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We present an inter-comparison of simulated sea-salt aerosols (SSA) in CMIP6 models, including an evaluation against station observations in the Artic and Antarctic regions and satellite data. Drivers of model diversity are investigated. Historical and future trends are also explored and connected to their driving mechanisms. Additionally, the sensitivity of the polar radiative budget to SSA in CMIP6 models is quantified and put in relation to present-day uncertainties and future trends. Comparisons suggest (i) a large inter-model spread in SSA surface concentrations mostly driven by the diversity in source functions, (ii) an important overestimation of SSA surface concentrations compared to measurement stations but reasonable agreement with optical depth from satellite data, (iii) difficulties in properly capturing the annual cycle of SSA at both poles, particularly at higher latitude. A generally increasing trend in SSA concentrations is found in CMIP6 over the last decades and in future scenarios. CMIP6 models show that SSA contribute to cooling the poles significantly, implying possible uncertainties of several W/m2 in the present-day polar radiative budget.

Air pollution in the central zone of Chile not only is a public health concern, but also threatens water resources and climate, in connection with the transport and deposition of black carbon (BC) from urban centers onto the glaciers of the Andes Cordillera. Chemistry-transport simulations reveal a seasonal dichotomy in the flux and latitudinal pattern of BC deposition on glaciers of the central Chilean Andes. The average deposition flux of BC on glaciers between 30° S and 37° S is 4 times larger in winter, affecting mostly low elevation glaciers, whereas the smaller summertime flux affects glaciers evenly, irrespective of their elevation. The contribution of emissions from Santiago city is dominant in summertime with more than 50 % along the Andes, but minor in wintertime with less than 20 % even close to the capital city. Transport at larger scales and more local sources likely account for the remaining flux. The superimposition of synoptic-scale circulation and local mountain-valley circulation along the Andes cordillera drives the differences between summertime and wintertime deposition fluxes and generates a greater meteorological export potential during summer months. Future emissions and climate projections suggest that under the RCP8.5 scenario the gap between summertime and wintertime BC export and deposition flux could decrease, thereby pointing to summertime emission control gaining relevance. The chemistry-transport modeling approach for BC deposition on the Andes sheds light on the importance of the often disregarded summertime emissions on the radiative balance of its glaciers, particularly in the vicinity of Santiago.

Near-surface mercury and ozone depletion events occur in the lowest part of the atmosphere during Arctic spring. Mercury depletion is the first step in a process that transforms long-lived elemental mercury to more reactive forms within the Arctic that are deposited to the cryosphere, ocean, and other surfaces, which can ultimately get integrated into the Arctic food web. Depletion of both mercury and ozone occur due to the presence of reactive halogen radicals that are released from snow, ice, and aerosols. In this work, we added a detailed description of the Arctic atmospheric mercury cycle to our recently published version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem 4.3.3) that includes Arctic bromine and chlorine chemistry and activation/recycling on snow and aerosols. The major advantage of our modelling approach is the online calculation of bromine concentrations and emission/recycling that is required to simulate the hourly and daily variability of Arctic mercury depletion. We used this model to study coupling between reactive cycling of mercury, ozone, and bromine during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) spring season in 2020 and evaluated results compared to land-based, ship-based, and remote sensing observations. The model predicts that elemental mercury oxidation is driven largely by bromine chemistry and that particulate mercury is the major form of oxidized mercury. The model predicts that the majority (74%) of oxidized mercury deposited to land-based snow is re-emitted to the atmosphere as gaseous elemental mercury, while a minor fraction (4%) of oxidized mercury that is deposited to sea ice is re-emitted during spring. Our work demonstrates that hourly differences in bromine/ozone chemistry in the atmosphere must be considered to capture the springtime Arctic mercury cycle, including its integration into the cryosphere and ocean.

In wintertime, high concentrations of atmospheric fine particulate matter (PM2.5) are commonly observed in the metropolitan area of Santiago, Chile. Hourly peaks can be very strong, up to 10 times above average levels, but have barely been studied so far. Based on atmospheric composition measurements and chemistry-transport modeling (WRF-CHIMERE), the chemical signature of sporadic skyrocketing wintertime PM2.5 peaks is analyzed. This signature and the timing of such extreme events trace their origin back to massive barbecue cooking by Santiago's inhabitants during international soccer games. The peaks end up evacuated outside Santiago after a few hours but trigger emergency plans for the next day. Decontamination plans in Santiago focus on decreasing emissions from traffic, industry, and residential heating. Thanks to the air quality network of Santiago, this study shows that cultural habits such as barbecue cooking also need to be taken into account. For short-term forecast and emergency management, cultural events such as soccer games seem a good proxy to prognose possible PM2.5 peak events. Not only can this result have an informative value for the Chilean authorities but also a similar methodology could be reproduced for other cases throughout the world in order to estimate the burden on air quality of cultural habits.

