimuth of atmospheric infrasound signals is biased when cross-winds are present along the propagation path. Infrasound from 598 surface explosions from over 30 years in northern Finland is measured with high spatial resolution on an array 178 km almost due North. The array is situated in the classical shadow-zone distance from the explosions. However, strong infrasound is almost always observed, which is most plausibly due to partial reflections from stratospheric altitudes. The most probable propagation paths are subject to both tropospheric and stratospheric cross-winds, and the wave-propagation modelling in this study yields good correspondence between the observed backazimuth deviation and cross-winds from the European Centre for Medium-Range Weather Forecasts Reanalysis (ERA)-Interim reanalysis product. This study demonstrates that atmospheric cross-winds can be estimated directly from infrasound data using propagation time and backazimuth deviation observations. This study finds these cross-wind estimates to be in good agreement with the ERA-Interim reanalysis.
2019
Recent Trends in Maintenance Costs for Façades Due to Air Pollution in the Oslo Quadrature, Norway
This study assesses changes since 1980 in the maintenance cost of the façades of the historical 17th to 19th century buildings of the Oslo Quadrature, Norway, due to atmospheric chemical wear, including the influence of air pollution. Bottom up estimations by exposure–response functions for an SO2 dominated situation reported in the literature for 1979 and 1995 were compared with calculations for the present (2002–2014) multi-pollutant situation. The present maintenance cost, relative to the total façade area, due to atmospheric wear and soiling was found to be about 1.6 Euro/m2 per year. The exposure to local air pollution, mainly particulate matter and NOx gases, contributed to 0.6 Euro/m2 (38%), of which the cost due to wear of renderings was about 0.4 Euro/m2 (22%), that due to the cleaning of glass was 0.2 Euro/m2 (11%), and that due to wear of other façade materials was 0.07 Euro/m2 (5%). The maintenance cost due to the atmospheric wear was found to be about 3.5%, and that due to the local air pollution about 1.1% of the total municipal building maintenance costs. The present (2002–2014) maintenance costs, relative to the areas of the specific materials, due to atmospheric wear are probably the highest for painted steel surfaces, about 8–10 Euro/m2, then about 2 Euro/m2 for façade cleaning and the maintenance of rendering, and down to 0.3 Euro/m2 for the maintenance of copper roofs. These costs should be adjusted with the importance of the wear relative to other reasons for the façade maintenance.
2019
The Tibetan Plateau (TP) region, often referred to as the Third Pole, is the world's highest plateau and exerts a considerable influence on regional and global climate. The state of the snowpack over the TP is a major research focus due to its great impact on the headwaters of a dozen major Asian rivers. While many studies have attempted to validate atmospheric reanalyses over the TP area in terms of temperature or precipitation, there have been – remarkably – no studies aimed at systematically comparing the snow depth or snow cover in global reanalyses with satellite and in situ data. Yet, snow in reanalyses provides critical surface information for forecast systems from the medium to sub-seasonal timescales.
Here, snow depth and snow cover from four recent global reanalysis products, namely the European Centre for Medium-Range Weather Forecasts (ECMWF) ERA5 and ERA-Interim reanalyses, the Japanese 55-year Reanalysis (JRA-55) and the NASA Modern-Era Retrospective analysis for Research and Applications (MERRA-2), are inter-compared over the TP region. The reanalyses are evaluated against a set of 33 in situ station observations, as well as against the Interactive Multisensor Snow and Ice Mapping System (IMS) snow cover and a satellite microwave snow depth dataset. The high temporal correlation coefficient (0.78) between the IMS snow cover and the in situ observations provides confidence in the station data despite the relative paucity of in situ measurement sites and the harsh operating conditions.
While several reanalyses show a systematic overestimation of the snow depth or snow cover, the reanalyses that assimilate local in situ observations or IMS snow cover are better capable of representing the shallow, transient snowpack over the TP region. The latter point is clearly demonstrated by examining the family of reanalyses from the ECMWF, of which only the older ERA-Interim assimilated IMS snow cover at high altitudes, while ERA5 did not consider IMS snow cover for high altitudes. We further tested the sensitivity of the ERA5-Land model in offline experiments, assessing the impact of blown snow sublimation, snow cover to snow depth conversion and, more importantly, excessive snowfall. These results suggest that excessive snowfall might be the primary factor for the large overestimation of snow depth and cover in ERA5 reanalysis. Pending a solution for this common model precipitation bias over the Himalayas and the TP, future snow reanalyses that optimally combine the use of satellite snow cover and in situ snow depth observations in the assimilation and analysis cycles have the potential to improve medium-range to sub-seasonal forecasts for water resources applications.
