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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

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.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Signatures of aerosol-cloud interactions in GiOcean: a coupled global reanalysis with two-moment cloud microphysics

Aerosols influence the Earth's radiative balance through direct interactions with radiation and by affecting cloud properties. Anthropogenic aerosols have led to cooling during the industrial era through aerosol–cloud interactions (ACI), including aerosol effects on cloud microphysical properties and the subsequent adjustments. However, large uncertainties remain in Earth system models (ESMs) regarding the magnitude of this cooling. In part, ESMs substantially disagree on cloud properties, thermodynamics, the hydrological cycle, and general circulation. Reanalysis provides a useful avenue for exploring the impact of ACI on clouds and radiation because its atmosphere is forced to match realistic conditions through the assimilation of observations. Here, we explore the impact of ACI on clouds in the GiOcean reanalysis – the first to incorporate aerosol-cloud interactions. We contrast variables important for ACI between GiOcean and satellite observations and develop 2-dimensional lookup tables of ACI for both using a source-sink budget perspective to attribute the changes in cloud droplet number (Nd) and liquid water path (LWP) to aerosol and meteorology. A compositing analysis using lookup tables shows that GiOcean captures key aspects of aerosol–cloud–precipitation interactions, including (1) activation of aerosol into cloud droplets, (2) effective precipitation scavenging of Nd, (3) suppression of precipitation by high Nd in regions with heavy aerosol emissions. In contrast, satellite observations do not exhibit clear patterns for processes (2) and (3). Random Forest analysis shows that interannual variability in Nd and LWP over the Northern Hemisphere ocean in GiOcean is primarily driven by precipitation, consistent with satellite observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

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.

Huang, Meng [Pacific Northwest National Laboratory↗
DOE OSTI2025

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.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Overview of the Nephele Perturbed Parameter Ensemble for Aerosol‐Cloud Interactions in E3SMv3

Aerosol-cloud interactions (aci) are the leading source of uncertainty in inferring climate sensitivity from the historical record. Earth system models (ESMs) struggle to represent aci because the processes responsible for these phenomena occur at much finer time and space scales than can be resolved by any ESM. Observational constraints provide key benchmarks to test ESMs, but cannot be used alone to fully understand aci processes except in very specific cases where causality is controlled; some degree of modeling is required to infer aci and estimate radiative forcing. Here, we generate and characterize a perturbed parameter ensemble (PPE) in version 3 of the Energy Exascale ESM (E3SMv3). We perturb 25 parameters that govern aci processes over 250 members and integrate the model over present-day and preindustrial aerosol emissions. We find that the process representation in E3SMv3 is flexible and can generate global-mean effective radiative forcings due to aci (ERFaci) ranging from −3.0 to +0.9 W m −2 . The positive ERFaci values simulated by a portion of the PPE are implausible and result from parameter combinations that produce unrealistic top-of-atmosphere energy fluxes. While global-mean cloud droplet number concentration always increases in response to anthropogenic aerosol, cloud liquid water path can both increase and decrease, suggesting that precipitation suppression is not the only aerosol-cloud adjustment represented by E3SMv3. Analysis of which processes control liquid cloud adjustment in the PPE points toward stratiform precipitation processes and aerosol activation, which is consistent with many previous ESMs, as well as the new two-moment convective cloud microphysics in E3SMv3.

Nugent, Jacqueline M. [Univ. of Wyoming, Laramie, ↗
DOE OSTI2025

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.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

LAACI – Light Absorbing Aerosol-Cloud Interactions Experiment

The “Light Absorbing Aerosol-Cloud Interactions Experiment” project aimed at studying the interactions of light-absorbing aerosols from biomass burning (e.g., wildfires or prescribed fires) with clouds. The core of the project was carried out at the Michigan Technological University turbulent cloud chamber facility (hereafter referred to as the Pi-Chamber). Light-absorbing aerosols from biomass burning include black carbon (BC) and brown carbon (BrC) organic material.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

The U.S. DOE ARM User Facility Establishes a New Site for Studies of Land–Aerosol–Cloud Interactions in the Southeastern United States

