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The impact of biomass burning aerosols (BBA) emitted in central Africa on the tropical African climate is studied using the ocean–atmosphere global climate model CNRM-CM, including prognostic aerosols. The direct BBA forcing, cloud feedbacks (semi-direct effects), effects on surface solar radiation, atmospheric dynamics and precipitation are analysed for the 1990–2014 period. During the June–July–August (JJA) season, the CNRM-CM simulations reveal a BBA semi-direct effect exerted on low-level clouds with an increase in the cloud fraction of ∼5 %–10 % over a large part of the tropical ocean. The positive effect of BBA radiative effects on low-level clouds is found to be mainly due to the sea surface temperature response (decrease of ∼0.5 K) associated with solar heating at 700 hPa, which increases the lower-tropospheric stability. Over land, results also indicate a positive effect of BBA on the low-cloud fraction, especially for the coastal regions of Gabon and Angola, with a potentially enhanced impact in these coupled simulations that integrates the response (cooling) of the sea surface temperature (SST). In addition to the BBA radiative effect on SST, the ocean–atmosphere coupled simulations highlight that the oceanic temperature response is noticeable (about -0.2 to -0.4 K) down to ∼80 m depth in JJA between the African coast and 10° W. In parallel to low-level clouds, reductions of ∼5 %–10 % are obtained for mid-level clouds over central Africa, mainly due to BBA-induced surface cooling and lower-tropospheric heating inhibiting convection. In terms of cloud optical properties, the BBA radiative effects induced an increase in the optical depth of about ∼2 –3 over the ocean south of the Equator. The result of the BBA direct effect and feedback on tropical clouds modulates the surface solar radiation over the whole of tropical Africa. The strongest surface dimming is over central Africa (∼-30 W m−2), leading to a large reduction in the continental surface temperature (by ∼1 to 2 K), but the solar radiation at the oceanic surface is also affected up to the Brazilian coast. With respect to the hydrological cycle, the CNRM-CM simulations show a negative effect on precipitation over the western African coast, with a decrease of ∼1 to 2 mm d−1. This study also highlights a persistent impact of BBA radiative effects on low-level clouds (increase in cloud fraction, liquid water content and optical depth) during the September–October–November (SON) period, mainly explained by a residual cooling of sea surface temperature over most of the tropical ocean. In SON, the effect on precipitation is mainly simulated over the Gulf of Guinea, with a reduction of ∼1 mm d−1. As for JJA, the analysis clearly highlights the important role of the slow response of the ocean in SON and confirms the need to use coupled modelling platforms to study the impact of BBA on the tropical African climate. [ABSTRACT FROM AUTHOR]

Algae populate multiple habitats, including snow and ice, where they can form red blooms. These decrease snow albedo, accelerating snowmelt and potentially feeding back on snow and glacier decline caused by climate change. Quantifying this feedback requires the understanding of bloom evolution with climate change. Little, however, is known about the drivers of red snow blooms. Here, we develop an algorithm to analyze 5 y of satellite data from the European Alps and separate bloom occurrences from similarly colored Saharan dust depositions. In a second step, we combine the occurrences of blooms with meteorological data and snow simulations to identify the drivers of blooms. Results show that the upward migration of algae from the ground and blooming requires the presence of liquid water throughout the whole snow column for at least 46 d. Our limited data suggest that moderate dust amounts provide nutrients favorable to bloom, whereas large dust amounts hasten snowmelt and reduce its duration below the threshold required for blooming. Over the period studied, blooms cover 1.3% of the area above 1,800m elevation, advancing the snow melt-out date by 4 to 21 d in these areas. Under warmer climates, maximum snow mass will decrease whereas snowmelt duration, that controls algal blooms' occurrences, is less sensitive to global temperature increase. In this respect, the impact of bloom on snowmelt will either remain stable (RCP4.5) or decrease (RCP8.5). Algal blooms in the Alps therefore do not constitute a positive climate feedback. [ABSTRACT FROM AUTHOR]

