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 at https://doi.org/10.5281/zenodo.4626578 (Petrescu et al., 2020a).

Methane emission rates from wetland rice fields were determined in Los Banos (Philippines) using an automatic system that allows continuous measurements over time. Methane emission was monitored in an irrigated Aquandic Epiaqualf planted to rice cultivar IR72. Urea fertilizer was applied using four modes: (1) broadcast 10 days after transplanting, (2) broadcast at transplanting, (3) broadcast and incorporated at final harrowing, and (4) deep placement as sulfur-coated granules. The treatments were laid out in a randomized complete block design with four replicates. Measurements were done in the 1991 wet season, 1992 dry season (four treatments), and the 1992 wet season (only treatment 3). Methane emission rates from the experimental plots showed pronounced seasonal and diel variations. The diel pattern of methane emission rates followed a consistent pattern, with highest rates observed in the early afternoon and lowest rates in the early morning. Methane emission rate was generally hig hest at the ripening stage. The average methane emission rate during the 1992 dry season (190 mg CH4 m(-2) d(-1)) exceeded the average flux rates of the 1992 wet season (79 mg CH4 m(-2) d(- 1)) by a factor of 2.4. The total methane emitted from these flooded rice fields amounted to 19 g CH4 m(-2) in the dry season with rice yields of 5.2-6.3 t ha(-1) and 7 g CH4 m(-2) in the wet season with rice yields of 2.4-3.3 t ha(-1) regardless of the mode of N application. Significant amounts corresponding to 20 per cent of the methane released under waterlogged conditions were released when the soil was drained after harvest. Emission rates increased sharply when the floodwater receded and macropores started to drain. Emission of methane stopped only when the soil became fully aerated

A new organic aerosol (OA) module has been implemented into the EMEP chemical transport model. Four different volatility basis set (VBS) schemes have been tested in long-term simulations for Europe, covering the six years 2002–2007. Different assumptions regarding partitioning of primary OA (POA) and aging of POA and secondary OA (SOA), have been explored. Model results are compared to filter measurements, AMS-data and source-apportionment studies, as well as to other model studies. The present study indicates that many different sources contribute significantly to OA in Europe. Fossil POA and oxidised POA, biogenic and anthropogenic SOA (BSOA and ASOA), residential burning of biomass fuels and wildfire emissions may all contribute more than 10% each over substantial parts of Europe. Simple VBS based OA models can give reasonably good results for summer OA but more observational studies are needed to constrain the VBS parameterisations and to help improve emission inventories. The volatility distribution of primary emissions is an important issue for further work. This study shows smaller contributions from BSOA to OA in Europe than earlier work, but relatively greater ASOA. BVOC emissions are highly uncertain and need further validation. We can not reproduce winter levels of OA in Europe, and there are many indications that the present emission inventories substantially underestimate emissions from residential wood burning in large parts of Europe

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Results of the chemistry transport model CHIMERE are compared with the measurements performed during the MEGAPOLI summer campaign in the Greater Paris Region in July, 2009. The Volatility-Basis-Set approach (VBS) is implemented into this model, taking into account the volatility of primary organic aerosol (POA) and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations related to the volatility of POA and the scheme of secondary organic aerosol (SOA) formation. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated and four pollution regimes according to the air mass origin are defined. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC) shows the best correlation with measurements. All observed high concentration events are reproduced by the model mostly after long range transport, indicating that long range transport of SOA to Paris is well reproduced. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization), to emission input data, and to simulated OH levels can be responsible for this behavior. Despite these uncertainties, the implementation of the VBS scheme into the CHIMERE model allowed for much more realistic organic aerosol simulations for Paris during summer time. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from north-east (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during days with advection from Southern France and Spain