A exposição das vinhas mediterrâneas ao ozono troposférico: uma abordagem de modelação

The main objective of this Thesis is to develop and evaluate a modeling system capable of simulating in detail the exposure and uptake of ambient ozone (O₃) by vineyards in Mediterranean environments. It also aims to contribute to the state of the art on the influence of climate in viticulture in the context of climate change. The selected study area was the Douro Demarcated Region (DDR) in Portugal. The assessment on climate change potential impact was based on WRF downscaled ERA-Interim and MPI-ESM-LR global simulations forced with a RCP8.5 GHG emission scenario, for recent-past (1986–2005) and future periods (2046–2065, 2081–2100). For the evaluation of phytotoxic risk due to ozone, a validation of a simulation with the WRF-CHIMERE system was carried out. This simulation covered a grapevine growing season from April to September 2017. In the same period, a field campaign was carried out, including measurements of ambient ozone, phenology, and leaf gas-exchange and water relations for the grapevine along representative vineyards of the study area. The field campaign indicated that the phytotoxicity threshold for ambient O₃ (40 ppb) was reached in all stages of grapevine development, including a sensitive period such as flowering. Regarding ambient O₃ exposure standards, the measured May-Jun AOT40, 8 ppm-h, exceeded the long-term objective for the protection of vegetation, 3 ppm-h, and was close to that established as a general annual standard by the 2002/03 and 2008/50 European Directives, 9 ppm-h. The validated ambient ozone simulations by the WRF-CHIMERE system also indicated that grapevine-specific thresholds for Jun-Sep AOT40 could be exceeded, mainly in the drier, warmer Douro Superior eastern subregion. On the other hand, the standard based on the phytotoxic ozone dose introduced into the plant, POD, also indicated risk of phytotoxicity, this time mostly located in the Baixo and Cima Corgo western DDR subregions. The POD risk had a lesser extension when adjusted to the physiological behavior of local grapevine varieties, mainly due to the inclusion of the plant water stress effect throughout the region. It has also been possible to relate the WRF-ERA recent-past climate simulations with vintage yield and quality in the DDR. The mid-term and long term WRF-MPI climate scenarios revealed shifts to warmer and drier conditions not remaining within the ranges for quality and production. Important conclusions of this work are the relevance of including phenological and physiological parametrizations of local grapevine varieties to refine standards related with ozone phytotoxic risk and climate change. A current limitation is the lack of valid O₃ exposure and dose-effect relationships for the grapevine.O principal objectivo desta Tese consiste no desenvolvimento e validação de um sistema de modelação capaz de simular em detalhe a exposição e a absorção do ozono (O₃) ambiental pelas vinhas em ambientes mediterrânicos. Visa também contribuir para o estado da arte sobre a influência do clima na viticultura no contexto das alterações climáticas. A área de estudo seleccionada foi a Região Demarcada do Douro (DDR), em Portugal. A avaliação do impacto potencial das alterações climáticas baseou-se no refinamento da resolução das simulações globais de ERA-Interim e MPI-ESMLR, forçadas com um cenário de emissão de GEE RCP8.5 para períodos recentes (1986-2005) e futuros (2046-2065, 2081-2100), recorrendo ao modelo WRF. Para a avaliação do risco fitotóxico devido ao ozono, foi efetuada uma validação de uma simulação do sistema WRF-CHIMERE. Esta simulação abrangeu um período de crescimento para as vinhas entre Abril e Setembro de 2017. No mesmo período, foi realizada uma campanha experimental, incluindo medições do ozono ambiente, fenologia, troca de gases foliares e relações de água, ao longo de vinhas representativas da área de estudo. A campanha indicou que o limiar de fitotoxicidade para O₃ ambiental (40 ppb) foi atingido em todas as fases de desenvolvimento das vinhas, incluindo um período sensível como a floração. Em relação aos padrões de exposição ambiental ao O₃, o indicador AOT40 entre Maio-Junho, 8 ppm-h, excedeu o objetivo a longo prazo para a proteção da vegetação, 3 ppm-h, e aproximou-se do estabelecido como norma geral anual pelas Diretivas Europeias 2002/03 e 2008/50, 9 ppm-h. As simulações de ozono ambiente, validadas pelo sistema WRF-CHIMERE, também indicaram que os limiares específicos para as vinhas, para AOT40 entre Junho-Setembro, podiam ser excedidos, principalmente na sub-região mais seca e quente mais oriental da DDR, o Douro Superior. Por outro lado, o padrão baseado na dose de ozono fitotóxico introduzida na planta, POD, indicou também risco de fitotoxicidade, principalmente nas sub-regiões ocidentais da DDR, o Baixo Corgo e o Cima Corgo. O risco indicado pelo POD teve uma menor extensão quando ajustado ao comportamento fisiológico das castas de videira locais, sobretudo devido à inclusão do efeito de stress hídrico das plantas em toda a região. Os resultados das simulações climáticas WRFERA para o período recente revelaram também uma relação coerente com o rendimento e qualidade da vinha na DDR em clima presente. Os cenários climáticos de médio e longo prazo do WRF-MPI indicaram uma tendência para condições mais quentes e secas, que propiciarão valores de produção e de qualidade inferiores aos recomendados. Conclusões importantes deste trabalho são a relevância de incluir parametrizações fenológicas e fisiológicas das castas de videira locais para refinar as normas relacionadas com o risco fitotóxico do ozono e as alterações climáticas. Uma limitação atual é a falta de relações exposição ou dose-efeito válidas para o O₃ e as vinhas.Programa Doutoral em Ciências e Engenharia do Ambient

