Biogenic isoprene emissions, dry deposition velocity, and surface ozone concentration during summer droughts, heatwaves, and normal conditions in southwestern Europe

At high concentrations, tropospheric ozone (O3) deteriorates air quality, inducing adverse effects on human and ecosystem health. Meteorological conditions are key to understanding the variability in O3 concentration, especially during extreme weather events. In addition to modifying photochemistry and atmospheric transport, droughts and heatwaves affect the state of vegetation and thus the biosphere–troposphere interactions that control atmospheric chemistry, namely biogenic emissions of precursors and gas dry deposition. A major source of uncertainty and inaccuracy in the simulation of surface O3 during droughts and heatwaves is the poor representation of such interactions. This publication aims at quantifying the isolated and combined impacts of both extremes on biogenic isoprene (C5H8) emissions, O3 dry deposition, and surface O3 in southwestern Europe. First, the sensitivity of biogenic C5H8 emissions, O3 dry deposition, and surface O3 to two specific effects of droughts, the decrease in soil moisture and in biomass, is analysed for the extremely dry summer 2012 using the biogenic emission model MEGANv2.1 and the chemistry transport model CHIMEREv2020r1. Despite a significant decrease in biogenic C5H8 emissions and O3 dry deposition velocity, characterized by a large spatial variability, the combined effect on surface O3 concentration remains limited (between +0.5 % and +3 % over the continent). The variations in simulated biogenic C5H8 emissions, O3 dry deposition, and surface O3 during the heatwaves and agricultural droughts are then analysed for summer 2012 (warm and dry), 2013 (warm), and 2014 (relatively wet and cool). We compare the results with large observational data sets, namely O3 concentrations from Air Quality (AQ) e-Reporting (2000–2016) and total columns of formaldehyde (HCHO, which is used as a proxy for biogenic emissions of volatile organic compounds) from the Ozone Monitoring Instrument (OMI) of the Aura satellite (2005–2016). Based on a cluster approach using the percentile limit anomalies indicator, we find that C5H8 emissions increase by +33 % during heatwaves compared to normal conditions, do not vary significantly during all droughts (either accompanied or not by a heatwave), and decrease by −16 % during isolated droughts. OMI data confirm an average increase in HCHO during heatwaves (between +15 % and +31 % depending on the product used) and decrease in HCHO (between −2 % and −6 %) during isolated droughts over the 2005–2016 summers. Simulated O3 dry deposition velocity decreases by −25 % during heatwaves and −35 % during all droughts. Simulated O3 concentrations increase by +7 % during heatwaves and by +3 % during all droughts. Compared to observations, CHIMERE tends to underestimate the daily maximum O3. However, similar sensitivity to droughts and heatwaves are obtained. The analysis of the AQ e-Reporting data set shows an average increase of +14 % during heatwaves and +7 % during all droughts over the 2000–2016 summers (for an average daily concentration value of 69 µg m−3 under normal conditions). This suggests that identifying the presence of combined heatwaves is fundamental to the study of droughts on surface–atmosphere interactions and O3 concentration.</p

Source contributions to 2012 summertime aerosols in the Euro-Mediterranean region

International audienceIn the Mediterranean area, aerosols may originate from anthropogenic or natural emissions (biogenic, mineral dust, fire and sea salt) before undergoing complex chemistry. In case of a huge pollution event, it is important to know whether European pollution limits are exceeded and, if so, whether the pollution is due to anthropogenic or natural sources. In this study, the relative contribution of emissions to surface PM10, surface PM2.5 and total aerosol optical depth (AOD) is quantified. For Europe and the Mediterranean regions and during the summer of 2012, the WRF and CHIMERE models are used to perform a sensitivity analysis on a 50 km resolution domain (from −10° W to 40° E and from 30° N to 55° N): one simulation with all sources (reference) and all others with one source removed. The reference simulation is compared to data from the AirBase network and two ChArMEx stations, and from the AERONET network and the MODIS satellite instrument, to quantify the ability of the model to reproduce the observations. It is shown that the correlation ranges from 0.19 to 0.57 for surface particulate matter and from 0.35 to 0.75 for AOD. For the summer of 2012, the model shows that the region is mainly influenced by aerosols due to mineral dust and anthropogenic emissions (62 and 19 %, respectively, of total surface PM10 and 17 and 52 % of total surface PM2.5). The western part of the Mediterranean is strongly influenced by mineral dust emissions (86 % for surface PM10 and 44 % for PM2.5), while anthropogenic emissions dominate in the northern Mediterranean basin (up to 75 % for PM2.5). Fire emissions are more sporadic but may represent 20 % of surface PM2.5, on average, during the period near local sources. Sea salt mainly contributes for coastal sites (up to 29 %) and biogenic emissions mainly in central Europe (up to 20 %)

