Fant 10000 publikasjoner. Viser side 304 av 400:
We present an Observing System Simulation Experiment (OSSE) dedicated to the evaluation of the added value of the Sentinel-4 and Sentinel-5P missions for tropospheric nitrogen dioxide (NO2). Sentinel-4 is a geostationary (GEO) mission covering the European continent, providing observations with high temporal resolution (hourly). Sentinel-5P is a low Earth orbit (LEO) mission providing daily observations with a global coverage. The OSSE experiment has been carefully designed, with separate models for the simulation of observations and for the assimilation experiments and with conservative estimates of the total observation uncertainties. In the experiment we simulate Sentinel-4 and Sentinel-5P tropospheric NO2 columns and surface ozone concentrations at 7 by 7 km resolution over Europe for two 3-month summer and winter periods. The synthetic observations are based on a nature run (NR) from a chemistry transport model (MOCAGE) and error estimates using instrument characteristics. We assimilate the simulated observations into a chemistry transport model (LOTOS-EUROS) independent of the NR to evaluate their impact on modelled NO2 tropospheric columns and surface concentrations. The results are compared to an operational system where only ground-based ozone observations are ingested. Both instruments have an added value to analysed NO2 columns and surface values, reflected in decreased biases and improved correlations. The Sentinel-4 NO2 observations with hourly temporal resolution benefit modelled NO2 analyses throughout the entire day where the daily Sentinel-5P NO2 observations have a slightly lower impact that lasts up to 3–6 h after overpass. The evaluated benefits may be even higher in reality as the applied error estimates were shown to be higher than actual errors in the now operational Sentinel-5P NO2 products. We show that an accurate representation of the NO2 profile is crucial for the benefit of the column observations on surface values. The results support the need for having a combination of GEO and LEO missions for NO2 analyses in view of the complementary benefits of hourly temporal resolution (GEO, Sentinel-4) and global coverage (LEO, Sentinel-5P).
2019
2019
2019
2019
2019
2019
2019
Vinca Institute of Nuclear Sciences
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
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
Source apportionment of circum-Arctic atmospheric black carbon from isotopes and modeling
Black carbon (BC) contributes to Arctic climate warming, yet source attributions are inaccurate due to lacking observational constraints and uncertainties in emission inventories. Year-round, isotope-constrained observations reveal strong seasonal variations in BC sources with a consistent and synchronous pattern at all Arctic sites. These sources were dominated by emissions from fossil fuel combustion in the winter and by biomass burning in the summer. The annual mean source of BC to the circum-Arctic was 39 ± 10% from biomass burning. Comparison of transport-model predictions with the observations showed good agreement for BC concentrations, with larger discrepancies for (fossil/biomass burning) sources. The accuracy of simulated BC concentration, but not of origin, points to misallocations of emissions in the emission inventories. The consistency in seasonal source contributions of BC throughout the Arctic provides strong justification for targeted emission reductions to limit the impact of BC on climate warming in the Arctic and beyond.
2019
2019
2019
2019