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Analysis of aerosol cloud interactions with a consistent signal of meteorology and other influencing parameters

Quantifying the impact of aerosols on cloud micro/macro physical properties and estimating the signature of Aerosol Cloud Interactions (ACI) is one of the challenging tasks in atmospheric sciences. The Moderate Resolution Imaging Spectroradiometer and the European Centre for Medium-Range Weather Forecasts ERA-5 reanalysis data are employed to systematically study the ACI over the monsoon region in Pakistan. Based on the monsoon occurrence and rainfall intensity, the whole region is divided into three sub-regions labeled as highly intensive (R1), moderately intensive (R2) and weak (R3) monsoon region. The results indicate that the monthly mean Aerosol Optical Depth (AOD) peaks in the summer monsoon months (Jun, Jul, Aug, Sep). Here, the well-known Twomey effect whereby the Cloud Droplet Radius (CDR) decreases with increasing AOD holds only over R3; the opposite effects (Anti-Twomey effect) are found over R1 and R2, all passing the test of statistical significance (p<0.05). The multi-year AOD is found to be positively correlated with Cloud Liquid Water Path (CLWP) and Cloud Optical Depth (COD) over R1 and R2, suggesting that thicker clouds containing more water droplets are formed in polluted atmosphere. Over R3, decreases in CLWP and COD are found with increasing AOD only when AOD is less than~0.325. The analysis of ACI over R1 and R2 during the winter months shows similar but stronger responses of CDR, CLWP and COD to the variation in AOD. The weaker responses during the summer monsoon season may attributed to the occurrence of high level cloud and unstable atmospheric condition. Further investigation of the influences of Relative Humidity and pressure vertical velocity on the CDR-AOD relationships shows that although the magnitude of the CDR-AOD correlations change with meteorological conditions, the sign of correlations remain unchanged with meteorological conditions.

54 ENVIRONMENTAL SCIENCES↗

Impact of Wildfires on Solar Resource Availability in California in a Changing Climate

Wildfires can emit large amounts of atmospheric particulate matters and influence not only air quality but also availability of photovoltaic (PV) generation due to scattering and absorption of solar radiation. Under anthropogenic changing climate, wildfire activity is projected to increase over western North America due to drier and warmer climate, implying increasing impact on solar resource and larger uncertainty in solar generation especially in regions with faster PV penetration. This study focuses on quantifying the impact of wildfires on aerosol optical depth (AOD) and thus solar resource over California using National Solar Radiation Database (NSRDB), developed by the National Renewable Energy Laboratory (NREL). This assessment includes historical analysis and estimation of solar resource under wildfire scenarios (2020 wildfire and an enhanced wildfire scenario based on 2020 wildfires). Historical analysis for the period of July-October 2019/2020 (low/high fire activity period) shows that the averaged global horizontal irradiance (GHI) and direct normal irradiance (DNI) are reduced by about 30 and 90 W m-2 (5.6 and 15.3%), respectively, during high fire activity period. To create AOD dataset for enhanced fire scenario, 165% increase in burn area (in around 2050) is selected based on comprehensive literature review, which is further applied to the Fire INventory from NCAR (FINN) fire emission. WRF-Chem model with the enhanced FINN emissions is used to simulate and represent a preserving spatial distribution of burned areas and wildfire-emitted aerosols. Our initial analysis suggests that the"enhanced 2020 wildfire" AOD can increase by a factor of 1.3 - 2, which can significantly reduce solar irradiance and increase uncertainty in generation and reliability of power system in extreme wildfire events under a high solar penetration scenario. Overall, this study provides an estimate of the impacts of wildfires on solar resource to make informed decisions on reserve planning, generation scheduling, and reliability investments.