Lidar signal simulation for the evaluation of aerosols in chemistry transport models

International audienceWe present an adaptable tool, the OPTSIM (OPTical properties SIMulation) software, for the simulation of optical properties and lidar attenuated backscattered profiles (beta') from aerosol concentrations calculated by chemistry transport models (CTM). It was developed to model both Level 1 observations and Level 2 aerosol lidar retrievals in order to compare model results to measurements: the level 2 enables to estimate the main properties of aerosols plume structures, but may be limited due to specific assumptions. The level 1, originally developed for this tool, gives access to more information about aerosols properties (beta') requiring, at the same time, less hypothesis on aerosols types. In addition to an evaluation of the aerosol loading and optical properties, active remote sensing allows the analysis of aerosols' vertical structures. An academic case study for two different species (black carbon and dust) is presented and shows the consistency of the simulator. Illustrations are then given through the analysis of dust events in the Mediterranean region during the summer 2007. These are based on simulations by the CHIMERE regional CTM and observations from the CALIOP space-based lidar, and highlight the potential of this approach to evaluate the concentration, size and vertical structure of the aerosol plumes

Tracking the emission and transport of pollution from wildfires using the IASI CO retrievals: analysis of the summer 2007 Greek fires

International audienceIn this paper, we analyze the performance of the Infrared Atmospheric Sounding Interferometer (IASI), launched in October 2006 on board METOP-A, for the monitoring of carbon monoxide (CO) during extreme fire events, focusing on the record-breaking fires which devastated thousands of square kilometers of forest in Greece during the last week (23–30) of August 2007. After an assessment of the quality of the profiles retrieved using the Fast Optimal Retrievals on Layers for IASI (FORLI) algorithm, the information provided on fire emissions and subsequent pollution outflow is discussed. Large CO plumes were observed above the Mediterranean Basin and North Africa, with total CO columns exceeding 24×1018 molecules/cm2 and absolute volume mixing ratios up to 4 ppmv on the 25 August. Up to 30×1018 molecules/cm2 and 22 ppmv in the lower troposphere are retrieved close to the fires above the Peloponnese, but with larger uncertainty. The average root-mean-square (RMS) difference between simulated and observed spectra is close to the estimated radiometric noise level, slightly increasing (by ~14%) in the fresh fire plumes. CO profiles are retrieved with a vertical resolution of about 8 km, with ~1.7 pieces of independent information on the vertical in the region considered and a maximum sensitivity in the free troposphere (~4–5 km). Using the integrated total amount, the increase in CO burden due to these fires is estimated to 0.321 Tg, ~40% of the total annual anthropogenic emissions in Greece. The patterns of these CO enhancements are in good agreement with the aerosol optical depth (AOD) retrieved from the MODIS measurements, highlighting a rapid transport of trace gases and aerosols across the Mediterranean Basin (less than one day). While the coarse vertical resolution will not allow the location of the exact plume height, the large CO enhancements observed in the lower troposphere are consistent with the maximum aerosol backscatter coefficient at ~2 km detected by the CALIPSO lidar in space (CALIOP)

Impact of forest fires, biogenic emissions and high temperatures on the elevated Eastern Mediterranean ozone levels during the hot summer of 2007

