Anthropogenic Aerosol Radiative Forcing Research Articles

Assessing the sensitivity of aerosol mass budget and effective radiative forcing to horizontal grid spacing in E3SMv1 using a regional refinement approach

Abstract. Atmospheric aerosols have important impacts on air quality and the Earth–atmospheric energy balance. However, as computing power is limited, Earth system models generally use coarse spatial grids and parameterize finer-scale atmospheric processes. These parameterizations and the simulation of atmospheric aerosols are often sensitive to model horizontal resolutions. Understanding the sensitivities is necessary for the development of Earth system models at higher resolutions with the deployment of more powerful supercomputers. Using the Energy Exascale Earth System Model (E3SM) version 1, this study investigates the impact of horizontal grid spacing on the simulated aerosol mass budget, aerosol–cloud interactions, and the effective radiative forcing of anthropogenic aerosols (ERFaer) over the contiguous United States. We examine the resolution sensitivity by comparing the nudged simulation results for 2016 from the low-resolution model (LR) and the regional refinement model (RRM). As expected, the simulated emissions of natural dust, sea salt, and marine organic matter are substantially higher in the RRM than in the LR. In addition, RRM simulates stronger aqueous-phase production of sulfate through the enhanced oxidation of sulfur dioxide by hydrogen peroxide due to increased cloud liquid water content. In contrast, the gas-phase chemical production of sulfate is slightly suppressed. The RRM resolves more large-scale precipitation and produces less convective precipitation than the LR, leading to increased (decreased) aerosol wet scavenging by large-scale (convective) precipitation. Regarding aerosol effects on clouds, RRM produces larger temporal variabilities in the large-scale liquid cloud fractions than LR, resulting in increased microphysical cloud processing of aerosols (more interstitial aerosols are converted to cloud-borne aerosols via aerosol activation) in RRM. Water vapor condensation is also enhanced in RRM compared to LR. Consequently, the RRM simulation produces more cloud droplets, a larger cloud droplet radius, a higher liquid water path, and a larger cloud optical depth than the LR simulation. A comparison of the present-day and pre-industrial simulations indicates that, for this contiguous United States domain, the higher-resolution increases ERFaer at the top of the model by about 12 %, which is mainly attributed to the strengthened indirect effect associated with aerosol–cloud interactions.

Implications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019

Abstract. This study focuses on implications of differences between recent global emissions inventories for simulated trends in anthropogenic aerosol abundances and radiative forcing (RF) over the 1990–2019 period. We use the ECLIPSE version 6 (ECLv6) and CEDS year 2021 release (CEDS21) as input to the chemical transport model OsloCTM3 and compare the resulting aerosol evolution to corresponding results derived with the first CEDS release, as well as to observed trends in regional and global aerosol optical depth (AOD). Using CEDS21 and ECLv6 results in a 3 % and 6 % lower global mean AOD compared to CEDS in 2014, primarily driven by differences over China and India, where the area average AOD is up to 30 % lower. These differences are considerably larger than the satellite-derived interannual variability in AOD. A negative linear trend over 2005–2017 in global AOD following changes in anthropogenic emissions is found with all three inventories but is markedly stronger with CEDS21 and ECLv6. Furthermore, we confirm that the model better captures the sign and strength of the observed AOD trend over China with CEDS21 and ECLv6 compared to using CEDS, while the opposite is the case for South Asia. We estimate a net global mean aerosol-induced RF in 2014 relative to 1990 of 0.08 W m−2 for CEDS21 and 0.12 W m−2 for ECLv6, compared to 0.03 W m−2 with CEDS. Using CEDS21, we also estimate the RF in 2019 relative to 1990 to be 0.10 W m−2, reflecting the continuing decreasing trend in aerosol loads post-2014. Our results facilitate more rigorous comparison between existing and upcoming studies of climate and health effects of aerosols using different emission inventories.

