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We determine the global emission distribution of the potent greenhouse gas sulfur hexafluoride (SF6) for the period 2005–2021 using inverse modelling. The inversion is based on 50 d backward simulations with the Lagrangian particle dispersion model (LPDM) FLEXPART and on a comprehensive observation data set of SF6 mole fractions in which we combine continuous with flask measurements sampled at fixed surface locations and observations from aircraft and ship campaigns. We use a global-distribution-based (GDB) approach to determine baseline mole fractions directly from global SF6 mole fraction fields at the termination points of the backward trajectories. We compute these fields by performing an atmospheric SF6 re-analysis, assimilating global SF6 observations into modelled global three-dimensional mole fraction fields. Our inversion results are in excellent agreement with several regional inversion studies in the USA, Europe, and China. We find that (1) annual US SF6 emissions strongly decreased from 1.25 Gg in 2005 to 0.48 Gg in 2021; however, they were on average twice as high as the reported emissions to the United Nations. (2) SF6 emissions from EU countries show an average decreasing trend of −0.006 Gg yr−1 during the period 2005 to 2021, including a substantial drop in 2018. This drop is likely a direct result of the EU's F-gas regulation 517/2014, which bans the use of SF6 for recycling magnesium die-casting alloys as of 2018 and requires leak detection systems for electrical switch gear. (3) Chinese annual emissions grew from 1.28 Gg in 2005 to 5.16 Gg in 2021, with a trend of 0.21 Gg yr−1, which is even higher than the average global total emission trend of 0.20 Gg yr−1. (4) National reports for the USA, Europe, and China all underestimated their SF6 emissions. (5) Our results indicate increasing emissions in poorly monitored areas (e.g. India, Africa, and South America); however, these results are uncertain due to weak observational constraints, highlighting the need for enhanced monitoring in these areas. (6) Global total SF6 emissions are comparable to estimates in previous studies but are sensitive to a priori estimates due to the low network sensitivity in poorly monitored regions. (7) Monthly inversions indicate that SF6 emissions in the Northern Hemisphere were on average higher in summer than in winter throughout the study period.

Numerical methods and simulation codes are essential for the advancement of our understanding of complex atmospheric processes. As technology and computer hardware continue to evolve, the development of sophisticated code is vital for accurate and efficient simulations. In this paper, we present the recent advancements made in the FLEXible PARTicle dispersion model (FLEXPART), a Lagrangian particle dispersion model, which has been used in a wide range of atmospheric transport studies over the past 3 decades, extending from tracing radionuclides from the Fukushima nuclear disaster, to inverse modelling of greenhouse gases, and to the study of atmospheric moisture cycles. This version of FLEXPART includes notable improvements in accuracy and computational efficiency. (1) By leveraging the native vertical coordinates of European Centre for Medium Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS) instead of interpolating to terrain-following coordinates, we achieved an improvement in trajectory accuracy, leading to a ∼8 %–10 % reduction in conservation errors for quasi-conservative quantities like potential vorticity. (2) The shape of aerosol particles is now accounted for in the gravitational settling and dry-deposition calculation, increasing the simulation accuracy for non-spherical aerosol particles such as microplastic fibres. (3) Wet deposition has been improved by the introduction of a new below-cloud scheme, by a new cloud identification scheme, and by improving the interpolation of precipitation. (4) Functionality from a separate version of FLEXPART, the FLEXPART CTM (chemical transport model), is implemented, which includes linear chemical reactions. Additionally, the incorporation of Open Multi-Processing parallelisation makes the model better suited for handling large input data. Furthermore, we introduced novel methods for the input and output of particle properties and distributions. Users now have the option to run FLEXPART with more flexible particle input data, providing greater adaptability for specific research scenarios (e.g. effective backward simulations corresponding to satellite retrievals). Finally, a new user manual (https://flexpart.img.univie.ac.at/docs/, last access: 11 September 2024) and restructuring of the source code into modules will serve as a basis for further development.