International audienceThe hot summer of 2007 in southeast Europe has been studied using two regional atmospheric chemistry models; WRF-Chem and EMEP MSC-W. The region was struck by three heat waves and a number of forest fire episodes, greatly affecting air pollution levels. We have focused on ozone and its precursors using state-of-the-art inventories for anthropogenic, biogenic and forest fire emissions. The models have been evaluated against measurement data, and processes leading to ozone formation have been quantified. Heat wave episodes are projected to occur more frequently in a future climate, and therefore this study also makes a contribution to climate change impact research. The plume from the Greek forest fires in August 2007 is clearly seen in satellite observations of CO and NO2 columns, showing extreme levels of CO in and downwindof the fires. Model simulations reflect the location and influence of the fires relatively well, but the modelled magnitude of CO in the plume core is too low. Most likely, this is caused by underestimation of CO in the emission inventories, suggesting that the CO/NOx ratios of fire emissions should be re-assessed. Moreover, higher maximum values are seen in WRF-Chem than in EMEP MSC-W, presumably due to differences in plume rise altitudes as the first model emits a larger fraction of the fire emissions in the lowermost model layer. The model results are also in fairly good agreement with surface ozone measurements. Biogenic VOC emissions reacting with anthropogenic NOx emissions are calculated to contribute significantly to the levels of ozone in the region, but the magnitude and geographical distribution depend strongly on the model and biogenic emission module used. During the July and August heat waves, ozone levels increased substantially due to a combination of forest fire emissions and the effect of high temperatures. We found that the largest temperature impact on ozone was through the temperature dependence of the biogenic emissions, closely followed by the effect of reduced dry deposiion caused by closing of the plants' stomata at very high temperatures. The impact of high temperatures on the ozone chemistry was much lower. The results suggest that forest fire emissions, and the temperature effect on biogenic emissions and dry deposition, will potentially lead to substantial ozone increases in a warmer climate

Inventory of Boreal Fire Emissions for North America in 2004: The Importance of Peat Burning and Pyro-Convective Injection

The summer of 2004 was one of the largest fire seasons on record for Alaska and western Canada. We construct a daily bottom-up fire emission inventory for that season, including consideration of peat burning and high-altitude (buoyant) injection, and evaluate it in a global chemical transport model (the GEOS-Chem CTM) simulation of CO through comparison with MOPITT satellite and ICARTT aircraft observations. The inventory is constructed by combining daily area burned reports and MODIS fire hot spots with estimates of fuel consumption and emission factors based on ecosystem type. We estimate the contribution from peat burning using drainage and peat distribution maps for Alaska and Canada; 17% of the reported 5.1 × 106 ha burned were located in peatlands in 2004. Our total estimate of North American fire emissions during the summer of 2004 is 30 Tg CO, including 11 Tg from peat. Including peat burning in the GEOS-Chem simulation improves agreement with MOPITT observations. The long-range transport of fire plumes observed by MOPITT suggests that the largest fires injected a significant fraction of their emissions in the upper troposphere.Earth and Planetary SciencesEngineering and Applied Science

Impact of forest fires, biogenic emissions and high temperatures on the elevated Eastern Meditteranean ozone levels during the hot summer of 2007

The hot summer of 2007 in southeast Europe has been studied using two regional atmospheric chemistry models; WRF-Chem and EMEP MSC-W. The region was struck by three heat waves and a number of forest fire episodes, greatly affecting air pollution levels. We have focused on ozone and its precursors using state-of-the-art inventories for anthropogenic, biogenic and forest fire emissions. The models have been evaluated against measurement data, and processes leading to ozone formation have been quantified. Heat wave episodes are projected to occur more frequently in a future climate, and therefore this study also makes a contribution to climate change impact research. The plume from the Greek forest fires in August 2007 is clearly seen in satellite observations of CO and NO2 columns, showing extreme levels of CO in and downwind of the fires. Model simulations reflect the location and influence of the fires relatively well, but the modelled magnitude of CO in the plume core is too low. Most likely, this is caused by underestimation of CO in the emission inventories, suggesting that the CO/NOx ratios of fire emissions should be re-assessed. Moreover, higher maximum values are seen in WRF-Chem than in EMEP MSC-W, presumably due to differences in plume rise altitudes as the first model emits a larger fraction of the fire emissions in the lowermost model layer. The model results are also in fairly good agreement with surface ozone measurements. Biogenic VOC emissions reacting with anthropogenic NOx emissions are calculated to contribute significantly to the levels of ozone in the region, but the magnitude and geographical distribution depend strongly on the model and biogenic emission module used. During the July and August heat waves, ozone levels increased substantially due to a combination of forest fire emissions and the effect of high temperatures. We found that the largest temperature impact on ozone was through the temperature dependence of the biogenic emissions, closely followed by the effect of reduced dry deposition caused by closing of the plants’ stomata at very high temperatures. The impact of high temperatures on the ozone chemistry was much lower. The results suggest that forest fire emissions, and the temperature effect on biogenic emissions and dry deposition, will potentially lead to substantial ozone increases in a warmer climate

