Found 2696 publications. Showing page 53 of 270:
Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes.
Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1.
Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc.
Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment.
Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models.
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2021
How Atmospheric Chemistry and Transport Drive Surface Variability of N2O and CFC-11
Nitrous oxide (N2O) is a long-lived greenhouse gas that affects atmospheric chemistry and climate. In this work, we use satellite measurements of N2O, ozone (O3), and temperature from the Aura Microwave Limb Sounder (MLS) instrument to calculate stratospheric loss of N2O, and thus its atmospheric lifetime. Using three chemistry transport models simulating the Aura period 2005–2017, we verify the stratospheric sink using MLS data and follow that loss signal down to the surface and compare with surface observations. Stratospheric loss has a strong seasonal cycle and is further modulated by the Quasi-Biennial Oscillation (QBO); these cycles are seen equally in both observations and the models. When filtered for interannual variability, the modeled surface signal is QBO-caused, and it reproduces the observed pattern, highlighting the potential role of the QBO in tropospheric chemistry and composition, as well as in model evaluation. The observed annual surface signal in the northern hemisphere matches well with the models run without emissions, indicating the annual cycle is driven mostly by stratosphere-troposphere exchange (STE) flux of N2O-depleted air and not surface N2O emissions. In the southern hemisphere (SH), all three models disagree and thus provide no guidance, except for indicating that modeling annual STE in the SH remains a major model uncertainty. Parallel model simulations of CFCl3, which has greater stratospheric loss that N2O and possibly surreptitious emissions, show that its interannual variations parallel those of N2O, and thus the observed N2O variability can identify the stratospheric component of the observed CFCl3 variability.
2021
Atmospheric nitrogen and sulfur deposition is an important effect of atmospheric pollution and may affect forest ecosystems positively, for example enhancing tree growth, or negatively, for example causing acidification, eutrophication, cation depletion in soil or nutritional imbalances in trees. To assess and design measures to reduce the negative impacts of deposition, a good estimate of the deposition amount is needed, either by direct measurement or by modeling. In order to evaluate the precision of both approaches and to identify possible improvements, we compared the deposition estimates obtained using an Eulerian model with the measurements performed by two large independent networks covering most of Europe. The results are in good agreement (bias <25%) for sulfate and nitrate open field deposition, while larger differences are more evident for ammonium deposition, likely due to the greater influence of local ammonia sources. Modeled sulfur total deposition compares well with throughfall deposition measured in forest plots, while the estimate of nitrogen deposition is affected by the tree canopy. The geographical distribution of pollutant deposition and of outlier sites where model and measurements show larger differences are discussed.
2021
2021
Low-risk removal of embedded surface soiling on delicate heritage objects can require novel alternatives to traditional cleaning systems. Edvard Munch’s monumental Aula paintings (1911–16) have a long history of exposure to atmospheric pollution and cleaning campaigns that have compromised the appearance and the condition of these important artworks. Soiling removal from porous and water-sensitive, unvarnished oil paintings continues to be a major conservation challenge. This paper presents the approach and results of research into the effect and efficiency of three novel systems used for soiling removal: soft particle blasting, CO2-snow blasting, and Nanorestore Gel® Dry and Peggy series hydrogels. Cleaning tests were performed on accelerated-aged and artificially soiled mock-ups consisting of unvarnished oil paint and chalk-glue grounds. Visual and analytical assessment (magnification using a light microscope and scanning electron microscope, as well as colour- and gloss measurement) was carried out before and after mock-up cleaning tests and the results were compared to those obtained using the dry polyurethane sponges employed in the most recent Aula surface cleaning campaign (2009–11). Although the results varied, the Nanorestore Gel® series proved promising with respect to improved soiling removal efficiency, and reduced pigment loss for the water-sensitive surfaces evaluated, compared to dry sponges.
2021
We synthesized N2O emissions over North America using 17 bottom-up (BU) estimates from 1980–2016 and five top-down (TD) estimates from 1998 to 2016. The BU-based total emission shows a slight increase owing to U.S. agriculture, while no consistent trend is shown in TD estimates. During 2007–2016, North American N2O emissions are estimated at 1.7 (1.0–3.0) Tg N yr−1 (BU) and 1.3 (0.9–1.5) Tg N yr−1 (TD). Anthropogenic emissions were twice as large as natural fluxes from soil and water. Direct agricultural and industrial activities accounted for 68% of total anthropogenic emissions, 71% of which was contributed by the U.S. Our estimates of U.S. agricultural emissions are comparable to the EPA greenhouse gas (GHG) inventory, which includes estimates from IPCC tier 1 (emission factor) and tier 3 (process-based modeling) approaches. Conversely, our estimated agricultural emissions for Canada and Mexico are twice as large as the respective national GHG inventories.