Individual high-Alpine ice cores have been proven to contain a well-preserved history of past anthropogenic air pollution in western Europe. The question of how representative one ice core is with respect to the reconstruction of atmospheric composition in the source region has not been addressed so far. Here, we present the first study systematically comparing longer-term ice-core records (1750–2015 CE) of various anthropogenic compounds, such as major inorganic aerosol constituents (NH4+, NO3-, SO42-), black carbon (BC), and trace species (Cd, F−, Pb). Depending on the data availability for the different air pollutants, up to five ice cores from four high-Alpine sites located in the European Alps analysed by different laboratories were considered. Whereas absolute concentration levels can partly differ depending on the prevailing seasonal distribution of accumulated precipitation, all seven investigated anthropogenic compounds are in excellent agreement between the various sites for their respective, species-dependent longer-term concentration trends. This is related to common source regions of air pollution impacting the four sites less than 100 km away including western European countries surrounding the Alps. For individual compounds, the Alpine ice-core composites developed in this study allowed us to precisely time the onset of pollution caused by industrialization in western Europe. Extensive emissions from coal combustion and agriculture lead to an exceeding of pre-industrial (1750–1850) concentration levels already at the end of the 19th century for BC, Pb, exSO42- (non-dust, non-sea salt SO42-), and NH4+, respectively. However, Cd, F−, and NO3- concentrations started surpassing pre-industrial values only in the 20th century, predominantly due to pollution from zinc and aluminium smelters and traffic. The observed maxima of BC, Cd, F−, Pb, and exSO42- concentrations in the 20th century and a significant decline afterwards clearly reveal the efficiency of air pollution control measures such as the desulfurization of coal, the introduction of filters and scrubbers in power plants and metal smelters, and the ban of leaded gasoline improving the air quality in western Europe. In contrast, NO3- and NH4+ concentration records show levels in the beginning of the 21th century which are unprecedented in the context of the past 250 years, indicating that the introduced abatement measures to reduce these pollutants were insufficient to have a major effect at high altitudes in western Europe. Only four ice-core composite records (BC, F−, Pb, exSO42-) of the seven investigated pollutants correspond well with modelled trends, suggesting inaccuracies of the emission estimates or an incomplete representation of chemical reaction mechanisms in the models for the other pollutants. Our results demonstrate that individual ice-core records from different sites in the European Alps generally provide a spatially representative signal of anthropogenic air pollution trends in western European countries.

Using the example of sulfur hexafluoride (SF6), we investigate the use of Lagrangian particle dispersion models (LPDMs) for inverse modeling of greenhouse gas (GHG) emissions and explore the limitations of this approach. We put the main focus on the impacts of baseline methods and the LPDM backward simulation period on the a posteriori emissions determined by the inversion. We consider baseline methods that are based on a statistical selection of observations at individual measurement sites and a global-distribution-based (GDB) approach, where global mixing ratio fields are coupled to the LPDM back-trajectories at their termination points. We show that purely statistical baseline methods can cause large systematic errors, which lead to inversion results that are sensitive to the LPDM backward simulation period and can generate unrealistic global total a posteriori emissions. The GDB method produces a posteriori emissions that are far less sensitive to the backward simulation period and that show a better agreement with recognized global total emissions. Our results show that longer backward simulation periods, beyond the often used 5 to 10 d, reduce the mean squared error and increase the correlation between a priori modeled and observed mixing ratios. Also, the inversion becomes less sensitive to biases in the a priori emissions and the global mixing ratio fields for longer backward simulation periods. Further, longer periods might help to better constrain emissions in regions poorly covered by the global SF6 monitoring network. We find that the inclusion of existing flask measurements in the inversion helps to further close these gaps and suggest that a few additional and well-placed flask sampling sites would have great value for improving global a posteriori emission fields.

This study presents simulations of Greenland surface melt for the Eemian interglacial period (∼130 000 to 115 000 years ago) derived from regional climate simulations with a coupled surface energy balance model. Surface melt is of high relevance due to its potential effect on ice core observations, e.g., lowering the preserved total air content (TAC) used to infer past surface elevation. An investigation of surface melt is particularly interesting for warm periods with high surface melt, such as the Eemian interglacial period. Furthermore, Eemian ice is the deepest and most compressed ice preserved on Greenland, resulting in our inability to identify melt layers visually. Therefore, simulating Eemian melt rates and associated melt layers is beneficial to improve the reconstruction of past surface elevation. Estimated TAC, based on simulated melt during the Eemian, could explain the lower TAC observations. The simulations show Eemian surface melt at all deep Greenland ice core locations and an average of up to ∼30 melt days per year at Dye-3, corresponding to more than 600 mm water equivalent (w.e.) of annual melt. For higher ice sheet locations, between 60 and 150 mmw.e.yr-1 on average are simulated. At the summit of Greenland, this yields a refreezing ratio of more than 25 % of the annual accumulation. As a consequence, high melt rates during warm periods should be considered when interpreting Greenland TAC fluctuations as surface elevation changes. In addition to estimating the influence of melt on past TAC in ice cores, the simulated surface melt could potentially be used to identify coring locations where Greenland ice is best preserved.