Anthropogenic aerosols play a major role in the Earth–atmosphere system by influencing the Earth's radiative budget and precipitation and consequently the climate. The perturbation induced by changes in anthropogenic aerosols on the Earth's energy balance is quantified in terms of the effective radiative forcing (ERF). In this work, the present-day shortwave (SW), longwave (LW), and total (i.e., SW plus LW) ERF of anthropogenic aerosols is quantified using two different sets of experiments with prescribed sea surface temperatures (SSTs) from Earth system models (ESMs) participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6): (a) time-slice pre-industrial perturbation simulations with fixed SSTs (piClim) and (b) transient historical simulations with time-evolving SSTs (histSST) over the historical period (1850–2014). ERF is decomposed into three components for both piClim and histSST experiments: (a) ERFARI , representing aerosol–radiation interactions; (b) ERFACI , accounting for aerosol–cloud interactions (including the semi-direct effect); and (c) ERFALB , which is due to temperature, humidity, and surface albedo changes caused by anthropogenic aerosols. We present spatial patterns at the top-of-atmosphere (TOA) and global weighted field means along with inter-model variability (1 standard deviation) for all SW, LW, and total ERF components (ERFARI , ERFACI , and ERFALB) and for every experiment used in this study. Moreover, the inter-model agreement and the robustness of our results are assessed using a comprehensive method as utilized in the IPCC Sixth Assessment Report. Based on piClim experiments, the total present-day (2014) ERF from anthropogenic aerosol and precursor emissions is estimated to be - 1.11 ± 0.26 Wm-2 , mostly due to the large contribution of ERFACI to the global mean and to the inter-model variability. Based on the histSST experiments for the present-day period (1995–2014), similar results are derived, with a global mean total aerosol ERF of - 1.28 ± 0.37 Wm-2 and dominating contributions from ERFACI. The spatial patterns for total ERF and its components are similar in both the piClim and histSST experiments. Furthermore, implementing a novel approach to determine geographically the driving factor of ERF, we show that ERFACI dominates over the largest part of the Earth and that ERFALB dominates mainly over the poles, while ERFARI dominates over certain reflective surfaces. Analysis of the inter-model variability in total aerosol ERF shows that SW ERFACI is the main source of uncertainty predominantly over land regions with significant changes in aerosol optical depth (AOD), with eastern Asia contributing mostly to the inter-model spread of both ERFARI and ERFACI. The global spatial patterns of total ERF and its components from individual aerosol species, such as sulfates, organic carbon (OC), and black carbon (BC), are also calculated based on piClim experiments. The total ERF caused by sulfates (piClim- SO2) is estimated at - 1.11 ± 0.31 Wm-2 , and the OC ERF (piClim-OC) is - 0.35 ± 0.21 Wm-2 , while the ERF due to BC (piClim-BC) is 0.19 ± 0.18 Wm-2. For sulfates and OC perturbation experiments, ERFACI dominates over the globe, whereas for BC perturbation experiments ERFARI dominates over land in the Northern Hemisphere and especially in the Arctic. Generally, sulfates dominate ERF spatial patterns, exerting a strongly negative ERF especially over industrialized regions of the Northern Hemisphere (NH), such as North America, Europe, and eastern and southern Asia. Our analysis of the temporal evolution of ERF over the historical period (1850–2014) reveals that ERFACI clearly dominates over ERFARI and ERFALB for driving the total ERF temporal evolution. Moreover, since the mid-1980s, total ERF has become less negative over eastern North America and western and central Europe, while over eastern and southern Asia there is a steady increase in ERF magnitude towards more negative values until 2014. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is one of the most important climate forcers with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a 2-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi (PDM) located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded Aethalometer AE33, a thermal-optical analyser Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations in the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy were explained by the mass absorption cross section (MAC) that was too low and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentrations were below 25 µgCcm-2 , which is probably linked to the incorrect determination of the organic carbon (OC)–EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow for the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution is needed to accurately estimate MrBC over a larger size range. [ABSTRACT FROM AUTHOR]

Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM2.5) as major climate forcers. Yet the model performance for PM2.5 components remains little evaluated due in part to a lack of observational data. Here, we evaluate near-surface concentrations of PM2.5 and its five main components over China as simulated by 14 CMIP6 models, including organic carbon (OC; available in 14 models), black carbon (BC; 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM2.5 components. Seven models output total PM2.5 concentrations, and they all underestimate the observed total PM2.5 over eastern China, with GFDL-ESM4 (- 1.5 %) and MPI-ESM-1-2-HAM (- 1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM2.5 from the available component output, underestimate the total PM2.5 concentrations partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by - 71.2 % to - 37.8 % across the 14 models) and the smallest for BC (- 47.9 % to - 12.1 %). The multi-model mean (MMM) reproduces the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.74) fairly well, yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

Improving knowledge of current and future spatio-temporal variability of surface solar radiation is essential in the context of climate change and associated environmental and societal issues. Such an evolution will be influenced by changes in both meteorological parameters and atmospheric composition, notably by anthropogenic emissions. We investigate both all-sky and clear-sky surface solar radiation (SSR) variability, along with cloud cover, aerosols and water vapor content, over Northern France and Benelux. This region of Europe is largely influenced by cloudy conditions and anthropogenic aerosols, especially nitrate species. Our analysis relies on the CNRM-ALADIN64 regional climate model at 12.5 km x 12.5 km spatial resolution, which includes the TACTIC interactive aerosol scheme. First, hindcast reanalysis-driven simulations over 2010-2020 allow a regional evaluation of ALADIN outputs and to investigate recent spatial variability of SSR and associated atmospheric parameters. Secondly, their possible evolution at mid and end of the 21st century are investigated based on ALADIN climate simulations following two contrasted CMIP6 scenarios, namely the shared socioeconomic pathways (SSP), SSP1-1.9 and SSP3-7.0. Our regional evaluation of clear-sky and all-sky SSR, clear-sky frequency and aerosols over northern France and Benelux shows reasonable agreement between 2010-2020 ALADIN hindcast simulations and coincident multi-site groundbased measurements, despite some overestimation of nitrate aerosols in spring and an overall underestimation of organic particles by the model. Focusing on spring and summer seasons, hindcast simulations show maximum of solar radiation around the southern parts and over sea areas of the region. In addition to latitudinal effects, elevated aerosol loads over Benelux, and high cloud cover over the South West of England reduce the SSR. Compared to 2005-2014 atmospheric conditions, ALADIN mid and long-term simulations for SSP1-1.9 predict a significant reduction of aerosol loads, especially over the Benelux, associated with an increase in future clear-sky SSR but geographically limited all-sky SSR evolution. In contrast, SSP3-7.0 simulations projected pronounced and extended decreases of clear-sky and all-sky SSR over most of the Benelux/northern France region. These reductions are maximum in spring due to combined effects of cloud cover and nitrate aerosol increases over the Benelux starting in 2050, that are amplified by an additional water vapor increase in 2100. Thus, this regional climate model approach suggests that future SSR evolution over this part of western Europe will be drastically affected by combined effects of anthropogenic aerosol emissions trajectories, cloud cover and water vapor changes, which also induce strong spatial patterns. [ABSTRACT FROM AUTHOR]

The impact of biomass burning aerosols (BBA) emitted in Central Africa on the tropical African climate is studied using the ocean-atmosphere global climate model CNRM-CM, including prognostic aerosols. The direct BBA forcing, cloud feedbacks (semi-direct effects), effects on surface solar radiation, atmospheric dynamics and precipitation are analysed for the 1990-2014 period. During the June-July-August (JJA) season, the CNRM-CM simulations reveal a BBA semi-direct effect exerted on low-level clouds with an increase in cloud fraction of ∼5-10% over a large part of the tropical ocean. The positive feedback of BBA radiative effects on low-level clouds is found to be mainly due to the sea surface temperature response (decrease of ∼-0.5 K) associated with solar heating at 700 hPa, which increases the lower tropospheric stability. Over land, results also indicates a positive effect of BBA on the low cloud fraction especially for the coastal regions of Gabon and Angola with a potentially enhanced impact in these coupled simulations that integrate the response (cooling) of the