Uncertainty in Simulating Twentieth Century West African Precipitation Trends: The Role of Anthropogenic Aerosol Emissions

AbstractAnthropogenic aerosol emissions from North America and Europe have strong effects on the decadal variability of the West African monsoon (WAM). Anthropogenic aerosol effective radiative forcing is model dependent, but the impact of such uncertainty on the simulation of long‐term WAM variability is unknown. We use an ensemble of simulations with HadGEM3‐GC3.1 that span the most recent estimates in simulated anthropogenic aerosol effective radiative forcing. We show that uncertainty in anthropogenic aerosol radiative forcing leads to significant uncertainty at simulating multi‐decadal trends in West African precipitation. At the large scale, larger forcing leads to a larger decrease in the interhemispheric temperature gradients, in temperature over both the North Atlantic Ocean and northern Sahara. There are also differences in dynamic changes specific to the WAM (locations of the Saharan heat low and African Easterly Jet, of the strength of the West African westerly jet, and of African Easterly Wave activity). We also assess effects on monsoon precipitation characteristics and temperature. We show that larger aerosol forcing results in a decrease of the number of rainy days and of heavy and extreme precipitation events and warm spells. However, simulated changes in onset and demise dates do not appear to be sensitive to the magnitude of aerosol forcing. Our results demonstrate the importance of reducing the uncertainty in anthropogenic aerosol forcing for understanding and predicting multi‐decadal variability in the WAM.

Seasonal variability in size-resolved hygroscopicity of sub-micron aerosols over the Western Ghats, India: Closure and parameterization

Hygroscopicity of atmospheric aerosol primarily depends on the size and chemical composition of the particle and is important for estimating anthropogenic aerosol radiative forcing. There is limited information exists over the Indian region on size segregated aerosol hygroscopicity (κ) in different seasons. This study presents ‘κ’ as derived from a Humidified Tandem Differential Mobility Analyzer (HTDMA) over a High Altitude Cloud Physics Laboratory (HACPL) in the Western Ghats, India for more than a year (from May 2019 to May 2020). The average hygroscopicity values of aerosol particles of diameters 32, 50, 75, 110, 150, 210 and 260 nm at 90 % RH condition are 0.19, 0.18, 0.16, 0.17, 0.18, 0.20, 0.21 respectively during the entire observation period. κ was observed to decrease with an increase in size in the Aitken mode regime (32–75 nm) and an increase in the accumulation mode (110–260 nm). Seasonal variation of hygroscopicity for a wide range of particle diameters is reported which is highly demanding as there is a change in the air mass flow pattern in each of the seasons. The diurnal cycle of hygroscopicity showed a prominent peak during the midnight to early morning hours followed by a decrease in the forenoon hours and a secondary peak in the afternoon hours. κ is found to be higher in pre-monsoon compared to winter season as Chl is approximately 3 % higher in pre-monsoon and NH4Cl is highly hygroscopic among the assumed chemical composition. Hygroscopicity derived through chemical speciation observations assuming internal and external mixing of aerosols i.e. κinter and κexter are overestimating as compared to κHTDMA. However, the bias between kexter and kHTDMA is relatively lower as external mixing type of aerosol is evident through the growth factor data sets measured by HTDMA. Utilizing the hygroscopicity measurements available for discrete diameters by HTDMA, a parameterization of hygroscopicity with the dry diameter of sub-micron particles is developed.

Natural and anthropogenic contributions to the hurricane drought of the 1970s–1980s

Atlantic hurricane activity experienced a pronounced lull during the 1970s and 1980s. The current explanation that anthropogenic aerosol radiative forcing cooled the sea surface locally fails to capture the magnitude of this large decrease in activity. To explain this hurricane drought, we propose that the radiative effects of sulfate aerosols from Europe and North-America decreased precipitation in the Sahara-Sahel region, leading to an enhancement of dust regional emissions and transport over the Atlantic. This dust in turn enhanced the local decrease of sea-surface temperature and of hurricane activity. Here, we show that dust emissions from the Sahara peaked in phase with regional sulfate aerosol optical thickness and Sahel drought conditions, and that dust optical depth variations alone can explain nearly half of the sea-surface temperature depression in the 1970s and 1980s.