The Greenland ice sheet contributes increasingly to global sea level rise. Its history during past warm intervals is a valuable reference for future sea level projections. We present ice sheet simulations for the Eemian interglacial period (∼130 000 to 115 000 years ago), a period with warmer-than-present summer climate over Greenland. The evolution of the Eemian Greenland ice sheet is simulated with a 3-D higher-order ice sheet model, forced with a surface mass balance derived from regional climate simulations. Sensitivity experiments with various surface mass balances, basal friction, and ice flow approximations are discussed. The surface mass balance forcing is identified as the controlling factor setting the minimum in Eemian ice volume, emphasizing the importance of a reliable surface mass balance model. Furthermore, the results indicate that the surface mass balance forcing is more important than the representation of ice flow for simulating the large-scale ice sheet evolution. This implies that modeling of the future contribution of the Greenland ice sheet to sea level rise highly depends on an accurate surface mass balance.

Understanding the behavior of the Greenland ice sheet in a warmer climate, and particularly its surface mass balance (SMB), is important for assessing Greenland's potential contribution to future sea level rise. The Eemian interglacial period, the most recent warmer-than-present period in Earth's history approximately 125 000 years ago, provides an analogue for a warm summer climate over Greenland. The Eemian is characterized by a positive Northern Hemisphere summer insolation anomaly, which complicates Eemian SMB calculations based on positive degree day estimates. In this study, we use Eemian global and regional climate simulations in combination with three types of SMB models – a simple positive degree day, an intermediate complexity, and a full surface energy balance model – to evaluate the importance of regional climate and model complexity for estimates of Greenland's SMB. We find that all SMB models perform well under the relatively cool pre-industrial and late Eemian. For the relatively warm early Eemian, the differences between SMB models are large, which is associated with whether insolation is included in the respective models. For all simulated time slices, there is a systematic difference between globally and regionally forced SMB models, due to the different representation of the regional climate over Greenland. We conclude that both the resolution of the simulated climate as well as the method used to estimate the SMB are important for an accurate simulation of Greenland's SMB. Whether model resolution or the SMB method is most important depends on the climate state and in particular the prevailing insolation pattern. We suggest that future Eemian climate model intercomparison studies should include SMB estimates and a scheme to capture SMB uncertainties.

The new mission concept of microwave and infrared-laser occultation between low-Earth-orbit satellites (LMIO) is designed to provide accurate and long-term stable profiles of atmospheric thermodynamic variables, greenhouse gases (GHGs), and line-of-sight (l.o.s.) wind speed with focus on the upper troposphere and lower stratosphere (UTLS). While the unique quality of GHG retrievals enabled by LMIO over the UTLS has been recently demonstrated based on end-to-end simulations, the promise of l.o.s. wind retrieval, and of joint GHG and wind retrieval, has not yet been analyzed in any realistic simulation setting. Here we use a newly developed l.o.s. wind retrieval algorithm, which we embedded in an end-to-end simulation framework that also includes the retrieval of thermodynamic variables and GHGs, and analyze the performance of both stand-alone wind retrieval and joint wind and GHG retrieval. The wind algorithm utilizes LMIO laser signals placed on the inflection points at the wings of the highly symmetric C18OO absorption line near 4767 cm−1 and exploits transmission differences from a wind-induced Doppler shift. Based on realistic example cases for a diversity of atmospheric conditions, ranging from tropical to high-latitude winter, we find that the retrieved l.o.s. wind profiles are of high quality over the lower stratosphere under all conditions, i.e., unbiased and accurate to within about 2 m s−1 over about 15 to 35 km. The wind accuracy degrades into the upper troposphere due to the decreasing signal-to-noise ratio of the wind-induced differential transmission signals. The GHG retrieval in windy air is not vulnerable to wind speed uncertainties up to about 10 m s−1 but is found to benefit in the case of higher speeds from the integrated wind retrieval that enables correction of wind-induced Doppler shift of GHG signals. Overall both the l.o.s. wind and GHG retrieval results are strongly encouraging towards further development and implementation of a LMIO mission.

