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In this paper, the fate of biomass burning emissions of carbon monoxide is studied with the global chemistry–transport model MOCAGE (MOdélisation de Chimie Atmosphérique à Grande Échelle) and IAGOS (In-Service Aircraft for a Global Observing System) airborne measurements for the year 2013. The objectives are firstly to improve their representation within the model and secondly to analyse their contribution to carbon monoxide concentrations in the upper troposphere. At first, a new implementation of biomass burning injection is developed for MOCAGE, using the latest products available in Global Fire Assimilation System (GFAS) biomass burning inventory on plume altitude and injection height. This method is validated against IAGOS observations of CO made in fire plumes, identified thanks to the SOFT-IO source attribution data. The use of these GFAS products leads to improved MOCAGE skill to simulate fire plumes originating from boreal forest wildfires. It is also shown that this new biomass burning injection method modifies the distribution of carbon monoxide in the free and upper troposphere, mostly at northern boreal latitudes. Then, MOCAGE performance is evaluated in general in the upper troposphere and lower stratosphere in comparison to the IAGOS observations and is shown to be very good, with very low bias and good correlations between the model and the observations. Finally, we analyse the contribution of biomass burning to upper tropospheric carbon monoxide concentrations. This is done by comparing simulations where biomass are toggled on and off in different source regions of the world to assess their individual influence. The two regions contributing the most to upper tropospheric CO are found to be the boreal forests and equatorial Africa, in accordance with the quantities of CO they emit each year and the fact that they undergo fast vertical transport: deep convection in the tropics and pyroconvection at high latitudes. It is also found that biomass burning contributes more than 11 % on average to the CO concentrations in the upper troposphere and up to 50 % at high latitudes during the wildfire season.

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.

In situ measurements from the In-service Aircraft for a Global Observing System (IAGOS) are used to characterise extreme values of carbon monoxide (CO) in large regions of the globe in the troposphere between 2002 and 2019. The SOFT-IO model, combining the FLEXPART Lagrangian dispersion model with emission inventories over the footprint region, is used to identify the origins of the CO in the sampled plumes. The impact of biomass burning and anthropogenic emissions on such CO plumes is characterised through CO mixing ratios and simultaneously recorded ozone (O3) ones. In the Northern Hemisphere, CO reaches its maximum values in DJF in the lower troposphere, which can be attributed to elevated anthropogenic emissions and reduced convective activity during the season. Due to the low photochemistry and the fresh age of the air masses, the O3 values of these plumes are low. CO plumes in the upper troposphere (UT) result from intense emissions and efficient vertical transport, peaking during JJA. The largest values of CO in the Northern Hemisphere are found in eastern Asia in the lower troposphere (LT) and middle troposphere (MT) and in Siberia in the upper troposphere. Among the anomalies detected in the upper troposphere in JJA, the ones with higher associated O3 values are the ones associated with biomass-burning emissions. The middle troposphere is a combination of the characteristics of the LT and the UT, with contributions from both local emissions and long-range transport. Among the studied regions, the troposphere above the Middle East and the UT above Siberia presented extremely high O3 values. Indian CO anomalies have different characteristics depending on the season, as the wet and dry phases of the monsoon have a strong impact on the transport of the pollutant in this region. Similarly, the shift in the intertropical convergence zone (ITCZ) strongly impacts the seasonality of the emissions and the transport patterns above Africa. In that region, convection is no longer the limiting factor, and the transport of the CO plumes is driven by the ITCZ shift, trade winds, and the upper branch of the Hadley cell redistributing the pollution to higher latitudes.