Evaluating uncertainty in aerosol forcing of tropical precipitation shifts

Abstract. An observed southward shift in tropical rainfall over land between 1950 and 1985, followed by a weaker recovery post-1985, has been attributed to anthropogenic aerosol radiative forcing and cooling of the Northern Hemisphere relative to the Southern Hemisphere. We might therefore expect models that have a strong historic hemispheric contrast in aerosol forcing to simulate a further northward tropical rainfall shift in the near-term future when anthropogenic aerosol emission reductions will predominantly warm the Northern Hemisphere. We investigate this paradigm using a perturbed parameter ensemble (PPE) of transient coupled ocean–atmosphere climate simulations that span a range of aerosol radiative forcing comparable to multi-model studies. In the 20th century, in our single-model ensemble, we find no relationship between the magnitude of pre-industrial to 1975 inter-hemispheric anthropogenic aerosol radiative forcing and tropical precipitation shifts. Instead, tropical precipitation shifts are associated with major volcanic eruptions and are strongly affected by internal variability. However, we do find a relationship between the magnitude of pre-industrial to 2005 inter-hemispheric anthropogenic aerosol radiative forcing and future tropical precipitation shifts over 2006 to 2060 under scenario RCP8.5. Our results suggest that projections of tropical precipitation shifts will be improved by reducing aerosol radiative forcing uncertainty, but predictive gains may be offset by temporary shifts in tropical precipitation caused by future major volcanic eruptions.

Use of Machine Learning to Reduce Uncertainties in Particle Number Concentration and Aerosol Indirect Radiative Forcing Predicted by Climate Models

AbstractThe radiative forcing of anthropogenic aerosols associated with aerosol‐cloud interactions (RFaci) remains the largest source of uncertainty in climate prediction. The calculation of particle number concentration (PNC), one of the critical parameters affecting RFaci, is generally simplified in climate models. Here we employ outputs from long‐term (30‐year) simulations of a global size‐resolved (sectional) aerosol microphysics model and a machine‐learning tool to develop a Random Forest Regression Model (RFRM) for PNC. We have implemented the PNC RFRM in GISS‐ModelE2.1 with a mass‐based One‐Moment Aerosol module, which is one of CMIP6 models. Compared to the default setting, the GISS‐ModelE2.1 simulation based on RFRM reduces the changes of cloud droplet number concentration associated with anthropogenic emissions, and decreases the RFaci from −1.46 to −1.11 W·m−2. This work highlights a promising approach based on machine learning to reduce uncertainties of climate models in predicting PNC and RFaci without compromising their computing efficiency.

Effective radiative forcing of anthropogenic aerosols in E3SM version 1: historical changes, causality, decomposition, and parameterization sensitivities

Abstract. The effective radiative forcing of anthropogenic aerosols (ERFaer) is an important measure of the anthropogenic aerosol effects simulated by a global climate model. Here we analyze ERFaer simulated by the E3SM version 1 (E3SMv1) atmospheric model using both century-long free-running atmosphere–land simulations and short nudged simulations. We relate the simulated ERFaer to characteristics of the aerosol composition and optical properties, and we evaluate the relationships between key aerosol and cloud properties. In terms of historical changes from the year 1870 to 2014, our results show that the global mean anthropogenic aerosol burden and optical depth increase during the simulation period as expected, but the regional averages show large differences in the temporal evolution. The largest regional differences are found in the emission-induced evolution of the burden and optical depth of the sulfate aerosol: a strong decreasing trend is seen in the Northern Hemisphere high-latitude region after around 1970, while a continued increase is simulated in the tropics. The relationships between key aerosol and cloud properties (relative changes between pre-industrial and present-day conditions) also show evident changes after 1970, diverging from the linear relationships exhibited for the period of 1870–1969. In addition to the regional differences in the simulated relationships, a reduced sensitivity in cloud droplet number and other cloud properties to aerosol perturbations is seen when the aerosol perturbation is large. Consequently, the global annual mean ERFaer magnitude does not increase after around 1970. The ERFaer in E3SMv1 is relatively large compared to the recently published multi-model estimates; the primary reason is the large indirect aerosol effect (i.e., through aerosol–cloud interactions). Compared to other models, E3SMv1 features large relative changes in the cloud droplet effective radius in response to aerosol perturbations. Large sensitivity is also seen in the liquid cloud optical depth, which is determined by changes in both the effective radius and liquid water path. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 are found to have a strong correlation, as the evolution of anthropogenic sulfate aerosols affects both the liquid cloud formation and the homogeneous ice nucleation in cirrus clouds (that causes a large effect on longwave ERFaer). As suggested by a previous study, the large ERFaer appears to be one of the reasons why the model cannot reproduce the observed global mean temperature evolution in the second half of the 20th century. Sensitivity simulations are performed to understand which parameterization and/or parameter changes have a large impact on the simulated ERFaer. The ERFaer estimates in E3SMv1 for the shortwave and longwave components are sensitive to the parameterization changes in both liquid and ice cloud processes. When the parameterization of ice cloud processes is modified, the top-of-model forcing changes in the shortwave and longwave components largely offset each other, so the net effect is negligible. This suggests that, to reduce the magnitude of the net ERFaer, it would be more effective to reduce the anthropogenic aerosol effect through liquid or mixed-phase clouds.