The Pantanal biome, at the confluence of Brazil, Bolivia and Paraguay, is the largest continental wetland on the planet and an invaluable reserve of biodiversity. The exceptional 2020 fire season in Pantanal drew particular attention due to the severe wildfires and the catastrophic natural and socio-economic impacts witnessed within the biome. So far, little progress has been made in order to better understand the influence of climate extremes on fire occurrence in Pantanal. Here, we evaluate how extreme hot conditions, through heatwave events, are related to the occurrence and the exacerbation of fires in this region. A historical analysis using a statistical regression model found that heatwaves during the dry season explained 82% of the interannual variability of burned area during the fire season. In a future perspective, an ensemble of CORDEX-CORE simulations assuming different Representative Concentration Pathways (RCP2.6 and RCP8.5), reveal a significant increasing trend in heatwave occurrence over Pantanal. Compared to historical levels, the RCP2.6 scenario leads to more than a doubling in the Pantanal heatwave incidence during the dry season by the second half of the 21st century, followed by a plateauing. Alternatively, RCP8.5 projects a steady increase of heatwave incidence until the end of the century, pointing to a very severe scenario in which heatwave conditions would be observed nearly over all the Pantanal area and during practically all the days of the dry season. Accordingly, favorable conditions for fire spread and consequent large burned areas are expected to occur more often in the future, posing a dramatic short-term threat to the ecosystem if no preservation action is undertaken.

The configuration of the Santiago basin, Chile (33.5°S 70.65°W) is quite unique in that it combines very strong emissions of urban anthropogenic pollutants with the steep topography of the coastal and Andes cordilleras surrounding the Metropolitan area. Interactions between atmospheric pollution and mountain meteorology are therefore exacerbated, and the potential for black carbon (BC) deposition on glaciers is strong. Based on chemistry-transport modeling with WRF-CHIMERE, we investigate (i) the pathways leading to deposition of BC from Santiago up to Andean glaciers in wintertime and (ii) the differences in magnitude and time dynamics of such deposition between wintertime and summertime.Ice and snow in the central Andes contain significant amounts of BC often attributed to emissions from Santiago. However, given the usually stable conditions in wintertime and the height of the obstacle to overcome for urban air masses (Santiago is 500 m a.s.l., summits are above 4000 m a.s.l.) the pathways for such deposition are not straightforward. We find that, for a typical winter month, up to 40% of BC dry deposition on snow- or ice-covered areas in the central Andes directly downwind from the Metropolitan area can indeed be attributed to emissions from Santiago. The adjacent network of canyons plays a key role in this export: for the case of the Maipo canyon, polluted urban air masses follow gentle slopes upward in the afternoon, consistently with mountain-valley circulation, before being vertically exported when reaching the tip of the main canyon. Statistical analysis shows that zonal wind speed in the urban area and vertical diffusion deep into the canyon account for most of the variance in BC deposition.In summertime, more intense convection takes place, and mountain-valley circulation is seldom perturbed by cloud cover, resulting in a greater export potential. Accordingly, summertime dry deposition of BC on glaciers occurs on a regular basis with equivalent amounts each day, contrarily to a more chaotic time series in wintertime. The contribution of wet deposition in winter (nonexistent in summer) exacerbates this irregularity. However, as a consequence of weaker emissions, average monthly dry deposition of BC over the central Andes glaciers (29°S to 38°S) is found to be less than half in summertime (135 µg/m2) compared to wintertime (320 µg/m2). Given the lesser role played by wood burning for residential heating in summertime, emissions from Santiago through traffic and industry dominate the signal leading to 55% of dry deposition, while it accounts for only 14% in wintertime, at the regional scale, due to more scattered sources.

