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Observations of fog-aerosol interactions over central Greenland
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Numerical case study of the aerosol–cloud interactions in warm boundary layer clouds over the eastern North Atlantic with an interactive chemistry module
The presence of warm boundary layer stratiform clouds over the eastern North Atlantic (ENA) region is commonly influenced by the Azores High, especially during the summer season. To investigate comprehensive aerosol–cloud interactions, this study employs the Weather Research and Forecasting model coupled with a chemistry component (WRF-Chem), incorporating aerosol chemical components that are relevant to the formation of cloud condensation nuclei (CCN) and accounting for aerosol spatiotemporal variation. This study focuses on aerosol indirect effects, particularly the long-range transport of aerosols, in the ENA region under three different weather regimes: a ridge with a surface high-pressure system, a post-trough with a surface high-pressure system, and a weak trough. The WRF-Chem simulations conducted at a near-large-eddy scale offer valuable insights into the model's performance, especially in terms of its ability to use high spatial resolution to capture mesoscale cloud features across various weather regimes. Our result shows that introducing 5 times more aerosols to either non-precipitating or precipitating clouds significantly increases ambient CCN numbers, resulting in, to varying degrees, higher liquid water path (LWP) values. The substantial aerosol–cloud interaction especially occurs in the precipitating clouds and demonstrates the susceptibility of the LWP to changes in CCN under different regimes. Conversely, thin, non-rain clouds at the edges of a cloud system are prone to evaporation, exhibiting an aerosol drying effect. The aerosols released during this process transition back to the accumulation mode, facilitating future activation. This dynamic behavior is not adequately represented in prescribed-aerosol simulations.
Large-Eddy Simulations of Marine Boundary Layer Clouds Associated with Cold-Air Outbreaks during the ACTIVATE Campaign. Part II: Aerosol–Meteorology–Cloud Interaction
Aerosol effects on micro/macrophysical properties of marine stratocumulus clouds over the western North Atlantic Ocean (WNAO) are investigated using in situ measurements and large-eddy simulations (LES) for two cold-air outbreak (CAO) cases (28 February and 1 March 2020) during the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). The LES is able to reproduce the vertical profiles of liquid water content (LWC), effective radius reff and cloud droplet number concentration Nc from fast cloud droplet probe (FCDP) in situ measurements for both cases. Furthermore, we show that aerosols affect cloud properties (N c , r eff , and LWC) via the prescribed bulk hygroscopicity of aerosols (¯k) and aerosol size distribution characteristics. N c , r eff , and liquid water path (LWP) are positively correlated to ¯κ and aerosol number concentration (N a ) while cloud fractional cover (CFC) is insensitive to ¯κ and aerosol size distributions for the two cases. The realistic changes to aerosol size distribution (number concentration, width, and the geometrical diameter) with the same meteorology state allow us to investigate aerosol effects on cloud properties without meteorological feedback. We also use the LES results to evaluate cloud properties from two reanalysis products, ERA5 and MERRA-2. Compared to LES, the ERA5 is able to capture the time evolution of LWP and total cloud coverage within the study domain during both CAO cases while MERRA-2 underestimates them.
Large-Eddy Simulations of Marine Boundary Layer Clouds Associated with Cold-Air Outbreaks during the ACTIVATE Campaign. Part II: Aerosol–Meteorology–Cloud Interaction
Aerosol effects on micro/macrophysical properties of marine stratocumulus clouds over the western North Atlantic Ocean (WNAO) are investigated using in situ measurements and large-eddy simulations (LES) for two cold-air outbreak (CAO) cases (28 February and 1 March 2020) during the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). The LES is able to reproduce the vertical profiles of liquid water content (LWC), effective radius r eff and cloud droplet number concentration N c from fast cloud droplet probe (FCDP) in situ measurements for both cases. Furthermore, we show that aerosols affect cloud properties (N c , r eff , and LWC) via the prescribed bulk hygroscopicity of aerosols ($\bar{κ}$) and aerosol size distribution characteristics. N c , r eff , and liquid water path (LWP) are positively correlated to $\bar{κ}$ and aerosol number concentration (N a ) while cloud fractional cover (CFC) is insensitive to $\bar{κ}$ and aerosol size distributions for the two cases. The realistic changes to aerosol size distribution (number concentration, width, and the geometrical diameter) with the same meteorology state allow us to investigate aerosol effects on cloud properties without meteorological feedback. We also use the LES results to evaluate cloud properties from two reanalysis products, ERA5 and MERRA-2. Compared to LES, the ERA5 is able to capture the time evolution of LWP and total cloud coverage within the study domain during both CAO cases while MERRA-2 underestimates them.