The consolidated European synthesis of CH4 and N2O emissions for the European Union and United Kingdom : 1990-2019

Funding Information: We thank Aurélie Paquirissamy, Géraud Moulas and the ARTTIC team for the great managerial support offered during the project. FAOSTAT statistics are produced and disseminated with the support of its member countries to the FAO regular budget. Annual, gap-filled and harmonized NGHGI uncertainty estimates for the EU and its member states were provided by the EU GHG inventory team (European Environment Agency and its European Topic Centre on Climate change mitigation). Most top-down inverse simulations referred to in this paper rely for the derivation of optimized flux fields on observational data provided by surface stations that are part of networks like ICOS (datasets: 10.18160/P7E9-EKEA , Integrated Non-CO Observing System, 2018a, and 10.18160/B3Q6-JKA0 , Integrated Non-CO Observing System, 2018b), AGAGE, NOAA (Obspack Globalview CH: 10.25925/20221001 , Schuldt et al., 2017), CSIRO and/or WMO GAW. We thank all station PIs and their organizations for providing these valuable datasets. We acknowledge the work of other members of the EDGAR group (Edwin Schaaf, Jos Olivier) and the outstanding scientific contribution to the VERIFY project of Peter Bergamaschi. Timo Vesala thanks ICOS-Finland, University of Helsinki. The TM5-CAMS inversions are available from https://atmosphere.copernicus.eu (last access: June 2022); Arjo Segers acknowledges support from the Copernicus Atmosphere Monitoring Service, implemented by the European Centre for Medium-Range Weather Forecasts on behalf of the European Commission (grant no. CAMS2_55). This research has been supported by the European Commission, Horizon 2020 Framework Programme (VERIFY, grant no. 776810). Ronny Lauerwald received support from the CLand Convergence Institute. Prabir Patra received support from the Environment Research and Technology Development Fund (grant no. JPMEERF20182002) of the Environmental Restoration and Conservation Agency of Japan. Pierre Regnier received financial support from the H2020 project ESM2025 – Earth System Models for the Future (grant no. 101003536). David Basviken received support from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (METLAKE, grant no. 725546). Greet Janssens-Maenhout received support from the European Union's Horizon 2020 research and innovation program (CoCO, grant no. 958927). Tuula Aalto received support from the Finnish Academy (grants nos. 351311 and 345531). Sönke Zhaele received support from the ERC consolidator grant QUINCY (grant no. 647204).Peer reviewedPublisher PD

Inverse modelling of European CH4 emissions during 2006-2012 using different inverse models and reassessed atmospheric observations

We present inverse modelling (top down) estimates of European methane (CH4) emissions for 2006-2012 based on a new quality-controlled and harmonised in situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions.The inverse models infer total CH4 emissions of 26.8 (20.2-29.7) TgCH(4) yr(-1) (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006-2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom up, based on statistical data and emissions factors) amount to only 21.3 TgCH(4) yr(-1) (2006) to 18.8 TgCH(4) yr(-1) (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP), total wetland emissions of 4.3 (2.3-8.2) TgCH(4) yr(-1) from the EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Taking into account the wetland emissions from the WETCHIMP ensemble, the top-down estimates are broadly consistent with the sum of anthropogenic and natural bottom-up inventories. However, the contribution of natural sources and their regional distribution remain rather uncertain.Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon Cycle (IMECC) aircraft campaign. We present a novel approach to estimate the biases in the derived emissions, based on the comparison of simulated and measured enhancements of CH4 compared to the background, integrated over the entire boundary layer and over the lower troposphere. The estimated average regional biases range between -40 and 20% at the aircraft profile sites in France, Hungary and Poland.</p