SST. In addition to the BBA radiative effect on sea surface temperature, the ocean-atmosphere coupled simulations highlight that the oceanic temperature response is noticeable (about -0.2 to -0.4 K) down to ∼80 m depth in the JJA between the African coast and 10°W. In parallel to low-level clouds, reductions of ∼5-10% are obtained for mid-level clouds over central Africa, mainly due to BBA-induced surface cooling and lower tropospheric heating inhibiting convection. In terms of cloud optical properties, the BBA radiative effects induced an increase of the optical depth by about ∼2-3 south of the equator over the ocean. The result of the BBA direct effect and feedback on tropical clouds modulates the surface solar radiation over the whole Tropical Africa. The strongest surface dimming is over central Africa (∼-30 W m-2), leading to a large reduction of the continental surface temperature (by ∼-1 to -2 K), but the solar radiation at the oceanic surface is also affected up to the Brazilian coast. With respect to the hydrological cycle, the CNRM-CM simulations show a negative feedback on precipitation over theWest African coast with a decrease of ∼-1 to -2 mm per day. This study highlights also a persistent impact of BBA radiative effects on low-level clouds (increase in cloud fraction, liquid water content and optical depth) during the September-October-November (SON) period, mainly explained by a residual cooling of sea surface temperature over most of the tropical ocean. In SON, the feedback on precipitation is mainly simulated over the Gulf of Guinea with a reduction by ∼-1 mm per day. As for JJA, the analysis clearly highlights the important role of the slow response of the ocean in SON and confirms the need to use coupled modelling platforms to study the impact of BBA on tropical African climate. [ABSTRACT FROM AUTHOR]

Black-carbon-containing particles strongly absorb light, causing substantial radiative heating of the atmosphere. The climate-relevant properties of black carbon (BC) are poorly constrained in high-altitude mountain regions, where many complex interactions between BC, radiation, clouds and snow have important climate implications. This study presents 2-year measurements of BC microphysical and optical properties at the Pic du Midi (PDM) research station, a high-altitude observatory located at 2877 m above sea level in the French Pyrenees. Among the long-term monitoring sites in the world, PDM is subject to limited influence from the planetary boundary layer (PBL), making it a suitable site for characterizing the BC in the free troposphere (FT). The classification of the dominant aerosol type using aerosol spectral optical properties indicates that BC is the predominant aerosol absorption component at PDM and controls the variation in single-scattering albedo (SSA) throughout the 2 years. Single-particle soot photometer (SP2) measurements of refractory BC (rBC) show a mean mass concentration (MrBC) of 35 ngm-3 and a relatively constant rBC core mass-equivalent diameter of about 180 nm, which are typical values for remote mountain sites. Combining the MrBC with in situ absorption measurements, a rBC mass absorption cross-section (MAC rBC) of 9.2 ± 3.7 m2g-1 at λ=880 nm has been obtained, which corresponds to an absorption enhancement (Eabs) of ∼2.2 compared to that of bare rBC particles with equal rBC core size distribution. A significant reduction in the ΔMrBC/ΔCO ratio when precipitation occurred along the air mass transport suggests wet removal of rBC. However we found that the wet removal process did not affect the rBC size, resulting in unchanged Eabs. We observed a large seasonal contrast in rBC properties with higher MrBC and Eabs in summer than in winter. In winter a high diurnal variability in MrBC (Eabs) with higher (lower) values in the middle of the day was linked to the injection of rBC originating from the PBL. On the contrary, in summer, MrBC showed no diurnal variation despite more frequent PBL conditions, implying that MrBC fluctuations are rather dominated by regional and long-range transport in the FT. Combining the ΔMrBC/ΔCO ratio with air mass transport analysis, we observed additional sources from biomass burning in summer leading to an increase in MrBC and Eabs. The diurnal pattern of Eabs in summer was opposite to that observed in winter with maximum values of ∼2.9 observed at midday. We suggest that this daily variation may result from a photochemical process driving the rBC mixing state rather than a change in BC emission sources. Such direct 2-year observations of BC properties provide quantitative constraints for both regional and global climate models and have the potential to close the gap between model-predicted and observed effects of BC on the regional radiation budget and climate. The results demonstrate the complex influence of BC emission sources, transport pathways, atmospheric dynamics and chemical reactivity in driving the light absorption of BC. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is one of the most important climate forcer with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a two-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded aethalometer AE33, a thermal-optical analyzer Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations of the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type, despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy was explained by the too low MAC and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentration were below 25 µ gC cm−2 , which is probably linked to the incorrect determination of the OC-EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution are needed to accurately estimate MrBC over a larger size range. [ABSTRACT FROM AUTHOR]

Anthropogenic aerosols play a major role for the Earth-Atmosphere system by influencing the Earth’s radiative budget and climate. The effect of the perturbation induced by changes in anthropogenic aerosols on the Earth's energy balance is quantified in terms of the effective radiative forcing (ERF) which is the recommended metric for perturbations affecting the Earth’s top-of-atmosphere energy budget since it is a better way to link this perturbation to subsequent global mean surface temperature change. In this work, the present-day ERF of anthropogenic aerosols is quantified using simulations from Earth system models (ESMs) participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The ERFs of individual aerosol species, such as sulphates, organic carbon (OC), and black carbon (BC) are calculated along with the ERF due to all anthropogenic aerosols and the transient ERF over the historical period (1850–2014). Additionally, ERF is analyzed into three components: (a) ERFARI, representing aerosol-radiation interactions, (b) ERFACI, accounting for aerosol-cloud interactions, and (c) ERFALB, which is mainly due to the contribution of surface albedo changes caused by anthropogenic aerosols. Here, the total anthropogenic aerosol ERF (calculated using the piClim-aer experiment) is estimated to be -1.11 ± 0.26 W m-2, mostly due to the large contribution of ERFACI (-1.14 ± 0.33 W m-2), compared to ERFARI (-0.02 ± 0.20 W m-2) and ERFALB (0.05 ± 0.07 W m-2). The total ERF caused by sulphates (piClim-SO2) is estimated at -1.11 ± 0.31 W m-2, the OC ERF (piClim-OC) is -0.35 ± 0.21 W m-2, whereas the ERF exerted by BC (piClim-BC) is 0.19 ± 0.18 W m-2. On top of that, our analysis reveals that ERFACI clearly prevails over the largest part of the Earth except for the BC experiment where ERFARI prevails over land. By the end of the historical period (1995–2014), the global mean total aerosol ERF is estimated at -1.28 ± 0.37 W m-2 (calculated using the histSST experiment). We find that sulphates dominate both present-day and transient ERF spatial patterns at the top of the atmosphere, exerting a strongly negative ERF especially over industrialized regions of the Northern Hemisphere, such as North America, Europe, East and South Asia. Since the mid-1980s ERF has become less negative over Eastern North America and Western and Central Europe, while over East and South Asia there is a steady increase in ERF magnitude towards more negative values until 2014. [ABSTRACT FROM AUTHOR]

Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM2.5) as major climate forcers. Yet the model performance for PM2.5 components remains little evaluated due in part to lack of observational data. Here, we evaluate near-surface concentrations of PM2.5 and its five main components over China as simulated by fourteen CMIP6 models, including organic carbon (OC, available in 14 models), black carbon (BC, 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM2.5 components. Seven models output total PM2.5 concentrations, and they all underestimate the observed total PM2.5 over eastern China, with GFDL-ESM4 (–1.5 %) and MPI-ESM-1-2-HAM (–1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM2.5 from the available components output, underestimate the total PM2.5 concentrations, partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by –71.2 % to –37.8 % across the 14 models) and the smallest for BC (–47.9 % to –12.1 %). The multi-model mean (MMM) reproduces fairly well the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.75), yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