2019
Socioeconomic position, lifestyle habits and biomarkers of epigenetic aging: A multi-cohort analysis
Differences in health status by socioeconomic position (SEP) tend to be more evident at older ages, suggesting the involvement of a biological mechanism responsive to the accumulation of deleterious exposures across the lifespan. DNA methylation (DNAm) has been proposed as a biomarker of biological aging that conserves memory of endogenous and exogenous stress during life.
We examined the association of education level, as an indicator of SEP, and lifestyle-related variables with four biomarkers of age-dependent DNAm dysregulation: the total number of stochastic epigenetic mutations (SEMs) and three epigenetic clocks (Horvath, Hannum and Levine), in 18 cohorts spanning 12 countries.
The four biological aging biomarkers were associated with education and different sets of risk factors independently, and the magnitude of the effects differed depending on the biomarker and the predictor. On average, the effect of low education on epigenetic aging was comparable with those of other lifestyle-related risk factors (obesity, alcohol intake), with the exception of smoking, which had a significantly stronger effect.
Our study shows that low education is an independent predictor of accelerated biological (epigenetic) aging and that epigenetic clocks appear to be good candidates for disentangling the biological pathways underlying social inequalities in healthy aging and longevity.
2019
2019
Although aerosols in the Arctic have multiple and complex impacts on the regional climate, their removal due to deposition is still not well quantified. We combined meteorological, aerosol, precipitation, and snowpack observations with simulations to derive information about the deposition of sea salt components and black carbon (BC) from November 2011 to April 2012 to the Arctic snowpack at two locations close to Ny-Ålesund, Svalbard. The dominating role of sea salt and the contribution of dust for the composition of atmospheric aerosols were reflected in the seasonal composition of the snowpack. The strong alignment of the concentrations of the major sea salt components in the aerosols, the precipitation, and the snowpack is linked to the importance of wet deposition for transfer from the atmosphere to the snowpack. This agreement was less strong for monthly snow budgets and deposition, indicating important relocation of the impurities inside the snowpack after deposition. Wet deposition was less important for the transfer of nitrate, non-sea-salt sulfate, and BC to the snow during the winter period. The average BC concentration in the snowpack remains small, with a limited impact on snow albedo and melting. Nevertheless, the observations also indicate an important redistribution of BC in the snowpack, leading to layers with enhanced concentrations. The complex behavior of bromide due to modifications during sea salt aerosol formation and remobilization in the atmosphere and in the snow were not resolved because of the lack of bromide measurements in aerosols and precipitation.
2019
2019
The Mineral Aerosol Profiling from Infrared Radiances (MAPIR) algorithm retrieves vertical dust concentration profiles from cloud-free Infrared Atmospheric Sounding Interferometer (IASI) thermal infrared (TIR) radiances using Rodgers' optimal estimation method (OEM). We describe the new version 4.1 and evaluation results. Main differences with respect to previous versions are the Levenberg–Marquardt modification of the OEM, the use of the logarithm of the concentration in the retrieval and the use of Radiative Transfer for TOVS (RTTOV) for in-line radiative transfer calculations. The dust aerosol concentrations are retrieved in seven 1 km thick layers centered at 0.5 to 6.5 km. A global data set of the daily dust distribution was generated with MAPIR v4.1 covering September 2007 to June 2018, with further extensions planned every 6 months. The post-retrieval quality filters reject about 16 % of the retrievals, a huge improvement with respect to the previous versions in which up to 40 % of the retrievals were of bad quality. The median difference between the observed and fitted spectra of the good-quality retrievals is 0.32 K, with lower values over oceans. The information content of the retrieved profiles shows a dependence on the total aerosol load due to the assumption of a lognormal state vector. The median degrees of freedom in dusty scenes (min 10 µm AOD of 0.5) is 1.4. An evaluation of the aerosol optical depth (AOD) obtained from the integrated MAPIR v4.1 profiles was performed against 72 AErosol RObotic NETwork (AERONET) stations. The MAPIR AOD correlates well with the ground-based data, with a mean correlation coefficient of 0.66 and values as high as 0.88. Overall, there is a mean AOD (550 nm) positive bias of only 0.04 with respect to AERONET, which is an extremely good result. The previous versions of MAPIR were known to largely overestimate AOD (about 0.28 for v3). A second evaluation exercise was performed comparing the mean aerosol layer altitude from MAPIR with the mean dust altitude from Cloud–Aerosol LIdar with Orthogonal Polarization (CALIOP). A small underestimation was found, with a mean difference of about 350 m (standard deviation of about 1 km) with respect to the CALIOP cumulative extinction altitude, which is again considered very good as the vertical resolution of MAPIR is 1 km. In the comparisons against AERONET and CALIOP, a dependence of MAPIR on the quality of the temperature profiles used in the retrieval is observed. Finally, a qualitative comparison of dust aerosol concentration profiles was done against lidar measurements from two ground-based stations (M'Bour and Al Dhaid) and from the Cloud–Aerosol Transport System (CATS) instrument on board the International Space Station (ISS). MAPIR v4.1 showed the ability to detect dust plumes at the same time and with a similar extent as the lidar instruments. This new MAPIR version shows a great improvement of the accuracy of the aerosol profile retrievals with respect to previous versions, especially so for the integrated AOD. It now offers a unique 3-D dust data set, which can be used to gain more insight into the transport and emission processes of mineral dust aerosols.
