Global Aerosol-climate Model Research Articles

Impacts of spatial heterogeneity of anthropogenic aerosol emissions in a regionally refined global aerosol–climate model

Abstract. Emissions of anthropogenic aerosol and their precursors are often prescribed in global aerosol models. Most of these emissions are spatially heterogeneous at model grid scales. When remapped from low-resolution data, the spatial heterogeneity in emissions can be lost, leading to large errors in the simulation. It can also cause the conservation problem if non-conservative remapping is used. The default anthropogenic emission treatment in the Energy Exascale Earth System Model (E3SM) is subject to both problems. In this study, we introduce a revised emission treatment for the E3SM Atmosphere Model (EAM) that ensures conservation of mass fluxes and preserves the original emission heterogeneity at the model-resolved grid scale. We assess the error estimates associated with the default emission treatment and the impact of improved heterogeneity and mass conservation in both globally uniform standard-resolution (∼ 165 km) and regionally refined high-resolution (∼ 42 km) simulations. The default treatment incurs significant errors near the surface, particularly over sharp emission gradient zones. Much larger errors are observed in high-resolution simulations. It substantially underestimates the aerosol burden, surface concentration, and aerosol sources over highly polluted regions, while it overestimates these quantities over less-polluted adjacent areas. Large errors can persist at higher elevation for daily mean estimates, which can affect aerosol extinction profiles and aerosol optical depth (AOD). We find that the revised treatment significantly improves the accuracy of the aerosol emissions from surface and elevated sources near sharp spatial gradient regions, with significant improvement in the spatial heterogeneity and variability of simulated surface concentration in high-resolution simulations. In the next-generation E3SM running at convection-permitting scales where the resolved spatial heterogeneity is significantly increased, the revised emission treatment is expected to better represent the aerosol emissions as well as their lifecycle and impacts on climate.

Impacts of ice-nucleating particles on cirrus clouds and radiation derived from global model simulations with MADE3 in EMAC

Abstract. Atmospheric aerosols can act as ice-nucleating particles (INPs) and influence the formation and the microphysical properties of cirrus clouds, resulting in distinct climate effects. We employ a global aerosol–climate model, including a two-moment cloud microphysical scheme and a parameterization for aerosol-induced ice formation in cirrus clouds, to quantify the climate impact of INPs on cirrus clouds (simulated period 2001–2010). The model considers mineral dust, soot, crystalline ammonium sulfate, and glassy organics as INPs in the cirrus regime. Several sensitivity experiments are performed to analyse various aspects of the simulated INP–cirrus effect regarding (i) the ice-nucleating potential of the INPs, (ii) the inclusion of ammonium sulfate and organic particles as INPs in the model, and (iii) the model representations of vertical updraughts. The resulting global radiative forcing of the total INP–cirrus effect, considering all different INP types, assuming a smaller and a larger ice-nucleating potential of INPs, to explore the range of possible forcings due to uncertainties in the freezing properties of INPs, is simulated as −28 and −55 mW m−2, respectively. While the simulated impact of glassy organic INPs is mostly small and not statistically significant, ammonium sulfate INPs contribute a considerable radiative forcing, which is nearly as large as the combined effect of mineral dust and soot INPs. Additionally, the anthropogenic INP–cirrus effect is analysed considering the difference between present-day (2014) and pre-industrial conditions (1750) and amounts to −29 mW m−2, assuming a larger ice-nucleating potential of INPs. In a further sensitivity experiment we analyse the effect of highly efficient INPs proposed for cirrus cloud seeding as a means to reduce global warming by climate engineering. However, the results indicate that this approach risks an overseeding of cirrus clouds and often results in positive radiative forcings of up to 86 mW m−2 depending on number concentration of seeded INPs. Idealized experiments with prescribed vertical velocities highlight the crucial role of the model dynamics for the simulated INP–cirrus effects. For example, resulting forcings increase about 1 order of magnitude (−42 to −340 mW m−2) when increasing the prescribed vertical velocity (from 1 to 50 cm s−1). The large discrepancy in the magnitude of the simulated INP–cirrus effect between different model studies emphasizes the need for future detailed analyses and efforts to reduce this uncertainty and constrain the resulting climate impact of INPs.

