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Enhancements in Cloud Condensation Nuclei Activity From Turbulent Fluctuations in Supersaturation

Abstract The effect of aerosols on the properties of clouds is a large source of uncertainty in predictions of weather and climate. These aerosol‐cloud interactions depend critically on the ability of aerosol particles to form cloud droplets. A challenge in modeling aerosol‐cloud interactions is the representation of interactions between turbulence and cloud microphysics. Turbulent mixing leads to small‐scale fluctuations in water vapor and temperature that are unresolved in large‐scale atmospheric models. To quantify the impact of turbulent fluctuations on cloud condensation nuclei (CCN) activation, we used a high‐resolution Large Eddy Simulation of a convective cloud chamber to drive particle‐based cloud microphysics simulations. We show small‐scale fluctuations strongly impact CCN activity. Once activated, the relatively long timescales of evaporation compared to fluctuations causes droplets to persist in subsaturated regions, which further increases droplet concentrations.

54 ENVIRONMENTAL SCIENCES↗

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E– 150°E) During the Spring and Summer: Results From MARCUS (I)

The Atmospheric Radiation Measurement Mobile Facility-2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017-2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60 degrees S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra-High-Sensitivity Aerosol Spectrometer show that both the number concentration (N-CCN) and size distribution of CCN-active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50 degrees S-60 degrees S) and the South Southern Ocean (SSO) (62 degrees S-68 degrees S). The average NSO N-CCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat-labile and presumably proteinacous INPs suggests an increase of ice nucleating-active microbes in summer.

Niu, Qing↗

Effective radiative forcing and adjustments in CMIP6 models

Abstract. The effective radiative forcing, which includes the instantaneous forcing plus adjustments from the atmosphere and surface, has emerged as the key metric of evaluating human and natural influence on the climate. We evaluate effective radiative forcing and adjustments in 17 contemporary climate models that are participating in the Coupled Model Intercomparison Project (CMIP6) and have contributed to the Radiative Forcing Model Intercomparison Project (RFMIP). Present-day (2014) global-mean anthropogenic forcing relative to pre-industrial (1850) levels from climate models stands at 2.00 (±0.23) W m−2, comprised of 1.81 (±0.09) W m−2 from CO2, 1.08 (± 0.21) W m−2 from other well-mixed greenhouse gases, −1.01 (± 0.23) W m−2 from aerosols and −0.09 (±0.13) W m−2 from land use change. Quoted uncertainties are 1 standard deviation across model best estimates, and 90 % confidence in the reported forcings, due to internal variability, is typically within 0.1 W m−2. The majority of the remaining 0.21 W m−2 is likely to be from ozone. In most cases, the largest contributors to the spread in effective radiative forcing (ERF) is from the instantaneous radiative forcing (IRF) and from cloud responses, particularly aerosol–cloud interactions to aerosol forcing. As determined in previous studies, cancellation of tropospheric and surface adjustments means that the stratospherically adjusted radiative forcing is approximately equal to ERF for greenhouse gas forcing but not for aerosols, and consequentially, not for the anthropogenic total. The spread of aerosol forcing ranges from −0.63 to −1.37 W m−2, exhibiting a less negative mean and narrower range compared to 10 CMIP5 models. The spread in 4×CO2 forcing has also narrowed in CMIP6 compared to 13 CMIP5 models. Aerosol forcing is uncorrelated with climate sensitivity. Therefore, there is no evidence to suggest that the increasing spread in climate sensitivity in CMIP6 models, particularly related to high-sensitivity models, is a consequence of a stronger negative present-day aerosol forcing and little evidence that modelling groups are systematically tuning climate sensitivity or aerosol forcing to recreate observed historical warming.