The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility has established a new site in the Bankhead National Forest (BNF) in northern Alabama that will gather data on how clouds, the land surface, and aerosols interact at a hierarchy of scales important to understanding and simulating the Earth system. Starting its operations in October 2024, the BNF site provides a multi-year opportunity for scientists to unravel complex land-atmosphere interactions. A suite of ground-based sensors, elevated tower-based instrumentation, and aerial facilities will enable scientists to investigate those interactions from within the canopy to the clouds. The Southeastern United States was recommended by the DOE ARM and its collaborators in the broader community as an important region to address their common scientific questions given the region’s abundant surface-forced convective clouds and mesoscale convective systems that pose ongoing challenges in Earth system models. The region is also home to significant terrain complexity and land-use heterogeneity that will unleash new understanding of anthropogenic and biogenic aerosol processes, boundary-layer aerosol-cloud interactions, and the interactions between the terrestrial ecosystem and coupled aerosol-cloud-radiation processes.

Aerosols↗
DOE OSTI2026

The Amazon River‐Breeze Circulation Limits Detection of Aerosol‐Cloud Interactions in Warm Clouds

Increased aerosol concentrations can brighten low-level clouds and extend their lifetimes, but aerosol–cloud interactions (ACI) remain highly uncertain and difficult to quantify. We show that part of this uncertainty is caused by topographical influences on clouds, that is, those arising from land–water contrasts. This is demonstrated using satellite retrievals in regions with extensive river networks, such as the Amazon Basin. 15 years of MODerate resolution Imaging Spectroradiometer (MODIS) satellite data show cloud formation over the Amazon River basin is suppressed by 26% with warm low clouds above the river exhibiting a 22% smaller droplet effective radius and 18% higher droplet concentration ($N_d$) compared to adjacent land clouds. Thus, clouds above the river may appear polluted but are actually influenced by river-breeze circulations driven by the thermal contrast between the river and the surrounding land. These responses are robust in both wet and dry seasons, and tests using an improved MODIS retrieval product show cloud differences are unlikely due to retrieval artifacts. In situ measurements from the Green Ocean Amazon Experiment (GoAmazon) confirm that $N_d$ is elevated above rivers and are also higher when carbon monoxide concentrations are elevated near the large city of Manaus. Lagrangian airmass tracking over Manaus shows that regional-scale river-breeze circulations impact $N_d$ as much as the urban aerosol plume, complicating ACI attribution and highlighting the need to isolate land-surface effects to assess ACI in continental regions.

Aerosol-Cloud Interactions↗
DOE OSTI2026

Laboratory Investigations of Aerosol-Cloud Interactions in an Entraining, Turbulent Environment (Final Technical Report)

The effects that aerosol particles have on clouds in Earth’s atmosphere and the role that clouds play in determining the fate of aerosol particles play a crucial role in determining the human experience on this planet. These interwoven interactions can determine whether it rains or snows, is comfortable, hot or cold, or whether the cloud you gaze at in the sky looks like a tiger or a lump of porridge. How clouds mix with the air surrounding them, a process known as entrainment, further affects these processes. We conducted laboratory experiments of aerosol-cloud interactions in a setting in which we can measure the effects of entrainment – the first laboratory experiments since the pioneering work of Latham and Reed in 1977. We measured the effects of entrainment on aerosol-cloud interactions in the Pi Chamber and also used a state-of-the-art large eddy simulation (LES) to investigate processes in fine detail.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

On the Prediction of Aerosol-Cloud Interactions Within a Data-Driven Framework

Aerosol-cloud interactions (ACI) pose the largest uncertainty for climate projection. Among many challenges of understanding ACI, the question of whether ACI can be deterministically predicted has not been explicitly answered. Here we attempt to answer this question by predicting cloud droplet number concentration N c from aerosol number concentration N a and ambient conditions using a data-driven framework. We use aerosol properties, vertical velocity fluctuations, and meteorological states from the ACTIVATE field observations (2020–2022) as predictors to estimate N c . We show that the campaign-wide N c can be successfully predicted using machine learning models despite the strongly nonlinear and multi-scale nature of ACI. However, the observation-trained machine learning model fails to predict N c in individual cases while it successfully predicts N c of randomly selected data points that cover a broad spatiotemporal scale. This suggests that, within a data-driven framework, the N c prediction is uncertain at fine spatiotemporal scales.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Regime-based aerosol–cloud interactions from CALIPSO-MODIS and the Energy Exascale Earth System Model version 2 (E3SMv2) over the Eastern North Atlantic