The global impact of the transport sectors on the atmospheric aerosol and the resulting climate effects under the Shared Socioeconomic Pathways (SSPs)

Abstract. A global aerosol–climate model is applied to quantify the impact of the transport sectors (land transport, shipping, and aviation) on aerosol and climate. Global simulations are performed for the present day (2015), based on the emission inventory of the Climate Model Intercomparison Project Phase 6 (CMIP6), and for near-term (2030) and mid-term (2050) future projections, under the Shared Socioeconomic Pathways (SSPs). The results for the present day show that land transport emissions have a large impact on near-surface concentrations of black carbon and aerosol nitrate over the most populated areas of the globe, but with contrasting patterns in terms of relative contributions between developed and developing countries. In spite of the recently introduced regulations to limit the fuel sulfur content in the shipping sector, shipping emissions are still responsible for a considerable impact on aerosol sulfate near-surface concentrations, about 0.5 to 1 µg m−3 in the most travelled regions, with significant effects on continental air pollution and in the northern polar regions as well. Aviation impacts on aerosol mass are found to be quite small, of the order of a few nanograms per cubic metre, while this sector considerably affects particle number concentrations, contributing up to 20 %–30 % of the upper-tropospheric particle number concentration at the northern mid-latitudes. The transport-induced impacts on aerosol mass and number concentrations result in a present-day radiative forcing of −164, −145, and −64 mW m−2 for land transport, shipping, and aviation, respectively, with a dominating contribution by aerosol–cloud interactions. These forcings represent a marked offset to the CO2 warming from the transport sectors and are therefore very relevant for climate policy. The projections under the SSPs show that the impact of the transport sectors on aerosol and climate are generally consistent with the narratives underlying these scenarios: the lowest impacts of transport on both aerosol and climate are simulated under SSP1, especially for the land transport sector, while SSP3 is generally characterized by the largest effects. Notable exceptions to this picture, however, exist, as the emissions of other anthropogenic sectors also contribute to the overall aerosol concentrations and thus modulate the relevance of the transport sectors in the different scenarios, not always consistently with their underlying storyline. On a qualitative level, the results for the present day mostly confirm the findings of our previous assessment for the year 2000, which used a predecessor version of the same model and the CMIP5 emission data. Some important quantitative differences are found, which can mostly be ascribed to the improved representation of aerosol background concentrations in the present study.

Assimilation of POLDER observations to estimate aerosol emissions

Abstract. We apply a local ensemble transform Kalman smoother (LETKS) in combination with the global aerosol–climate model ECHAM–HAM to estimate aerosol emissions from POLDER-3/PARASOL (POLarization and Directionality of the Earth's Reflectances) observations for the year 2006. We assimilate aerosol optical depth at 550 mnm (AOD550), the Ångström exponent at 550 and 865 nm (AE550–865), and single-scattering albedo at 550 nm (SSA550) in order to improve modeled aerosol mass, size and absorption simultaneously. The new global aerosol emissions increase to 1419 Tg yr−1 (+28 %) for dust, 1850 Tg yr−1 (+75 %) for sea salt, 215 Tg yr−1 (+143 %) for organic aerosol and 13.3 Tg yr−1 (+75 %) for black carbon, while the sulfur dioxide emissions increase to 198 Tg yr−1 (+42 %) and the total deposition of sulfates to 293 Tg yr−1 (+39 %). Organic and black carbon emissions are much higher than their prior values from bottom-up inventories, with a stronger increase in biomass burning sources (+193 % and +90 %) than in anthropogenic sources (115 % and 70 %). The evaluation of the experiments with POLDER (assimilated) and AERONET as well as MODIS Dark Target (independent) observations shows a clear improvement compared with the ECHAM–HAM control run. Specifically based on AERONET, the global mean error in AOD550 improves from −0.094 to −0.006, while absorption aerosol optical depth at 550 nm (AAOD550) improves from −0.009 to −0.004 after the assimilation. A smaller improvement is also observed in the AE550–865 mean absolute error (from 0.428 to 0.393), with a considerably higher improvement over isolated island sites at the ocean. The new dust emissions are closer to the ensemble median of AEROCOM I, AEROCOM III and CMIP5 as well as some of the previous assimilation studies. The new sea salt emissions have become closer to the reported emissions from previous studies. Indications of a missing fraction of coarse dust and sea salt particles are discussed. The biomass burning changes (based on POLDER) can be used as alternative biomass burning scaling factors for the Global Fire Assimilation System (GFAS) inventory distinctively estimated for organic carbon (2.93) and black carbon (1.90) instead of the recommended scaling of 3.4 (Kaiser et al., 2012). The estimated emissions are highly sensitive to the relative humidity due to aerosol water uptake, especially in the case of sulfates. We found that ECHAM–HAM, like most of the global climate models (GCMs) that participated in AEROCOM and CMIP6, overestimated the relative humidity compared with ERA5 and as a result the water uptake by aerosols, assuming the kappa values are not underestimated. If we use the ERA5 relative humidity, sulfate emissions must be further increased, as modeled sulfate AOD is lowered. Specifically, over East Asia, the lower AOD can be attributed to the underestimated precipitation and the lack of simulated nitrates in the model.

