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Knowledge architecture for the wise governance of sustainability transitions

Oliver, Tom H.; Benini, Lorenzo; Borja, Angel; Dupont, Claire; Doherty, Bob; Grodzinska-Jurczak, Malgorzata; Iglesias, Ana; Jordan, Andrew; Kass, Gary; Lung, Tobias; Maguire, Kathy; McGonigle, Dan; Mickwitz, Per; Spangenberg, Joachim H.; Tarrasón, Leonor

The need for sustainability transitions is widely recognised, along with a concurrent need for the evolution of knowledge systems to inform more effective policy action. Although there are many new policy targets relating to net zero emissions and other sustainability challenges, cities, regional and national governments are struggling to rapidly develop transformational policies to achieve them. As academics and practitioners who work at the science-policy interface, we identify specific knowledge and competency needs for governing sustainability transitions related to the interlinked phases of envisioning, implementing and evaluating. In short, coordinated reforms of both policy and knowledge systems are urgently needed to address the speed and scale of sustainability challenges. These include embedding systems thinking literacy, mainstreaming participatory policy making, expanding the capacity to undertake transdisciplinary research, more adaptive governance and continuous organisational learning. These processes must guide further knowledge development, uptake and use as part of an iterative and holistic process. Such deep-seated change in policy-knowledge systems will be disruptive and presents challenges for traditional organisational models of knowledge delivery, but is essential for successful sustainability transformations.

2021

Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo

Hamer, Paul David; Marécal, Virginie; Hossaini, Ryan; Pirre, Michel; Krysztofiak, Gisele; Ziska, Franziska; Engel, Andreas; Sala, Stephan; Keber, Timo; Bönisch, Harald; Atlas, Elliot; Krüger, Kirstin; Chipperfield, Martyn; Catoire, Valery; Samah, Azizan A.; Dorf, Marcel; Moi, Phang Siew; Schlager, Hans; Pfeilsticker, Klaus

This paper presents a modelling study on the fate of CHBr3 and its product gases in the troposphere within the context of tropical deep convection. A cloud-scale case study was conducted along the west coast of Borneo, where several deep convective systems were triggered on the afternoon and early evening of 19 November 2011. These systems were sampled by the Falcon aircraft during the field campaign of the SHIVA project and analysed using a simulation with the cloud-resolving meteorological model C-CATT-BRAMS at 2×2 km resolution that represents the emissions, transport by large-scale flow, convection, photochemistry, and washout of CHBr3 and its product gases (PGs). We find that simulated CHBr3 mixing ratios and the observed values in the boundary layer and the outflow of the convective systems agree. However, the model underestimates the background CHBr3 mixing ratios in the upper troposphere, which suggests a missing source at the regional scale. An analysis of the simulated chemical speciation of bromine within and around each simulated convective system during the mature convective stage reveals that >85 % of the bromine derived from CHBr3 and its PGs is transported vertically to the point of convective detrainment in the form of CHBr3 and that the remaining small fraction is in the form of organic PGs, principally insoluble brominated carbonyls produced from the photo-oxidation of CHBr3. The model simulates that within the boundary layer and free troposphere, the inorganic PGs are only present in soluble forms, i.e. HBr, HOBr, and BrONO2, and, consequently, within the convective clouds, the inorganic PGs are almost entirely removed by wet scavenging. We find that HBr is the most abundant PG in background lower-tropospheric air and that this prevalence of HBr is a result of the relatively low background tropospheric ozone levels at the regional scale. Contrary to a previous study in a different environment, for the conditions in the simulation, the insoluble Br2 species is hardly formed within the convective systems and therefore plays no significant role in the vertical transport of bromine. This likely results from the relatively small quantities of simulated inorganic bromine involved, the presence of HBr in large excess compared to HOBr and BrO, and the relatively efficient removal of soluble compounds within the convective column.

2021

Real-time UV index retrieval in Europe using Earth observation-based techniques: system description and quality assessment

Kosmopoulos, Panagiotis G.; Kazadzis, Stelios; Schmalwieser, Alois W.; Raptis, Panagiotis I.; Papachristopoulou, Kyriakoula; Fountoulakis, Ilias; Masoom, Akriti; Bais, Alkiviadis F.; Bilbao, Julia; Blumthaler, Mario; Kreuter, Axel; Siani, Anna Maria; Eleftheratos, Kostas; Topaloglou, Chrystanthi; Gröbner, Julian; Johnsen, Bjørn; Svendby, Tove Marit; Vilaplana, Jose Manuel; Doppler, Lionel; Webb, Ann R; Khazova, Marina; Backer, Hugo De; Heikkilä, Anu; Lakkala, Kaisa; Jaroslawski, Janusz; Meleti, Charikleia; Diémoz, Henri; Hülsen, Gregor; Klotz, Barbara; Rimmer, John; Kontoes, Charalampos

This study introduces an Earth observation (EO)-based system which is capable of operationally estimating and continuously monitoring the ultraviolet index (UVI) in Europe. UVIOS (i.e., UV-Index Operating System) exploits a synergy of radiative transfer models with high-performance computing and EO data from satellites (Meteosat Second Generation and Meteorological Operational Satellite-B) and retrieval processes (Tropospheric Emission Monitoring Internet Service, Copernicus Atmosphere Monitoring Service and the Global Land Service). It provides a near-real-time nowcasting and short-term forecasting service for UV radiation over Europe. The main atmospheric inputs for the UVI simulations include ozone, clouds and aerosols, while the impacts of ground elevation and surface albedo are also taken into account. The UVIOS output is the UVI at high spatial and temporal resolution (5 km and 15 min, respectively) for Europe (i.e., 1.5 million pixels) in real time. The UVI is empirically related to biologically important UV dose rates, and the reliability of this EO-based solution was verified against ground-based measurements from 17 stations across Europe. Stations are equipped with spectral, broadband or multi-filter instruments and cover a range of topographic and atmospheric conditions. A period of over 1 year of forecasted 15 min retrievals under all-sky conditions was compared with the ground-based measurements. UVIOS forecasts were within ±0.5 of the measured UVI for at least 70 % of the data compared at all stations. For clear-sky conditions the agreement was better than 0.5 UVI for 80 % of the data. A sensitivity analysis of EO inputs and UVIOS outputs was performed in order to quantify the level of uncertainty in the derived products and to identify the covariance between the accuracy of the output and the spatial and temporal resolution and the quality of the inputs. Overall, UVIOS slightly overestimated the UVI due to observational uncertainties in inputs of cloud and aerosol. This service will hopefully contribute to EO capabilities and will assist the provision of operational early warning systems that will help raise awareness among European Union citizens of the health implications of high UVI doses.