aerosol optical depth↗

All-sky aerosol direct radiative effects at the ARM SGP site

All-sky aerosol direct radiative effect (DRE) was estimated for the first time at the Atmospheric Radiation Measurement Southern Great Plains site using multi-year ground-based observations. The NASA Langley Fu-Liou radiation model was employed. Observed inputs for the radiation model include aerosol and cloud vertical extinction profile from Raman lidar; spectral aerosol optical depth, single-scattering albedo, and asymmetry factor from Aerosol Robotic Network; cloud water content profiles from radars; temperature and water vapor profiles from radiosondes; and surface shortwave spectral albedo from radiometers. A cloudy-sky radiative closure experiment was performed. The relative mean differences between modeled and observed surface downwelling shortwave total fluxes were 6% (7%) for transparent (opaque) cloudy-skies. The estimated annual mean all-sky aerosol DRE is -2.13±0.54W m -2 at the top of atmosphere (TOA) and -5.95±0.87 W m -2 at the surface, compared to -3.00±0.58 W m -2 AND -6.85±1.00 W m -2 , respectively, under clear-sky conditions. The seasonal cycle of all-sky aerosol DRE is similar to that of the clear-sky, except with secondary influences of the clouds: The cloud radiative effect is strongest (most negative) in the spring, which reduces the all-sky aerosol DRE. The relative uncertainties in all-sky aerosol DRE due to measurement errors are generally comparable to those in clear-sky conditions except for the aerosol single-scattering albedo. Finally, the TOA all-sky aerosol DRE relative uncertainty due to aerosol single-scattering albedo uncertainty is larger than that in clear-sky, leading to a larger total relative uncertainty. The measurement errors in cloud properties have small effects on the all-sky aerosol DRE.

54 ENVIRONMENTAL SCIENCES↗

Aerosol Direct Radiative Effects at the ARM SGP and TWP Sites: Clear Skies

The clear-sky aerosol direct radiative effect (DRE) was estimated at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) and Tropical Western Pacific (TWP) sites. The NASA Langley Fu-Liou radiation model was used with observed inputs including aerosol vertical extinction profile from the Raman lidar; spectral aerosol optical depth (AOD), single-scattering albedo and asymmetry factor from Aerosol Robotic Network; temperature and water vapor profiles from radiosondes; and surface shortwave (SW) spectral albedo from radiometers. A radiative closure experiment was conducted for clear-sky conditions. The mean differences of modeled and observed surface downwelling SW total fluxes were 1 W m-2 at SGP and 2 W m -2 at TWP, which are within observational uncertainty. At SGP, the estimated annual mean clear-sky aerosol DRE is -3.00 W m -2 at the top of atmosphere (TOA) and -6.85 W m -2 at the surface. The strongest aerosol DRE of -4.81 (-10.77) W m -2 at the TOA (surface) are in the summer when AODs are largest. The weakest aerosol DRE of -.28 (-2.77) W m -2 at the TOA (surface) are in November–January when AODs and single-scattering albedos are lowest. At TWP, the annual mean clear-sky DRE is -2.82 W m-2 at the TOA and -10.34 W m -2 at the surface. The strongest aerosol DRE of -5.95 (-22.20) W m -2 at the TOA (surface) are in November (October) due to the biomass burning season’s peak. The weakest aerosol DRE of -0.96 (-4.16) W m -2 at the TOA (surface) are in March (April) when AODs are smallest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Sensitivity of aerosol optical properties to the aerosol size distribution over central Europe and the Mediterranean Basin using the WRF-Chem v.3.9.1.1 coupled model