How the extreme 2019–2020 Australian wildfires affected global circulation and adjustments

Abstract. Wildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019–2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17 km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol–climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5 W m−2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5 W m−2, for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2 %. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing.

A global climatology of ice-nucleating particles under cirrus conditions derived from model simulations with MADE3 in EMAC

Abstract. Atmospheric aerosols can act as ice-nucleating particles (INPs), thereby influencing the formation and the microphysical properties of cirrus clouds, resulting in distinct climate effects. In addition to mineral dust and soot particles, laboratory experiments suggest crystalline ammonium sulfate and glassy organic particles as effective INPs in the cirrus regime. However, the impact of these new particle types at the global scale is still highly uncertain. Here, we present and analyse a global climatology of INPs derived from model simulations performed with a global aerosol–climate model coupled to a two-moment cloud microphysical scheme and a parametrization for aerosol-induced ice formation in cirrus clouds. This global INP climatology comprises mineral dust and soot particles as well as crystalline ammonium sulfate and glassy organics, including a simplified formulation of the particle phase state for the latter. By coupling the different INP types to the microphysical cirrus cloud scheme, their ice nucleation potential under cirrus conditions is analysed, considering possible competition mechanisms between different INPs. The simulated INP concentrations in the range of about 1 to 100 L−1 agree well with in situ observations and other global model studies. We show that INP concentrations of glassy organics and crystalline ammonium sulfate are strongly related to the ambient conditions which often inhibit the glassy or crystalline phase respectively. Our model results suggest that glassy organic particles probably only have a minor influence, as INP concentrations are mostly low in the cirrus regime. On the other hand, crystalline ammonium sulfate often shows large INP concentrations, has the potential to influence ice nucleation in cirrus clouds, and should be taken into account in future model applications.

Insect Herbivory Caused Plant Stress Emissions Increases the Negative Radiative Forcing of Aerosols.

Plant stress in a changing climate is predicted to increase plant volatile organic compound (VOC) emissions and thus can affect the formed secondary organic aerosol (SOA) concentrations, which in turn affect the radiative properties of clouds and aerosol. However, global aerosol‐climate models do not usually consider plant stress induced VOCs in their emission schemes. In this study, we modified the monoterpene emission factors in biogenic emission model to simulate biotic stress caused by insect herbivory on needleleaf evergreen boreal and broadleaf deciduous boreal trees and studied the consequent effects on SOA formation, aerosol‐cloud interactions as well as direct radiative effects of formed SOA. Simulations were done altering the fraction of stressed and healthy trees in the latest version of ECHAM‐HAMMOZ (ECHAM6.3‐HAM2.3‐MOZ1.0) global aerosol‐climate model. Our simulations showed that increasing the extent of stress to the aforementioned tree types, substantially increased the SOA burden especially over the areas where these trees are located. This indicates that increased VOC emissions due to increasing stress enhance the SOA formation via oxidation of VOCs to low VOCs. In addition, cloud droplet number concentration at the cloud top increased with increasing extent of biotic stress. This indicates that as SOA formation increases, it further enhances the number of particles acting as cloud condensation nuclei. The increase in SOA formation also decreased both all‐sky and clear‐sky radiative forcing. This was due to a shift in particle size distributions that enhanced aerosol reflecting and scattering of incoming solar radiation.