2021

Global intercomparison of polyurethane foam passive air samplers evaluating sources of variability in SVOC measurements

Melymuk, Lisa; Bohlin-Nizzetto, Pernilla; Harner, Tom; White, Kevin B.; Wang, Xianyu; Tominaga, Maria Yumiko; He, Jun; Li, Jun; Ma, Jianmin; Ma, Wan-Lin; Aristizábal, Beatriz H.; Dreyer, Annekatrin; Jiménez, Begoña; Muñoz-Arnanz, Juan; Odabasi, Mustafa; Dumanoglu, Yetikin; Yaman, Baris; Graf, Carola; Sweetman, Andrew; Klánova, Jana

Polyurethane foam passive air samplers (PUF-PAS) are the most common type of passive air sampler used for a range of semi-volatile organic compounds (SVOCs), including regulated persistent organic pollutants (POPs) and polycyclic aromatic hydrocarbons (PAHs), and emerging contaminants (e.g., novel flame retardants, phthalates, current-use pesticides). Data from PUF-PAS are key indicators of effectiveness of global regulatory actions on SVOCs, such as the Global Monitoring Plan of the Stockholm Convention on Persistent Organic Pollutants. While most PUF-PAS use similar double-dome metal shielding, there is no standardized dome size, shape, or deployment configuration, with many different PUF-PAS designs used in regional and global monitoring. Yet, no information is available on the comparability of data from studies using different PUF-PAS designs. We brought together 12 types of PUF-PAS used by different research groups around the world and deployed them in a multi-part intercomparison to evaluate the variability in reported concentrations introduced by different elements of PAS monitoring. PUF-PAS were deployed for 3 months in outdoor air in Kjeller, Norway in 2015–2016 in three phases to capture (1) the influence of sampler design on data comparability, (2) the influence of analytical variability when samplers are analyzed at different laboratories, and (3) the overall variability in global monitoring data introduced by differences in sampler configurations and analytical methods. Results indicate that while differences in sampler design (in particular, the spacing between the upper and lower sampler bowls) account for up to 50 % differences in masses collected by samplers, the variability introduced by analysis in different laboratories far exceeds this amount, resulting in differences spanning orders of magnitude for POPs and PAHs. The high level of variability due to analysis in different laboratories indicates that current SVOC air sampling data (i.e., not just for PUF-PAS but likely also for active air sampling) are not directly comparable between laboratories/monitoring programs. To support on-going efforts to mobilize more SVOC data to contribute to effectiveness evaluation, intercalibration exercises to account for uncertainties in air sampling, repeated at regular intervals, must be established to ensure analytical comparability and avoid biases in global-scale assessments of SVOCs in air caused by differences in laboratory performance.

2021

A Bad Start in Life? Maternal Transfer of Legacy and Emerging Poly- And Perfluoroalkyl Substances to Eggs in an Arctic Seabird.

Jouanneau, William; Leándri-Breton, Don-Jean; Corbeau, Alexandre; Herzke, Dorte; Moe, Børge; Nikiforov, Vladimir; Gabrielsen, Geir W.; Chastel, Olivier

In birds, maternal transfer is a major exposure route for several contaminants, including poly- and perfluoroalkyl substances (PFAS). Little is known, however, about the extent of the transfer of the different PFAS compounds to the eggs, especially for alternative fluorinated compounds. In the present study, we measured legacy and emerging PFAS, including Gen-X, ADONA, and F-53B, in the plasma of prelaying black-legged kittiwake females breeding in Svalbard and the yolk of their eggs. We aimed to (1) describe the contaminant levels and patterns in both females and eggs, and (2) investigate the maternal transfer, that is, biological variables and the relationship between the females and their eggs for each compound. Contamination of both females and eggs were dominated by linPFOS then PFUnA or PFTriA. We notably found 7:3 fluorotelomer carboxylic acid─a precursor of long-chain carboxylates─in 84% of the egg yolks, and provide the first documented finding of ADONA in wildlife. Emerging compounds were all below the detection limit in female plasma. There was a linear association between females and eggs for most of the PFAS. Analyses of maternal transfer ratios in females and eggs suggest that the transfer is increasing with PFAS carbon chain length, therefore the longest chain perfluoroalkyl carboxylic acids (PFCAs) were preferentially transferred to the eggs. The mean ∑PFAS in the second-laid eggs was 73% of that in the first-laid eggs. Additional effort on assessing the outcome of maternal transfers on avian development physiology is essential, especially for PFCAs and emerging fluorinated compounds which are under-represented in experimental studies.
black-legged kittiwake Rissa tridactyla top predator Svalbard PFAS emerging contaminants

2021

Seasonality of the particle number concentration and size distribution: a global analysis retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories

Rose, Clemence; Coen, Martine Collaud; Andrews, Elisabeth; Lin, Yong; Bossert, Isaline; Myhre, Cathrine Lund; Tuch, Thomas; Wiedensohler, Alfred; Fiebig, Markus; Aalto, Pasi; Alastuey, Andrés; Alonso-Blanco, Elisabeth; Andrade, Marcos; Artiñano, Begoña; Arsov, Todor; Baltensprenger, Urs; Bastian, Susanne; Bath, Olaf; Beukes, Johan Paul; Brem, Benjamin T.; Bukowiecki, Nicolas; Casquero-Vera, Juan Andres; Conil, Sébastien; Eleftheriadis, Konstantinos; Favez, Olivier; Flentje, Harald; Gini, Maria I.; Gómez-Moreno, Francisco Javier; Gysel-Beer, Martin; Hallar, Anna Gannet; Kalapov, Ivo; Kalivitis, Nikos; Kasper-Giebl, Anne; Keywood, Melita; Kim, Jeong Eun; Kim, Sang-Woo; Kristensson, Adam; Kulmala, Markku; Lihavainen, Heikki; Lin, Neng-Huei; Lyamani, Hassan; Marinoni, Angela; Santos, Sebastiao Martins Dos; Mayol-Bracero, Olga; Meinhardt, Frank; Merkel, Maik; Metzger, Jean-Marc; Mihalopoulos, Nikolaos; Ondráček, Jakub; Pandolfi, Marco; Pérez, Noemi; Petäjä, Tuukka; Petit, Jean-Eudes; Picard, David; Pichon, Jean-Marc; Pont, Veronique; Putaud, Jean-Philippe; Reisen, Fabienne; Sellegri, Karine; Sharma, Sangeeta; Schauer, Gerhard; Sheridan, Patrick; Sherman, James Patrick; Schwerin, Andreas; Sohmer, Ralf; Sorribas, Mar; Sun, Junying; Tulet, Pierre; Vakkari, Ville; Zyl, Pieter Gideon van; Velarde, Fernando; Villani, Paolo; Vratolis, Stergios; Wagner, Zdenek; Wang, Sheng-Hsiang; Weinhold, Kay; Weller, Rolf; Yela, Margarita; Ždímal, Vladimir; Laj, Paolo G.

Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle.

Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 102 cm−3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 103–104 cm−3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (∼ 102–103 cm−3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm−3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot.

Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.

2021

Introducing a nested multimedia fate and transport model for organic contaminants (NEM)

Breivik, Knut; Eckhardt, Sabine; McLachlan, Michael S; Wania, Frank

Some organic contaminants, including the persistent organic pollutants (POPs), have achieved global distribution through long range atmospheric transport (LRAT). Regulatory efforts, monitoring programs and modelling studies address the LRAT of POPs on national, continental (e.g. Europe) and/or global scales. Whereas national and continental-scale models require estimates of the input of globally dispersed chemicals from outside of the model domain, existing global-scale models either have relatively coarse spatial resolution or are so computationally demanding that it limits their usefulness. Here we introduce the Nested Exposure Model (NEM), which is a multimedia fate and transport model that is global in scale yet can achieve high spatial resolution of a user-defined target region without huge computational demands. Evaluating NEM by comparing model predictions for PCB-153 in air with measurements at nine long-term monitoring sites of the European Monitoring and Evaluation Programme (EMEP) reveals that nested simulations at a resolution of 1° × 1° yield results within a factor of 1.5 of observations at sites in northern Europe. At this resolution, the model attributes more than 90% of the atmospheric burden within any of the grid cells containing an EMEP site to advective atmospheric transport from elsewhere. Deteriorating model performance with decreasing resolution (15° × 15°, 5° × 5° and 1° × 1°), manifested by overestimation of concentrations across most of northern Europe by more than a factor of 3, illustrates the effect of numerical diffusion. Finally, we apply the model to demonstrate how the choice of spatial resolution affect predictions of atmospheric deposition to the Baltic Sea. While we envisage that NEM may be used for a wide range of applications in the future, further evaluation will be required to delineate the boundaries of applicability towards chemicals with divergent fate properties as well as in environmental media other than air.

2021

Assessment of Low-Cost Particulate Matter Sensor Systems against Optical and Gravimetric Methods in a Field Co-Location in Norway

Vogt, Matthias; Schneider, Philipp; Castell, Nuria; Hamer, Paul David

The increased availability of commercially-available low-cost air quality sensors combined with increased interest in their use by citizen scientists, community groups, and professionals is resulting in rapid adoption, despite data quality concerns. We have characterized three out-the-box PM sensor systems under different environmental conditions, using field colocation against reference equipment. The sensor systems integrate Plantower 5003, Sensirion SPS30 and Alphasense OCP-N3 PM sensors. The first two use photometry as a measuring technique, while the third one is an optical particle counter. For the performance evaluation, we co-located 3 units of each manufacturer and compared the results against optical (FIDAS) and gravimetric (KFG) methods for a period of 7 weeks (28 August to 19 October 2020). During the period from 2nd and 5th October, unusually high PM concentrations were observed due to a long-range transport episode. The results show that the highest correlations between the sensor systems and the optical reference are observed for PM1, with coefficients of determination above 0.9, followed by PM2.5. All the sensor units struggle to correctly measure PM10, and the coefficients of determination vary between 0.45 and 0.64. This behavior is also corroborated when using the gravimetric method, where correlations are significantly higher for PM2.5 than for PM10, especially for the sensor systems based on photometry. During the long range transport event the performance of the photometric sensors was heavily affected, and PM10 was largely underestimated. The sensor systems evaluated in this study had good agreement with the reference instrumentation for PM1 and PM2.5; however, they struggled to correctly measure PM10. The sensors also showed a decrease in accuracy when the ambient size distribution was different from the one for which the manufacturer had calibrated the sensor, and during weather conditions with high relative humidity. When interpreting and communicating air quality data measured using low-cost sensor systems, it is important to consider such limitations in order not to risk misinterpretation of the resulting data.