2021
The rise of advanced ICT technologies has made it possible to apply low-cost sensor systems for measuring air quality in citizen science projects, including education. High school students in Norway used these sensor systems in a citizen science project to design, carry out, and evaluate their own research projects on air quality. An impact assessment framework was designed to assess the impact of these activities, considering five areas of impact: scientific, social, economic, political, and environmental. In addition, the framework also considers the transformative potential of the citizen science pilot, i.e., the degree to which the pilot can help to change, alter, or replace current systems, and the business-as-usual in one or more fields such as knowledge production or environmental protection. Data for this assessment were gathered in the form of questionnaires that the students had to complete before starting and after finalizing the pilot activities. The results showed positive impacts on learning, a pro-environmental world view, and an increase in pro-science attitudes and interest in scientific and environmental-related topics at the end of the pilot activities. Only weak impacts were measured for behavioral change. The activities showed transformative potential, which makes the student activities an example of good practice for citizen science activities on air quality with low-cost sensors.
2021
The Arctic middle atmosphere was affected by major sudden stratospheric warmings (SSW) in February 2018 and January 2019, respectively. In this article, we report for the first time the impact of these two events on the middle atmospheric nitric oxide (NO) abundance. The study is based on measurements obtained during two dedicated observation campaigns, using the Sub-Millimetre Radiometer (SMR) aboard the Odin satellite, measuring NO globally since 2003. The SSW of February 2018 was similar to other, more dynamically quiet, Arctic winters in term of NO downward transport from the upper mesosphere–lower thermosphere to lower altitudes (referred to as energetic particle precipitation indirect effect EPP-IE). On the contrary, the event of January 2019 led to one of the strongest EPP-IE cases observed within the Odin operational period. Important positive NO anomalies were indeed observed in the lower mesosphere–upper stratosphere during the three months following the SSW onset, corresponding to NO volume mixing ratios more than 50 times higher than the climatological values. These different consequences on the middle atmospheric composition are explained by very different dynamical characteristics of these two SSW events.
2021
2021
Long-term monitoring of regulated organic chemicals, such as legacy persistent organic pollutants (POPs) and polycyclic aromatic hydrocarbons (PAHs), in ambient air provides valuable information about the compounds' environmental fate as well as temporal and spatial trends. This is the foundation to evaluate the effectiveness of national and international regulations for priority pollutants. Extracts of high-volume air samples, collected on glass fibre filters (GFF for particle phase) and polyurethane foam plugs (PUF for gaseous phase), for targeted analyses of legacy POPs are commonly cleaned by treatment with concentrated sulfuric acid, resulting in extracts clean from most interfering compounds and matrices that are suitable for multi-quantitative trace analysis. Such standardised methods, however, severely restrict the number of analytes for quantification and are not applicable when targeting new and emerging compounds as some may be less stable under acid treatment. Recently developed suspect and non-target screening analytical strategies (SUS and NTS, respectively) are shown to be effective evaluation tools aimed at identifying a high number of compounds of emerging concern. These strategies, combining highly sophisticated analytical technology with extensive data interpretation and statistics, are already widely accepted in environmental sciences for investigations of various environmental matrices, but their application to air samples is still very limited. In order to apply SUS and NTS for the identification of organic contaminants in air samples, an adapted and more wide-scope sample clean-up method is needed compared to the traditional method, which uses concentrated sulfuric acid. Analysis of raw air sample extracts without clean-up would generate extensive contamination of the analytical system, especially with PUF matrix-based compounds, and thus highly interfered mass spectra and detection limits which are unacceptable high for trace analysis in air samples.
In this study, a novel wide-scope sample clean-up method for high-volume air samples has been developed and applied to real high-volume air samples, which facilitates simultaneous target, suspect and non-target analyses. The scope and efficiency of the method were quantitatively evaluated with organic compounds covering a wide range of polarities (logP 2–11), including legacy POPs, brominated flame retardants (BFRs), chlorinated pesticides and currently used pesticides (CUPs). In addition, data reduction and selection strategies for SUS and NTS were developed for comprehensive two-dimensional gas chromatography separation with low-resolution time-of-flight mass spectrometric detection (GC × GC-LRMS) data and applied to real high-volume air samples. Combination of the newly developed clean-up procedure and data treatment strategy enabled the prioritisation of over 600 compounds of interest in the particle phase (on GFF) and over 850 compounds in the gas phase (on PUF) out of over 25 000 chemical features detected in the raw dataset. Of these, 50 individual compounds were identified and confirmed with reference standards, 80 compounds were identified with a probable structure, and 774 compounds were assigned to various compound classes. In the dataset available here, 11 hitherto unknown halogenated compounds were detected. These unknown compounds were not yet listed in the available mass spectral libraries.
2021