Assessing the potential for simplification in global climate model cloud microphysics

Abstract. Cloud properties and their evolution influence Earth's radiative balance. The cloud microphysical (CMP) processes that shape these properties are therefore important to represent in global climate models. Historically, parameterizations in these models have grown more detailed and complex. However, a simpler formulation of CMP processes may leave the model results mostly unchanged while enabling an easier interpretation of model results and helping to increase process understanding. This study employs sensitivity analysis of an emulated perturbed parameter ensemble of the global aerosol–climate model ECHAM-HAM to illuminate the impact of selected CMP cloud ice processes on model output. The response to the perturbation of a process serves as a proxy for the effect of a simplification. Autoconversion of ice crystals is found to be the dominant CMP process in influencing key variables such as the ice water path and cloud radiative effects, while riming of cloud droplets on snow has the most influence on the liquid phase. Accretion of ice and snow and self-collection of ice crystals have a negligible influence on model output and are therefore identified as suitable candidates for future simplifications. In turn, the dominating role of autoconversion suggests that this process has the greatest need to be represented correctly. A seasonal and spatially resolved analysis employing a spherical harmonics expansion of the data corroborates the results. This study introduces a new application for the combination of statistical emulation and sensitivity analysis to evaluate the sensitivity of a complex numerical model to a specific parameterized process. It paves the way for simplifications of CMP processes leading to more interpretable climate model results.

Exploring the uncertainties in the aviation soot–cirrus effect

Abstract. A global aerosol–climate model, including a two-moment cloud microphysical scheme and a parametrization for aerosol-induced ice formation in cirrus clouds, is applied in order to quantify the impact of aviation soot on natural cirrus clouds. Several sensitivity experiments are performed to assess the uncertainties in this effect related to (i) the assumptions on the ice nucleation abilities of aviation soot, (ii) the representation of vertical updrafts in the model, and (iii) the use of reanalysis data to relax the model dynamics (the so-called nudging technique). Based on the results of the model simulations, a radiative forcing from the aviation soot–cirrus effect in the range of −35 to 13 mW m−2 is quantified, depending on the assumed critical saturation ratio for ice nucleation and active fraction of aviation soot but with a confidence level below 95 % in several cases. Simple idealized experiments with prescribed vertical velocities further show that the uncertainties on this aspect of the model dynamics are critical for the investigated effect and could potentially add a factor of about 2 of further uncertainty to the model estimates of the resulting radiative forcing. The use of the nudging technique to relax model dynamics is proved essential in order to identify a statistically significant signal from the model internal variability, while simulations performed in free-running mode and with prescribed sea-surface temperatures and sea-ice concentrations are shown to be unable to provide robust estimates of the investigated effect. A comparison with analogous model studies on the aviation soot–cirrus effect show a very large model diversity, with a conspicuous lack of consensus across the various estimates, which points to the need for more in-depth analyses on the roots of such discrepancies.

Vertical grid refinement for stratocumulus clouds in the radiation scheme of the global climate model ECHAM6.3-HAM2.3-P3

Abstract. In this study, we implement a vertical grid refinement scheme in the radiation routine of the global aerosol–climate model ECHAM-HAM, aiming to improve the representation of stratocumulus clouds and address the underestimation of their cloud cover. The scheme is based on a reconstruction of the temperature inversion as a physical constraint for the cloud top. On the refined grid, the boundary layer and the free troposphere are separated and the cloud's layer is made thinner. The cloud cover is recalculated either by conserving the cloud volume (SC-VOLUME) or by using the Sundqvist cloud cover routine on the new grid representation (SC-SUND). In global climate simulations, we find that the SC-VOLUME approach is inadequate, as there is a mismatch, in most cases, between the layer of the inversion and the layer of the stratocumulus cloud, which prevents its application and is itself likely caused by an overly low vertical resolution. Additionally, we find that the occurrence frequency of stratocumulus clouds is underestimated in ECHAM-HAM, limiting a priori the potential benefits of a scheme like SC-VOLUME targeting only cloud amount when present. With the SC-SUND approach, the possibility for new clouds to be formed on the refined grid results in a large increase in mean total cloud cover in stratocumulus regions. In both cases, however, the changes exerted in the radiation routine are too weak to produce a significant improvement in the simulated stratocumulus cloud cover. We investigate and discuss the reasons behind this. The grid refinement scheme could be used more effectively for this purpose if implemented directly in the model's cloud microphysics and cloud cover routines, but other possible ways forward are also discussed.