The Importance of an Ensemble Approach for Modeling Aerosol‐Convection Interactions
Aerosol-convection interactions modulate cloud microphysics, thermodynamics, and updraft intensity, contributing to climate-scale aerosol-radiative forcing. However, quantifying aerosol indirect effects in mixed-phase deep convection remains challenging due to uncertainties in parameterized physics and initial conditions driving nonlinear evolution of convective processes. This study investigates the convective updraft sensitivity to random initial temperature perturbations using an idealized ensemble modeling framework informed by in situ thermodynamic and aerosol observations from the DOE TRACER field campaign. We analyze the impact of small-scale initial perturbations on updraft velocity and supersaturation, and determine the ensemble size required to minimize stochastic internal variability. Results show that minor thermodynamic perturbations can produce updraft variability comparable to aerosol-induced changes reported in prior work. An ensemble of 10 members sufficiently reduces variability, enabling robust investigation of aerosol-related updraft invigoration and informing the design of future ensemble-based aerosol-convection interaction studies in environments with significant spatiotemporal mesoscale thermodynamic and aerosol heterogeneity.
Aerosol-Cloud Interactions and the Intersection of Climate Forcing and Feedback
The goal of this project has been to understand at the process level how the interaction of aerosols and cloud microphysics may alter the cloud response to climate change from the scale of turbulence to the global scale. Atmospheric aerosols (suspended particulates) have a unique role to play in the climate system. Anthropogenic aerosols may be an air pollution hazard and degrade human health. Their presence also results in the direct scattering or absorption of sunlight, with small net impacts on climate. But aerosols are also a key part of cloud formation, as the locations on which cloud droplets and ice crystals form. Understanding these Aerosol Cloud Interactions (ACI) is a critical uncertainty for climate models, including the Energy Exascale Earth System Model (E3SM), and affects how well models like E3SM can simulate the past and future. This work aims to understand cloud microphysics as well as the interaction of aerosol forcing and cloud feedback through improving our understanding of aerosol-cloud interactions (ACI) by looking at their uncertainty in critical environments at the process level. It will also contribute to the development of E3SM. Specific goals include: first, high level analysis of Perturbed Parameter Ensemble (PPE) simulations already available from the Community Earth System Model (CESM) and E3SM. Second, detailed analysis of recent changes to temperature and the role of aerosols.
An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin
Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3-5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.
An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin
Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~ 350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~ 100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.
Increased importance of aerosol–cloud interactions for surface PM 2.5 pollution relative to aerosol–radiation interactions in China with the anthropogenic emission reductions
Surface fine particulate matter (PM 2.5 ) pollution can be enhanced by feedback processes induced by aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). Many previous studies have reported enhanced PM 2.5 concentrations induced by ARIs and ACIs for episodic events in China. However, few studies have examined the changes in the ARI- and ACI-induced PM 2.5 enhancements over a long period, though the anthropogenic emissions have changed substantially in the last decade. In this study, we quantify the ARI- and ACI-induced PM 2.5 changes for 2013–2021 under different meteorology and emission scenarios using the Weather Research and Forecasting model with Chemistry (WRF-Chem), and we investigate the driving factors behind the changes. Our results show that, in January 2013, when China suffered from the worst PM 2.5 pollution, the PM 2.5 enhancement induced by ARIs in eastern China (5.59 µg m −3 ) was larger than that induced by ACIs (3.96 µg m −3 ). However, the ACI-induced PM 2.5 enhancement showed a significantly smaller decrease ratio (51 %) than the ARI-induced enhancement (75 %) for 2013–2021, making ACIs more important for enhancing PM 2.5 concentrations in January 2021. Our analyses suggest that the anthropogenic emission reductions played a key role in this shift. Owing to only anthropogenic emission reductions, the ACI-induced