54 ENVIRONMENTAL SCIENCES↗

A Model Intercomparison Study of Aerosol‐Cloud‐Turbulence Interactions in a Cloud Chamber: 1. Model Results

This study presents the first model intercomparison of aerosol‐cloud‐turbulence interactions in a controlled cloudy Rayleigh‐Bénard Convection chamber environment, utilizing the Pi Chamber at Michigan Technological University. We analyzed simulated cloud chamber‐averaged statistics of microphysics and thermodynamics in a warm‐phase, cloudy environment under steady‐state conditions at varying aerosol injection rates. Simulation results from seven distinct models (DNS, LES, and a 1D turbulence model) were compared. Our findings demonstrate that while all models qualitatively capture observed trends in droplet number concentration, mean radius, and droplet size distributions at both high and low aerosol injection rates, significant quantitative differences were observed. Notably, droplet number concentrations varied by over two orders of magnitude between models for the same injection rates, indicating sensitivities to the model treatments in droplet activation and removal and wall fluxes. Furthermore, inconsistencies in vertical relative humidity profiles and in achieving steady‐state liquid water content suggest the need for further investigation into the mechanisms driving these variations. Despite these discrepancies, the models generally reproduced consistent power‐law relationships between the microphysical variables. This model intercomparison underscores the importance of controlled cloud chamber experiments for validating and improving cloud microphysical parameterizations. Recommendations for future modeling studies are also highlighted, including constraining wall conditions and processes, investigating droplet/aerosol removal (including sidewall losses), and conducting simplified experiments to isolate specific processes contributing to model divergence and reduce model uncertainties.

54 ENVIRONMENTAL SCIENCES↗

Tracking Aerosol Convection Interactions Experiment (TRACER) Field Campaign Report

Convective clouds serve a critical role in the Earth’s energy and water cycles through their transport of heat, moisture, momentum, and chemical species through the troposphere driving the global circulation (e.g., Hartmann et al. 1984, Del Genio et al. 2012, Su et al. 2014). On more local scales, convective clouds impact the atmospheric heating profile through diabatic heating effects, removal of water from the atmospheric column through precipitation, and conditioning of the local environment impacting further development of clouds (e.g., Sullivan and Voigt 2021). These critical roles underscore the importance of realistic representation of convective processes across scales of models from large-eddy simulation (LES), to convection-permitting models (CPM; e.g., Kendon et al. 2020, Marinescu et al. 2021), to numerical weather prediction (NWP) models used for operational weather forecasting, to Earth system models used to predict climate sensitivity (Sanderson et al. 2011, Sherwood et al. 2014, Tomassini et al. 2014, Zhao et al. 2016, Cronin et al. 2017). A key component of improving model representation of convective clouds is better quantification and parameterization of updraft microphysics and dynamics, including their interactions with the surrounding environment and storm organization (Bony et al. 2015, Hagos and Houze 2016, Donner et al. 2016, Morrison et al. 2020). Aerosol is an important environmental factor that could affect convective clouds and precipitation since cloud droplet and ice formation processes are initiated by it. Andrae et al. (2004) hypothesized that aerosols associated with increased biomass burning particles acting as cloud condensation nuclei (CCN) result in smaller and more monodisperse cloud droplets leading to suppression of warm rain formation, ultimately leading to more cloud water being lofted above the freezing level based on observations in the Amazon region. The subsequent increase in latent heat release increases the buoyancy of rising convective parcels invigorating the deep convection. This work was followed by a description of the theoretical basis for this “cold-phase invigoration” by Rosenfeld et al. (2008), who argued that it could have a significant effect for deep convective clouds with warm cloud-bases. Several modeling studies (e.g., Khain et al. 2005, 2009, van den Heever et al. 2006, Fan et al. 2007, 2009, 2012, Lee et al. 2008, Storer et al. 2010, Lebo et al. 2012, Storer and van den Heever 2013, Chen et al. 2020, Dagan et al. 2022) have investigated these aerosol-convection interactions and the environmental factors that influence their relative importance and magnitude. More recently, several studies have indicated that “warm-phase invigoration”, the enhancement of convection through condensational heating, also appears to play a role in enhancing both shallow cumuli (Seiki and Nakajima 2014, Saleeby et al 2015) and deeper tropical convection (Lebo and Seinfeld 2011, Khain et al. 2012, Sheffield et al 2015, Fan et al. 2018, Igel and van den Heever 2021), as well as Houston thunderstorms (Fan et al. 2007, 2020). However, still other studies have provided additional evidence of systematic biases in simulated convective outflow ice size distribution properties, which are consistent with a lack of poorly understood secondary ice production within convective updrafts (e.g., Fridlind et al. 2017). To help address these critical gaps in our understanding of cloud processes, aerosol processes and aerosol-cloud interactions, the Tracking Aerosol Convection Interactions Experiment was designed building upon efforts by the Aerosol, Cloud, Precipitation and Climate (ACPC) Initiative (http://acpcintiative.org/), a joint effort of the International Geosphere-Biosphere Programme (IGBP) and the World Climate Research Program (WCRP) that focused on resolving uncertainties in the interactions between aerosol and clouds towards better understanding the role that these interactions play in the climate system. The TRACER campaign was motivated by recommendations from a number of pilot studies undertaken by ACPC (van den Heever et al. 2017, Fridlind et al. 2019, Hu et al. 2019, Fan et al. 2020, Marinescu et al. 2021, Hernandez-Deckers et al. 2022) that pointed towards the southeastern Texas region as a locale where aerosol-convection interactions could be studied owing to the copious occurrence of isolated convection during the summer months accompanied by diverse and significant sources of aerosols from both anthropogenic and natural sources. The TRACER campaign began on 01 October 2021 and extended through 30 September 2022 with an intensive operational period (IOP) during June-September 2022. Three main sites (Table 1) were managed by the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility.