Incorrect Asian aerosols affecting the attribution and projection of regional climate change in CMIP6 models

Anthropogenic aerosol (AA) forcing has been shown as a critical driver of climate change over Asia since the mid-20th century. Here we show that almost all Coupled Model Intercomparison Project Phase 6 (CMIP6) models fail to capture the observed dipole pattern of aerosol optical depth (AOD) trends over Asia during 2006–2014, last decade of CMIP6 historical simulation, due to an opposite trend over eastern China compared with observations. The incorrect AOD trend over China is attributed to problematic AA emissions adopted by CMIP6. There are obvious differences in simulated regional aerosol radiative forcing and temperature responses over Asia when using two different emissions inventories (one adopted by CMIP6; the other from Peking university, a more trustworthy inventory) to driving a global aerosol-climate model separately. We further show that some widely adopted CMIP6 pathways (after 2015) also significantly underestimate the more recent decline in AA emissions over China. These flaws may bring about errors to the CMIP6-based regional climate attribution over Asia for the last two decades and projection for the next few decades, previously anticipated to inform a wide range of impact analysis.

Tracing devastating fires in Portugal to a snow archive in the Swiss Alps: a case study

Abstract. Recent large wildfires, such as those in Portugal in 2017, have devastating impacts on societies, economy, ecosystems and environments. However, wildfires are a natural phenomenon, which has been exacerbated by land use during the past millennia. Ice cores are one of the archives preserving information on fire occurrences over these timescales. A difficulty is that emission sensitivity of ice cores is often unknown, which constitutes a source of uncertainty in the interpretation of such archives. Information from specific and well-documented case studies is therefore useful to better understand the spatial representation of ice-core burning records. The wildfires near Pedrógão Grande in central Portugal in 2017 provided a test bed to link a fire event to its footprint left in a high-alpine snowpack considered a surrogate for high-alpine ice-core sites. Here, we (1) analysed black carbon (BC) and microscopic charcoal particles deposited in the snowpack close to the high-alpine research station Jungfraujoch in the Swiss Alps; (2) calculated backward trajectories based on ERA-Interim reanalysis data and simulated the transport of these carbonaceous particles using a global aerosol-climate model; and (3) analysed the fire spread, its spatial and temporal extent, and its intensity with remote-sensing (e.g. MODIS) Active Fire and Burned Area products. According to modelled emissions of the FINN v1.6 database, the fire emitted a total amount of 203.5 t BC from a total burned area of 501 km2 as observed on the basis of satellite fire products. Backward trajectories unambiguously linked a peak of atmospheric-equivalent BC observed at the Jungfraujoch research station on 22 June – with elevated levels until 25 June – with the highly intensive fires in Portugal. The atmospheric signal is in correspondence with an outstanding peak in microscopic charcoal observed in the snow layer, depositing nearly as many charcoal particles as during an average year in other ice archives. In contrast to charcoal, the amount of atmospheric BC deposited during the fire episode was minor due to a lack of precipitation. Simulations with a global aerosol-climate model suggest that the observed microscopic charcoal particles originated from the fires in Portugal and that their contribution to the BC signal in snow was negligible. Our study revealed that microscopic charcoal can be transported over long distances (1500 km) and that snow and ice archives are much more sensitive to distant events than sedimentary archives, for which the signal is dominated by local fires. The findings are important for future ice-core studies as they document that, for BC as a fire tracer, the signal preservation depends on precipitation. Single events, like this example, might not be preserved due to unfavourable meteorological conditions.

Robust observational constraint of uncertain aerosol processes and emissions in a climate model and the effect on aerosol radiative forcing

Abstract. The effect of observational constraint on the ranges of uncertain physical and chemical process parameters was explored in a global aerosol–climate model. The study uses 1 million variants of the Hadley Centre General Environment Model version 3 (HadGEM3) that sample 26 sources of uncertainty, together with over 9000 monthly aggregated grid-box measurements of aerosol optical depth, PM2.5, particle number concentrations, sulfate and organic mass concentrations. Despite many compensating effects in the model, the procedure constrains the probability distributions of parameters related to secondary organic aerosol, anthropogenic SO2 emissions, residential emissions, sea spray emissions, dry deposition rates of SO2 and aerosols, new particle formation, cloud droplet pH and the diameter of primary combustion particles. Observational constraint rules out nearly 98 % of the model variants. On constraint, the ±1σ (standard deviation) range of global annual mean direct radiative forcing (RFari) is reduced by 33 % to −0.14 to −0.26 W m−2, and the 95 % credible interval (CI) is reduced by 34 % to −0.1 to −0.32 W m−2. For the global annual mean aerosol–cloud radiative forcing, RFaci, the ±1σ range is reduced by 7 % to −1.66 to −2.48 W m−2, and the 95 % CI by 6 % to −1.28 to −2.88 W m−2. The tightness of the constraint is limited by parameter cancellation effects (model equifinality) as well as the large and poorly defined “representativeness error” associated with comparing point measurements with a global model. The constraint could also be narrowed if model structural errors that prevent simultaneous agreement with different measurement types in multiple locations and seasons could be improved. For example, constraints using either sulfate or PM2.5 measurements individually result in RFari±1σ ranges that only just overlap, which shows that emergent constraints based on one measurement type may be overconfident.