This study investigates aerosol-cloud interactions in marine boundary layer (MBL) clouds using an advanced deep-learning-driven synoptic-regime-based framework, combining satellite data (CALIPSO vertically resolved aerosol extinction and MODIS cloud properties) with 1° nudged Energy Exascale Earth System Model version 2 (E3SMv2) simulation over the Eastern North Atlantic (ENA; ∼10°×10°, 2006–2014). The E3SMv2 captures observed seasonal variations in cloud droplet number concentrations (N d ) and liquid water path (LWP), though it systematically underestimates N d . We then partition ENA meteorology into four synoptic regimes (Pre-Trough, Post-Trough, Ridge, Trough) via a deep-learning clustering of ERA5 reanalysis fields, enabling regime-dependent aerosol-cloud interactions analyses. Both satellite and E3SMv2 exhibit an inverted-V LWP-N d relationship. In Post-Trough and Ridge regimes, the satellite shows stronger negative LWP-N d sensitivities than in Pre-Trough regime. The Trough regime displays a muted satellite LWP response. In comparison, the model predicts more exaggerated LWP responses across regimes, with LWP increasing too quickly at low N d and decreasing more sharply at high N d , especially in Pre-Trough and Trough regimes. These exaggerated model LWP sensitivities may stem from uncertainties in representing drizzle processes, entrainment, and turbulent mixing. As for N d susceptibility to aerosols, N d increases with MBL aerosol extinction in both datasets, but the simulated aerosol-cloud interactions appear oversensitive to meteorological conditions. Overall, E3SMv2 better captures aerosol effects under regimes that favor stratiform clouds (Post-Trough, Ridge), but performance deteriorates for regimes with deeper, dynamically complex clouds (Trough), highlighting the need for improved representations of those cloud processes in climate models.

Environmental sciences↗
DOE OSTI2026

Advancing the quantification of aerosol-cloud interactions with the CALIPSO-CloudSat-Aqua/MODIS record

Aerosol-cloud-precipitation interactions are assessed over the non-polar ocean using more than 11 years of combined Aqua-MODIS, CALIPSO-CALIOP, and CloudSat products. The analysis first shows the benefit of incorporating vertically resolved aerosol extinction coefficient (σext) in aerosol-cloud interactions (ACI) assessments, demonstrating that: σext vertically collocated with the cloud layer () correlates best with cloud droplet number concentration (Nd), column-integrated aerosol optical depth (AOD) cannot explain the Nd variability in the extratropics, and the S-shape of the AOD-Nd relationship reported in previous studies is not replicated when using instead of AOD, with a Nd- linearity more consistent with in-situ studies over the ocean. ACI metric, estimated as the log-scale regression between CALIOP and MODIS Nd reveals that the eastern Pacific is the region with the strongest ACI, followed by the Southern Ocean. The susceptibility of clouds to changes in their liquid water path (LWP) and frequency of precipitation followed a 2-step calculation by combining the Nd- regression (ACI) with the regression between these macrophysical variables and Nd. LWP susceptibility is negative (LWP decreases with aerosol loading) and statistically significant over the eastern Pacific, eastern Atlantic, and extratropics. In contrast, vast areas of the tropical and subtropical ocean feature negligible changes in LWP with aerosol. Precipitation frequency susceptibility is negative, but the values are only significant over the coastal eastern Pacific and Atlantic. The findings suggest that previous modeling assessments relying on AOD may need to be revisited by taking advantage of the synergy between passive and active sensors.

