| 1. |
- Berchet, Antoine, et al.
(författare)
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The Community Inversion Framework v1.0 : A unified system for atmospheric inversion studies
- 2021
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Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 14:8, s. 5331-5354
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric inversion approaches are expected to play a critical role in future observation-based monitoring systems for surface fluxes of greenhouse gases (GHGs), pollutants and other trace gases. In the past decade, the research community has developed various inversion software, mainly using variational or ensemble Bayesian optimization methods, with various assumptions on uncertainty structures and prior information and with various atmospheric chemistry-Transport models. Each of them can assimilate some or all of the available observation streams for its domain area of interest: flask samples, in situ measurements or satellite observations. Although referenced in peer-reviewed publications and usually accessible across the research community, most systems are not at the level of transparency, flexibility and accessibility needed to provide the scientific community and policy makers with a comprehensive and robust view of the uncertainties associated with the inverse estimation of GHG and reactive species fluxes. Furthermore, their development, usually carried out by individual research institutes, may in the future not keep pace with the increasing scientific needs and technical possibilities. We present here the Community Inversion Framework (CIF) to help rationalize development efforts and leverage the strengths of individual inversion systems into a comprehensive framework. The CIF is primarily a programming protocol to allow various inversion bricks to be exchanged among researchers. In practice, the ensemble of bricks makes a flexible, transparent and open-source Python-based tool to estimate the fluxes of various GHGs and reactive species both at the global and regional scales. It will allow for running different atmospheric transport models, different observation streams and different data assimilation approaches. This adaptability will allow for a comprehensive assessment of uncertainty in a fully consistent framework. We present here the main structure and functionalities of the system, and we demonstrate how it operates in a simple academic case.
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| 2. |
- Martinsson, Johan, et al.
(författare)
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Exploring sources of biogenic secondary organic aerosol compounds using chemical analysis and the FLEXPART model
- 2017
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:18, s. 11025-11040
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Tidskriftsartikel (refereegranskat)abstract
- Molecular tracers in secondary organic aerosols (SOAs) can provide information on origin of SOA, as well as regional scale processes involved in their formation. In this study 9 carboxylic acids, 11 organosulfates (OSs) and 2 nitrooxy organosulfates (NOSs) were determined in daily aerosol particle filter samples from Vavihill measurement station in southern Sweden during June and July 2012. Several of the observed compounds are photo-oxidation products from biogenic volatile organic compounds (BVOCs). Highest average mass concentrations were observed for carboxylic acids derived from fatty acids and monoterpenes (12. 3 ± 15. 6 and 13. 8 ± 11. 6 ng mg-3, respectively). The FLEXPART model was used to link nine specific surface types to single measured compounds. It was found that the surface category sea and ocean was dominating the air mass exposure (56 %) but contributed to low mass concentration of observed chemical compounds. A principal component (PC) analysis identified four components, where the one with highest explanatory power (49 %) displayed clear impact of coniferous forest on measured mass concentration of a majority of the compounds. The three remaining PCs were more difficult to interpret, although azelaic, suberic, and pimelic acid were closely related to each other but not to any clear surface category. Hence, future studies should aim to deduce the biogenic sources and surface category of these compounds. This study bridges micro-level chemical speciation to air mass surface exposure at the macro level.
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| 3. |
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| 4. |
- McGrath, Matthew J., et al.