Anthropogenic Aerosols Effects on Ice Clouds: A Review

Since the ability of anthropogenic aerosols to act as ice nucleation particles has been recognized, the effect of anthropogenic aerosols on ice clouds has attracted increasing attentions. In recent years, some progress has been made in investigating the effects of anthropogenic aerosols on ice clouds. In this paper, we briefly review the study on the impact of anthropogenic aerosols on ice nuclei, properties and radiative forcing of ice clouds. Anthropogenic aerosols can form ice nuclei through homogeneous nucleation and heterogeneous nucleation. Convective strength can modulate the response of ice clouds to anthropogenic aerosols by affecting the nucleation activities. There have been large uncertainties in calculating the radiative forcing of anthropogenic aerosols on ice clouds in climate models. Further studies on the impact of anthropogenic aerosols on ice clouds are imperative to provide better parameterization schemes and reduce the uncertainties of aerosol indirect effects.

Beyond SOx reductions from shipping: assessing the impact of NOx and carbonaceous-particle controls on human health and climate

Historically, cargo ships have been powered by low-grade fossil fuels, which emit particles and particle-precursor vapors that impact human health and climate. We used a global chemical-transport model with online aerosol microphysics (GEOS-Chem-TOMAS) to estimate the aerosol health and climate impacts of four emission-control policies: (1) 85% reduction in sulfur oxide (SOx) emissions (Sulf); (2) 85% reduction in SOx and black carbon (BC) emissions (Sulf-BC); (3) 85% reduction in SOx, BC, and organic aerosol (OA) emissions (Sulf-BC-OA); and (4) 85% reduction in SOx, BC, OA, and nitrogen oxide (NOx) emissions (Sulf-BC-OA-NOx). The SOx reductions reflect the 0.5% fuel-sulfur cap implemented by the International Maritime Organization (IMO) on 1 January 2020. The other reductions represent realistic estimates of future emission-control policies. We estimate that these policies could reduce fine particulate matter (PM2.5)-attributable mortalities by 13 300 (Sulf) to 38 600 (Sulf-BC-OA-NOx) mortalities per year. These changes represent 0.3% and 0.8%, respectively, of annual PM2.5-attributable mortalities from anthropogenic sources. Comparing simulations, we estimate that adding the NOx cap has the greatest health benefit. In contrast to the health benefits, all scenarios lead to a simulated climate warming tendency. The combined aerosol direct radiative effect and cloud-albedo indirect effects (AIE) are between 27 mW m−2 (Sulf) and 41 mW m−2 (Sulf-BC-OA-NOx). These changes are about 2.1% (Sulf) to 3.2% (Sulf-BC-OA-NOx) of the total anthropogenic aerosol radiative forcing. The emission control policies examined here yield larger relative changes in the aerosol radiative forcing (2.1%–3.2%) than in health effects (0.3%–0.8%), because most shipping emissions are distant from populated regions. Valuation of the impacts suggests that these emissions reductions could produce much larger marginal health benefits ($129–$374 billion annually) than the marginal climate costs ($12–$17 billion annually).

