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DOE OSTI2024

General circulation models simulate negative liquid water path–droplet number correlations, but anthropogenic aerosols still increase simulated liquid water path

General circulation models' (GCMs) estimates of the liquid water path adjustment to anthropogenic aerosol emissions differ in sign from other lines of evidence. This reduces confidence in estimates of the effective radiative forcing of the climate by aerosol–cloud interactions (ERFaci). The discrepancy is thought to stem in part from GCMs' inability to represent the turbulence–microphysics interactions in cloud-top entrainment, a mechanism that leads to a reduction in liquid water in response to an anthropogenic increase in aerosols. In the real atmosphere, enhanced cloud-top entrainment is thought to be the dominant adjustment mechanism for liquid water path, weakening the overall ERFaci. We show that the latest generation of GCMs includes models that produce a negative correlation between the present-day cloud droplet number and liquid water path, a key piece of observational evidence supporting liquid water path reduction by anthropogenic aerosols and one that earlier-generation GCMs could not reproduce. However, even in GCMs with this negative correlation, the increase in anthropogenic aerosols from preindustrial to present-day values still leads to an increase in the simulated liquid water path due to the parameterized precipitation suppression mechanism. This adds to the evidence that correlations in the present-day climate are not necessarily causal. We investigate sources of confounding to explain the noncausal correlation between liquid water path and droplet number. These results are a reminder that assessments of climate parameters based on multiple lines of evidence must carefully consider the complementary strengths of different lines when the lines disagree.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Magnitude and timescale of liquid water path adjustments to cloud droplet number concentration perturbations for nocturnal non-precipitating marine stratocumulus

Cloud liquid water path (L) adjusts to perturbations in cloud droplet number concentration (N) over time. We explore the magnitude and timescale of this adjustment in nocturnal non-precipitating marine stratocumuli using large eddy simulations of baseline conditions and aerosol seeding experiments for 22 meteorological conditions. The results confirm that the L adjustment (δL) slope (k) is more negative for simulation pairs with relatively low N and less negative for high N. Overall, k is unlikely to be lower than −0.4 within 24 h of seeding start, meaning the L adjustment is unlikely to fully offset the brightening due to the Twomey effect. After seeding, the δL becomes increasingly negative, which can be characterized by an exponential convergence. This evolution is governed by a short timescale around 5 h and lasts for around 8–12 h. It is driven by the feedback between entrainment, L, and boundary layer (BL) turbulence. Other processes, including radiation, surface fluxes, and subsidence, respond to the seeding weakly. This short timescale is insensitive to the amount of seeding, making the evolution of δL and some other deviations similar for different seeding amounts after appropriate scaling. The timescale of k evolution is closely related to the δL timescale and hence also short, while it could also be affected by the δN evolution. The results are most relevant to conditions where seeding is applied to a large area of marine stratocumulus in well-mixed and overcast BL where shear is not a primary source of turbulence.

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 OSTI2021

Graupel Precipitating From Thin Arctic Clouds With Liquid Water Paths Less Than 50 g m -2

Rimed precipitation growth can efficiently remove moisture and aerosols from the boundary layer, yet thin low-level Arctic mixed-phase clouds are generally thought to precipitate pristine and aggregated ice crystals. Here we present automated surface photographic measurements showing that only 34% of precipitation particles exhibit negligible riming and that graupel particles ≥ in diameter commonly fall from clouds with liquid water paths less than 50 g m -2 . Analyses indicate that significant riming enhancement can occur provided sustained updrafts of 0.4 m s -1 , consistent with those measured in Arctic clouds. A Lagrangian numerical simulation that tracks falling particles suggests that similar updraft speeds can account for about one half of the observed riming enhancement. Riming enhancement appears particularly likely when weak temperature inversions are observed at cloud top, but a full explanation remains to be determined.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Atmospheric temperature, water vapour and liquid water path from two microwave radiometers during MOSAiC