(författare)
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The consolidated European synthesis of CO2 emissions and removals for the European Union and United Kingdom : 1990-2020
- 2023
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Ingår i: Earth System Science Data. - 1866-3508. ; 15:10, s. 4295-4370
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Tidskriftsartikel (refereegranskat)abstract
- Quantification of land surface-atmosphere fluxes of carbon dioxide (CO2) and their trends and uncertainties is essential for monitoring progress of the EU27+UK bloc as it strives to meet ambitious targets determined by both international agreements and internal regulation. This study provides a consolidated synthesis of fossil sources (CO2 fossil) and natural (including formally managed ecosystems) sources and sinks over land (CO2 land) using bottom-up (BU) and top-down (TD) approaches for the European Union and United Kingdom (EU27+UK), updating earlier syntheses (Petrescu et al., 2020, 2021). Given the wide scope of the work and the variety of approaches involved, this study aims to answer essential questions identified in the previous syntheses and understand the differences between datasets, particularly for poorly characterized fluxes from managed and unmanaged ecosystems. The work integrates updated emission inventory data, process-based model results, data-driven categorical model results, and inverse modeling estimates, extending the previous period 1990-2018 to the year 2020 to the extent possible. BU and TD products are compared with the European national greenhouse gas inventory (NGHGI) reported by parties including the year 2019 under the United Nations Framework Convention on Climate Change (UNFCCC). The uncertainties of the EU27+UK NGHGI were evaluated using the standard deviation reported by the EU member states following the guidelines of the Intergovernmental Panel on Climate Change (IPCC) and harmonized by gap-filling procedures. Variation in estimates produced with other methods, such as atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), originate from within-model uncertainty related to parameterization as well as structural differences between models. By comparing the NGHGI with other approaches, key sources of differences between estimates arise primarily in activities. System boundaries and emission categories create differences in CO2 fossil datasets, while different land use definitions for reporting emissions from land use, land use change, and forestry (LULUCF) activities result in differences for CO2 land. The latter has important consequences for atmospheric inversions, leading to inversions reporting stronger sinks in vegetation and soils than are reported by the NGHGI. For CO2 fossil emissions, after harmonizing estimates based on common activities and selecting the most recent year available for all datasets, the UNFCCC NGHGI for the EU27+UK accounts for 926g±g13gTggCgyr-1, while eight other BU sources report a mean value of 948 [937,961]gTggCgyr-1 (25th, 75th percentiles). The sole top-down inversion of fossil emissions currently available accounts for 875gTggC in this same year, a value outside the uncertainty of both the NGHGI and bottom-up ensemble estimates and for which uncertainty estimates are not currently available. For the net CO2 land fluxes, during the most recent 5-year period including the NGHGI estimates, the NGHGI accounted for -91g±g32gTggCgyr-1, while six other BU approaches reported a mean sink of -62 [-117,-49]gTggCgyr-1, and a 15-member ensemble of dynamic global vegetation models (DGVMs) reported -69 [-152,-5]gTggCgyr-1. The 5-year mean of three TD regional ensembles combined with one non-ensemble inversion of -73gTggCgyr-1 has a slightly smaller spread (0th-100th percentiles of [-135,+45]gTggCgyr-1), and it was calculated after removing net land-atmosphere CO2 fluxes caused by lateral transport of carbon (crop trade, wood trade, river transport, and net uptake from inland water bodies), resulting in increased agreement with the NGHGI and bottom-up approaches. Results at the category level (Forest Land, Cropland, Grassland) generally show good agreement between the NGHGI and category-specific models, but results for DGVMs are mixed. Overall, for both CO2 fossil and net CO2 land fluxes, we find that current independent approaches are consistent with the NGHGI at the scale of the EU27+UK. We conclude that CO2 emissions from fossil sources have decreased over the past 30 years in the EU27+UK, while land fluxes are relatively stable: positive or negative trends larger (smaller) than 0.07 (-0.61)gTggCgyr-2 can be ruled out for the NGHGI. In addition, a gap on the order of 1000gTggCgyr-1 between CO2 fossil emissions and net CO2 uptake by the land exists regardless of the type of approach (NGHGI, TD, BU), falling well outside all available estimates of uncertainties. However, uncertainties in top-down approaches to estimate CO2 fossil emissions remain uncharacterized and are likely substantial, in addition to known uncertainties in top-down estimates of the land fluxes. The data used to plot the figures are available at 10.5281/zenodo.8148461 (McGrath et al., 2023).
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| 5. |
- Monteil, Guillaume, et al.