Radiative forcing of anthropogenic aerosols on cirrus clouds using a hybrid ice nucleation scheme

Abstract. Anthropogenic aerosols impact cirrus clouds through ice nucleation, thereby changing the Earth's radiation budget. However, the magnitude and sign of anthropogenic forcing in cirrus clouds is still very uncertain depending on the treatments for ice-nucleating particles (INPs), the treatments for haze particle freezing, and the ice nucleation scheme. In this study, a new ice nucleation scheme (hereafter the HYBRID scheme) is developed to combine the best features of two previous ice nucleation schemes, so that global models are able to calculate the ice number concentration in both updrafts and downdrafts associated with gravity waves, and it has a robust sensitivity to the change of aerosol number. The scheme is applied in a box model, and the ice number concentrations (9.52±2.08 L−1) are somewhat overestimated but are in reasonable agreement with those from an adiabatic parcel model (9.40±2.31 L−1). Then, the forcing and cloud changes associated with changes in aircraft soot, sulfur emission, and all anthropogenic emissions between the preindustrial (PI) period and the present day (PD) are examined using the CESM/IMPACT global model with the HYBRID scheme. Aircraft soot emissions decrease the global average ice number concentration (Ni) by -1.0±2.4×107 m−2 (−1 %) (over the entire column) due to the inhibition of homogeneous nucleation and lead to a radiative forcing of -0.14±0.07 W m−2, while the increase in sulfur emissions increases the global average Ni by 7.3±2.9×107 m−2 (5 %) due to the increase in homogeneous nucleation and leads to a radiative forcing of -0.02±0.06 W m−2. The possible effects of aerosol and cloud feedbacks to the meteorological state in remote regions partly contribute to reduce the forcing and the change in Ni due to anthropogenic emissions. The radiative forcing due to all increased anthropogenic emissions from PI to PD is estimated to be -0.20±0.05 W m−2. If newly formed secondary organic aerosols (SOAs) act as INPs and inhibit homogeneous nucleation, the Ni formed from heterogeneous nucleation is increased. As a result, the inclusion of INPs from SOA increases the change in Ni to 12.0±2.3×107 m−2 (9 %) and increases (makes less negative) the anthropogenic forcing on cirrus clouds to -0.04±0.08 W m−2 from PI to PD.

Decadal Attribution of Historic Temperature and Ocean Heat Content Change to Anthropogenic Emissions

AbstractWe present an alternative method of calculating the historical effective radiative forcing using the observed temperature record and a kernel based on the 5th Climate Model Intercomparison Project (CMIP5) temperature response. This estimate is the effective radiative forcing time series that the average climate model would need to simulate the observed global mean surface temperature anomalies. We further infer the anthropogenic aerosols radiative forcing as a residual using the better‐known greenhouse gas radiative forcing. This allows an independent estimate of anthropogenic aerosol radiative forcing, which suggests a cooling influence due to aerosols in the early part of the twentieth century. The temporal kernels are also used to calculate decadal contributions from the dominant forcing agents to present‐day temperature, ocean heat content, and thermosteric sea level rise. The current global mean temperature anomaly is dominated by emissions in the past two decades, while current ocean heat content is more strongly affected by earlier decades.

Concentrations and radiative forcing of anthropogenic aerosols from 1750 to 2014 simulated with the Oslo CTM3 and CEDS emission inventory

Abstract. We document the ability of the new-generation Oslo chemistry-transport model, Oslo CTM3, to accurately simulate present-day aerosol distributions. The model is then used with the new Community Emission Data System (CEDS) historical emission inventory to provide updated time series of anthropogenic aerosol concentrations and consequent direct radiative forcing (RFari) from 1750 to 2014. Overall, Oslo CTM3 performs well compared with measurements of surface concentrations and remotely sensed aerosol optical depth. Concentrations are underestimated in Asia, but the higher emissions in CEDS than previous inventories result in improvements compared to observations. The treatment of black carbon (BC) scavenging in Oslo CTM3 gives better agreement with observed vertical BC profiles relative to the predecessor Oslo CTM2. However, Arctic wintertime BC concentrations remain underestimated, and a range of sensitivity tests indicate that better physical understanding of processes associated with atmospheric BC processing is required to simultaneously reproduce both the observed features. Uncertainties in model input data, resolution, and scavenging affect the distribution of all aerosols species, especially at high latitudes and altitudes. However, we find no evidence of consistently better model performance across all observables and regions in the sensitivity tests than in the baseline configuration. Using CEDS, we estimate a net RFari in 2014 relative to 1750 of −0.17 W m−2, significantly weaker than the IPCC AR5 2011–1750 estimate. Differences are attributable to several factors, including stronger absorption by organic aerosol, updated parameterization of BC absorption, and reduced sulfate cooling. The trend towards a weaker RFari over recent years is more pronounced than in the IPCC AR5, illustrating the importance of capturing recent regional emission changes.