Central Chile faces atmospheric pollution issues all year long, in relation with elevated concentrations of fine particulate matter during the cold months and tropospheric ozone during the warm season. In addition to public health issues, environmental problems regarding vegetation growth and water supply, as well as meteorological feedback are at stake. Sharp spatial gradients in regional emissions along with a complex geographical situation make for variable and heterogeneous dynamics in the localization and long-range transport of pollutants, with seasonal differences. Based on chemistry-transport modeling with WRF-CHIMERE, this work studies for one winter period and one summer period: (i) the contribution of emissions from the Santiago Metropolitan Area to air pollution in central Chile, (ii) the reciprocal contribution of regional pollutants transported into the Santiago basin. The underlying 3-dimensional advection patterns are investigated. We find that on average for the winter period 5 μg m−3 to 10 μg m−3 of fine particulate matter in Santiago come from regional transport, corresponding to 13 % to 15 % of average concentrations. In turn, emissions from the Metropolitan Area contribute to 5 % to 10 % of fine particulate matter pollution as far as 4° north and 4° south. Wintertime transport occurs mostly close to the surface. In summertime, exported precursors from Santiago, in combination with mountain-valley circulation dynamics, are found to account for most of ozone formation in the adjacent Andes cordillera and to create a persistent plume of ozone of more than 50 ppb, extending along 80 km horizontally and 1.5 km vertically, and located several hundred meters above ground, slightly north of Santiago. This work constitutes the first description of such an ozone bubble formation mechanism. Emissions of precursors from the capital city also affect daily maxima of surface ozone hundreds of kilometers away. In parallel, cutting emissions of precursors in the Santiago basin results in an increase of surface ozone mixing ratios in its western area.

Ice and snow in the Central Andes contain significant amounts of light-absorbing particles such as black carbon. The consequent accelerated melting of the cryosphere is not only a threat from a climate perspective but also for water resources and snow-dependent species and activities, worsened by the mega-drought affecting the region since the last decade. Given its proximity to the Andes, emissions from the Metropolitan Area of Santiago, Chile, are believed to be among the main contributors to deposition on glaciers. However, no evidence backs such an assertion, especially given the usually subsident and stable conditions in wintertime, when the snowpack is at its maximum extent. Based on high-resolution chemistry-transport modeling with WRF-CHIMERE, the present work shows that, for the month of July 2015, up to 40% of black carbon dry deposition on snow or ice covered areas in the Central Andes downwind from the Metropolitan area can be attributed to emissions from Santiago. Through the analysis of aerosol tracers we determine (i) that the areas of the Metropolitan Area where emissions matter most when it comes to export towards glaciers are located in Eastern Santiago near the foothills of the Andes, (ii) the crucial role of the network of Andean valleys that channels pollutants up to remote locations near glaciers, following gentle slopes. A direct corollary is that severe urban pollution, and deposition of impurities on the Andes, are anti-correlated phenomena. Finally, a two-variable meteorological index is developed that accounts for the dynamics of aerosol export towards the Andes, based on the zonal wind speed over the urban area, and the vertical diffusion coefficient in the valleys close to ice and snow covered terrain. Numerous large urban areas are found along the Andes so that the processes studied here can shed light on similar investigations for other glaciers-dependent Andean regions.

In wintertime, high background concentrations of atmospheric fine particulate matter (PM2.5) are commonly observed in the metropolitan area of Santiago, Chile. Although the frequency of alert events has been decreasing in the recent years, two short-lived peak events reaching up to 600µg/m3 for a few hours were observed in the city on June 18th and June 26th 2016, triggering emergency measures for the next day.The observed meteorological conditions at the time of these peaks are not unusual. In addition, a high-resolution meteorology and chemistry-transport simulation with the WRF meteorological model and the CHIMERE chemistry-transport model reproduces fairly well the meteorology and levels of PM for June 2016, except for those two particular events that are not captured by the model. The combination of these elements leads to the conclusion that sporadic strong emissions are at play.The analysis of recorded concentration ratios of PM2.5, NOx and CO points to a specific source, departing significantly from the average signal for the season. Based on the literature and HTAP emission ratios, usual sources of PM such as traffic, residential heating and industry can be ruled out. The temporal correlation of the events with soccer games of the Chilean team and the recorded chemical footprint lead to conclude to the dominant contribution of massive barbecue cooking at the peak times.Following the source identification via surface stations analysis, the next question was to quantify the potential transport and impact of such pollution peaks in the Santiago Metropolitan area. An additional source term was added in the chemistry-transport simulation, and maps of PM changes were analyzed. For both events, the same region in the Southwest of Santiago was impacted by the plume.A natural continuation of this work is the study through modeling of the dispersion patterns of polluted plumes outside of the Santiago basin on a longer time scale. In particular, significant deposition of light-absorbing particles has been measured on glaciers near the capital city, without a clear identification of their source or the underlying processes of transport.