2019
DNA double‐strand breaks in Arctic char (Salvelinus alpinus) from Bjørnøya in the Norwegian Arctic
High levels of organochlorine contaminants (OCs) have been found in arctic char (Salvelinus alpinus) from Lake Ellasjøen, Bjørnøya (Norwegian Arctic). The aim of the present study was to investigate the potential genotoxic effect of environmental organochlorine contaminant exposure in arctic char from Ellasjøen compared with arctic char from the low‐contaminated Lake Laksvatn nearby. Blood was analyzed using agarose gel electrophoresis and image data analysis to quantify the fraction of total DNA that migrated into the gel (DNA‐FTM) as a relative measure of DNA double‐strand breaks (DSBs). Analysis by GC‐MS of muscle samples showed an average 43 times higher concentration of ΣOCs in arctic char from Ellasjøen (n = 18) compared with Laksvatn char (n = 21). Char from Lake Ellasjøen had a much higher frequency of DSBs, as measured by DNA‐FTM, than char from Lake Laksvatn. Principal component analysis and multiple linear regressions show that there was a significant positive relationship between DSBs and levels of organochlorine contaminants in the char. In addition, DSBs were less frequent in reproductively mature char than in immature char. The results suggest that organochlorine contaminants are genotoxic to arctic char.
2019
Information on the origin of pollution constitutes an essential step of air quality management as it helps identifying measures to control air pollution. In this work, we review the most widely used source-apportionment methods for air quality management. Using theoretical and real-case datasets we study the differences among these methods and explain why they result in very different conclusions to support air quality planning. These differences are a consequence of the intrinsic assumptions that underpin the different methodologies and determine/limit their range of applicability. We show that ignoring their underlying assumptions is a risk for efficient/successful air quality management as these methods are sometimes used beyond their scope and range of applicability. The simplest approach based on increments (incremental approach) is often not suitable to support air quality planning. Contributions obtained through mass-transfer methods (receptor models or tagging approaches built in air quality models) are appropriate to support planning but only for specific pollutants. Impacts obtained via “brute-force” methods are the best suited but it is important to assess carefully their application range to make sure they reproduce correctly the prevailing chemical regimes.
2019
2019
Peroxisome proliferator-activated receptor alfa (PPARA/NR1C1) is a ligand activated nuclear receptor that is a key regulator of lipid metabolism in tissues with high fatty acid catabolism such as the liver. Here, we cloned PPARA from polar bear liver tissue and studied in vitro transactivation of polar bear and human PPARA by environmental contaminants using a luciferase reporter assay. Six hinge and ligand-binding domain amino acids have been substituted in polar bear PPARA compared to human PPARA. Perfluorocarboxylic acids (PFCA) and perfluorosulfonic acids induced the transcriptional activity of both human and polar bear PPARA. The most abundant PFCA in polar bear tissue, perfluorononanoate, increased polar bear PPARA-mediated luciferase activity to a level comparable to that of the potent PPARA agonist WY-14643 (~8-fold, 25 μM). Several brominated flame retardants were weak agonists of human and polar bear PPARA. While single exposures to polychlorinated biphenyls did not, or only slightly, increase the transcriptional activity of PPARA, a technical mixture of PCBs (Aroclor 1254) strongly induced the transcriptional activity of human (~8-fold) and polar bear PPARA (~22-fold). Polar bear PPARA was both quantitatively and qualitatively more susceptible than human PPARA to transactivation by less lipophilic compounds.