The microwave radiometers HATPRO (Humidity and Temperature Profiler) and MiRAC-P (Microwave Radiometer for Arctic Clouds - Passive) continuously measured radiation emitted from the atmosphere throughout the Multidisciplinary drifting Observatory for the Study of the Arctic Climate (MOSAiC) expedition on board the research vessel Polarstern. From the measured brightness temperatures, we have retrieved atmospheric variables using statistical methods in a temporal resolution of 1 s covering October 2019 to October 2020. The integrated water vapour (IWV) is derived individually from both radiometers. In addition, we present the liquid water path (LWP), temperature and absolute humidity profiles from HATPRO. To prove the quality and to estimate uncertainty, the data sets are compared to radiosonde measurements from Polarstern. The comparison shows an extremely good agreement for IWV, with standard deviations of 0.08–0.19 kg m -2 (0.39–1.47 kg m -2 ) in dry (moist) situations. The derived profiles of temperature and humidity denote uncertainties of 0.7–1.8 K and 0.6–0.45 gm -3 in 0–2 km altitude.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Atmospheric temperature, water vapour and liquid water path from two microwave radiometers during MOSAiC

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54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Coastal-Fog Microphysics Using In-Situ Observations and GOES-R Retrievals

Here, the objective of this work is to evaluate GOES-R based fog conditions occurred during the C-FOG (Toward Improving Coastal Fog Prediction) field campaign. C-FOG is designed to advance understanding of fog formation, development, and dissipation over coastal environments to improve its predictability. The project took place along coastlines and open water environments of Eastern Canada (Nova Scotia, NS and the Island of Newfoundland, NL) during August-October of 2018 where environmental conditions play an important role for late season’s fog formation. During the C-FOG field campaign, instruments were located at the Ferryland Supersite, NL, with 2 main sites, and five satellite sites, as well as on the Research Vessel (R/V) Hugh R. Sharp. Key measurement instruments included a Gondola carrying a CDP (cloud droplet probe) and a BCP (backscatter cloud probe) was used for measuring droplet spectra from 1-75 µm on the R/V. A LPM (laser precipitation monitor) with 100 µm-1 cm size range and an OPC (optical particle counter) with 0.3-17 µm at 16 spectral channels provided information for fog and drizzle discrimination. Remote sensing platforms (e.g. profiling microwave radiometer, PMWR), Ceilometer, Lidar), meteorological towers, tethered balloons, and GOES-R products (e.g. fog coverage and droplet size and liquid water path) were used to evaluate fog over horizontal and vertical dimensions. Results suggest that effective radius, phase, liquid water path, and liquid water content values obtained from GOES-R and PMWR were comparable to ground based in-situ observations. It is concluded that integration of observations and nowcasting products may help improve short term local fog predictions.

54 ENVIRONMENTAL SCIENCES↗

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 OSTI2023

Evaluating EAMv2 Simulated High Latitude Clouds Using ARM Measurements in the Northern and Southern Hemispheres

Here, this study evaluates high latitude stratiform mixed-phase clouds (SMPC) in the atmosphere model of the Energy Exascale Earth System Model version 2 (EAMv2) by utilizing one-year-long ground-based remote sensing measurements from the Atmospheric Radiation and Measurement (ARM) program. A nudging approach is applied to model simulations for a constrained comparison with the ARM observations. Observed and modeled SMPCs are sampled and collocated to address the difference in data resolution, so that we can consistently evaluate their macrophysical properties at the North Slope of Alaska (NSA) site in the Arctic and the McMurdo (AWR) site in the Antarctic. We found that EAMv2 overestimates SMPC frequency of occurrence at both sites. However, the model captures the observed larger cloud frequency of occurrence at the NSA site. For collocated SMPCs, the annual statistics of observed cloud macrophysics are generally reproduced at the NSA site, while at the AWR site, there are larger biases. Compared to the AWR site, the lower cloud top and cloud base and the warmer cloud top temperature observed at NSA are well simulated. On the other hand, simulated cloud phase is substantially biased. The model largely overestimates liquid water path, and the ice water path is underestimated at NSA, but at AWR, the liquid water path is frequently underestimated due to the dominance of snow in Antarctic SMPCs. As a result, the observed hemispheric difference in cloud phase partitioning is misrepresented in EAMv2. This study implies that additional model development is needed for high latitude mixed-phase clouds.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Surface radiation trends at North Slope of Alaska influenced by large-scale circulation and atmospheric rivers