Source attribution of Arctic black carbon and sulfate aerosols and associated Arctic surface warming during 1980–2018

Abstract. Observations show that the concentrations of Arctic sulfate and black carbon (BC) aerosols have declined since the early 1980s. Previous studies have reported that reducing sulfate aerosols potentially contributed to the recent rapid Arctic warming. In this study, a global aerosol–climate model (Community Atmosphere Model, version 5) equipped with Explicit Aerosol Source Tagging (CAM5-EAST) is applied to quantify the source apportionment of aerosols in the Arctic from 16 source regions and the role of aerosol variations in affecting changes in the Arctic surface temperature from 1980 to 2018. The CAM5-EAST simulated surface concentrations of sulfate and BC in the Arctic had a decrease of 43 % and 23 %, respectively, in 2014–2018 relative to 1980–1984 mainly due to the reduction of emissions from Europe, Russia and local Arctic sources. Increases in emissions from South and East Asia led to positive trends in Arctic sulfate and BC in the upper troposphere. All aerosol radiative impacts are considered including aerosol–radiation and aerosol–cloud interactions, as well as black carbon deposition on snow- and ice-covered surfaces. Within the Arctic, sulfate reductions caused a top-of-atmosphere (TOA) warming of 0.11 and 0.25 W m−2 through aerosol–radiation and aerosol–cloud interactions, respectively. While the changes in Arctic atmospheric BC has little impact on local radiative forcing, the decrease in BC in snow and ice led to a net cooling of 0.05 W m−2. By applying climate sensitivity factors for different latitudinal bands, global changes in sulfate and BC during 2014–2018 (with respect to 1980–1984) exerted a +0.088 and 0.057 K Arctic surface warming, respectively, through aerosol–radiation interactions. Through aerosol–cloud interactions, the sulfate reduction caused an Arctic warming of +0.193 K between the two time periods. The weakened BC effect on snow–ice albedo led to an Arctic surface cooling of −0.041 K. The changes in atmospheric sulfate and BC outside the Arctic produced a total Arctic warming of +0.25 K, the majority of which is due to the midlatitude changes in radiative forcing. Our results suggest that changes in aerosols over the midlatitudes of the Northern Hemisphere have a larger impact on Arctic temperature than other regions through enhanced poleward heat transport. The combined total effects of sulfate and BC produced an Arctic surface warming of +0.297 K, explaining approximately 20 % of the observed Arctic warming since the early 1980s.

Global response of parameterised convective cloud fields to anthropogenic aerosol forcing

Abstract. The interactions between aerosols and convective clouds represent some of the greatest uncertainties in the climate impact of aerosols in the atmosphere. A wide variety of mechanisms have been proposed by which aerosols may invigorate, suppress or change the properties of individual convective clouds, some of which can be reproduced in high-resolution limited-area models. However, there may also be mesoscale, regional or global adjustments which modulate or dampen such impacts which cannot be captured in the limited domain of such models. The Convective Cloud Field Model (CCFM) provides a mechanism to simulate a population of convective clouds, complete with microphysics and interactions between clouds, within each grid column at resolutions used for global climate modelling, so that a representation of the microphysical aerosol response within each parameterised cloud type is possible. Using CCFM within the global aerosol–climate model ECHAM–HAM, we demonstrate how the parameterised cloud field responds to the present-day anthropogenic aerosol perturbation in different regions. In particular, we show that in regions with strongly forced deep convection and/or significant aerosol effects via large-scale processes, the changes in the convective cloud field due to microphysical effects are rather small; however in a more weakly forced regime such as the Caribbean, where large-scale aerosol effects are small, a signature of convective invigoration does become apparent.