2021

Modeling study of the impact of SO2 volcanic passive emissions on the tropospheric sulfur budget

Lamotte, Claire; Guth, Jonathan; Marécal, Virginie; Cussac, Martin; Hamer, Paul David; Theys, Nicolas; Schneider, Philipp

Well constrained volcanic emissions inventories in chemistry transport models are necessary to study the impacts induced by these sources on the tropospheric sulfur composition and on sulfur species concentrations and depositions at the surface. In this paper, the changes induced by the update of the volcanic sulfur emissions inventory are studied using the global chemistry transport model MOCAGE (MOdèle de Chimie Atmosphérique à Grande Échelle). Unlike the previous inventory (Andres and Kasgnoc, 1998), the updated one (Carn et al., 2016, 2017) uses more accurate information and includes contributions from both passive degassing and eruptive emissions. Eruptions are provided as daily total amounts of sulfur dioxide (SO2) emitted by volcanoes in the Carn et al. (2016, 2017) inventories, and degassing emissions are provided as annual averages with the related mean annual uncertainties of those emissions by volcano. Information on plume altitudes is also available and has been used in the model. We chose to analyze the year 2013, for which only a negligible amount of eruptive volcanic SO2 emissions is reported, allowing us to focus the study on the impact of passive degassing emissions on the tropospheric sulfur budget. An evaluation against the Ozone Monitoring Instrument (OMI) SO2 total column and MODIS (Moderate-Resolution Imaging Spectroradiometer) aerosol optical depth (AOD) observations shows the improvements of the model results with the updated inventory. Because the global volcanic SO2 flux changes from 13 Tg yr−1 in Andres and Kasgnoc (1998) to 23.6 Tg yr−1 in Carn et al. (2016, 2017), significant differences appear in the global sulfur budget, mainly in the free troposphere and in the tropics. Even though volcanic SO2 emissions represent 15 % of the total annual sulfur emissions, the volcanic contribution to the tropospheric sulfate aerosol burden is 25 %, which is due to the higher altitude of emissions from volcanoes. Moreover, a sensitivity study on passive degassing emissions, using the annual uncertainties of emissions per volcano, also confirmed the nonlinear link between tropospheric sulfur species content with respect to volcanic SO2 emissions. This study highlights the need for accurate estimates of volcanic sources in chemistry transport models in order to properly simulate tropospheric sulfur species.

2021

Differentiation of coarse-mode anthropogenic, marine and dust particles in the High Arctic islands of Svalbard

Song, Congbo; Dall'Osto, Manuel; Lupi, Angelo; Mazzola, Mauro; Traversi, Rita; Becagli, Silvia; Gilardoni, Stefania; Vratolis, Stergios; Yttri, Karl Espen; Beddows, David C.S.; Schmale, Julia; Brean, James; Kramawijaya, Agung Ghani; Harrison, Roy M.; Shi, Zongbo

Understanding aerosol–cloud–climate interactions in the Arctic is key to predicting the climate in this rapidly changing region. Whilst many studies have focused on submicrometer aerosol (diameter less than 1 µm), relatively little is known about the supermicrometer aerosol (diameter above 1 µm). Here, we present a cluster analysis of multiyear (2015–2019) aerodynamic volume size distributions, with diameter ranging from 0.5 to 20 µm, measured continuously at the Gruvebadet Observatory in the Svalbard archipelago. Together with aerosol chemical composition data from several online and offline measurements, we apportioned the occurrence of the coarse-mode aerosols during the study period (mainly from March to October) to anthropogenic (two sources, 27 %) and natural (three sources, 73 %) origins. Specifically, two clusters are related to Arctic haze with high levels of black carbon, sulfate and accumulation mode (0.1–1 µm) aerosol. The first cluster (9 %) is attributed to ammonium sulfate-rich Arctic haze particles, whereas the second one (18 %) is attributed to larger-mode aerosol mixed with sea salt. The three natural aerosol clusters were open-ocean sea spray aerosol (34 %), mineral dust (7 %) and an unidentified source of sea spray-related aerosol (32 %). The results suggest that sea-spray-related aerosol in polar regions may be more complex than previously thought due to short- and long-distance origins and mixtures with Arctic haze, biogenic and likely blowing snow aerosols. Studying supermicrometer natural aerosol in the Arctic is imperative for understanding the impacts of changing natural processes on Arctic aerosol.

2021

Growing Atmospheric Emissions of Sulfuryl Fluoride

Gressent, Alicia; Rigby, Matthew; Ganesan, Anita L.; Prinn, Ronald G.; Manning, Alistair J.; Mühle, Jens; Salameh, Peter K.; Krummel, Paul; Fraser, Paul J.; Steele, Paul; Mitrevski, Blagoj; Weiss, Ray F.; Harth, Christina M.; Wang, Ray H.; O'Doherty, S.; Young, Dickon; Park, Sunyoung; Li, S.; Yao, Bo; Reimann, Stefan; Vollmer, Martin K.; Maione, Michela; Arduini, Jgor; Lunder, Chris Rene

The potent greenhouse gas sulfuryl fluoride (SO2F2) is increasingly used as a fumigant, replacing methyl bromide, whose structural and soil fumigation uses have been phased out under the Montreal Protocol. We use measurements on archived air samples and in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE) and a box model of the global atmosphere to show a global increase of SO2F2 mole fraction from 0.3 ± 0.02 to 2.5 ± 0.08 ppt along with a global increase in emissions from 0.5 ± 0.4 Gg yr−1 to 2.9 ± 0.4 Gg yr−1 from 1978 to 2019. Based on a hybrid model incorporating bottom-up industry data and a top-down downscaling approach, we estimate the spatial distribution and trend in SO2F2 regional emissions between 2000 and 2019 and propose that the global emissions increase is driven by the growing use of SO2F2 in structural fumigation in North America and in postharvest treatment of grains and other agricultural products worldwide.