Earth system models (ESMs) participating in the latest Coupled Model Intercomparison Project Phase 6 (CMIP6) simulate various components of fine particulate matter (PM2.5) as major climate forcers. Yet the model performance for PM2.5 components remains little evaluated due in part to lack of observational data. Here, we evaluate near-surface concentrations of PM2.5 and its five main components over China as simulated by fourteen CMIP6 models, including organic carbon (OC, available in 14 models), black carbon (BC, 14 models), sulfate (14 models), nitrate (4 models), and ammonium (5 models). For this purpose, we collect observational data between 2000 and 2014 from a satellite-based dataset for total PM2.5 and from 2469 measurement records in the literature for PM2.5 components. Seven models output total PM2.5 concentrations, and they all underestimate the observed total PM2.5 over eastern China, with GFDL-ESM4 (–1.5 %) and MPI-ESM-1-2-HAM (–1.1 %) exhibiting the smallest biases averaged over the whole country. The other seven models, for which we recalculate total PM2.5 from the available components output, underestimate the total PM2.5 concentrations, partly because of the missing model representations of nitrate and ammonium. Concentrations of the five individual components are underestimated in almost all models, except that sulfate is overestimated in MPI-ESM-1-2-HAM by 12.6 % and in MRI-ESM2-0 by 24.5 %. The underestimation is the largest for OC (by –71.2 % to –37.8 % across the 14 models) and the smallest for BC (–47.9 % to –12.1 %). The multi-model mean (MMM) reproduces fairly well the observed spatial pattern for OC (R = 0.51), sulfate (R = 0.57), nitrate (R = 0.70) and ammonium (R = 0.75), yet the agreement is poorer for BC (R = 0.39). The varying performances of ESMs on total PM2.5 and its components have important implications for the modeled magnitude and spatial pattern of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

Black Carbon containing particles (BC) are strong light absorbers, causing substantial radiative heating of the atmosphere. The climate-relevant properties of BC are poorly constrained in high-elevation mountain regions, where numerous complex interactions between BC, radiation, clouds and snow have important climate implications. This study presents twoyear measurements of BC microphysical and optical properties at the research station of Pic du Midi (PDM), a high-altitude observatory located at 2877 m above sea level in the French Pyrenees. Among the worldwide existing long-term monitoring sites, PDM has experiences limited influence of the planetary boundary layer (PBL), making it an appropriate site for characterizing free tropospheric (FT) BC. The classification of the dominant aerosol type using the spectral optical properties of the aerosols indicates that BC was the predominant absorption component of aerosols at PDM and controlled the variation of Single Scattering Albedo (SSA) throughout the two years. Single-particle soot photometer (SP2) measurements showed a mean mass concentrations of BC (MBC) of 35 ng m-3 and a relatively constant BC core mass-equivalent diameter of around 180 nm, which are typical values for remote mountain sites. Combining the MBC with in situ absorption measurements yielded BC mass absorption coefficient (MACBC) of 9.8 ± 2.7 m² g-1 at 880 nm, which corresponds to an absorption enhancement Eabs) of 2.4 compared to that of bare BC particles with equal BC core size distribution. A significant reduction of the ratio ΔBC/ΔCO when precipitation occurred along the air mass transport suggests wet removal of BC. However we found that the wet removal process did not affect the size of BC, resulting in unchanged Eabs. We observed a large seasonal contrast in BC properties with higher MBC and Eabs in summer than winter. In winter a strong diurnal variability of MBC (Eabs) with higher lower) values in the middle of the day was linked to the injection of BC originating from the PBL. During summer in contrast, MBC showed no diurnal variation was rather constant despite more frequent PBL-conditions, implying that MBC fluctuations were rather dominated by regional and long-range transport in the FT. A body of evidence suggests that biomass burning emissions effectively altered the concentration and optical properties of BC at PDM, leading to higher Eabs in summer compared to winter. The diurnal pattern of Eabs in summer was opposite to that observed in winter with maximum values of 2.9 observed at noon. We suggest that this daily variation results from photochemical processing driving BC mixing state rather than a change in BC emission source. Such direct two-year observations of BC properties provide quantitative constraints for both regional and global climate models and have the potential to close the gap between model predicted and observed effects of BC on regional radiation budget and climate. The results demonstrates the complex influence of BC emission sources, transport pathways, atmospheric dynamics and chemical reactivity in driving the light absorption of BC. [ABSTRACT FROM AUTHOR]