Circulation responses to regional aerosol climate forcing in summer over East Asia

For East Asia, circulation responses to anthropogenic aerosol radiative forcing dominate aerosol-precipitation interactions. To gain insights, this study analyzed CESM simulated circulation changes related to the ‘north drought and south flood’ pattern caused by aerosol increases between two cases. One case was driven by the year-1850 global emission inventory, whereas the other used identical emissions for all regions except East Asia where anthropogenic emissions of aerosols and precursors of the year-2000 were imposed. Results show that the cooling caused by increased aerosols, which peaks at the middle latitudes, induces two intervened anomalous circulations in the troposphere. Near the surface, the increased land pressure weakens the southerlies and reduces the moisture transport for the entire eastern China. Meanwhile, in the free troposphere, the anomalous circulation exhibits remarkable meridional variations. While convergence occurs over 25°–45°N which partially compensates the decrease of moisture transport from lower levels, divergence develops over regions to the north which enhances the moisture deficiency. In addition, the southward shift of the jet stream stimulates anomalous rising and sinking motions over the south and north of 32°N. The combination of these changes leads to precipitation increase in the Yangtze River Valley but decrease over North China.

Aerosols at the poles: an AeroCom Phase II multi-model evaluation

Abstract. Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes.The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (−0.12 W m−2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of the AeroCom models (GISS modelE) to investigate how regional emissions of BC and sulfate and the lifetime of BC influence the Arctic and Antarctic AOD. A doubling of emissions in eastern Asia results in a 33 % increase in Arctic AOD of BC. A doubling of the BC lifetime results in a 39 % increase in Arctic AOD of BC. However, these radical changes still fall within the AeroCom model range.

Estimates of Health Impacts and Radiative Forcing in Winter Haze in Eastern China through Constraints of Surface PM2.5 Predictions.

The Gridpoint Statistical Interpolation (GSI) Three-Dimensional Variational (3DVAR) data assimilation system is extended to treat the MOSAIC aerosol model in WRF-Chem, and to be capable of assimilating surface PM2.5 concentrations. The coupled GSI-WRF-Chem system is applied to reproduce aerosol levels over China during an extremely polluted winter month, January 2013. After assimilating surface PM2.5 concentrations, the correlation coefficients between observations and model results averaged over the assimilated sites are improved from 0.67 to 0.94. At nonassimilated sites, improvements (higher correlation coefficients and lower mean bias errors (MBE) and root-mean-square errors (RMSE)) are also found in PM2.5, PM10, and AOD predictions. Using the constrained aerosol fields, we estimate that the PM2.5 concentrations in January 2013 might have caused 7550 premature deaths in Jing-Jin-Ji areas, which are 2% higher than the estimates using unconstrained aerosol fields. We also estimate that the daytime monthly mean anthropogenic aerosol radiative forcing (ARF) to be -29.9W/m2 at the surface, 27.0W/m2 inside the atmosphere, and -2.9W/m2 at the top of the atmosphere. Our estimates update the previously reported overestimations along Yangtze River region and underestimations in North China. This GSI-WRF-Chem system would also be potentially useful for air quality forecasting in China.