The size distribution of atmospheric aerosols plays a key role for understanding and quantifying the uncertainties related to aerosol–radiation and aerosol–cloud interactions. These interactions ultimately depend on the size distribution through optical properties (such as aerosol optical depth, AOD) or cloud microphysical properties. Hence, the main objective of this contribution is to disentangle the impact of the representation of aerosol size distribution on aerosol optical properties over central Europe, particularly over the Mediterranean Basin, during a summertime aerosol episode. To fulfill this objective, a sensitivity test has been conducted using the coupled chemistry–meteorology model WRF-Chem (Weather Research Forecast model coupled with Chemistry). The test modified the parameters defining a lognormal size distribution (geometric diameter and standard deviation) by 10 %, 20 %, and 50 %. Results reveal that the reduction in the standard deviation of the accumulation mode leads to the largest impacts on AOD due to a transfer of particles from the accumulation mode to the coarse mode. A reduction in the geometric diameter of the accumulation mode also has an influence on AOD representation since particles in this mode are assumed to be smaller. In addition, an increase in the geometric diameter of the coarse mode produces a redistribution through the total size distribution by relocating particles from the finer modes to the coarse.

54 ENVIRONMENTAL SCIENCES↗

Distinct Seasonality in Aerosol Responses to Emission Control Over Northern China

Despite intensive research exploring how aerosols respond to emission control over Northern China, efforts mostly focus on the environmental benefit, especially in winter. Here we found that unlike the most substantial PM 2.5 concentration reduction in winter, aerosol optical depth (AOD) declines more than 2 times faster in summer, causing an increase in aerosol radiative effects of 1.2 (5.7)Wm -2 on all-sky (clear-sky) conditions over 2013–2019 and largely shaping the climate impact. Low-level aerosols are shown to be the prime contributor under the synergetic effects of aerosol composition and ambient relative humidity (RH). The dominance of the highly hygroscopic sulfate combined with high RH enables a strong extinction efficiency of the reduced summertime aerosols, while the insignificant AOD decline in wintertime result from the dominance of organic aerosols with weak hygroscopicity, and is further offset by the increased frequencies of extremely high RH. We show the environmental and climatic responses of aerosols to emission control exhibit distinctively different seasonality.

54 ENVIRONMENTAL SCIENCES↗

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.

54 ENVIRONMENTAL SCIENCES↗

A Lagrangian analysis of pockets of open cells over the southeastern Pacific

Abstract. Pockets of open cells (POCs) have been shown to develop within closed-cell stratocumulus (StCu), and a large body of evidence suggests that the development of POCs result from changes in small-scale processes internal to the boundary layer rather than large-scale forcings. Precipitation is widely viewed as a key process important to POC development and maintenance. In this study, GOES-16 satellite observations are used in conjunction with MERRA-2 winds to track and compare the microphysical and environmental evolution of two populations of closed-cell StCu selected by visual inspection over the southeastern Pacific Ocean: one group that transitions to POCs and another comparison group (CLOSED) that does not. The high spatiotemporal resolution of the new GOES-16 data allows for a detailed examination of the temporal evolution of POCs in this region. We find that POCs tend to develop near the coast, last tens of hours, are larger than 104 km2, and often (88 % of cases) do not re-close before they exit the StCu deck. Most POCs are observed to form at night and tend to exit the StCu during the day when the StCu is contracting in area. Relative to the CLOSED trajectories, POCs have systematically larger effective radii, lower cloud drop number concentrations, a comparable conditional in-cloud liquid water path, and a higher frequency of more intense precipitation. Meanwhile, no systematic environmental differences other than boundary layer height are observed between POC and CLOSED trajectories. Interestingly, there are no differences in reanalysis aerosol optical depth between both sets of trajectories, which may lead one to the interpretation that differences in aerosol concentrations are not influencing POC development or resulting in a large number that re-close. However, this largely depends on the reanalysis treatment of aerosol–cloud interactions, and the product used in this study has no explicit handling of these important processes. These results support the consensus view regarding the importance of precipitation on the formation and maintenance of POCs and demonstrate the utility of modern geostationary remote sensing data in evaluating the POC life cycle.