2021

Seasonal Variation of Wet Deposition of Black Carbon at Ny-Ålesund, Svalbard

Mori, Tatsuhiro; Kondo, Yutaka; Ohata, Sho; Goto-Azuma, Kumiko; Fukuda, Kaori; Ogawa-Tsukagawa, Yoshimi; Moteki, Nobuhiro; Yoshida, Atsushi; Koike, Makoto; Sinha, P. R.; Oshima, Naga; Matsui, Hitoshi; Tobo, Yutaka; Yabuki, Masanori; Aas, Wenche

Black carbon (BC) aerosol deposited in and onto Arctic snow increases the snow's absorption of solar radiation and accelerates snowmelt. Concentrations of BC in the Arctic atmosphere and snow are controlled by wet deposition; however, details of this process are poorly understood owing to the scarcity of time-resolved measurements of BC in hydrometeors. We measured mass concentrations of BC in hydrometeors (CMBC) and in air (MBC) with 16% and 15% accuracies, respectively, at Ny-Ålesund, Svalbard during 2012–2019. Median monthly MBC and CMBC values showed similar seasonal variations, being high in winter-spring and low in summer. Median monthly BC wet deposition mass flux (FMBC) was highest in winter and lowest in summer, associated with seasonal patterns of CMBC and precipitation. Seasonally averaged BC size distributions in hydrometeors were similar except for summer. Measurements of MBC and CMBC in spring 2017 showed a size-independent removal efficiency, indicating that BC-containing particles were efficiently activated into cloud droplets. These observations at Ny-Ålesund were compared with observations at Barrow, Alaska, during 2013–2017. The near-surface MBC at Ny-Ålesund and Barrow had similar seasonal patterns; however, the two sites differed in CMBC and FMBC. In summer, CMBC was low at Ny-Ålesund but moderate at Barrow, likely reflecting differences in MBC in the lower troposphere. Seasonally averaged BC size distributions in hydrometeors were similar at both sites, suggesting that average BC size distributions are similar in the Arctic lower troposphere. The efficiency of BC removal tends to be size-independent during transport, leading to the observed similarity.

2021

Main sources controlling atmospheric burdens of persistent organic pollutants on a national scale

Halvorsen, Helene Lunder; Bohlin-Nizzetto, Pernilla; Eckhardt, Sabine; Gusev, Alexey; Krogseth, Ingjerd Sunde; Möckel, Claudia; Shatalov, Victor; Skogeng, Lovise Pedersen; Breivik, Knut

National long-term monitoring programs on persistent organic pollutants (POPs) in background air have traditionally relied on active air sampling techniques. Due to limited spatial coverage of active air samplers, questions remain (i) whether active air sampler monitoring sites are representative for atmospheric burdens within the larger geographical area targeted by the monitoring programs, and thus (ii) if the main sources affecting POPs in background air across a nation are understood. The main objective of this study was to explore the utility of spatial and temporal trends in concert with multiple modelling approaches to understand the main sources affecting polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in background air across a nation. For this purpose, a comprehensive campaign was carried out in summer 2016, measuring POPs in background air across Norway using passive air sampling. Results were compared to a similar campaign in 2006 to assess possible changes over one decade. We furthermore used the Global EMEP Multi-media Modeling System (GLEMOS) and the Flexible Particle dispersion model (FLEXPART) to predict and evaluate the relative importance of primary emissions, secondary emissions, long-range atmospheric transport (LRAT) and national emissions in controlling atmospheric burdens of PCB-153 on a national scale. The concentrations in air of both PCBs and most of the targeted OCPs were generally low, with the exception of hexachlorobenzene (HCB). A limited spatial variability for all POPs in this study, together with predictions by both models, suggest that LRAT dominates atmospheric burdens across Norway. Model predictions by the GLEMOS model, as well as measured isomeric ratios, further suggest that LRAT of some POPs are dictated by secondary emissions. Our results illustrate the utility of combining observations and mechanistic modelling approaches to help identify the main factors affecting atmospheric burdens of POPs across a nation, which, in turn, may be used to inform both national monitoring and control strategies.

2021

Dimethyl Sulfide-Induced Increase in Cloud Condensation Nuclei in the Arctic Atmosphere

Park, Ki-Tae; Yoon, Young Jun; Lee, Kitack; Tunved, Peter; Krejci, Radovan; Ström, Johan; Jang, Eunho; Kang, Hyo Jin; Jang, Seyhun; Park, Jiyeon; Lee, Bang Young; Traversi, Rita; Becagli, Silvia; Hermansen, Ove

Oceanic dimethyl sulfide (DMS) emissions have been recognized as a biological regulator of climate by contributing to cloud formation. Despite decades of research, the climatic role of DMS remains ambiguous largely because of limited observational evidence for DMS-induced cloud condensation nuclei (CCN) enhancement. Here, we report concurrent measurement of DMS, physiochemical properties of aerosol particles, and CCN in the Arctic atmosphere during the phytoplankton bloom period of 2010. We encountered multiple episodes of new particle formation (NPF) and particle growth when DMS mixing ratios were both low and high. The growth of particles to sizes at which they can act as CCN accelerated in response to an increase in atmospheric DMS. Explicitly, the sequential increase in all relevant parameters (including the source rate of condensable vapor, the growth rate of particles, Aitken mode particles, hygroscopicity, and CCN) was pronounced at the DMS-derived NPF and particle growth events. This field study unequivocally demonstrates the previously unconfirmed roles of DMS in the growth of particles into climate-relevant size and eventual CCN activation.