Ancient texts and archaeological evidence indicate substantial lead exposure during antiquity that potentially impacted human health. Although lead exposure routes were many and included the use of glazed tablewares, paints, cosmetics, and even intentional ingestion, the most significant for the nonelite, rural majority of the population may have been through background air pollution from mining and smelting of silver and lead ores that underpinned the Roman economy. Here, we determined potential health effects of this air pollution using Arctic ice core measurements of Roman-era lead pollution, atmospheric modeling, and modern epidemiology-based relationships between air concentrations, blood lead levels (BLLs), and cognitive decline. Findings suggest air lead concentrations exceeded 150 ng/m3 near metallurgical emission sources, with average enhancements of >1.0 ng/m3 over Europe during the Pax Romana apogee of the Roman Empire. The result was blood lead enhancements in young children of about 2.4 µg/dl above an estimated Neolithic background of 1.0 µg/dl, leading to widespread cognitive decline including a 2.5-to-3 point reduction in intelligence quotient throughout the Roman Empire. [ABSTRACT FROM AUTHOR]

Atmospheric ammonia (NH3) is a key transboundary air pollutant that contributes to the impacts of nitrogen and acidity on terrestrial ecosystems. Ammonia also contributes to the atmospheric aerosol that affects air quality. Emission inventories indicate that NH3 was predominantly emitted by agriculture over the 19th and 20th centuries but, up to now, these estimates have not been compared to long-term observations. To document past atmospheric NH3 pollution in south-eastern Europe, ammonium (NH 4+) was analysed along an ice core extracted from Mount Elbrus in the Caucasus, Russia. The NH 4+ ice-core record indicates a 3.5-fold increase in concentrations between 1750 and 1990 CE. Remaining moderate prior to 1950 CE, the increase then accelerated to reach a maximum in 1989 CE. Comparison between ice-core trends and estimated past emissions using state-of-the-art atmospheric transport modelling of submicron-scale aerosols (FLEXPART (FLEXible PARTicle dispersion) model) indicates good agreement with the course of estimated NH3 emissions from south-eastern Europe since ∼ 1750 CE, with the main contributions from south European Russia, Türkiye, Georgia, and Ukraine. Examination of ice deposited prior to 1850 CE, when agricultural activities remained limited, suggests an NH 4+ ice concentration related to natural soil emissions representing ∼ 20 % of the 1980–2009 CE NH 4+ level, a level mainly related to current agricultural emissions that almost completely outweigh biogenic emissions from natural soil. These findings on historical NH3 emission trends represent a significant contribution to the understanding of ammonia emissions in Europe over the last 250 years. [ABSTRACT FROM AUTHOR]

Numerical methods and simulation codes are essential for the advancement of our understanding of complex atmospheric processes. As technology and computer hardware continue to evolve, the development of sophisticated code is vital for accurate and efficient simulations. In this paper, we present the recent advancements made in the FLEXible PARTicle dispersion model (FLEXPART), a Lagrangian particle dispersion model, which has been used in a wide range of atmospheric transport studies over the past 3 decades, extending from tracing radionuclides from the Fukushima nuclear disaster, to inverse modelling of greenhouse gases, and to the study of atmospheric moisture cycles. This version of FLEXPART includes notable improvements in accuracy and computational efficiency. (1) By leveraging the native vertical coordinates of European Centre for Medium Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS) instead of interpolating to terrain-following coordinates, we achieved an improvement in trajectory accuracy, leading to a ∼8 %–10 % reduction in conservation errors for quasi-conservative quantities like potential vorticity. (2) The shape of aerosol particles is now accounted for in the gravitational settling and dry-deposition calculation, increasing the simulation accuracy for non-spherical aerosol particles such as microplastic fibres. (3) Wet deposition has been improved by the introduction of a new below-cloud scheme, by a new cloud identification scheme, and by improving the interpolation of precipitation. (4) Functionality from a separate version of FLEXPART, the FLEXPART CTM (chemical transport model), is implemented, which includes linear chemical reactions. Additionally, the incorporation of Open Multi-Processing parallelisation makes the model better suited for handling large input data. Furthermore, we introduced novel methods for the input and output of particle properties and distributions. Users now have the option to run FLEXPART with more flexible particle input data, providing greater adaptability for specific research scenarios (e.g. effective backward simulations corresponding to satellite retrievals). Finally, a new user manual (https://flexpart.img.univie.ac.at/docs/ , last access: 11 September 2024) and restructuring of the source code into modules will serve as a basis for further development. [ABSTRACT FROM AUTHOR]