Black carbon transport from the Santiago Metropolitan Area, Chile, up to the adjacent Andes Cordillera and its glaciers is of major concern. Its deposition accelerates the melting of the snowpack, which could lead to stress on water supply in addition to climate feedback. A proposed pathway for this transport is the channelling through the network of canyons that connect the urban basin to the elevated summits, as suggested by modelling studies, although no observations have validated this hypothesis so far. In this work, atmospheric measurements from a dedicated field campaign conducted in winter 2015, under severe urban pollution conditions, in Santiago and the Maipo canyon, southeast of Santiago, are analysed. Wind (speed and direction) and particulate matter concentrations measured at the surface and along vertical profiles, demonstrate intrusions of thick layers (up to 600 m above ground) of urban black carbon deep into the canyon on several occasions. Transport of PM down-valley occurs mostly through shallow layers at the surface except in connection with deep valley intrusions, when a secondary layer in altitude with return flow (down-valley) at night is observed. The transported particulate matter is mostly from the vicinity of the entrance to the canyon and uncorrelated to concentrations observed in downtown Santiago. Reanalyses data show that for 10% of the wintertime days, deep intrusions into the Maipo canyon are prevented by easterly winds advecting air pollutants away from the Andes. Also, in 23% of the cases, intrusions proceed towards a secondary north-eastward branch of the Maipo canyon, leaving 67% of the cases with favourable conditions for deep penetrations into the main Maipo canyon. Reanalyses show that the wind directions associated to the 33% anomalous cases are related to thick cloud cover and/or the development of coastal lows.

In wintertime, high background concentrations of atmospheric fine particulate matter (PM2.5) are commonly observed in the metropolitan area of Santiago, Chile. Hourly peaks can be very strong, up to ten times average levels, but have barely been studied so far. Based on atmospheric composition measurements and chemistry-transport modeling (WRF-CHIMERE), the chemical signature of sporadic skyrocketing wintertime PM2.5 peaks is analyzed. This signature and the timing of such extreme events traces their origin back to massive barbecue cooking by Santiago's inhabitants during international soccer games. The peaks end up evacuated outside Santiago after a few hours but trigger emergency plans for the next day. Decontamination plans in Santiago focus on decreasing traffic, industrial and residential heating emissions. Thanks to the air quality network of Santiago, this study shows that cultural habits such as barbecue cooking also need to be taken into account. For short-term forecast and emergency management, cultural events such as soccer games seem a good proxy to prognose possible PM2.5 peak events. Not only this result can have an informative value for the Chilean authorities, but a similar methodology could also be reproduced for other cases throughout the world in order to estimate the burden on air quality of cultural habits. In particular, the present study shows that investigating the atmospheric composition in large cities during major events is key for the design of effective air pollution mitigation policies.

International audience; Natural aerosols and their interactions with clouds remain an important uncertainty within climate models, especially at the poles. Here, we study the behavior of sea salt aerosols (SSaer) in the Arctic and Antarctic within 12 climate models from CMIP6. We investigate the driving factors that control SSaer abundances and show large differences based on the choice of the source function, and the representation of aerosol processes in the atmosphere. Close to the poles, the CMIP6 models do not match observed seasonal cycles of surface concentrations, likely due to the absence of wintertime SSaer sources such as blowing snow. Further away from the poles, simulated concentrations have the correct seasonality, but have a positive mean bias of up to one order of magnitude. SSaer optical depth is derived from the MODIS data and compared to modeled values, revealing good agreement, except for winter months. Better agreement for AOD than surface concentration may indicate a need for improving the vertical distribution, the size distribution and/or hygroscopicity of modeled polar SSaer. Source functions used in CMIP6 emit very different numbers of small SSaer, potentially exacerbating cloud-aerosol interaction uncertainties in these remote regions. For future climate scenarios SSP126 and SSP585, we show that SSaer concentrations increase at both poles at the end of the 21st century, with more than two times mid-20th century values in the Arctic. The pre-industrial climate CMIP6 experiments suggest there is a large uncertainty in the polar radiative budget due to SSaer.