In situ measurements in the upper troposphere–lower stratosphere (UTLS) have been performed in the framework of the European research infrastructure IAGOS (In-service Aircraft for a Global Observing System) for ozone since 1994 and for carbon monoxide (CO) since 2002. The flight tracks cover a wide range of longitudes in the northern extratropics, extending from the North American western coast (125° W) to the eastern Asian coast (135° E) and more recently over the northern Pacific Ocean. Several tropical regions are also sampled frequently, such as the Brazilian coast, central and southern Africa, southeastern Asia, and the western half of the Maritime Continent. As a result, a new set of climatologies for O3 (August 1994–December 2013) and CO (December 2001–December 2013) in the upper troposphere (UT), tropopause layer, and lower stratosphere (LS) are made available, including gridded horizontal distributions on a semi-global scale and seasonal cycles over eight well-sampled regions of interest in the northern extratropics. The seasonal cycles generally show a summertime maximum in O3 and a springtime maximum in CO in the UT, in contrast to the systematic springtime maximum in O3 and the quasi-absence of a seasonal cycle of CO in the LS. This study highlights some regional variabilities in the UT, notably (i) a west–east difference of O3 in boreal summer with up to 15 ppb more O3 over central Russia compared with northeast America, (ii) a systematic west–east gradient of CO from 60 to 140° E, especially noticeable in spring and summer with about 5 ppb by 10 degrees longitude, (iii) a broad spring/summer maximum of CO over northeast Asia, and (iv) a spring maximum of O3 over western North America. Thanks to almost 20 years of O3 and 12 years of CO measurements, the IAGOS database is a unique data set to derive trends in the UTLS at northern midlatitudes. Trends in O3 in the UT are positive and statistically significant in most regions, ranging from +0.25 to +0.45 ppb yr−1, characterized by the significant increase in the lowest values of the distribution. No significant trends of O3 are detected in the LS. Trends of CO in the UT, tropopause, and LS are almost all negative and statistically significant. The estimated slopes range from −1.37 to −0.59 ppb yr−1, with a nearly homogeneous decrease in the lowest values of the monthly distribution (5th percentile) contrasting with the high interregional variability in the decrease in the highest values (95th percentile).

The Gradient in Longitude of Atmospheric constituents above the Mediterranean basin (GLAM) campaign was set up in August 2014, as part of the Chemistry and Aerosol Mediterranean Experiment (ChArMEx) project. This campaign aimed to study the chemical variability of gaseous pollutants and aerosols in the troposphere along a west–east transect above the Mediterranean Basin (MB). In the present work, we focus on two biomass burning events detected at 5.4 and 9.7 km altitude above sea level (a.s.l.) over Sardinia (from 39∘12′ N–9∘15′ E to 35∘35′ N–12∘35′ E and at 39∘30′ N–8∘25′ E, respectively). Concentration variations in trace gas carbon monoxide (CO), ozone (O3) and aerosols were measured thanks to the standard instruments on board the Falcon 20 aircraft operated by the Service des Avions Français Instrumentés pour la Recherche en Environnement (SAFIRE) and the Spectromètre InfraRouge In situ Toute Altitude (SPIRIT) developed by LPC2E. Twenty-day backward trajectories with Lagrangian particle dispersion model FLEXPART (FLEXible PARTicle) help to understand the transport processes and the origin of the emissions that contributed to this pollution detected above Sardinia. Biomass burning emissions came (i) on 10 August from the North American continent with air masses transported during 5 days before arriving over the MB, and (ii) on 6 August from Siberia, with air masses travelling during 12 days and enriched in fire emission products above Canada 5 days before arriving over the MB. In combination with the Global Fire Assimilation System (GFAS) inventory and the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite fire locations, FLEXPART reproduces well the contribution of those fires to CO and aerosols enhancements under adjustments of the injection height to 10 km in both cases and application of an amplification factor of 2 on CO GFAS emissions for the 10 August event. The chemistry transport model (CTM) MOCAGE is used as a complementary tool for the case of 6 August to confirm the origin of the emissions by tracing the CO global atmospheric composition reaching the MB. For this event, both models agree on the origin of air masses with CO concentrations simulated with MOCAGE lower than the observed ones, likely caused by the coarse model horizontal resolution that yields the dilution of the emissions and diffusion during transport. In combination with wind fields, the analysis of the transport of the air mass documented on 6 August suggests the subsidence of CO pollution from Siberia towards North America and then a transport to the MB via fast jet winds located at around 5.5 km in altitude. Finally, using the ratio ΔO3 ∕ ΔCO, the plume age can be estimated and the production of O3 during the transport of the air mass is studied using the MOCAGE model.