2021

Good Agreement Between Modeled and Measured Sulfur and Nitrogen Deposition in Europe, in Spite of Marked Differences in Some Sites

Marchetto, Aldo; Simpson, David; Aas, Wenche; Fagerli, Hilde; Hansen, Karin; Pihl-Karlsson, Gunilla; Karlsson, Per Erik; Rogora, Michela; Sanders, Tanja G.M.; Schmitz, Andreas; Seidling, Walter; Thimonier, Anne; Tsyro, Svetlana; Vries, Wim de; Waldner, Peter

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

Black Carbon Emission Reduction Due to COVID-19 Lockdown in China

Jia, Mengwei; Evangeliou, Nikolaos; Eckhardt, Sabine; Huang, Xin; Gao, Jian; Ding, Aijun; Stohl, Andreas

During the Lunar New Year Holiday of 2020, China implemented an unprecedented lockdown to fight the COVID-19 outbreak, which strongly affected the anthropogenic emissions. We utilized elemental carbon observations (equivalent to black carbon, BC) from 42 sites and performed inverse modeling to determine the impact of the lockdown on the weekly BC emissions and quantify the effect of the stagnant conditions on BC observations in densely populated eastern and northern China. BC emissions declined 70% (eastern China) and 48% (northern China) compared to the first half of January. In northern China, under the stagnant conditions of the first week of the lockdown, the observed BC concentrations rose unexpectedly (29%) even though the BC emissions fell. The emissions declined substantially thereafter until a week after the lockdown ended. On the contrary, in eastern China, BC emissions dropped sharply in the first week and recovered synchronously with the end of the lockdown.

2021

Integrated water vapor during rain and rain-free conditions above the Swiss Plateau

Hocke, Klemens; Bernet, Leonie; Wang, Wenyue; Mätzler, Christian; Hervo, Maxime; Haefele, Alexander

Water vapor column density, or vertically-integrated water vapor (IWV), is monitored by ground-based microwave radiometers (MWR) and ground-based receivers of the Global Navigation Satellite System (GNSS). For rain periods, the retrieval of IWV from GNSS Zenith Wet Delay (ZWD) neglects the atmospheric propagation delay of the GNSS signal by rain droplets. Similarly, it is difficult for ground-based dual-frequency single-polarisation microwave radiometers to separate the microwave emission of water vapor and cloud droplets from the rather strong microwave emission of rain. For ground-based microwave radiometry at Bern (Switzerland), we take the approach that IWV during rain is derived from linearly interpolated opacities before and after the rain period. The intermittent rain periods often appear as spikes in the time series of integrated liquid water (ILW) and are indicated by ILW ≥ 0.4 mm. In the present study, we assume that IWV measurements from radiosondes are not affected by rain. We intercompare the climatologies of IWV(rain), IWV(no rain), and IWV(all) obtained by radiosonde, ground-based GNSS atmosphere sounding, ground-based MWR, and ECMWF reanalysis (ERA5) at Payerne and Bern in Switzerland. In all seasons, IWV(rain) is 3.75 to 5.94 mm greater than IWV(no rain). The mean IWV differences between GNSS and radiosonde at Payerne are less than 0.26 mm. The datasets at Payerne show a better agreement than the datasets at Bern. However, the MWR at Bern agrees with the radiosonde at Payerne within 0.41 mm for IWV(rain) and 0.02 mm for IWV(no rain). Using the GNSS and rain gauge measurements at Payerne, we find that IWV(rain) increases with increase of the precipitation rate during summer as well as during winter. IWV(rain) above the Swiss Plateau is quite well estimated by GNSS and MWR though the standard retrievals are limited or hampered during rain periods.

2021

The influence of probe spacing and probe bias in a double Langmuir probe setup

Kjølerbakken, Kai Morgan; Miloch, Wojciech Jacek; Røed, Ketil

Multi-needle Langmuir probes are mounted on satellites and sounding rockets for high-frequency characterization of plasma in the ionosphere. Mounted on a spacecraft, the recorded probe current often differs from expected results. In this paper, we perform a numerical study using a particle in cell model to see how the spacing between the individual probes used in a multi-needle setup influences the measured current. We also study how the applied probe bias voltage can contribute to deviations. In our study, we use realistic electron temperatures and electron densities for the relevant part of the ionosphere. However, the results should be generally applicable and valid for other space environments as well as for laboratory Langmuir probe applications. From our study, we can see that when the distance is short, less than two Debye lengths, the current is highly affected, and we can see deviations of more than 60% compared to a single probe setup.

2021

The who, why and where of Norway's CO2 emissions from tourist travel

Grythe, Henrik; Lopez-Aparicio, Susana

We present emissions from Norway’s tourist travel by the available transport modes, i.e., aviation, maritime (ferries and cruises) and land-based transport (road and railways). Our study includes detailed information on both domestic and international tourist travel within, from and to Norway. We have coupled statistics from several large surveys with detailed emission data to allow us to separate the purpose of the travel (holiday or business).

Total transport emissions for tourists in 2018 were estimated to be 8 530 kt, equivalent to 19% of the reported Norwegian national emissions. Of these emissions, international tourists visiting Norway were responsible for 3 273 kt , whereas travel by Norwegians accounted for 4 875 kt , most of which occur outside Norway’s reporting obligations. Aviation and maritime transport were found to be the largest emission sources, responsible for 71% and 21% of total emissions, respectively. The reduction due to the COVID-19 pandemic was approximately 60% in 2020, and was sustained throughout the year.

Our study shows that officially reported emissions, as limited to the countries territory, are not suitable for accurate evaluation of transport emissions related to tourism. A consumer or tourist-based calculation gives a marked redistribution of emission responsibility. Our results indicate that emissions from Norwegian residents travelling abroad are 1 602 kt higher than those from tourists coming to Norway. This is driven by frequent trips to popular tourist destinations such as Spain, Thailand, Turkey and Greece. Globally consumer based calculations would shift the responsibility of emissions by tourists to the large wealthy nations, with the most international tourists. The understanding of emission distributed by population group or market support in addition the developing of marketing strategies to attract low emission tourist markets and create awareness among the nations with higher shares of international tourist.