54 ENVIRONMENTAL SCIENCES↗

Using CESM-RESFire to understand climate–fire–ecosystem interactions and the implications for decadal climate variability

Large wildfires exert strong disturbance on regional and global climate systems and ecosystems by perturbing radiative forcing as well as the carbon and water balance between the atmosphere and land surface, while short- and long-term variations in fire weather, terrestrial ecosystems, and human activity modulate fire intensity and reshape fire regimes. The complex climate–fire–ecosystem interactions were not fully integrated in previous climate model studies, and the resulting effects on the projections of future climate change are not well understood. Here we use the fully interactive REgion-Specific ecosystem feedback Fire model (RESFire) that was developed in the Community Earth System Model (CESM) to investigate these interactions and their impacts on climate systems and fire activity. We designed two sets of decadal simulations using CESM-RESFire for present-day (2001–2010) and future (2051–2060) scenarios, respectively, and conducted a series of sensitivity experiments to assess the effects of individual feedback pathways among climate, fire, and ecosystems. Our implementation of RESFire, which includes online land–atmosphere coupling of fire emissions and fire-induced land cover change (LCC), reproduces the observed aerosol optical depth (AOD) from space-based Moderate Resolution Imaging Spectroradiometer (MODIS) satellite products and ground-based AErosol RObotic NETwork (AERONET) data; it agrees well with carbon budget benchmarks from previous studies. We estimate the global averaged net radiative effect of both fire aerosols and fire-induced LCC at –0.59±0.52 W m –2 , which is dominated by fire aerosol–cloud interactions (–0.82±0.19 W m –2 ), in the present-day scenario under climatological conditions of the 2000s. The fire-related net cooling effect increases by ~170 % to –1.60±0.27 W m –2 in the 2050s under the conditions of the Representative Concentration Pathway 4.5 (RCP4.5) scenario. Such considerably enhanced radiative effect is attributed to the largely increased global burned area (+19 %) and fire carbon emissions (+100 %) from the 2000s to the 2050s driven by climate change. The net ecosystem exchange (NEE) of carbon between the land and atmosphere components in the simulations increases by 33 % accordingly, implying that biomass burning is an increasing carbon source at short-term timescales in the future. High-latitude regions with prevalent peatlands would be more vulnerable to increased fire threats due to climate change, and the increase in fire aerosols could counter the projected decrease in anthropogenic aerosols due to air pollution control policies in many regions. We also evaluate two distinct feedback mechanisms that are associated with fire aerosols and fire-induced LCC, respectively. On a global scale, the first mechanism imposes positive feedbacks to fire activity through enhanced droughts with suppressed precipitation by fire aerosol–cloud interactions, while the second one manifests as negative feedbacks due to reduced fuel loads by fire consumption and post-fire tree mortality and recovery processes. These two feedback pathways with opposite effects compete at regional to global scales and increase the complexity of climate–fire–ecosystem interactions and their climatic impacts.

54 ENVIRONMENTAL SCIENCES↗

Southwest Pacific tropical cyclone development classification utilizing machine learning and synoptic composites

This study evaluates the ability of machine learning algorithms to classify tropical depressions (TDs) and tropical storms (TSs) in the western region of the southwest Pacific Ocean (SWPO). Decision rules are generated to predict the environment required for a depression to fully develop into a mature storm, and the most influential predictors in the classification decision are ranked. TD and TS are discriminated based on a maximum sustained wind speed threshold (≥17 ms -1 ). Various aerosol, thermodynamic, and dynamic parameters are extracted closest to the initiation point of each non-developing and developing sample. The covariates associated with each labelled sample are used to train a decision tree and random forest model. Results using a testing dataset suggest the random forest approach more accurately distinguishes between non-developing and developing samples. The classification accuracy of the decision tree and random forest are 72% and 91%, respectively. Random forest outperformed the decision tree by providing higher accuracy in test data. The most important variables for binary classification are sea salt aerosol optical depth (AOD), 1,000 mb relative humidity, and sea surface temperature. AOD is a quantitative estimate of the aerosols presents in the air through the extinction of a ray of light as it passes through the atmosphere. Mean composite maps constructed in an unsupervised manner have been created for the most important variables identified by the random forest classifier during TD and TS events to highlight the difference in geophysical and aerosol variables' climatology during the two different classifications. This work will advance the risk management strategies for northeastern Australia and other SWPO basin islands to control their tropical cyclone related losses through prioritizing forecasting variables that are the strongest predictors of the strengthening of tropical depressions into tropical cyclones.