PM 2.5 enhancement decreased by 43 % in January, which was lower than the decrease ratio of the ARI-induced enhancement (57 %). The relative change in ARI- and ACI-induced PM 2.5 enhancement in July was similar to the pattern observed in January, caused by anthropogenic emission reductions. The primary reason for this phenomenon is that the decrease in ambient PM 2.5 for 2013–2021 caused a disproportionately small decrease in the liquid water path (LWP) and an increase in the cloud effective radius (Re) under the condition of high PM 2.5 concentrations. Therefore, the surface solar radiation attenuation (and, hence, the boundary layer height reduction) caused by ACIs decreased slower than that caused by ARIs. Moreover, the lower decrease ratio of the ACI-induced PM 2.5 enhancement was dominated by the lower decrease ratio of ACI-induced secondary PM 2.5 component enhancement, which was additionally caused by the smaller decrease ratio of the air temperature reduction and the relative humidity (RH) increase. Our findings indicate that, with the decrease in ambient PM 2.5 , the ACI-induced PM 2.5 enhancement inevitably becomes more important. This needs to be considered in the formulation of control policies to meet the national PM 2.5 air quality standard.
An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin
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Evaluation of Aerosol-cloud Interaction in the GISS Model E Using ARM Observations
Observations from the US Department of Energy's Atmospheric Radiation Measurement (ARM) program are used to evaluate the ability of the NASA GISS ModelE global climate model in reproducing observed interactions between aerosols and clouds. Included in the evaluation are comparisons of basic meteorology and aerosol properties, droplet activation, effective radius parameterizations, and surface-based evaluations of aerosol-cloud interactions (ACI). Differences between the simulated and observed ACI are generally large, but these differences may result partially from vertical distribution of aerosol in the model, rather than the representation of physical processes governing the interactions between aerosols and clouds. Compared to the current observations, the ModelE often features elevated droplet concentrations for a given aerosol concentration, indicating that the activation parameterizations used may be too aggressive. Additionally, parameterizations for effective radius commonly used in models were tested using ARM observations, and there was no clear superior parameterization for the cases reviewed here. This lack of consensus is demonstrated to result in potentially large, statistically significant differences to surface radiative budgets, should one parameterization be chosen over another.
Evaluation of E3SM Simulated Aerosols and Aerosol‐Cloud Interactions Across GCM and Convection‐Permitting Scales
This paper introduces an Earth system modeling testbed for predicting aerosols and aerosol‐cloud interactions (ACIs) at convection‐permitting scales. Using the Energy Exascale Earth System Model (E3SM) version 2 with a four‐mode Modal Aerosol Module, we conduct simulations at 3.25 km resolution on a regionally refined mesh (RRM) across four regions with distinct aerosol and cloud regimes. Results are compared with the standard 100 km E3SM configuration and evaluated against satellite, aircraft, and ground‐based observations. We find that increasing model resolution improves heavy precipitation simulation but amplifies positive bias in light drizzle at coarse resolution. These resolution‐induced changes affect cloud and aerosol properties to varying degrees across regions. Generally, cloud cover and liquid water path (LWP) show better agreement with satellite retrievals at 3.25 km, though surface‐based comparisons suggest otherwise. Aerosol composition remains poorly represented at both resolutions. The RRM increases Aitken mode aerosol number concentrations via enhanced new particle formation. However, accumulation mode aerosols are decreased at higher resolution as aerosol removals become more efficient. This partially contributes to fewer cloud condensation nuclei (CCN) and lower cloud droplet number concentrations (N d ), which produces larger model biases in some scenarios. These findings suggest that solely increasing horizontal resolution to kilometer scales is insufficient to broadly improve aerosol and cloud predictions without concurrent advancements in physical and chemical process representations. Nonetheless, the RRM moderately improves key ACI relationships such as CCN‐N d correlation, reflecting enhanced aerosol activation representation. The LWP‐N d relationship is also better captured by RRM, suggesting a better characterization of LWP adjustment.