We determine the global emission distribution of the potent greenhouse gas sulfur hexafluoride (SF6) for the period 2005–2021 using inverse modelling. The inversion is based on 50 d backward simulations with the Lagrangian particle dispersion model (LPDM) FLEXPART and on a comprehensive observation data set of SF6 mole fractions in which we combine continuous with flask measurements sampled at fixed surface locations and observations from aircraft and ship campaigns. We use a global-distribution-based (GDB) approach to determine baseline mole fractions directly from global SF6 mole fraction fields at the termination points of the backward trajectories. We compute these fields by performing an atmospheric SF6 re-analysis, assimilating global SF6 observations into modelled global three-dimensional mole fraction fields. Our inversion results are in excellent agreement with several regional inversion studies in the USA, Europe, and China. We find that (1) annual US SF6 emissions strongly decreased from 1.25 Gg in 2005 to 0.48 Gg in 2021; however, they were on average twice as high as the reported emissions to the United Nations. (2) SF6 emissions from EU countries show an average decreasing trend of -0.006 Gg yr−1 during the period 2005 to 2021, including a substantial drop in 2018. This drop is likely a direct result of the EU's F-gas regulation 517/2014, which bans the use of SF6 for recycling magnesium die-casting alloys as of 2018 and requires leak detection systems for electrical switch gear. (3) Chinese annual emissions grew from 1.28 Gg in 2005 to 5.16 Gg in 2021, with a trend of 0.21 Gg yr−1, which is even higher than the average global total emission trend of 0.20 Gg yr−1. (4) National reports for the USA, Europe, and China all underestimated their SF6 emissions. (5) Our results indicate increasing emissions in poorly monitored areas (e.g. India, Africa, and South America); however, these results are uncertain due to weak observational constraints, highlighting the need for enhanced monitoring in these areas. (6) Global total SF6 emissions are comparable to estimates in previous studies but are sensitive to a priori estimates due to the low network sensitivity in poorly monitored regions. (7) Monthly inversions indicate that SF6 emissions in the Northern Hemisphere were on average higher in summer than in winter throughout the study period. [ABSTRACT FROM AUTHOR]

Antibody-mediated complement-dependent cytotoxicity (CDC) on malignant cells is regulated by several complement control proteins, including the inhibitory complement factor H (fH). fH consists of 20 short consensus repeat elements (SCRs) with specific functional domains. Previous research revealed that the fH-derived SCRs 19-20 (SCR1920) can displace full-length fH on the surface of chronic lymphocytic leukemia (CLL) cells, which sensitizes CLL cells for e.g. CD20-targeting therapeutic monoclonal antibody (mAb) induced CDC. Therefore, we constructed lentiviral vectors for the generation of cell lines that stably produce mAb-SCR-fusion variants starting from the clinically approved parental mAbs rituximab, obinutuzumab and ofatumumab, respectively. Flowcytometry revealed that the modification of the mAbs by the SCRs does not impair the binding to CD20. Increased in vitro lysis potency compared to their parental mAbs was corroborated by showing specific and dose dependent target cell elimination by CDC when compared to their parental mAbs. Lysis of CLL cells was not affected by the depletion of NK cells, suggesting that antibodydependent cellular cytotoxicity plays a minor role in this context. Overall, this study emphasizes the crucial role of CDC in the elimination of CLL cells by mAbs and introduces a novel approach for enhancing CDC by directly fusing fH SCR1920 with mAbs. [ABSTRACT FROM AUTHOR]

This paper focuses on nonpharmaceutical interventions (NPIs) to explain fertility dynamics during the pandemic, while considering countries' institutional context. We argue that containment policies disrupted people's lives and increased their uncertainty more in countries with weak welfare support systems, while health‐related and economic support NPIs mitigated such disruptions much more there, as they were less expected by citizens. We estimate monthly "excess" crude birth rates (CBRs) and find that countries with low public support—Southern Europe, East Asia, and Eastern Europe—experienced larger decreases and less of a rebound in CBRs than countries with histories of high public spending—Western, Central, and Northern Europe. However, in low support countries, NPIs are much more strongly associated with excess CBRs—containment NPIs more negatively and health and economic support NPIs more positively—with the exception of the one‐month lag of containment NPIs, for which the opposite holds. When putting these coefficients into broader perspective, our findings suggest that the actual implementation of all NPIs taken together mitigated fertility declines. This is especially the case for low public support countries, whereas one might have seen a birth decline even in high support countries if the NPIs were not implemented. [ABSTRACT FROM AUTHOR]