54 ENVIRONMENTAL SCIENCES↗

ARM data-oriented metrics and diagnostics package for climate model evaluation (ARM-DIAGS-V3) version 3

A Python-based metrics and diagnostics package is currently being developed by the ARM Infrastructure Team at Lawrence Livermore National Laboratory to facilitate the use of long-term high frequency measurements from the ARM program in evaluating the regional climate simulation of clouds, radiation, precipitation, and aerosols. This metrics and diagnostics package computes climatological means of targeted climate model simulation and generates tables and plots for comparing the model simulation with ARM observational data. The CMIP model data sets are also included in the package to enable model inter-comparison as demonstrated in Zhang et al. (2018) and Zhang et al. (2020). The mean of the CMIP model can be served as a reference for individual models. Basic performance metrics are computed to measure the accuracy of mean state and variability of climate models. The evaluated physical quantities include cloud fraction, temperature, relative humidity, cloud liquid water path, total column water vapor, precipitation, sensible and latent heat fluxes, aerosol optical depth, and radiative fluxes, with plan to extend to more fields, such as the evaluation of model simulated aerosol physicochemical properties and cloud microphysics properties. Process-oriented diagnostics focusing on aerosol, cloud, and precipitation-related phenomena are also being developed for the evaluation and development of specific model physical parameterizations. In addition to the Southern Great Plains (SGP), North Slope of Alaska (NSA) and Tropical Western Pacific (TWP) atmospheric observatories in the ARMDIAGS version 2.0, the version 3.0 package have extended to the data collected at the ARM Eastern North Atlantic (ENA) atmospheric observatory and the Observation and Modeling of the Green Ocean Amazon (GOAMAZON) field campaign. The metrics and diagnostics package are currently built upon standard Python libraries and additional Python packages developed by DOE (CDAT). The ARM metrics and diagnostic package is available publicly with the hope that it can serve as an easy entry point for climate modelers to compare their models with ARM data. In this report, we first provide an overview of major metrics in section 2. The input data, which constitutes the core content of the metrics and diagnostics package, is summarized in section 3. A user's guide documenting the workflow/structure of the version 3.0 codes and including step-by-step instruction for running the package is described in section 4.

54 ENVIRONMENTAL SCIENCES↗

Constraining the Twomey effect from satellite observations: issues and perspectives

Abstract. The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd, ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd, ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, ΔNd, ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of metres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining ΔNd, ant, namely the quantification of (i) the cloud-active aerosol – the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-to-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

54 ENVIRONMENTAL SCIENCES↗

On the relationship between eastern China aerosols and western North Pacific tropical cyclone activity

How aerosols affect the weather and climate system has received increasing attention. This study finds a significant negative correlation between March–May eastern China aerosol optical depth (AOD) and July–November western North Pacific (WNP) tropical cyclone (TC) frequency during 2003–2020. This time period spans when several aerosol reanalyses are available and both Terra and Aqua Moderate Resolution Imaging Spectroradiometer AOD retrievals are assimilated therein. Composite analyses and budget analyses of dynamical genesis potential indices indicate the importance of large-scale environmental factors, especially vertical velocity and vertical wind shear, associated with changes in AOD that in turn modulate changes in WNP TC frequency. Increased eastern China AOD may facilitate negative Pacific meridional mode development via modulation of the westerly jet, which then forces an anticyclonic circulation over the WNP basin. Increased AOD can also directly decrease the inter-hemispheric temperature differential and increases the intra-hemispheric temperature differential between the equator and the mid-latitudes, thus weakening ascending motion and enhancing vertical wind shear over the WNP, especially the southeastern portion of the basin. Further, all of these large-scale environment changes induced by increased eastern China AOD tend to suppress WNP TCs. This study highlights the potential influence of eastern China aerosol loadings on WNP TCs, thus improving our understanding of TC climate variability over the WNP.