The modeling study presented here aims to estimate how uncertainties in global hydroxyl radical (OH) distributions, variability, and trends may contribute to resolving discrepancies between simulated and observed methane (CH4) changes since 2000. A multi-model ensemble of 14 OH fields was analyzed and aggregated into 64 scenarios to force the offline atmospheric chemistry transport model LMDz (Laboratoire de Meteorologie Dynamique) with a standard CH4 emission scenario over the period 2000–2016. The multi-model simulated global volume-weighted tropospheric mean OH concentration ([OH]) averaged over 2000–2010 ranges between 8.7×105 and 12.8×105 molec cm−3. The inter-model differences in tropospheric OH burden and vertical distributions are mainly determined by the differences in the nitrogen oxide (NO) distributions, while the spatial discrepancies between OH fields are mostly due to differences in natural emissions and volatile organic compound (VOC) chemistry. From 2000 to 2010, most simulated OH fields show an increase of 0.1–0.3×105 molec cm−3 in the tropospheric mean [OH], with year-to-year variations much smaller than during the historical period 1960–2000. Once ingested into the LMDz model, these OH changes translated into a 5 to 15 ppbv reduction in the CH4 mixing ratio in 2010, which represents 7 %–20 % of the model-simulated CH4 increase due to surface emissions. Between 2010 and 2016, the ensemble of simulations showed that OH changes could lead to a CH4 mixing ratio uncertainty of >±30 ppbv. Over the full 2000–2016 time period, using a common state-of-the-art but nonoptimized emission scenario, the impact of [OH] changes tested here can explain up to 54 % of the gap between model simulations and observations. This result emphasizes the importance of better representing OH abundance and variations in CH4 forward simulations and emission optimizations performed by atmospheric inversions.

A 2-degree global warming is likely to affect the production, deposition, and transport of air pollutants, leading to impacts on air quality and health. In the present study we use an ensemble of four regional chemistry-transport models, driven by meteorological data from different climate models, to assess such changes and their uncertainties for PM2.5 and SOMO35. Changes and uncertainties are compared to the inter-model variability. We find that the impact of regional climate change on PM2.5, averaged over the model ensemble, ranges from −0.5 μg.m −3 to +1.3 μg.m −3 over Europe. It mainly results from changes in natural and biogenic emissions, such as desert dust, sea salt and biogenic VOCs. Statistically significant decreases in PM2.5 are found over southwestern Russia and Ukraine as well as an increase over Southern Spain. Modeled changes in summer ozone levels range from −1.7 to 1.6 ppbv. We find a smaller ensemble-mean evolution of SOMO35 as compared to inter-model variability. We also investigate the uncertainty due to inter-decadal variability and find that 10-year periods may not be sufficient to allow the detection of statistically significant change signals.