(författare)
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Regional CO2 inversions with LUMIA, the Lund University modular inversion algorithm, v1.0
- 2021
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Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 14:6, s. 3383-3406
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric inversions are used to derive constraints on the net sources and sinks of CO2 and other stable atmospheric tracers from their observed concentrations. The resolution and accuracy that the fluxes can be estimated with depends, among other factors, on the quality and density of the observational coverage, on the precision and accuracy of the transport model used by the inversion to relate fluxes to observations, and on the adaptation of the statistical approach to the problem studied. In recent years, there has been an increasing demand from stakeholders for inversions at higher spatial resolution (country scale), in particular in the framework of the Paris agreement. This step up in resolution is in theory enabled by the growing availability of observations from surface in situ networks (such as ICOS in Europe) and from remote sensing products (OCO-2, GOSAT-2). The increase in the resolution of inversions is also a necessary step to provide efficient feedback to the bottom-up modeling community (vegetation models, fossil fuel emission inventories, etc.). However, it calls for new developments in the inverse models: diversification of the inversion approaches, shift from global to regional inversions, and improvement in the computational efficiency. In this context, we developed LUMIA, the Lund University Modular Inversion Algorithm. LUMIA is a Python library for inverse modeling built around the central idea of modularity: it aims to be a platform that enables users to construct and experiment with new inverse modeling setups while remaining easy to use and maintain. It is in particular designed to be transport-model-agnostic, which should facilitate isolating the transport model errors from those introduced by the inversion setup itself. We have constructed a first regional inversion setup using the LUMIA framework to conduct regional CO2 inversions in Europe using in situ data from surface and tall-tower observation sites. The inversions rely on a new offline coupling between the regional high-resolution FLEXPART Lagrangian particle dispersion model and the global coarse-resolution TM5 transport model. This test setup is intended both as a demonstration and as a reference for comparison with future LUMIA developments. The aims of this paper are to present the LUMIA framework (motivations for building it, development principles and future prospects) and to describe and test this first implementation of regional CO2 inversions in LUMIA.
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| 6. |
- Monteil, Guillaume, et al.
(författare)
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The regional European atmospheric transport inversion comparison, EUROCOM : First results on European-wide terrestrial carbon fluxes for the period 2006-2015
- 2020
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:20, s. 12063-12091
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric inversions have been used for the past two decades to derive large-scale constraints on the sources and sinks of CO2 into the atmosphere. The development of dense in situ surface observation networks, such as ICOS in Europe, enables in theory inversions at a resolution close to the country scale in Europe. This has led to the development of many regional inversion systems capable of assimilating these high-resolution data, in Europe and elsewhere. The EUROCOM (European atmospheric transport inversion comparison) project is a collaboration between seven European research institutes, which aims at producing a collective assessment of the net carbon flux between the terrestrial ecosystems and the atmosphere in Europe for the period 2006 2015. It aims in particular at investigating the capacity of the inversions to deliver consistent flux estimates from the country scale up to the continental scale. The project participants were provided with a common database of in situ-observed CO2 concentrations (including the observation sites that are now part of the ICOS network) and were tasked with providing their best estimate of the net terrestrial carbon flux for that period, and for a large domain covering the entire European Union. The inversion systems differ by the transport model, the inversion approach, and the choice of observation and prior constraints, enabling us to widely explore the space of uncertainties. This paper describes the intercomparison protocol and the participating systems, and it presents the first results from a reference set of inversions, at the continental scale and in four large regions. At the continental scale, the regional inversions support the assumption that European ecosystems are a relatively small sink (-0:21 ± 0:2 Pg C yr-1). We find that the convergence of the regional inversions at this scale is not better than that obtained in state-of-the-art global inversions. However, more robust results are obtained for subregions within Europe, and in these areas with dense observational coverage, the objective of delivering robust countryscale flux estimates appears achievable in the near future.
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| 7. |
- Munassar, Saqr, et al.