54 ENVIRONMENTAL SCIENCES↗

Vertical Gradient of Size-Resolved Aerosol Compositions over the Arctic Reveals Cloud Processed Aerosol in-Cloud and above Cloud

Arctic aerosols play a significant role in the aerosol-radiation and aerosol-cloud interactions, but ground-based measurements are insufficient to explain the interaction of aerosols and clouds in a vertically stratified Arctic atmosphere. This study shows the vertical variability of aerosol particle composition via tethered balloon system at Oliktok Point, Alaska, in August 2019, at different cloud layers for two case studies (background aerosol condition and polluted condition). Multi-modal micro-spectroscopy analysis of samples during the background case reveals a broadening of chemically specific size distribution above cloud top with a high abundance of sulfate and core-shell morphology, suggesting possible cloud processing of aerosols. The pollution case also indicates a broadening of size distribution at the upper cloud layer with the dominance of carbonaceous aerosol, which suggests the potential of carbonaceous aerosols for Arctic cloud formation. Here this study provides insights into the vertical profile of Arctic aerosols on cloud formation.

54 ENVIRONMENTAL SCIENCES↗

Enhanced mid-latitude warming due to poleward shift of sea salt aerosols in a warmer future

Natural aerosols provide large uncertainties regarding the quantification of the climate effects of aerosols, especially those related to aerosol-cloud interactions. Advancing research on the interaction of natural aerosols and climate can provide a better assessment of the climate impacts of anthropogenic activities. Furthermore, as one of the most dominant natural aerosols, sea salt has the highest proportion of mass in natural aerosols. Sea salt can be regarded as a purely scattering aerosol, causing a negative radiative effect by scattering shortwave solar radiation and acting as cloud condensation nuclei (CCN) through aerosol-cloud interactions. Future climate change will influence sea salt distribution, thus modifying the radiative effects of sea salt, which will further affect the climate. However, few previous studies have explored the interactions between sea salt changes under warming scenarios and climate change.