Li, Zhujun↗
DOE OSTI2025

Exploring Causal Relationships and Adjustment Timescales of Aerosol-Cloud Interactions in Geostationary Satellite Observations and CAM6 Using Wavelet Phase Coherence Analysis

We present for the first time within the cloud physics context, the application of wavelet phase coherence analysis to disentangle counteracting physical processes associated with the lead-lag phase difference between cloud-proxy liquid water path (LWP) and aerosol-proxy cloud droplet number concentration ( N d ) in an Eulerian framework using satellite-based observations and climate model outputs. This approach allows us to identify the causality and dominant adjustment timescales governing the correlation between LWP and N d . Satellite observations indicate a more prevalent positive correlation between daytime LWP and N d regardless of whether LWP leads or lags N d . The positive cloud water response, associated with precipitation processes, typically occurs within 1 hr, while the negative response resulting from entrainment drying, usually takes 2–4 hr. CAM6 displays excessively rapid negative responses along with overly strong negative cloud water response and insufficient positive response, leading to a more negative correlation between LWP and N d compared to observations.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Understanding the causes of satellite–model discrepancies in aerosol–cloud interactions using near-LES simulations of marine boundary layer clouds

Aerosol–cloud interactions (ACI) remain the largest source of uncertainty in model estimates of anthropogenic radiative forcing, primarily because of deficiencies in representing aerosol–cloud microphysical processes that lead to inconsistent cloud liquid water path (LWP) responses to aerosol perturbations between observations and models. To investigate this discrepancy, we conducted a series of large-eddy-scale simulations driven by realistic meteorology over the eastern North Atlantic, and evaluated LWP susceptibility, precipitation processes, and boundary layer thermodynamics using satellite and ground-based observations. Simulated LWP responses show a strong dependence on cloud state. Non-precipitating thin clouds exhibit a modest LWP decrease with increasing cloud droplet number concentration (N d ), consistent in sign but weaker in magnitude than satellite estimates, reflecting enhanced turbulent mixing and evaporation. The largest model-observation discrepancy occurs in non-precipitating thick clouds, where simulated LWP susceptibilities are strongly positive (+0.32) while observations indicate large negative values (−0.69). This discrepancy stems from excessive precipitation driven by underestimated entrainment, overly active accretion, and overly broad drop-size distributions in polluted conditions. While our high-resolution setup mitigates the excessive drizzling common in coarser models and captures key regime transitions, these biases persist – highlighting that improved parameterizations of cloud-top processes, precipitation, and aerosol effects are needed beyond simply increasing model resolution. Additionally, misrepresented moisture inversions in reanalysis introduce a moist bias in cloud-top relative humidity, further amplifying positive LWP susceptibility. Our results also suggest that large negative N d –LWP relationships in observations may reflect internal cloud processes rather than true ACI effects.

Aerosol-cloud interaction↗
DOE OSTI2025

RCEMIP‐ACI: Aerosol‐Cloud Interactions in a Multimodel Ensemble of Radiative‐Convective Equilibrium Simulations

Aerosol‐cloud interactions are a persistent source of uncertainty in climate research. This study presents findings from a model intercomparison project examining the impact of aerosols on clouds and climate in convection‐permitting radiative‐convective equilibrium (RCE) simulations. Specifically, 11 different modeling teams conducted RCE simulations under varying aerosol concentrations, domain configurations, and sea surface temperatures (SSTs). We analyze the response of domain‐mean cloud and radiative properties to imposed aerosol concentrations across different SSTs. Additionally, we explore the potential impact of aerosols on convective aggregation and large‐scale circulation in large‐domain simulations. The results reveal that the cloud and radiative responses to aerosols vary substantially across models. However, a common trend across models, SSTs, and domain configurations is that increased aerosol loading tends to suppress warm rain formation, enhance cloud water content in the mid‐troposphere, and consequently increase mid‐tropospheric humidity and upper‐tropospheric temperature, thereby impacting static stability. The warming of the upper troposphere can be attributed to reduced lateral entrainment effects due to the higher environmental humidity in the mid‐troposphere. However, models do not agree on aerosol impacts on convective updraft velocity based on the preliminary examination of high‐percentiles of vertical velocity at a single mid‐troposheric layer (500 hPa). In large‐domain simulations, where convection tends to self‐organize, aerosol loading does not consistently influence self‐organization but tends to reduce the intensity of large‐scale circulation forming between convective clusters and dry regions. This reduction in circulation intensity can be explained by the increase in static stability due to the upper tropospheric warming.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Can general circulation models (GCMs) represent cloud liquid water path adjustments to aerosol–cloud interactions?