A new method for diagnosing effective radiative forcing from aerosol–cloud interactions in climate models
Aerosol–cloud interactions (ACIs) are a leading source of uncertainty in estimates of the historical effective radiative forcing (ERF). One reason for this uncertainty is the difficulty in estimating the ERF from aerosol–cloud interactions (ERFaci) in climate models, which typically requires multiple calls to the radiation code. Most commonly used methods also cannot disentangle the contributions from different processes to ERFaci. Here, we develop a new, computationally efficient method for estimating the shortwave (SW) ERFaci from liquid clouds using histograms of monthly averaged cloud fraction partitioned by cloud droplet effective radius (r e ) and liquid water path (LWP). Multiplying the histograms with SW cloud radiative kernels gives the total SW ERFaci from liquid clouds, which can be decomposed into contributions from the Twomey effect, LWP adjustments, and cloud fraction (CF) adjustments. We test the method with data from five CMIP6-era models, using the Moderate Resolution Imaging Spectroradiometer (MODIS) satellite instrument simulator to generate the histograms. Our method gives similar total SW ERFaci estimates to other established methods in regions of prevalent liquid cloud and indicates that the Twomey effect, LWP adjustments, and CF adjustments have contributed -0.34 ± 0.23, -0.22 ± 0.13, and -0.09 ± 0.11 W m -2 , respectively, to the effective radiative forcing of the climate since 1850 in the ensemble mean (95 % confidence). These results demonstrate that widespread adoption of a MODIS r e –LWP joint histogram diagnostic would allow the SW ERFaci and its components to be quickly and accurately diagnosed from climate model outputs, a crucial step for reducing uncertainty in the historical ERF.
Impact of biomass burning aerosols on radiation, clouds, and precipitation over the Amazon: relative importance of aerosol–cloud and aerosol–radiation interactions
Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of –0.2 and 1.5 W m –2 , respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.
Local limits of detection for anthropogenic aerosol-cloud interactions
Ship tracks are quasi-linear cloud patterns produced from the interaction of ship emissions with low boundary layer clouds. They are visible throughout the diurnal cycle in satellite images from space-borne assets like the Advanced Baseline Imagers (ABI) aboard the National Oceanic and Atmospheric Administration Geostationary Operational Environmental Satellites (GOES-R). However, complex atmospheric dynamics often make it difficult to identify and characterize the formation and evolution of tracks. Ship tracks have the potential to increase a cloud's albedo and reduce the impact of global warming. Thus, it is important to study these patterns to better understand the complex atmospheric interactions between aerosols and clouds to improve our climate models, and examine the efficacy of climate interventions, such as marine cloud brightening. Over the course of this 3-year project, we have developed novel data-driven techniques that advance our ability to assess the effects of ship emissions on marine environments and the risks of future marine cloud brightening efforts. The three main innovative technical contributions we will document here are a method to track aerosol injections using optical flow, a stochastic simulation model for track formations and an automated detection algorithm for efficient identification of ship tracks in large datasets.
Observations of Aerosol‐Cloud Interactions During the North Atlantic Aerosol and Marine Ecosystem Study
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Overview of ACTIVATE’s First Year of Flights Targeting Aerosol-Cloud-Meteorology Interactions
The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) included 40 research flights in the winter and summer months of 2020 using a two-aircraft approach to simultaneously obtain in situ and remote sensing data of regions below, inside, and above boundary layer clouds. This presentation will summarize early findings from the first year of ACTIVATE flights with focus on aerosol and cloud droplet number concentration behavior, formation and evolution of clouds, and analysis of remote sensing retrievals of aerosol and cloud properties. There is a clear annual cycle in cloud droplet number concentration suggesting a marked annual cycle in aerosol-cloud interactions. Although aerosol particles are more abundant in spring and summer, the conditions needed to activate those particles into cloud droplets are weaker than in other colder months. Several flights targeted post-frontal clouds associated with cold air outbreaks pointing to enhanced levels of nucleated particles immediately above such clouds, and that ice formation hastens the transition from closed to open cloud structures in the sampled CAO events. Also observed in the marine boundary layer during CAOs is the frequent occurrence of non-spherical sea salt particles, which has significant implications for remote sensing retrievals.