Yang, Yang [Nanjing Univ. of Information Science a↗

Atmospheric Research Over the Extended Western North Atlantic Ocean Region and North American East Coast: A Review of Past Work and Challenges Ahead

Decades of atmospheric research have focused on the extended Western North Atlantic Ocean (WNAO) region, including the East Coast of North America and the island of Bermuda, because of its unique location that offers accessibility, gradients in important atmospheric parameters, and a range of meteorological regimes leading to diverse conditions that are poorly understood. This work reviews decades of scientific investigations for the extended WNAO region. Approximately 40 combined field campaigns and long-term monitoring programs, in addition to 563 peer-reviewed publications between 1950 and 2019 have provided a firm foundation of knowledge for the extended WNAO region. Of particular importance in this region has been extensive work at the island of Bermuda that is host to important time series records of oceanic and atmospheric variables. Our review categorizes WNAO research into eight major categories, with some studies fitting into multiple categories (relative %): Aerosols (26%), Gases (23%), Development/Validation of Techniques, Models, and Retrievals (17%), Meteorology and Transport (10%), Air-Sea Interactions (9%), Wet Deposition (6%), Clouds/Storms (6%), and Aerosol-Cloud Interactions (3%). These extensive works have revealed a series of major knowledge gaps. For instance, a disproportionately low number of studies have been devoted to aerosol-cloud interactions, which is identified here as one of the most pressing research needs for the extended WNAO region. Recommendations for future research are provided in the categories highlighted above. Part 2 of this paper series will summarize major spatial and temporal features for the extended WNAO region.

Sorooshian, Armin↗

Using aircraft measurements to characterize subgrid-scale variability of aerosol properties near the Atmospheric Radiation Measurement Southern Great Plains site

Abstract. Complex distributions of aerosol properties evolve in space and time as a function of emissions, new particle formation, coagulation, condensational growth, chemical transformation, phase changes, turbulent mixing and transport, removal processes, and ambient meteorological conditions. The ability of chemical transport models to represent the multi-scale processes affecting the life cycle of aerosols depends on their spatial resolution since aerosol properties are assumed to be constant within a grid cell. Subgrid-scale-dependent processes that affect aerosol populations could have a significant impact on the formation of particles, their growth to cloud condensation nuclei (CCN) sizes, aerosol–cloud interactions, dry deposition and rainout and hence their burdens, lifetimes, and radiative forcing. To address this issue, we characterize subgrid-scale variability in terms of measured aerosol number, size, composition, hygroscopicity, and CCN concentrations made by repeated aircraft flight paths over the Atmospheric Radiation Measurement (ARM) program's Southern Great Plains (SGP) site during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystem (HI-SCALE) campaign. Subgrid variability is quantified in terms of both normalized frequency distributions and percentage difference percentiles using grid spacings of 3, 9, 27, and 81 km that represent those typically used by cloud-system-resolving models as well as the current and next-generation climate models. Even though the SGP site is a rural location, surprisingly large horizontal gradients in aerosol properties were frequently observed. For example, 90 % of the 3, 9, and 27 km cell mean organic matter concentrations differed from the 81 km cell around the SGP site by as much as ∼ 46 %, large spatial variability in aerosol number concentrations and size distributions were found during new particle formation events, and consequently 90 % of the 3, 9, and 27 km cell mean CCN number concentrations differed from the 81 km cell mean by as much as ∼ 38 %. The spatial variability varied seasonally for some aerosol properties, with some having larger spatial variability during the spring and others having larger variability during the late summer. While measurements at a single surface site cannot reflect the surrounding variability of aerosol properties at a given time, aircraft measurements that are averaged within an 81 km cell were found to be similar to many, but not all, aerosol properties measured at the ground SGP site. This analysis suggests that it is reasonable to directly compare most ground SGP site aerosol measurements with coarse global climate model predictions. In addition, the variability quantified by the aircraft can be used as an uncertainty range when comparing the surface point measurements with model predictions that use coarse grid spacings.