Abstract. General circulation models (GCMs), unlike other lines of evidence, indicate that anthropogenic aerosols cause a global-mean increase in cloud liquid water path (ℒ) and thus a negative adjustment to radiative forcing of the climate by aerosol–cloud interactions. In part 1 of this series of papers, we showed that this is true even in models that reproduce the negative correlation observed in present-day internal variability in ℒ and cloud droplet number concentration (Nd). We studied several possible confounding mechanisms that could explain the noncausal cloud–aerosol correlations in GCMs and that possibly contaminate observational estimates of radiative adjustments. Here, we perform single-column and full-atmosphere GCM experiments to investigate the causal model-physics mechanisms underlying the model radiative adjustment estimate. We find that both aerosol–cloud interaction mechanisms thought to be operating in real clouds – precipitation suppression and entrainment evaporation enhancement – are active in GCMs and behave qualitatively in agreement with physical process understanding. However, the modeled entrainment enhancement has a negligible global-mean effect. This raises the question of whether the GCM estimate is incorrect due to parametric or base-state representation errors or whether the process understanding gleaned from a limited set of canonical cloud cases is insufficiently representative of the diversity of clouds in the real climate. Regardless, even at limited resolution, the GCM physics appears able to parameterize the small-scale microphysics–turbulence interplay responsible for the entrainment enhancement mechanism. We suggest ways to resolve tension between current and future (storm-resolving) global modeling systems and other lines of evidence in synthesis climate projections.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

The role of local shipping emissions in aerosol-cloud interactions in the central Arctic

Arctic shipping is projected to increase as sea ice retreats, yet the impact of modern low-sulfur ship emissions on Arctic clouds and radiation remain poorly constrained. We use year-long in situ observations from the MOSAiC expedition to characterize ship-aerosol-cloud interactions for an icebreaker burning ultra-low sulfur fuel (0.1% mass per mass). Exhaust plumes were found to be strongly enriched in Aitken-mode particles, organic aerosol, and black carbon, but showed no detectable enhancement in particulate sulfate. Despite reduced hygroscopicity relative to ambient aerosols, ship emissions substantially increased local cloud condensation nuclei concentrations. A droplet activation parameterization was applied to quantify responses in cloud droplet number concentration ( N d ) to ship-induced perturbations in low-level Arctic clouds. In winter, abundant background accumulation-mode particles from Arctic haze supplied nearly all cloud droplets, while additional particles from ship emissions had little impact on N d . In contrast, during summer months, when unperturbed background aerosol concentrations are low, ship emissions nearly doubled N d compared to average background conditions and increased N d by a factor of five compared to very clean background conditions (25th percentile of background aerosol number concentrations). Longwave radiative transfer simulations for typical conditions of summer Arctic low-level clouds/fog suggest that these ship-induced increases in N d locally (i.e. <100 km downwind) lead to enhanced net surface longwave fluxes and consequent warming, primarily for optically thin clouds (liquid water path (LWP) ⩽ 30 g·m −2 ). For LWP = 10 g · m −2 , ship emissions lead to an increase of 1 W · m −2 in cloud longwave forcing at the surface compared to average unperturbed conditions (+7% relative increase), and up to 4 W · m −2 when compared to very clean background conditions (+22% relative increase). Even ultra-low sulfur fuel emissions can therefore locally and episodically modify Arctic cloud microphysics and radiative properties, especially during summer, implying that future increases in Arctic shipping could have non-negligible regional climate impacts.

Arctic↗