Arctic amplification manifests as a pervasive warming trend emerging over the past century in near-surface air temperature throughout the Arctic that is double the globally averaged temperature increase throughout most of the year. It results from complex processes involving oceanic, atmospheric and terrestrial components which require detailed study to discern roles of the fundamental processes involved to improve predictions of the Arctic environment. We report on signals that are beginning to emerge, on a timescale predicted by recent satellite remote sensing studies, from the unique 25 year record of detailed surface-based radiometer measurements obtained by the US Department of Energy Atmospheric Radiation Measurement (ARM) Facility North Slope of Alaska (NSA) site at Utqiaġvik, Alaska. Statistically significant warming trends are found at the site in the boreal fall, while a decrease in net radiation occurs in late summer. This decrease is driven primarily by the decrease in shortwave radiation resulting from increasing cloud liquid water path as observed by the microwave radiometer. The magnitude of the liquid water path trends is slightly larger than the root mean square error (RMSE) due to natural variability, while the magnitude of the net radiation trends is smaller than the RMSE natural variability, emphasizing that these signals are only just emerging. Analysis of prevailing meteorological regimes linking NSA with the Arctic Ocean and subarctic latitudes, and atmospheric rivers, suggests that specific changing circulation patterns are the primary driver for these summertime trends.

Lubin, Dan [Univ. of California, San Diego, CA (Un↗

DOE OSTI2021

Large-Eddy Simulations of Marine Boundary Layer Clouds Associated with Cold-Air Outbreaks during the ACTIVATE Campaign. Part I: Case Setup and Sensitivities to Large-Scale Forcings

Large-eddy simulation (LES) is able to capture key boundary layer (BL) turbulence and cloud processes. Yet, large-scale forcing and surface turbulent fluxes of sensible and latent heat are often poorly prescribed for LESs. We derive these quantities from measurements and reanalysis obtained for two cold-air outbreak (CAO) events during Phase I of the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE) in February–March 2020. We study the two contrasting CAO cases by performing LES and test the sensitivity of BL structure and clouds to large-scale forcings and turbulent heat fluxes. Profiles of atmospheric state and large-scale divergence and surface turbulent heat fluxes obtained from ERA5 data agree reasonably well with those derived from ACTIVATE field measurements for both cases at the sampling time and location. Therefore, we adopt the time-evolving heat fluxes, wind, and advective tendencies profiles from ERA5 data to drive the LES. We find that large-scale thermodynamic advective tendencies and wind relaxations are important for the LES to capture the evolving observed BL meteorological states characterized by the hourly ERA5 data and validated by the observations. We show that the divergence (or vertical velocity) is important in regulating the BL growth driven by surface heat fluxes in LESs. The evolution of liquid water path is largely affected by the evolution of surface heat fluxes. The liquid water path simulated in LES agrees reasonably well with the ACTIVATE measurements. This study paves the path to investigate aerosol–cloud–meteorology interactions using LES informed and evaluated by ACTIVATE field measurements.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

On the Role of Macrophysics and Microphysics in Km-Scale Simulations of Mixed-Phase Clouds During Cold Air Outbreaks

Regional atmospheric models struggle to maintain supercooled liquid in mixed-phase clouds during polar cold-air outbreaks (CAOs). Previous studies focused on the parameterization of aerosol, microphysics and turbulence to understand the origin of this widespread model bias. This study investigates the role of sub-grid cloud fraction parameterizations (CFP) in the simulation of mixed-phase cloud. Km-scale simulations are performed for a large number of CAO cases over Norway, for which continuous ground observations were collected at one site over 6 months. We use a novel analysis that attributes the cloud-radiative errors to deficiencies in specific cloud regimes. We show that the CFP matters for cloud-radiative effects in CAOs, but that it is probably not the primary cause of the lack of liquid water in simulated mixed-phase clouds. Of all the CFP sensitivities explored in this study, the prognostic representation of both liquid and ice shows most promise in increasing the liquid water path. A newly proposed hybrid CFP with prognostic frozen and diagnostic liquid cloud fraction reproduces some of the benefits of the prognostic scheme at reduced cost and complexity. All simulations appear to produce too large precipitation particles. As a result, reducing the snow deposition rate increases the liquid water path and improves the precipitation size distributions, while simulations are less sensitive to reduced riming rates.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Evaluating cloud liquid detection against Cloudnet using cloud radar Doppler spectra in a pre-trained artificial neural network