54 ENVIRONMENTAL SCIENCES↗

Comparing the interactions between particulate matter and cloud properties over two populated cities in Texas using WRF-Chem fine-resolution modeling

Accurate modeling of aerosol-cloud interactions is essential for reliable weather and air quality simulations, given their significant impact on precipitation patterns, cloud dynamics, and aerosol distributions. This study employed the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to examine the impact of enhanced meteorological simulations, achieved through advanced microphysics parameterization supported by data assimilation techniques, on air quality across Texas on August 19 and 20, 2022. We tested four distinct configurations: (1) the Morrison two-moment bulk microphysics scheme, (2) Morrison's with observation nudging, (3) the Spectral Bin Microphysics (SBM), and (4) SBM with observation nudging. While the SBM scheme is known for its detailed representation of aerosol-cloud interactions, our focus was on how improvements in meteorological accuracy translate to more precise air quality simulations. Our findings demonstrated a progressive improvement in simulation accuracy, starting with the Morrison's scheme and further enhanced by adopting the SBM scheme, complemented by incorporating observation nudging. Specifically, the combination of the SBM scheme and the nudging substantially enhanced the model's ability to capture convective precipitation events, as shown by better alignment with NEXRAD radar reflectivity, with R increasing from –0.21 to 0.82, IOA from 0.10 to 0.87, and NMB decreasing from 99% to 34% in Houston. The enhanced meteorology translated into more accurate PM 2.5 concentration simulations, particularly through the more accurate representation of aerosol washout during precipitation events. In Houston, the SBM scheme with nudging improved the model's PM 2.5 simulations significantly, with NMB decreasing from –20% to 5% and IOA improving from 0.43 to 0.61. In San Antonio, improvements were also notable, with NMB improved from –27% to –22%, R increased from 0.48 to 0.82, and IOA increased from 0.66 to 0.86. Furthermore, our results underscore the crucial role of accurate meteorological simulations in refining our understanding of aerosol behaviors in relation to precipitation patterns, directly enhancing the reliability and effectiveness of air quality modeling.

54 ENVIRONMENTAL SCIENCES↗

Characterization of the aerosol vertical distributions and their impacts on warm clouds based on multi-year ARM observations

Aerosol vertical distribution plays a crucial role in cloud development and thus precipitation since both aerosol indirect and semi-direct effects significantly depend on the relative position of aerosol layer in reference to cloud, but its precise influence on cloud remains unclear. In this study, we integrated multi-year Raman Lidar measurements of aerosol vertical profiles from the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) facility with available Value-Added Products of cloud features to characterize aerosol vertical distributions and their impacts on warm clouds over the continental and marine ARM atmospheric observatories, i.e., Southern Great Plains (SGP) and Eastern North Atlantic (ENA). A unimodal seasonal distribution of aerosol optical depths (AODs) with a peak in summer is found at upper boundary layer over SGP, while a bimodal distribution is observed at ENA for the AODs at lower levels with a major winter-spring maximum. The diurnal mean of upper-level AOD at SGP shows a maximum in the early evening. According to the relative positions of aerosol layers to clouds we further identify three primary types of aerosol vertical distribution, including Random, Decreasing, and Bottom. It is found that the impacts of aerosols on cloud may or may not vary with aerosol vertical distribution depending on environmental conditions, as reflected by the wide variations of the relations between AOD and cloud properties. For example, as AOD increases, the liquid water paths (LWPs) tend to be reduced at SGP but enhanced at ENA. The relations of cloud droplet effective radius with AOD largely depend on aerosol vertical distributions, particularly showing positive values in the Random type under low-LWP condition (<50gm -2 ). In conclusion, the distinct features of aerosol-cloud interactions in relation to aerosol vertical distribution are likely attributed to the continental-marine contrast in thermodynamic environments and aerosol conditions between SGP and ENA.

54 ENVIRONMENTAL SCIENCES↗

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.