Impact of isolated atmospheric aging processes on the cloud condensation nuclei activation of soot particles

Abstract. The largest contributors to the uncertainty in assessing the anthropogenic contribution in radiative forcing are the direct and indirect effects of aerosol particles on the Earth's radiative budget. Soot particles are of special interest since their properties can change significantly due to aging processes once they are emitted into the atmosphere. Probably the largest obstacle for the investigation of these processes in the laboratory is the long atmospheric lifetime of 1 week, requiring tailored experiments that cover this time span. This work presents results on the ability of two types of soot, obtained using a miniCAST soot generator, to act as cloud condensation nuclei (CCN) after exposure to atmospherically relevant levels of ozone (O3) and humidity. Aging times of up to 12 h were achieved by successful application of the continuous-flow stirred tank reactor (CSTR) concept while allowing for size selection of particles prior to the aging step. Particles of 100 nm diameter and rich in organic carbon (OC) that were initially CCN inactive showed significant CCN activity at supersaturations (SS) down to 0.3 % after 10 h of exposure to 200 ppb of O3. While this process was not affected by different levels of relative humidity in the range of 5 %–75 %, a high sensitivity towards the ambient/reaction temperature was observed. Soot particles with a lower OC content required an approximately 4-fold longer aging duration to show CCN activity at the same SS. Prior to the slow change in the CCN activity, a rapid increase in the particle diameter was detected which occurred within several minutes. This study highlights the applicability of the CSTR approach for the simulation of atmospheric aging processes, as aging durations beyond 12 h can be achieved in comparably small aerosol chamber volumes (<3 m3). Implementation of our measurement results in a global aerosol-climate model, ECHAM6.3-HAM2.3, showed a statistically significant increase in the regional and global CCN burden and cloud droplet number concentration.

The importance of the representation of air pollution emissions for the modeled distribution and radiative effects of black carbon in the Arctic

Abstract. Aerosol particles can contribute to the Arctic amplification (AA) by direct and indirect radiative effects. Specifically, black carbon (BC) in the atmosphere, and when deposited on snow and sea ice, has a positive warming effect on the top-of-atmosphere (TOA) radiation balance during the polar day. Current climate models, however, are still struggling to reproduce Arctic aerosol conditions. We present an evaluation study with the global aerosol-climate model ECHAM6.3-HAM2.3 to examine emission-related uncertainties in the BC distribution and the direct radiative effect of BC. The model results are comprehensively compared against the latest ground and airborne aerosol observations for the period 2005–2017, with a focus on BC. Four different setups of air pollution emissions are tested. The simulations in general match well with the observed amount and temporal variability in near-surface BC in the Arctic. Using actual daily instead of fixed biomass burning emissions is crucial for reproducing individual pollution events but has only a small influence on the seasonal cycle of BC. Compared with commonly used fixed anthropogenic emissions for the year 2000, an up-to-date inventory with transient air pollution emissions results in up to a 30 % higher annual BC burden locally. This causes a higher annual mean all-sky net direct radiative effect of BC of over 0.1 W m−2 at the top of the atmosphere over the Arctic region (60–90∘ N), being locally more than 0.2 W m−2 over the eastern Arctic Ocean. We estimate BC in the Arctic as leading to an annual net gain of 0.5 W m−2 averaged over the Arctic region but to a local gain of up to 0.8 W m−2 by the direct radiative effect of atmospheric BC plus the effect by the BC-in-snow albedo reduction. Long-range transport is identified as one of the main sources of uncertainties for ECHAM6.3-HAM2.3, leading to an overestimation of BC in atmospheric layers above 500 hPa, especially in summer. This is related to a misrepresentation in wet removal in one identified case at least, which was observed during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) summer aircraft campaign. Overall, the current model version has significantly improved since previous intercomparison studies and now performs better than the multi-model average in the Aerosol Comparisons between Observation and Models (AEROCOM) initiative in terms of the spatial and temporal distribution of Arctic BC.