2021

Observed and Modeled Black Carbon Deposition and Sources in the Western Russian Arctic 1800−2014

Ruppel, Meri M.; Eckhardt, Sabine; Pesonen, Antto; Mizohata, Kenichiro; Oinonen, Markku J.; Stohl, Andreas; Andersson, August; Jones, Vivienne; Manninen, Sirkku; Gustafsson, Örjan

Black carbon (BC) particles contribute to climate warming by heating the atmosphere and reducing the albedo of snow/ice surfaces. The available Arctic BC deposition records are restricted to the Atlantic and North American sectors, for which previous studies suggest considerable spatial differences in trends. Here, we present first long-term BC deposition and radiocarbon-based source apportionment data from Russia using four lake sediment records from western Arctic Russia, a region influenced by BC emissions from oil and gas production. The records consistently indicate increasing BC fluxes between 1800 and 2014. The radiocarbon analyses suggest mainly (∼70%) biomass sources for BC with fossil fuel contributions peaking around 1960–1990. Backward calculations with the atmospheric transport model FLEXPART show emission source areas and indicate that modeled BC deposition between 1900 and 1999 is largely driven by emission trends. Comparison of observed and modeled data suggests the need to update anthropogenic BC emission inventories for Russia, as these seem to underestimate Russian BC emissions and since 1980s potentially inaccurately portray their trend. Additionally, the observations may indicate underestimation of wildfire emissions in inventories. Reliable information on BC deposition trends and sources is essential for design of efficient and effective policies to limit climate warming.

2021

GUV long-term measurements of total ozone column and effective cloud transmittance at three Norwegian sites

Svendby, Tove Marit; Johnsen, Bjørn; Kylling, Arve; Dahlback, Arne; Bernhard, Germar H.; Hansen, Georg H.; Petkov, Boyan; Vitale, Vito

Measurements of total ozone column and effective cloud transmittance have been performed since 1995 at the three Norwegian sites Oslo/Kjeller, Andøya/Tromsø, and in Ny-Ålesund (Svalbard). These sites are a subset of nine stations included in the Norwegian UV monitoring network, which uses ground-based ultraviolet (GUV) multi-filter instruments and is operated by the Norwegian Radiation and Nuclear Safety Authority (DSA) and the Norwegian Institute for Air Research (NILU). The network includes unique data sets of high-time-resolution measurements that can be used for a broad range of atmospheric and biological exposure studies. Comparison of the 25-year records of GUV (global sky) total ozone measurements with Brewer direct sun (DS) measurements shows that the GUV instruments provide valuable supplements to the more standardized ground-based instruments. The GUV instruments can fill in missing data and extend the measuring season at sites with reduced staff and/or characterized by harsh environmental conditions, such as Ny-Ålesund. Also, a harmonized GUV can easily be moved to more remote/unmanned locations and provide independent total ozone column data sets. The GUV instrument in Ny-Ålesund captured well the exceptionally large Arctic ozone depletion in March/April 2020, whereas the GUV instrument in Oslo recorded a mini ozone hole in December 2019 with total ozone values below 200 DU. For all the three Norwegian stations there is a slight increase in total ozone from 1995 until today. Measurements of GUV effective cloud transmittance in Ny-Ålesund indicate that there has been a significant change in albedo during the past 25 years, most likely resulting from increased temperatures and Arctic ice melt in the area surrounding Svalbard.

2021

Spatiotemporal Patterns in Data Availability of the Sentinel-5P NO2 Product over Urban Areas in Norway

Schneider, Philipp; Hamer, Paul David; Kylling, Arve; Shetty, Shobitha; Stebel, Kerstin

Due to its comparatively high spatial resolution and its daily repeat frequency, the tropospheric nitrogen dioxide product provided by the TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor platform has attracted significant attention for its potential for urban-scale monitoring of air quality. However, the exploitation of such data in, for example, operational assimilation of local-scale dispersion models is often complicated by substantial data gaps due to cloud cover or other retrieval limitations. These challenges are particularly prominent in high-latitude regions where significant cloud cover and high solar zenith angles are often prevalent. Using the example of Norway as a representative case for a high-latitude region, we here evaluate the spatiotemporal patterns in the availability of valid data from the operational TROPOMI tropospheric nitrogen dioxide (NO2) product over five urban areas (Oslo, Bergen, Trondheim, Stavanger, and Kristiansand) and a 2.5 year period from July 2018 through November 2020. Our results indicate that even for relatively clean environments such as small Norwegian cities, distinct spatial patterns of tropospheric NO2 are visible in long-term average datasets from TROPOMI. However, the availability of valid data on a daily level is limited by both cloud cover and solar zenith angle (during the winter months), causing the fraction of valid retrievals in each study site to vary from 20% to 50% on average. A temporal analysis shows that for our study sites and the selected period, the fraction of valid pixels in each domain shows a clear seasonal cycle reaching a maximum of 50% to 75% in the summer months and 0% to 20% in winter. The seasonal cycle in data availability shows the inverse behavior of NO2 pollution in Norway, which typically has its peak in the winter months. However, outside of the mid-winter period we find the TROPOMI NO2 product to provide sufficient data availability for detailed mapping and monitoring of NO2 pollution in the major urban areas in Norway and see potential for the use of the data in local-scale data assimilation and emission inversions applications.

2021

SAMIRA-SAtellite Based Monitoring Initiative for Regional Air Quality

Stebel, Kerstin; Stachlewska, Iwona S.; Nemuc, Anca; Horálek, Jan; Schneider, Philipp; Ajtai, Nicolae; Diamandi, Andrei; Benesova, Nina; Boldeanu, M.; Botezan, Camelia; Markova, Jana; Dumitrache, R.; Iriza-Burca, Amalia; Juras, R.; Nicolae, Doina; Nicolae, V.; Novotný, Petr; Stefanie, Horatiu; Vanek, Lumir; Vlcek, O.; Zawadzka-Manko, Olga; Zehner, Claus