MACv2-SP: a parameterization of anthropogenic aerosol optical properties and an associated Twomey effect for use in CMIP6

Abstract. A simple plume implementation of the second version (v2) of the Max Planck Institute Aerosol Climatology, MACv2-SP, is described. MACv2-SP provides a prescription of anthropogenic aerosol optical properties and an associated Twomey effect. It was created to provide a harmonized description of post-1850 anthropogenic aerosol radiative forcing for climate modeling studies. MACv2-SP has been designed to be easy to implement, change and use, and thereby enable studies exploring the climatic effects of different patterns of aerosol radiative forcing, including a Twomey effect. MACv2-SP is formulated in terms of nine spatial plumes associated with different major anthropogenic source regions. The shape of the plumes is fit to the Max Planck Institute Aerosol Climatology, version 2, whose present-day (2005) distribution is anchored by surface-based observations. Two types of plumes are considered: one predominantly associated with biomass burning, the other with industrial emissions. These differ in the prescription of their annual cycle and in their optical properties, thereby implicitly accounting for different contributions of absorbing aerosol to the different plumes. A Twomey effect for each plume is prescribed as a change in the host model's background cloud-droplet population density using relationships derived from satellite data. Year-to-year variations in the amplitude of the plumes over the historical period (1850–2016) are derived by scaling the plumes with associated national emission sources of SO2 and NH3. Experiments using MACv2-SP are performed with the Max Planck Institute Earth System Model. The globally and annually averaged instantaneous and effective aerosol radiative forcings are estimated to be −0.6 and −0.5 W m−2, respectively. Forcing from aerosol–cloud interactions (the Twomey effect) offsets the reduction of clear-sky forcing by clouds, so that the net effect of clouds on the aerosol forcing is small; hence, the clear-sky forcing, which is more readily measurable, provides a good estimate of the total aerosol forcing.

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

Global fine-mode aerosol radiative effect, as constrained by comprehensive observations

Abstract. Aerosols directly affect the radiative balance of the Earth through the absorption and scattering of solar radiation. Although the contributions of absorption (heating) and scattering (cooling) of sunlight have proved difficult to quantify, the consensus is that anthropogenic aerosols cool the climate, partially offsetting the warming by rising greenhouse gas concentrations. Recent estimates of global direct anthropogenic aerosol radiative forcing (i.e., global radiative forcing due to aerosol–radiation interactions) are −0.35 ± 0.5 W m−2, and these estimates depend heavily on aerosol simulation. Here, we integrate a comprehensive suite of satellite and ground-based observations to constrain total aerosol optical depth (AOD), its fine-mode fraction, the vertical distribution of aerosols and clouds, and the collocation of clouds and overlying aerosols. We find that the direct fine-mode aerosol radiative effect is −0.46 W m−2 (−0.54 to −0.39 W m−2). Fine-mode aerosols include sea salt and dust aerosols, and we find that these natural aerosols result in a very large cooling (−0.44 to −0.26 W m−2) when constrained by observations. When the contribution of these natural aerosols is subtracted from the fine-mode radiative effect, the net becomes −0.11 (−0.28 to +0.05) W m−2. This net arises from total (natural + anthropogenic) carbonaceous, sulfate and nitrate aerosols, which suggests that global direct anthropogenic aerosol radiative forcing is less negative than −0.35 W m−2.

Impact of anthropogenic aerosols on summer precipitation in the Beijing–Tianjin–Hebei urban agglomeration in China: Regional climate modeling using WRF-Chem

The WRF model with chemistry (WRF-Chem) was employed to simulate the impacts of anthropogenic aerosols on summer precipitation over the Beijing–Tianjin–Hebei urban agglomeration in China. With the aid of a high-resolution gridded inventory of anthropogenic emissions of trace gases and aerosols, we conducted relatively long-term regional simulations, considering direct, semi-direct and indirect effects of the aerosols. Comparing the results of sensitivity experiments with and without emissions, it was found that anthropogenic aerosols tended to enhance summer precipitation over the metropolitan areas. Domain-averaged rainfall was increased throughout the day, except for the time around noon. Aerosols shifted the precipitation probability distribution from light or moderate to extreme rain. Further analysis showed that the anthropogenic aerosol radiative forcing had a cooling effect at the land surface, but a warming effect in the atmosphere. However, enhanced convective strength and updrafts accompanied by water vapor increases and cyclone-like wind shear anomalies were found in the urban areas. These responses may originate from cloud microphysical effects of aerosols on convection, which were identified as the primary cause for the summer rainfall enhancement.