Detection of liquid-containing cloud layers in thick mixed-phase clouds or multi-layer cloud situations from ground-based remote-sensing instruments still poses observational challenges, yet improvements are crucial since the existence of multi-layer liquid layers in mixed-phase cloud situations influences cloud radiative effects, cloud lifetime, and precipitation formation processes. Hydrometeor target classifications such as from Cloudnet that require a lidar signal for the classification of liquid are limited to the maximum height of lidar signal penetration and thus often lead to underestimations of liquid-containing cloud layers. Here we evaluate the Cloudnet liquid detection against the approach of Luke et al. (2010) which extracts morphological features in cloud-penetrating cloud radar Doppler spectra measurements in an artificial neural network (ANN) approach to classify liquid beyond full lidar signal attenuation based on the simulation of the two lidar parameters particle backscatter coefficient and particle depolarization ratio. We show that the ANN of Luke et al. (2010) which was trained under Arctic conditions can successfully be applied to observations at the mid-latitudes obtained during the 7-week-long ACCEPT field experiment in Cabauw, the Netherlands, in 2014. In a sensitivity study covering the whole duration of the ACCEPT campaign, different liquid-detection thresholds for ANN-predicted lidar variables are applied and evaluated against the Cloudnet target classification. Independent validation of the liquid mask from the standard Cloudnet target classification against the ANN-based technique is realized by comparisons to observations of microwave radiometer liquid-water path, ceilometer liquid-layer base altitude, and radiosonde relative humidity. In addition, a case-study comparison against the cloud feature mask detected by the space-borne lidar aboard the CALIPSO satellite is presented. Three conclusions were drawn from the investigation. First, it was found that the threshold selection criteria of liquid-related lidar backscatter and depolarization alone control the liquid detection considerably. Second, all threshold values used in the ANN framework were found to outperform the Cloudnet target classification for deep or multi-layer cloud situations where the lidar signal is fully attenuated within low liquid layers and the cloud radar is able to detect the microphysical fingerprint of liquid in higher cloud layers. Third, if lidar data are available, Cloudnet is at least as good as the ANN. The times when Cloudnet outperforms the ANN in liquid detections are often associated with situations where cloud dynamics smear the imprint of cloud microphysics on the radar Doppler spectra.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Substantial Diel Changes of Cloud Adjustments to Aerosols in Ship‐Tracks

Clouds adjust their albedo, amount and liquid water path to anthropogenic aerosols, and produce a climate forcing. Such cloud adjustments are complex functions of both environmental conditions and interaction time. However, direct observations of temporal changes in cloud adjustments are limited. Here, we develop a method to show observational evidence of substantial diel changes in cloud adjustments within ship-tracks. Polluted clouds experiencing extended nighttime exposure exhibit higher increases in cloud fraction while liquid-water path adjustments follow a non-monotonic evolution. The higher cloud fraction increase persists through daytime. Such diel variations likely stem from diel changes in solar heating and background cloud precipitation, and are important because nighttime changes persist and affect solar radiation during the day. Accounting for diel variations produces a stronger aerosol forcing, by −0.1 ∼−0.4 W⁢m −2 . Our approach reveals how the temporal evolution of cloud adjustments can have important implications for aerosol-cloud interactions.