Fire is the primary form of terrestrial ecosystem disturbance on a global scale and an important Earth system process. Most Earth system models (ESMs) have incorporated fire modeling, with 19 of them submitting model outputs of fire-related variables to the Coupled Model Intercomparison Project Phase 6 (CMIP6). This study provides the first comprehensive evaluation of CMIP6 historical fire simulations by comparing them with multiple satellite-based products and charcoal-based historical reconstructions. Our results show that most CMIP6 models simulate the present-day global burned area and fire carbon emissions within the range of satellite-based products. They also capture the major features of observed spatial patterns and seasonal cycles, the relationship of fires with precipitation and population density, and the influence of the El Niño–Southern Oscillation (ENSO) on the interannual variability of tropical fires. Regional fire carbon emissions simulated by the CMIP6 models from 1850 to 2010 generally align with the charcoal-based reconstructions, although there are regional mismatches, such as in southern South America and eastern temperate North America prior to the 1910s and in temperate North America, eastern boreal North America, Europe, and boreal Asia since the 1980s. The CMIP6 simulations have addressed three critical issues identified in CMIP5: (1) the simulated global burned area being less than half of that of the observations, (2) the failure to reproduce the high burned area fraction observed in Africa, and (3) the weak fire seasonal variability. Furthermore, the CMIP6 models exhibit improved accuracy in capturing the observed relationship between fires and both climatic and socioeconomic drivers and better align with the historical long-term trends indicated by charcoal-based reconstructions in most regions worldwide. However, the CMIP6 models still fail to reproduce the decline in global burned area and fire carbon emissions observed over the past 2 decades, mainly attributed to an underestimation of anthropogenic fire suppression, and the spring peak in fires in the Northern Hemisphere mid-latitudes, mainly due to an underestimation of crop fires. In addition, the model underestimates the fire sensitivity to wet–dry conditions, indicating the need to improve fuel wetness estimation. Based on these findings, we present specific guidance for fire scheme development and suggest a post-processing methodology for using CMIP6 multi-model outputs to generate reliable fire projection products.

The Infrared Atmospheric Sounding Interferometer (IASI) is an essential instrument for numerical weather prediction (NWP). It measures radiances at the top of the atmosphere using 8461 channels. The huge amount of observations provided by IASI has led the community to develop techniques to reduce observations while conserving as much information as possible. Thus, a selection of the 300 most informative channels was made for NWP based on the concept of information theory. One of the main limitations of this method was to neglect the covariances between the observation errors of the different channels. However, many centres have shown a significant benefit for weather forecasting to use them. Currently, the observation-error covariances are only estimated on the current IASI channel selection, but no studies to make a new selection of IASI channels taking into account the observation-error covariances have yet been carried out. The objective of this paper was therefore to perform a new selection of IASI channels by taking into account the observation-error covariances. The results show that with an equivalent number of channels, accounting for the observation-error covariances, a new selection of IASI channels can reduce the analysis error on average in temperature by 3 %, humidity by 1.8 % and ozone by 0.9 % compared to the current selection. Finally, we go one step further by proposing a robust new selection of 400 IASI channels to further reduce the analysis error for NWP.

In this study, we focus on the eruption of Mount Etna on Christmas 2018, which emitted great amounts of SO2 from 24th to 30th December into the free troposphere. Simulations based on two different estimations of SO2 emission fluxes are conducted with the chemistry-transport model MOCAGE in order to study the impact of these estimations on the volcanic plume modeling. The two flux emissions used are retrieved (1) from the ground-based network FLAME, located on the flank of the volcano, and (2) from the spaceborne instrument SEVIRI onboard the geostationary satellite MSG. Multiple spaceborne observations, in the infrared and ultraviolet bands, are used to evaluate the model results. Overall, the model results match well with the plume location over the period of the eruption showing the good transport of the volcanic plume by the model, which is linked to the use of a realistic estimation of the altitude of injection of the emissions. However, there are some discrepancies in the plume concentrations of SO2 between the two simulations, which are due to the differences between the two emission flux estimations used that are large on some of the days. These differences are linked to uncertainties in the retrieval methods and observations used to derive SO2 volcanic fluxes. We find that the uncertainties in the satellite-retrieved column of SO2 used for the evaluation of the simulations, linked to the instrument sensitivity and/or the retrieval algorithm, are sometimes nearly as large as the differences between the two simulations. This shows a limitation of the use of satellite retrievals of SO2 concentrations to quantitatively validate modeled volcanic plumes. In the paper, we also discuss approaches to improve the simulation of SO2 concentrations in volcanic plumes through model improvements and also via more advanced methods to more effectively use satellite-derived products.