Adjoint of the global Eulerian-Lagrangian coupled atmospheric transport model (A-GELCA v1.0): development and validation

We present the development of the Adjoint of the Global Eulerian–Lagrangian Coupled Atmospheric (A-GELCA) model that consists of the National Institute for Environmental Studies (NIES) model as an Eulerian three-dimensional transport model (TM), and FLEXPART (FLEXible PARTicle dispersion model) as the Lagrangian Particle Dispersion Model (LPDM). The forward tangent linear and adjoint components of the Eulerian model were constructed directly from the original NIES TM code using an automatic differentiation tool known as TAF (Transformation of Algorithms in Fortran; http://www.FastOpt.com), with additional manual pre- and post-processing aimed at improving transparency and clarity of the code and optimizing the performance of the computing, including MPI (Message Passing Interface). The Lagrangian component did not require any code modification, as LPDMs are self-adjoint and track a significant number of particles backward in time in order to calculate the sensitivity of the observations to the neighboring emission areas. The constructed Eulerian adjoint was coupled with the Lagrangian component at a time boundary in the global domain. The simulations presented in this work were performed using the A-GELCA model in forward and adjoint modes. The forward simulation shows that the coupled model improves reproduction of the seasonal cycle and short-term variability of CO2. Mean bias and standard deviation for five of the six Siberian sites considered decrease roughly by 1 ppm when using the coupled model. The adjoint of the Eulerian model was shown, through several numerical tests, to be very accurate (within machine epsilon with mismatch around to ±6 e−14) compared to direct forward sensitivity calculations. The developed adjoint of the coupled model combines the flux conservation and stability of an Eulerian discrete adjoint formulation with the flexibility, accuracy, and high resolution of a Lagrangian backward trajectory formulation. A-GELCA will be incorporated into a variational inversion system designed to optimize surface fluxes of greenhouse gases

Quantification des sources de méthane en Sibérie par inversion atmosphérque à la méso-échelle

Anthopogenic and natural methane emissions in Siberia significantly contribute to theglobal methane budget, but the magnitude of these emissions is uncertain (3–11% of globalemissions). To the South, anthropogenic emissions are related to big urban centres. To theNorth, oil and gas extraction in West Siberia is responsible for conspicuous point sources.These regions are also covered by large natural wetlands emitting methane during the snowfreeseason, roughly from May to September. Regional atmospheric inversions at a meso-scaleprovide a mean for improving our knowledge on all emission process. But inversions sufferfrom the uncertainties in the assimilated observations, in the atmospheric transport modeland in the emission magnitude and distribution. I developp a new inversion method based onerror statistic marginalization in order to account for these uncertainties. I test this methodon case study and explore its robustness. I then apply it to Siberia. Using measurements ofmethane atmospheric concentrations gathered at Siberian surface observation sites, I founda regional methane budget in Siberia of 5–28 TgCH4.a−1 (1–5% of global emissions). Thisimplies a reduction of 50% in the uncertainties on the regional budget. With the new method,I also can detect emission patterns at a resolution of a few thousands km2 and emissionvariability at a resolution of 2–4 weeks.Les émissions anthropiques et naturelles de méthane en Sibérie contribuent de manièrenotable, mais mal quantifiée au budget mondial de méthane (3–11% des émissions mondiales).Au Sud de la région, les émissions anthropiques sont liées aux grands centres urbains.Au Nord, l’extraction de gaz et de pétrole en Sibérie occidentale induit d’importantessources anthropiques ponctuelles. Ces régions sont aussi couvertes de vastes zones humidesnaturelles émettant du méthane durant l’été (typiquement de mai à septembre). Nous utilisonsdes inversions atmosphériques régionales à la méso-échelle pour mieux comprendreles contributions de chaque processus dans le budget sibérien. Les inversions souffrent desincertitudes dans les observations, dans la simulation du transport et dans l’amplitude et ladistribution des émissions. Pour prendre en compte ces incertitudes, je développe une nouvelleméthode d’inversion basée sur une marginalisation des statistiques d’erreurs. Je testecette méthode et documente sa robustesse sur un cas test. Je l’applique ensuite à la Sibérie.À l’aide de mesures de concentrations atmosphériques de méthane collectées par des sitesd’observation de surface en Sibérie, j’estime le budget régional de méthane sibérien à 5–28 TgCH4.a−1 (1–5% des émissions mondiales), soit une réduction de 50% des incertitudespar rapport aux précédentes études dans la région. Grâce à cette méthode, je suis de plus enmesure de détecter des structures d’émissions par zones de quelques milliers de km2 et leurvariabilité à une résolution de 2–4 semaines