(författare)
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Why do inverse models disagree? A case study with two European CO2 inversions
- 2023
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 23:4, s. 2813-2828
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Tidskriftsartikel (refereegranskat)abstract
- We present an analysis of atmospheric transport impact on estimating CO2 fluxes using two atmospheric inversion systems (CarboScope-Regional (CSR) and Lund University Modular Inversion Algorithm (LUMIA)) over Europe in 2018. The main focus of this study is to quantify the dominant drivers of spread amid CO2 estimates derived from atmospheric tracer inversions. The Lagrangian transport models STILT (Stochastic Time-Inverted Lagrangian Transport) and FLEXPART (FLEXible PARTicle) were used to assess the impact of mesoscale transport. The impact of lateral boundary conditions for CO2 was assessed by using two different estimates from the global inversion systems CarboScope (TM3) and TM5-4DVAR. CO2 estimates calculated with an ensemble of eight inversions differing in the regional and global transport models, as well as the inversion systems, show a relatively large spread for the annual fluxes, ranging between -0.72 and 0.20gPgCgyr-1, which is larger than the a priori uncertainty of 0.47gPgCgyr-1. The discrepancies in annual budget are primarily caused by differences in the mesoscale transport model (0.51gPgCgyr-1), in comparison with 0.23 and 0.10gPgCgyr-1 that resulted from the far-field contributions and the inversion systems, respectively. Additionally, varying the mesoscale transport caused large discrepancies in spatial and temporal patterns, while changing the lateral boundary conditions led to more homogeneous spatial and temporal impact. We further investigated the origin of the discrepancies between transport models. The meteorological forcing parameters (forecasts versus reanalysis obtained from ECMWF data products) used to drive the transport models are responsible for a small part of the differences in CO2 estimates, but the largest impact seems to come from the transport model schemes. Although a good convergence in the differences between the inversion systems was achieved by applying a strict protocol of using identical prior fluxes and atmospheric datasets, there was a non-negligible impact arising from applying a different inversion system. Specifically, the choice of prior error structure accounted for a large part of system-to-system differences.
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| 8. |
- Pandey, Sudhanshu, et al.
(författare)
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Enhanced methane emissions from tropical wetlands during the 2011 la Niña
- 2017
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 7
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Tidskriftsartikel (refereegranskat)abstract
- Year-to-year variations in the atmospheric methane (CH4) growth rate show significant correlation with climatic drivers. The second half of 2010 and the first half of 2011 experienced the strongest La Niña since the early 1980s, when global surface networks started monitoring atmospheric CH4 mole fractions. We use these surface measurements, retrievals of column-averaged CH4 mole fractions from GOSAT, new wetland inundation estimates, and atmospheric δ13C-CH4 measurements to estimate the impact of this strong La Niña on the global atmospheric CH4 budget. By performing atmospheric inversions, we find evidence of an increase in tropical CH4 emissions of ∼6-9 TgCH4 yr-1 during this event. Stable isotope data suggest that biogenic sources are the cause of this emission increase. We find a simultaneous expansion of wetland area, driven by the excess precipitation over the Tropical continents during the La Niña. Two process-based wetland models predict increases in wetland area consistent with observationally-constrained values, but substantially smaller per-area CH4 emissions, highlighting the need for improvements in such models. Overall, tropical wetland emissions during the strong La Niña were at least by 5% larger than the long-term mean.
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| 9. |
- Petrescu, Ana Maria Roxana, et al.