The satellite based monitoring initiative for regional air quality (SAMIRA) initiative was set up to demonstrate the exploitation of existing satellite data for monitoring regional and urban scale air quality. The project was carried out between May 2016 and December 2019 and focused on aerosol optical depth (AOD), particulate matter (PM), nitrogen dioxide (NO2), and sulfur dioxide (SO2). SAMIRA was built around several research tasks: 1. The spinning enhanced visible and infrared imager (SEVIRI) AOD optimal estimation algorithm was improved and geographically extended from Poland to Romania, the Czech Republic and Southern Norway. A near real-time retrieval was implemented and is currently operational. Correlation coefficients of 0.61 and 0.62 were found between SEVIRI AOD and ground-based sun-photometer for Romania and Poland, respectively. 2. A retrieval for ground-level concentrations of PM2.5 was implemented using the SEVIRI AOD in combination with WRF-Chem output. For representative sites a correlation of 0.56 and 0.49 between satellite-based PM2.5 and in situ PM2.5 was found for Poland and the Czech Republic, respectively. 3. An operational algorithm for data fusion was extended to make use of various satellite-based air quality products (NO2, SO2, AOD, PM2.5 and PM10). For the Czech Republic inclusion of satellite data improved mapping of NO2 in rural areas and on an annual basis in urban background areas. It slightly improved mapping of rural and urban background SO2. The use of satellites based AOD or PM2.5 improved mapping results for PM2.5 and PM10. 4. A geostatistical downscaling algorithm for satellite-based air quality products was developed to bridge the gap towards urban-scale applications. Initial testing using synthetic data was followed by applying the algorithm to OMI NO2 data with a direct comparison against high-resolution TROPOMI NO2 as a reference, thus allowing for a quantitative assessment of the algorithm performance and demonstrating significant accuracy improvements after downscaling. We can conclude that SAMIRA demonstrated the added value of using satellite data for regional- and urban-scale air quality monitoring.

2021

Towards FAIR nanosafety data

Jeliazkova, Nina; Apostolova, Margarita D.; Andreoli, Cristina; Barone, Flavia; Barrick, Andrew; Battistelli, Chiara L.; Bossa, Cecilia; Botea-Petcu, Alina; Chatel, Amelie; Angelis, Isabella De; Dusinska, Maria; Yamani, Naouale El; Gheorghe, Daniela; Giusti, Anna; Gómez-Fernández, Paloma; Grafström, Roland; Gromelski, Maciej; Jacobsen, Nicklas Raun; Jeliazkov, Vedrin; Jensen, Keld Alstrup; Kochev, Nikolay; Kohonen, Pekka; Manier, Nicolas; Mariussen, Espen; Mech, Agnieszka; Navas, José María; Paskaleva, Vesselina; Precupas, Aurica; Puzyn, Tomasz; Rasmussen, Kirsten; Ritchie, Peter; Llopis, Isabel Rodriguez; Rundén-Pran, Elise; Sandu, Romica; Shandilya, Neeraj; Tanasescu, Sperenta; Haase, Andrea; Nymark, Penny

2021

The Monitoring Nitrous Oxide Sources (MIN2OS) satellite project

Ricaud, Philippe; Attié, Jean-Luc; Chalinel, Rémi; Pasternak, Frédérick; Léonard, Joël; Pison, Isabelle; Pattey, Elizabeth; Thompson, Rona Louise; Zelinger, Zdenek; Lelieveld, Jos; Sciare, Jean; Saitoh, Naoko; Warner, Juying; Fortems-Cheiney, Audrey; Reynal, Hélène; Vidot, Jérôme; Brooker, Laure; Berdeu, Laurent; Saint-Pé, Olivier; Patra, Prabir K.; Dostál, Michal; Suchánek, Jan; Nevrlý, Václav; Zwaaftink, Christine Groot

The Monitoring Nitrous Oxide Sources (MIN2OS) satellite project aims at monitoring global-scale nitrous oxide (N2O) sources by retrieving N2O surface fluxes from the inversion of space-borne N2O measurements that are sensitive to the lowermost atmospheric layers under favorable conditions. MIN2OS will provide emission estimates of N2O at a horizontal resolution of 1° × 1° on the global scale and 10 × 10 km2 on the regional scale on a weekly to monthly basis depending on the application (e.g., agriculture, national inventories, policy, scientific research). Our novel approach is based on the development of: 1) a space-borne instrument operating in the Thermal InfraRed domain providing, in clear sky conditions, N2O mixing ratio in the lowermost atmosphere (900 hPa) under favorable conditions (summer daytime) over land and under favorable and unfavorable (winter nighttime) conditions over the ocean and 2) an atmospheric inversion framework to estimate N2O surface fluxes from the atmospheric satellite observations. After studying three N2O spectral bands (B1 at 1240–1350 cm−1, B2 at 2150–2260 cm−1 and B3 at 2400–2600 cm−1), a new TIR instrument will be developed, centered at 1250–1330 cm−1, with a resolution of 0.125 cm−1, a Full Width at Half Maximum of 0.25 cm−1 and a swath of 300 km. To optimally constrain the retrieval of N2O vertical profiles, the instrument will be on-board a platform at ~830 km altitude in a sun-synchronous orbit crossing the Equator in descending node at 09:30 local time in synergy with two other platforms (Metop-SG and Sentinel-2 NG) expected to fly in 2031–32 aiming at detecting surface properties, agricultural information on the field scale and vertical profiles of atmospheric constituents and temperature. The lifetime of the MIN2OS project would be 4–5 years to study the interannual variability of N2O surface fluxes. The spectral noise can be decreased by at least a factor of 5 compared to the lowest noise accessible to date with the Infrared Atmospheric Sounding Interferometer-New Generation (IASI-NG) mission. The N2O total error is expected to be less than ~1% (~3 ppbv) along the vertical. The preliminary design of the MIN2OS project results in a small instrument (payload of 90 kg, volume of 1200 × 600 × 300 mm3) with, in addition to the spectrometer, a wide field and 1-km resolution imager for cloud detection. The instruments could be hosted on a small platform, the whole satellite being largely compatible with a dual launch on VEGA-C. The MIN2OS project has been submitted to the European Space Agency Earth Explorer 11 mission ideas.

2021

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