54 ENVIRONMENTAL SCIENCES↗

Intensifying heat extremes in China attributed to rising greenhouse gases and declining aerosols since the 2010s

Rising temperatures have increased the frequency, duration, and intensity of extreme temperature events over China in recent decades. The upward trends in heat extremes in China in the warm season (May–September) and their relationships with changes in aerosols and greenhouse gases are investigated using observations, reanalysis data and model results. Significant increasing trends in China are observed in daily maximum temperatures (TXx), heatwave frequency, and heatwave mean duration during 2011–2023, with increasing rates of 0.70 °C/decade, 3.77 d/decade and 0.31 d/event/decade, respectively. This study shows that 43 ± 3% of the TXx increases in China are attributed to the rising CO2 concentrations. Aerosol optical depth in China decreased at a rate of 0.054 per decade from 2011 to 2023 due to significant air quality improvements. The weakened aerosol cooling effect due to declining aerosols contributes 27 ± 3% to the observed TXx trend. In eastern China, where aerosol reductions were most significant, aerosol reduction even accounts for 79 ± 10% of the TXx increasing trend. The intensifying heat waves attributed to GHGs and aerosols are in accordance with the increasing extreme high temperatures. The results highlight the significant impacts of rising GHGs and decreasing aerosols on heat extreme events over China in recent years, emphasizing the need of considering both GHGs and aerosols to address the issue of intensification of heat extremes in a warming future.

Zou, Aili↗

Anthropogenic–biogenic interaction amplifies warming from emission reduction over the southeastern US

A decline of surface biogenic secondary organic aerosols through the mediation of reduced anthropogenic aerosols has been recognized as an air quality co-benefit of anthropogenic emission control over the southeastern US. However, the climate impacts of this anthropogenic–biogenic interaction remain poorly understood. Here, we identified a substantial decline of summertime aerosol loading aloft over the southeastern US in recent decades through the interaction, which leads to a stronger decline in column-integrated aerosol optical depth and a greater increase in radiative fluxes over the southeastern than northeastern US, different from trends of anthropogenic emissions and near-surface aerosol loading. The anthropogenic–biogenic interaction is shown to explain more than 60% of the coherent increasing trend of 5.3 Wm -2 decade -1 in clear-sky surface downward radiative fluxes. We show that current climate models fail to represent this interaction. The interaction is further projected to amplify the positive radiative forcing from emission control by 42.3% regionally over the southeastern US and globally by 5.4% in 2050 under RCP4.5 compared to 2005. This amplification effect implies greater challenges to achieving the Paris Agreement temperature targets with continuous emission control in future.

54 ENVIRONMENTAL SCIENCES↗

Exploring the Constraints on Simulated Aerosol Sources and Transport across the North Atlantic with Island-Based Sun Photometers

Atmospheric aerosol over the North Atlantic Ocean impact regional clouds and climate. In this work, we use a set of sun photometer observations of Aerosol Optical Depth (AOD) located on the Graciosa and Cape Verde islands, along with the GEOS-Chem chemical transport model to investigate the sources of these aerosol and their transport over the North Atlantic Ocean. At both locations, the largest simulated contributor to aerosol extinction is the local source of sea-salt aerosol. In addition to this large source, we find that signatures consistent with long-range transport of anthropogenic, biomass burning, and dust emissions are apparent throughout the year at both locations. Model simulations suggest that this signal of long-range transport in AOD is more apparent at higher elevation locations; the influence of anthropogenic and biomass burning aerosol extinction is particularly pronounced at the height of Pico Mountain, near the Graciosa Island site. Using a machine learning approach, we further show that simulated observations at these three sites (near Graciosa, Pico Mountain, and Cape Verde) can be used to predict the simulated background aerosol imported into cities on the European mainland, particularly during the local winter months, highlighting the utility of background AOD monitoring for understanding downwind air quality.