(författare)
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The consolidated European synthesis of CO2emissions and removals for the European Union and United Kingdom : 1990-2018
- 2021
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Ingår i: Earth System Science Data. - : Copernicus GmbH. - 1866-3508 .- 1866-3516. ; 13:5, s. 2363-2406
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Forskningsöversikt (refereegranskat)abstract
- Reliable quantification of the sources and sinks of atmospheric carbon dioxide (CO2), including that of their trends and uncertainties, is essential to monitoring the progress in mitigating anthropogenic emissions under the Kyoto Protocol and the Paris Agreement. This study provides a consolidated synthesis of estimates for all anthropogenic and natural sources and sinks of CO2 for the European Union and UK (EU27 + UK), derived from a combination of state-of-the-art bottom-up (BU) and top-down (TD) data sources and models. Given the wide scope of the work and the variety of datasets involved, this study focuses on identifying essential questions which need to be answered to properly understand the differences between various datasets, in particular with regards to the less-well-characterized fluxes from managed ecosystems. The work integrates recent emission inventory data, process-based ecosystem model results, data-driven sector model results and inverse modeling estimates over the period 1990-2018. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported under the UNFCCC in 2019, aiming to assess and understand the differences between approaches. For the uncertainties in NGHGIs, we used the standard deviation obtained by varying parameters of inventory calculations, reported by the member states following the IPCC Guidelines. Variation in estimates produced with other methods, like atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), arises from diverse sources including within-model uncertainty related to parameterization as well as structural differences between models. In comparing NGHGIs with other approaches, a key source of uncertainty is that related to different system boundaries and emission categories (CO2 fossil) and the use of different land use definitions for reporting emissions from land use, land use change and forestry (LULUCF) activities (CO2 land). At the EU27 + UK level, the NGHGI (2019) fossil CO2 emissions (including cement production) account for 2624 Tg CO2 in 2014 while all the other seven bottom-up sources are consistent with the NGHGIs and report a mean of 2588 (± 463 Tg CO2). The inversion reports 2700 Tg CO2 (± 480 Tg CO2), which is well in line with the national inventories. Over 2011-2015, the CO2 land sources and sinks from NGHGI estimates report-90 Tg C yr-1 ± 30 Tg C yr-1 while all other BU approaches report a mean sink of-98 Tg C yr-1 (± 362 Tg of C from dynamic global vegetation models only). For the TD model ensemble results, we observe a much larger spread for regional inversions (i.e., mean of 253 Tg C yr-1 ± 400 Tg C yr-1). This concludes that (a) current independent approaches are consistent with NGHGIs and (b) their uncertainty is too large to allow a verification because of model differences and probably also because of the definition of "CO2 flux"obtained from different approaches. The referenced datasets related to figures are visualized.
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| 10. |
- Prokopiou, Markella, et al.
(författare)
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Constraining N2O emissions since 1940 using firn air isotope measurements in both hemispheres
- 2017
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:7, s. 4539-4564
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Tidskriftsartikel (refereegranskat)abstract
- N2O is currently the third most important anthropogenic greenhouse gas in terms of radiative forcing and its atmospheric mole fraction is rising steadily. To quantify the growth rate and its causes over the past decades, we performed a multi-site reconstruction of the atmospheric N2O mole fraction and isotopic composition using new and previously published firn air data collected from Greenland and Antarctica in combination with a firn diffusion and densification model. The multi-site reconstruction showed that while the global mean N2O mole fraction increased from (290±1)nmolmol-1 in 1940 to (322±1)nmolmol-1 in 2008, the isotopic composition of atmospheric N2O decreased by (-2.2±0.2)% for δ15Nav, (-1.0±0.3)% for δ18O, (-1.3±0.6)% for δ15Nα, and (-2.8±0.6)% for δ15Nβ over the same period. The detailed temporal evolution of the mole fraction and isotopic composition derived from the firn air model was then used in a two-box atmospheric model (comprising a stratospheric box and a tropospheric box) to infer changes in the isotopic source signature over time. The precise value of the source strength depends on the choice of the N2O lifetime, which we choose to fix at 123 years. The average isotopic composition over the investigated period is δ15Nav Combining double low line (-7.6±0.8)% (vs. air-N2), δ18O Combining double low line (32.2±0.2)% (vs. Vienna Standard Mean Ocean Water-VSMOW) for δ18O, δ15Nα Combining double low line (-3.0±1.9)% and δ15Nβ Combining double low line (-11.7±2.3)%. δ15Nav, and δ15Nβ show some temporal variability, while for the other signatures the error bars of the reconstruction are too large to retrieve reliable temporal changes. Possible processes that may explain trends in 15N are discussed. The 15N site preference (Combining double low line δ15Nα-δ15Nβ) provides evidence of a shift in emissions from denitrification to nitrification, although the uncertainty envelopes are large.
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