54 ENVIRONMENTAL SCIENCES↗

Vertical Aerosol Profiling during SAIL (VAPS) Field Campaign Report

To more fully address the science goals of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s Surface Atmosphere Integrated Field Laboratory (SAIL) campaign, particularly the key science question of “How strongly do aerosols affect the surface energy and water balance by altering clouds, precipitation, and surface albedo, and how do these impacts vary seasonally?”, our campaign added instrumentation to planned tethered balloon system (TBS) flights in May and July of 2022. A key aspect of aerosol-cloud interactions is understanding cloud condensation nuclei (CCN) and ice nucleating particle (INP) populations, and how they vary seasonally and spatially. Because the interactions between aerosols and clouds is the target of this work, vertical distributions are particularly important to evaluate. Measurements of aerosol at ground level, below-cloud, and in-cloud will allow a better understanding of the airmasses that are feeding cloud-active particles into low- and mid-level clouds. Measurements of INP and aerosol populations often differ between the ground and aloft, with relationships that likely depend on regional and seasonal. Because of this, collocated measurements of aerosol, CCN, and INP, across different seasons, are crucial to reducing uncertainties in relationships between ground-level and cloud-base aerosol populations. Our campaign added online measurements of CCN using a compact CCN counter and offline filter collections for measurement of INP populations to the SAIL campaign TBS flights in May and July of 2022. The CCN instrument, the CloudPuck, flew and successfully collected data for a total of eight flights across both campaign periods. The IcePuck flew for most flights during the same period. Both instruments have continued to be used for other campaign requests in the SAIL domain. Analysis of this data was proposed through a concurrent DOE Atmospheric System Research (ASR) project submission, which was not funded in 2022. A similar proposal, which would involve analysis of the samples and data collected from this campaign, has been resubmitted in 2023 but a funding decision has not yet been made. If the proposal is again declined, we will seek other resources to ensure that this data can be analyzed.

54 ENVIRONMENTAL SCIENCES↗

Long-Term Trends in Aerosols, Low Clouds, and Large-Scale Meteorology Over the Western North Atlantic From 2003 to 2020

Here, a continuous decrease in aerosols over the Western North Atlantic Ocean (WNAO) on a decadal timescale provides a long-term benchmark to evaluate how various natural and anthropogenic processes affect the manifestation of aerosol-cloud interactions in this region. Furthermore, the WNAO serves as a natural laboratory with diverse aerosol sources, marine boundary layer clouds more variable than those in marine stratocumulus deck regions, and unique flow regimes established by the Gulf Stream and the semi-permanent Bermuda High. We investigate how satellite-retrieved macrophysical and microphysical properties of low clouds and the surface shortwave irradiance changed from 2003 to 2020, in tandem with this aerosol decrease. The decadal changes in large-scale meteorology related to the North Atlantic Oscillation (NAO) are also examined. We find a reduction in low-cloud optical thickness, accompanied by fewer and larger cloud droplets, yet observe no significant changes in low-cloud fraction and liquid water path. Despite the reduction in low-cloud optical thickness together with aerosol decrease, a corresponding increase in the trends of surface shortwave irradiance, also known as surface brightening, is lacking. This absence of brightening is potentially related to concomitant changes found in large-scale meteorology associated with NAO—Bermuda High strengthening, sea surface warming, and atmospheric moistening— as well as an increase in high-level cloud fraction that can counteract the surface brightening. Ultimately, our findings suggest that spatial patterns of decadal meteorological variability introduce complexities in the surface cloud radiative effect over the WNAO, thereby complicating the isolation and examination of aerosol-cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

Aerosol-boundary-layer-monsoon interactions amplify semi-direct effect of biomass smoke on low cloud formation in Southeast Asia

Low clouds play a key role in the Earth-atmosphere energy balance and influence agricultural production and solar-power generation. Smoke aloft has been found to enhance marine stratocumulus through aerosol-cloud interactions, but its role in regions with strong human activities and complex monsoon circulation remains unclear. Here we show that biomass burning aerosols aloft strongly increase the low cloud coverage over both land and ocean in subtropical southeastern Asia. The degree of this enhancement and its spatial extent are comparable to that in the Southeast Atlantic, even though the total biomass burning emissions in Southeast Asia are only one-fifth of those in Southern Africa. We find that a synergetic effect of aerosol-cloud-boundary layer interaction with the monsoon is the main reason for the strong semi-direct effect and enhanced low cloud formation in southeastern Asia.