2019
BACKGROUND: In order to use in situ measurements to constrain urban anthropogenic emissions of carbon dioxide (CO2), we use a Lagrangian methodology based on diffusive backward trajectory tracer reconstructions and Bayesian inversion. The observations of atmospheric CO2 were collected within the Tokyo Bay Area during the Comprehensive Observation Network for TRace gases by AIrLiner (CONTRAIL) flights, from the Tsukuba tall tower of the Meteorological Research Institute (MRI) of the Japan Meteorological Agency and at two surface sites (Dodaira and Kisai) from the World Data Center for Greenhouse Gases (WDCGG).
RESULTS: We produce gridded estimates of the CO2 emissions and calculate the averages for different areas within the Kanto plain where Tokyo is located. Using these inversions as reference we investigate the impact of perturbing different elements in the inversion system. We modified the observations amount and location (surface only sparse vs. including aircraft CO2 observations), the background representation, the wind data used to drive the transport model, the prior emissions magnitude and time resolution and error parameters of the inverse model.
CONCLUSIONS: Optimized fluxes were consistent with other estimates for the unperturbed simulations. Inclusion of CONTRAIL measurements resulted in significant differences in the magnitude of the retrieved fluxes, 13% on average for the whole domain and of up to 21% for the spatiotemporal cells with the highest fluxes. Changes in the background yielded differences in the retrieved fluxes of up to 50% and more. Simulated biases in the modelled transport cause differences in the retrieved fluxes of up to 30% similar to those obtained using different meteorological winds to advect the Lagrangian trajectories. Perturbations to the prior inventory can impact the fluxes by ~ 10% or more depending on the assumptions on the error covariances. All of these factors can cause significant differences in the estimated flux, and highlight the challenges in estimating regional CO2 fluxes from atmospheric observations.
2019
2019
Recent Trends in Stratospheric Chlorine From Very Short-Lived Substances
Very short‐lived substances (VSLS), including dichloromethane (CH2Cl2), chloroform (CHCl3), perchloroethylene (C2Cl4), and 1,2‐dichloroethane (C2H4Cl2), are a stratospheric chlorine source and therefore contribute to ozone depletion. We quantify stratospheric chlorine trends from these VSLS (VSLCltot) using a chemical transport model and atmospheric measurements, including novel high‐altitude aircraft data from the NASA VIRGAS (2015) and POSIDON (2016) missions. We estimate VSLCltot increased from 69 (±14) parts per trillion (ppt) Cl in 2000 to 111 (±22) ppt Cl in 2017, with >80% delivered to the stratosphere through source gas injection, and the remainder from product gases. The modeled evolution of chlorine source gas injection agrees well with historical aircraft data, which corroborate reported surface CH2Cl2 increases since the mid‐2000s. The relative contribution of VSLS to total stratospheric chlorine increased from ~2% in 2000 to ~3.4% in 2017, reflecting both VSLS growth and decreases in long‐lived halocarbons. We derive a mean VSLCltot growth rate of 3.8 (±0.3) ppt Cl/year between 2004 and 2017, though year‐to‐year growth rates are variable and were small or negative in the period 2015–2017. Whether this is a transient effect, or longer‐term stabilization, requires monitoring. In the upper stratosphere, the modeled rate of HCl decline (2004–2017) is −5.2% per decade with VSLS included, in good agreement to ACE satellite data (−4.8% per decade), and 15% slower than a model simulation without VSLS. Thus, VSLS have offset a portion of stratospheric chlorine reductions since the mid‐2000s.
2019
Using meteor wind data from the Super Dual Auroral Radar Network (SuperDARN) in the Northern Hemisphere, we (1) demonstrate that the migrating (Sun‐synchronous) tides can be separated from the nonmigrating components in the mesosphere and lower thermosphere (MLT) region and (2) use this to determine the response of the different components of the semidiurnal tide (SDT) to sudden stratospheric warming (SSW) conditions. The radars span a limited range of latitudes around 60°N and are located over nearly 180° of longitude. The migrating tide is extracted from the nonmigrating components observed in the meridional wind recorded from meteor ablation drift velocities around 95‐km altitude, and a 20‐year climatology of the different components is presented. The well‐documented late summer and wintertime maxima in the semidiurnal winds are shown to be due primarily to the migrating SDT, whereas during late autumn and spring the nonmigrating components are at least as strong as the migrating SDT. The robust behavior of the SDT components during SSWs is then examined by compositing 13 SSW events associated with an elevated stratopause recorded between 1995 and 2013. The migrating SDT is seen to reduce in amplitude immediately after SSW onset and then return anomalously strongly around 10–17 days after the SSW onset. We conclude that changes in the underlying wind direction play a role in modulating the tidal amplitude during the evolution of SSWs and that the enhancement in the midlatitude migrating SDT (previously reported in modeling studies) is observed in the MLT at least up to 60°N.
2019