The global aerosol–climate model ECHAM6.3–HAM2.3 – Part 2: Cloud evaluation, aerosol radiative forcing, and climate sensitivity

Abstract. The global aerosol–climate model ECHAM6.3–HAM2.3 (E63H23) as well as the previous model versions ECHAM5.5–HAM2.0 (E55H20) and ECHAM6.1–HAM2.2 (E61H22) are evaluated using global observational datasets for clouds and precipitation. In E63H23, the amount of low clouds, the liquid and ice water path, and cloud radiative effects are more realistic than in previous model versions. E63H23 has a more physically based aerosol activation scheme, improvements in the cloud cover scheme, changes in the detrainment of convective clouds, changes in the sticking efficiency for the accretion of ice crystals by snow, consistent ice crystal shapes throughout the model, and changes in mixed-phase freezing; an inconsistency in ice crystal number concentration (ICNC) in cirrus clouds was also removed. Common biases in ECHAM and in E63H23 (and in previous ECHAM–HAM versions) are a cloud amount in stratocumulus regions that is too low and deep convective clouds over the Atlantic and Pacific oceans that form too close to the continents (while tropical land precipitation is underestimated). There are indications that ICNCs are overestimated in E63H23. Since clouds are important for effective radiative forcing due to aerosol–radiation and aerosol–cloud interactions (ERFari+aci) and equilibrium climate sensitivity (ECS), differences in ERFari+aci and ECS between the model versions were also analyzed. ERFari+aci is weaker in E63H23 (−1.0 W m−2) than in E61H22 (−1.2 W m−2) (or E55H20; −1.1 W m−2). This is caused by the weaker shortwave ERFari+aci (a new aerosol activation scheme and sea salt emission parameterization in E63H23, more realistic simulation of cloud water) overcompensating for the weaker longwave ERFari+aci (removal of an inconsistency in ICNC in cirrus clouds in E61H22). The decrease in ECS in E63H23 (2.5 K) compared to E61H22 (2.8 K) is due to changes in the entrainment rate for shallow convection (affecting the cloud amount feedback) and a stronger cloud phase feedback. Experiments with minimum cloud droplet number concentrations (CDNCmin) of 40 cm−3 or 10 cm−3 show that a higher value of CDNCmin reduces ERFari+aci as well as ECS in E63H23.

The global aerosol–climate model ECHAM6.3–HAM2.3 – Part 1: Aerosol evaluation

Abstract. We introduce and evaluate aerosol simulations with the global aerosol–climate model ECHAM6.3–HAM2.3, which is the aerosol component of the fully coupled aerosol–chemistry–climate model ECHAM–HAMMOZ. Both the host atmospheric climate model ECHAM6.3 and the aerosol model HAM2.3 were updated from previous versions. The updated version of the HAM aerosol model contains improved parameterizations of aerosol processes such as cloud activation, as well as updated emission fields for anthropogenic aerosol species and modifications in the online computation of sea salt and mineral dust aerosol emissions. Aerosol results from nudged and free-running simulations for the 10-year period 2003 to 2012 are compared to various measurements of aerosol properties. While there are regional deviations between the model and observations, the model performs well overall in terms of aerosol optical thickness, but may underestimate coarse-mode aerosol concentrations to some extent so that the modeled particles are smaller than indicated by the observations. Sulfate aerosol measurements in the US and Europe are reproduced well by the model, while carbonaceous aerosol species are biased low. Both mineral dust and sea salt aerosol concentrations are improved compared to previous versions of ECHAM–HAM. The evaluation of the simulated aerosol distributions serves as a basis for the suitability of the model for simulating aerosol–climate interactions in a changing climate.

Modelling mineral dust in the Central Asian region

In Central Asia, climate and air quality are largely affected by local and long-travelled mineral dust. For the last century, the area has experienced severe land-use changes and water exploitation producing new dust sources. Today global warming causes rapid shrinking of mountain glaciers with yet unknow consequences for dust and its climate effects. Despite the importance for a growing population, only little is known about sources, transport pathways and properties of Central Asian dust. A transport study with a global aerosol-climate model is undertaken to investigate the life cycle of mineral dust in Central Asia for the period of a remote-sensing campaign in Tajikistan in 2015–2016. An initial evaluation with sun photometer measurements shows reasonable agreement for the average amount of dust, but a significant weakness of the model in reproducing the seasonality of local dust with maximum activity in summer. Source apportionment reveals a major contribution from Arabia throughout the year in accordance with observations. In the model, local sources mainly contribute in spring and autumn while summer-time dust production is underestimated. The results underline the importance of considering long-range transport and, locally, a detailed representation of atmospheric dynamics and surface characteristics for modelling dust in Central Asia.