Ozone-CO Correlations Determined by the TES Satellite Instrument in Continental Outflow Regions

Collocated measurements of tropospheric ozone (O3) and carbon monoxide (CO) from the Tropospheric Emission Spectrometer (TES) aboard the EOS Aura satellite provide information on O3-CO correlations to test our understanding of global anthropogenic influence on O3. We examine the global distribution of TES O3-CO correlations in the middle troposphere (618 hPa) for July 2005 and compare to correlations generated with the GEOS-Chem chemical transport model and with ICARTT aircraft observations over the eastern United States (July 2004). The TES data show significant O3-CO correlations downwind of polluted continents, with dO3/dCO enhancement ratios in the range 0.4–1.0 mol mol−1 and consistent with ICARTT data. The GEOS-Chem model reproduces the O3-CO enhancement ratios observed in continental outflow, but model correlations are stronger and more extensive. We show that the discrepancy can be explained by spectral measurement errors in the TES data. These errors will decrease in future data releases, which should enable TES to provide better information on O3-CO correlations.Earth and Planetary SciencesEngineering and Applied Science

Mesure de l'ozone troposphérique à partir d'observations satellitaires dans le domaine de l'infrarouge

Different forthcoming satellite missions will allow the global observation of several trace gases. The objective of this thesis was to evaluate the capabilities of an instrument measuring from space the thermal infrared radiation in a nadir viewing geometry for the measurement of tropospheric ozone.This work was undertaken in the framework of the preparation of the IASI mission (Infrared Atmospheric Sounding Interferometer), for which the Service d'Aéronomie develops an operational algorithm for the retrieval of trace gases CO, CH4, and O3. IASI is due for launch in 2005, 2010 and 2015 on board the three successive european satellites METOP. An inversion algorithm was developed for ozone retrieval, as well as an error analysis module. The satellite data provided by the IMG instrument, present on board the satellite ADEOS (1996-1997), and the balloon data provided by LPMA/IASI (august 2002), were used to test our developments on real data and to validate the method. A first interpretation of the IMG/ADEOS global distributions of tropospheric ozone has been undertaken by comparing the different informations available on its production and transport.These studies for IASI have been extended to the evaluation of the capacities of a similar instrument present on board a satellite in geostationary orbit for the observation of trace gases.Dans les années à venir, plusieurs missions spatiales permettront l'observation globale des concentrations de nombreux gaz traces dans l'atmosphère. L'objectif de cette thèse a été d'évaluer les capacités d'un instrument mesurant depuis l'espace le rayonnement du système Terre – atmosphère dans l'infrarouge thermique par visée au nadir pour l'observation de l'ozone troposphérique.Ces travaux ont été réalisés dans le cadre de la préparation de la mission IASI (Infrared Atmospheric Sounding Interferometer), pour laquelle le Service d'Aéronomie développe un algorithme opérationnel d'inversion des gaz traces CO, CH4 et O3. Les lancements des trois instruments IASI sont prévus en 2006, 2010 et 2015 sur les trois plates-formes successives MetOp. Un algorithme d'inversion de l'ozone a été développé, ainsi qu'un module d'analyse de l'erreur d'inversion. Les données satellitaires mesurées par l'instrument IMG (Interferometric Monitor for Greenhouse Gases), présent sur le satellite ADEOS (1996-1997), et les mesures ballon LPMA/IASI mesurées en août 2002, nous ont permis de tester les développements sur des mesures réelles et de valider la méthode. Une première interprétation des distributions globales d'ozone troposphérique IMG/ADEOS a été réalisée en comparant les différentes informations disponibles sur sa production et son transport.Les études entreprises pour IASI ont été étendues à l'évaluation des capacités d'un instrument similaire embarqué sur un satellite en orbite géostationnaire pour l'observation des gaz traces

Mesure de l'ozone troposhérique à partir d'observations satellitaires dans le domaine de l'infrarouge

PARIS-BIUSJ-Thèses (751052125) / SudocPARIS-BIUSJ-Sci.Terre recherche (751052114) / SudocSudocFranceF