54 ENVIRONMENTAL SCIENCES↗

Aquaplanets as a Framework for Examination of Aerosol Effects

Although fundamental to the planetary radiative balance, aerosol impacts are highly uncertain in climate simulations because of the uneven distribution of aerosol sources and the complex interactions with radiation and clouds that are difficult to represent in climate models. This study proposes that aquaplanet configurations represent an idealized framework to investigate aerosol effects. As a simple demonstration, a series of aquaplanet simulations with the Community Atmosphere Model version 6 shows that the spatial distribution of aerosol emissions changes the aerosol effective radiative forcing even with unchanged total emissions. Some statistical properties of the simulations are presented to show that relatively short model integrations yield robust results. Much of the aerosol effect is shown to arise from aerosol–cloud interactions, especially through rapid adjustments associated with the aerosol lifetime effect that alter the cloud optical thickness.

54 ENVIRONMENTAL SCIENCES↗

Characterization of Organosulfates and Organonitrates in Vertically Resolved Aerosols over the Southern Great Plains Field Campaign Report

Aerosol is the largest individual source of uncertainty in assessing the Earth’s radiative balance due to poorly understood aerosol processes and aerosol-cloud interactions. Thus, to constrain aerosol’s climate impacts, it is critical to understand aerosol compositions at high elevations. Organic material accounts for about 20-80% of total aerosol mass in the atmosphere and is known to play a key role in aerosol processes and cloud formation. In prior research, characterization of aerosol molecular composition has been mostly carried out at ground level. In these ground-level measurements, total speciated organosulfates and organonitrates may contribute significantly to organic aerosol mass on the order of 10-40%, most of which are from abundant biogenic volatile organic compounds such as isoprene and monoterpenes. Organosulfates and organonitrates have also been shown to be present in substantial amounts in cloud water, suggesting that they can be transported and/or directly formed at high elevations. On the other hand, the less common and more expensive aircraft studies have performed high-altitude measurements, but were often limited in the number of different altitudes sampled and in sample collection under consistent conditions. Therefore, the vertical distributions of key aerosol components such as organosulfates and organonitrates are not well understood and have not been extensively studied. Nevertheless, it is important to understand how organosulfates and organonitrates in aerosols are distributed, transformed, participate in aqueous-phase processes, and interact with high-altitude clouds.

54 ENVIRONMENTAL SCIENCES↗

Bounding Global Aerosol Radiative Forcing of Climate Change

Abstract Aerosols interact with radiation and clouds. Substantial progress made over the past 40 years in observing, understanding, and modeling these processes helped quantify the imbalance in the Earth's radiation budget caused by anthropogenic aerosols, called aerosol radiative forcing, but uncertainties remain large. This review provides a new range of aerosol radiative forcing over the industrial era based on multiple, traceable, and arguable lines of evidence, including modeling approaches, theoretical considerations, and observations. Improved understanding of aerosol absorption and the causes of trends in surface radiative fluxes constrain the forcing from aerosol‐radiation interactions. A robust theoretical foundation and convincing evidence constrain the forcing caused by aerosol‐driven increases in liquid cloud droplet number concentration. However, the influence of anthropogenic aerosols on cloud liquid water content and cloud fraction is less clear, and the influence on mixed‐phase and ice clouds remains poorly constrained. Observed changes in surface temperature and radiative fluxes provide additional constraints. These multiple lines of evidence lead to a 68% confidence interval for the total aerosol effective radiative forcing of ‐1.6 to ‐0.6 W m −2 , or ‐2.0 to ‐0.4 W m −2 with a 90% likelihood. Those intervals are of similar width to the last Intergovernmental Panel on Climate Change assessment but shifted toward more negative values. The uncertainty will narrow in the future by continuing to critically combine multiple lines of evidence, especially those addressing industrial‐era changes in aerosol sources and aerosol effects on liquid cloud amount and on ice clouds.

54 ENVIRONMENTAL SCIENCES↗