Yuan, Tianle [NASA Goddard Space Flight Center (GS↗

DOE OSTI2025

Multiscale ACI Satellite Database

The SATELLITE_EAGLES_PNNL NetCDF dataset contains a suite of satellite- and reanalysis-derived atmospheric and surface parameters on a regular latitude–longitude grid. The dataset includes core geophysical fields such as land fraction, aerosol optical depth at multiple wavelengths (465, 550, 667, and 865 nm), sea surface temperature, estimated inversion strength, and various thermodynamic and dynamic quantities (e.g., relative humidity, vertical velocity, boundary-layer height, and surface fluxes) from both MERRA and ERA reanalysis products, provided as daily-mean and instantaneous values. A major component of the dataset consists of MODIS-retrieved cloud microphysical properties, including cloud droplet number concentration, cloud effective radius, optical thickness, and liquid water path, provided for three compositing regimes (“All,” “Q06,” and “G18”). Corresponding cloud-top parameters—temperature, height, and pressure—along with total and domain-mean cloud fraction fields are also included. The file further integrates additional satellite data from AMSR-E (for cloud water, rain water, and surface precipitation retrievals) and CERES (for top-of-atmosphere radiative fluxes, cloud fractions, and albedo). This dataset is designed to evaluate aerosol–cloud interactions in warm clouds, emphasizing the use of MODIS for deriving cloud droplet number concentration and liquid water path statistics. The complementary satellite and reanalysis fields are co-located and time-matched to the same instantaneous MODIS observations, enabling consistent comparisons between cloud properties, aerosol loading, and large-scale meteorological conditions. The dataset is recently featured in Christensen et al. (2025), Machine Learning Reveals Strong Grid-Scale Dependence in the Satellite Nd–LWP Relationship, EGUsphere [preprint], https://doi.org/10.5194/egusphere-2025-3850, 2025.

Christensen, Matthew [Pacific Northwest National L↗

DOE OSTI2025

Multiscale ACI Satellite Database

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Effects of Wind Shear and Aerosol Conditions on the Organization of Precipitating Marine Stratocumulus Clouds

Here this study examines how wind shear affects precipitating marine stratocumulus clouds under different cloud droplet number concentrations (N d ). We performed a series of large eddy simulations (LES) of nocturnal marine stratocumulus clouds using Cloud Model 1 (CM1). The simulations show that N d is the dominant factor for cloud cellular organization in this cloud regime rather than wind shear. Low N d characterizes the open cellular structure with a high in-cloud liquid water path (LWP). When wind shear is increased, the cloud fraction tends to decrease along with LWP, suggesting the cloud top region is significantly influenced by the entrainment and mixing of dry air from the free troposphere. We also examine cold pools in open and closed cellular clouds. Open-cell clouds produce larger and deeper cold pools compared to closed-cell clouds. Interestingly, cold pools can exist without surface precipitation and are produced by evaporation of light precipitation (drizzle) below the cloud base with weak downdrafts. The evaporation of raindrops and drizzle play an important role in initiating new convection, particularly where colliding outflows occur downstream of the cloud. This secondary convection contributes to the development and maintenance of the cloud cellular organization and formation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Natural marine cloud brightening in the Southern Ocean

Abstract. The number of cloud droplets per unit volume (Nd) is a fundamentally important property of marine boundary layer (MBL) liquid clouds that, at constant liquid water path, exerts considerable controls on albedo. Past work has shown that regional Nd has a direct correlation to marine primary productivity (PP) because of the role of seasonally varying, biogenically derived precursor gases in modulating secondary aerosol properties. These linkages are thought to be observable over the high-latitude oceans, where strong seasonal variability in aerosol and meteorology covary in mostly pristine environments. Here, we examine Nd variability derived from 5 years of MODIS Level 2-derived cloud properties in a broad region of the summer eastern Southern Ocean and adjacent marginal seas. We demonstrate latitudinal, longitudinal and temporal gradients in Nd that are strongly correlated with the passage of air masses over high-PP waters that are mostly concentrated along the Antarctic Shelf poleward of 60∘ S. We find that the albedo of MBL clouds in the latitudes south of 60∘ S is significantly higher than similar liquid water path (LWP) clouds north of this latitude.

54 ENVIRONMENTAL SCIENCES↗