The consolidated European synthesis of CH4 and N2O emissions for the European Union and United Kingdom : 1990-2017

Reliable quantification of the sources and sinks of greenhouse gases, together with trends and uncertainties, is essential to monitoring the progress in mitigating anthropogenic emissions under the Paris Agreement. This study provides a consolidated synthesis of CH4 and N2O emissions with consistently derived state-of-the-art bottom-up (BU) and top-down (TD) data sources for the European Union and UK (EU27 C UK). We integrate recent emission inventory data, ecosystem process-based model results and inverse modeling estimates over the period 1990-2017. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported to the UN climate convention UNFCCC secretariat in 2019. For uncertainties, we used for NGHGIs the standard deviation obtained by varying parameters of inventory calculations, reported by the member states (MSs) following the recommendations of the IPCC Guidelines. For atmospheric inversion models (TD) or other inventory datasets (BU), we defined uncertainties from the spread between different model estimates or model-specific uncertainties when reported. In comparing NGHGIs with other approaches, a key source of bias is the activities included, e.g., anthropogenic versus anthropogenic plus natural fluxes. In inversions, the separation between anthropogenic and natural emissions is sensitive to the geospatial prior distribution of emissions. Over the 2011-2015 period, which is the common denominator of data availability between all sources, the anthropogenic BU approaches are directly comparable, reporting mean emissions of 20.8 TgCH(4) yr (-1) (EDGAR v5.0) and 19.0 TgCH(4) yr(-1) (GAINS), consistent with the NGHGI estimates of 18.9 +/- 1.7 TgCH(4) yr(-1). The estimates of TD total inversions give higher emission estimates, as they also include natural emissions. Over the same period regional TD inversions with higher-resolution atmospheric transport models give a mean emission of 28.8 TgCH(4) yr(-1). Coarser-resolution global TD inversions are consistent with regional TD inversions, for global inversions with GOSAT satellite data (23.3 TgCH(4) yr(-1)) and surface network (24.4 TgCH(4) yr (-1)). The magnitude of natural peatland emissions from the JSBACH-HIMMELI model, natural rivers and lakes emissions, and geological sources together account for the gap between NGHGIs and inversions and account for 5.2 TgCH(4) yr(-1). For N2O emissions, over the 2011-2015 period, both BU approaches (EDGAR v5.0 and GAINS) give a mean value of anthropogenic emissions of 0.8 and 0.9 TgN(2)Oyr(-1), respectively, agreeing with the NGHGI data (0.9 0.6 TgN(2)Oyr(-1)). Over the same period, the average of the three total TD global and regional inversions was 1.3 +/- 0.4 and 1.3 +/- 0.1 TgN(2)Oyr(-1), respectively. The TD and BU comparison method defined in this study can be operationalized for future yearly updates for the calculation of CH4 and N2O budgets both at the EU CUK scale and at the national scale.Peer reviewe

Fire emission heights in the climate system - Part 1: Global plume height patterns simulated by ECHAM6-HAM2

We use the global circulation model ECHAM6 extended by the aerosol module HAM2 to simulate global patterns in wildfire emission heights. Prescribed plume heights in ECHAM6 are replaced by an implementation of a simple, semi-empirical plume height parametrization. In a first step, the global performance of the plume height parametrization is evaluated for plumes reported in the Multiangle Imaging Spectroradiometer (MISR) Plume Height Project (MPHP) data set. Our results show that the parametrization simulates a largely reasonable global distribution of plume heights. While the modeled global mean plume height (1411 ± 646 m) is in good agreement with the observed mean (1382 ± 702 m), the upper and lower tails of the plume height distribution tend to be slightly underrepresented. Furthermore, we compare plume heights simulated by the simple parametrization to a more complex, analytical plume model. Major differences in global plume height distributions are found for the lowest 1.5 km, but reasonable agreement is observed for higher plumes. In a second step, fire radiative power (FRP) as reported in the global fire assimilation system (GFAS) is used to simulate plume heights for observed fires globally for the period 2005–2011. The global fraction of simulated daytime plumes injecting emissions into the free troposphere (FT) ranges from 3.7 ± 0.7 to 5.2 ± 1.0 %. This range is comparable to results from observational studies, but it is much lower than results for prescribed plume heights in the ECHAM6-HAM2 standard setup. Nevertheless, occasionally deep emission injections exceeding 5–7 km in height are simulated for intense fires and favorable meteorological conditions. The application of a prescribed diurnal cycle in FRP turns out to be of minor importance. For a hypothetical doubling in FRP, moderate changes in plume heights of 100–400 m are simulated. These small changes indicate that a potential future increase in fire intensity will only slightly impact the emission heights on a global scale