54 ENVIRONMENTAL SCIENCES↗

Why Does E3SMv2 Have High Aerosol Sensitivity?

The Energy Exascale Earth System Model’s (E3SM) high aerosol effective radiative forcing (ERF) is evaluated against results from the Radiative-Forcing-Model-Intercomparison-Project (RFMIP). ERF is decomposed into aerosol susceptibility and aerosol optical depth change (Δτ). E3SM’s Δτ is found to be larger than that of any RFMIP model – particularly over the ocean - while its radiative response to anthropogenic aerosol change is unremarkable. Sensitivity simulations which reduce E3SM’s unrealistically large Δτ are effective at damping E3SM’s unusually strong ERF and improve agreement with the historical temperature record but have little impact on present-day climatology. These results suggest that reducing anthropogenic aerosol concentrations is an essential ingredient in any plan to fix E3SM’s high ERF.

58 GEOSCIENCES↗

Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 1: Experimental protocols and surface changes

There is now substantial literature on climate model studies of equatorial or tropical stratospheric SO 2 injections that aim to counteract the surface warming produced by rising concentrations of greenhouse gases. Here we present the results from the first systematic intercomparison of climate responses in three Earth system models wherein the injection of SO 2 occurs at different latitudes in the lower stratosphere: CESM2-WACCM6, UKESM1.0 and GISS-E2.1-G. The first two use a modal aerosol microphysics scheme, while two versions of GISS-E2.1-G use a bulk aerosol (One-Moment Aerosol, OMA) and a two-moment (Multiconfiguration Aerosol TRacker of mIXing state, MATRIX) microphysics approach, respectively. Our aim in this work is to determine commonalities and differences between the climate model responses in terms of the distribution of the optically reflective sulfate aerosols produced from the oxidation of SO 2 and in terms of the surface response to the resulting reduction in solar radiation. A focus on understanding the contribution of characteristics of models transport alongside their microphysical and chemical schemes, and on evaluating the resulting stratospheric responses in different models, is given in the companion paper (Bednarz et al., 2023). The goal of this exercise is not to evaluate these single-point injection simulations as stand-alone proposed strategies to counteract global warming; instead we determine sources and areas of agreement and uncertainty in the simulated responses and, ultimately, the possibility of designing a comprehensive intervention strategy capable of managing multiple simultaneous climate goals through the combination of different injection locations. We find large disagreements between GISS-E2.1-G and the CESM2-WACCM6 and UKESM1.0 models regarding the magnitude of cooling per unit of aerosol optical depth (AOD) produced, which varies from 4.7 K per unit of AOD in CESM2-WACCM6 to 16.7 K in the GISS-E2.1-G version with two-moment aerosol microphysics. By normalizing the results with the global mean response in each of the models and thus assuming that the amount of SO 2 injected is a free parameter that can be managed independently, we highlight some commonalities in the overall distributions of the aerosols, in the inter-hemispheric surface temperature response and in shifts to the Intertropical Convergence Zone, as well as some areas of disagreement, such as the extent of the aerosol confinement in the equatorial region and the efficiency of the transport to polar latitudes. In conclusion, we demonstrate that it is possible to use these simulations to produce more comprehensive injection strategies in multiple climate models. However, large differences in the injection magnitudes can be expected, potentially increasing inter-model spreads in some stratospheric quantities (such as aerosol distribution) while reducing the spread in the surface response in terms of temperature and precipitation; furthermore, the selection of the injection locations may be dependent on the models' specific stratospheric transport.

54 ENVIRONMENTAL SCIENCES↗