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All sourcesNASA NTRSDOE OSTI
NASA NTRS2004

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-resolving Model Simulations

Cloud microphysics is inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, r d a U production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembe1 (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e. pristine ice crystals (columnar and platelike), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions. A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region and in the mid-latitude continent with different concentrations of CCN: a low "c1ean"concentration and a high "dirty" concentration. In addition, differences and similarities between bulk microphysics and spectral-bin microphysical schemes will be examined and discussed.

Tao, Wei-Kuo↗
NASA NTRS2004

Characterization of Individual Aerosol Particles Associated with Clouds (CRYSTAL-FACE)

The aim of our research was to obtain data on the chemical and physical properties of individual aerosol particles from near the bottoms and tops of the deep convective systems that lead to the generation of tropical cirrus clouds and to provide insights into the particles that serve as CCN or IN. We used analytical transmission electron microscopy (ATEM), including energy-dispersive X-ray spectrometry (EDS) and electron energy-loss spectroscopy (EELS), and field-emission electron microscopy (FESEM) to compare the compositions, concentrations, size distributions, shapes, surface coatings, and degrees of aggregation of individual particles from cloud bases and the anvils near the tropopause. Aggregates of sea salt and mineral dust, ammonium sulfate, and soot particles are abundant in in-cloud samples. Cirrus samples contain many H2SO4 droplets, but acidic sulfate particles are rare at the cloud bases. H2SO4 probably formed at higher altitudes through oxidation of SO2 in cloud droplets. The relatively high extent of ammoniation in the upper troposphere in-cloud samples appears to have resulted from vertical transport by strong convection. The morphology of H2SO4 droplets indicates that they had been at least yartiy ammoniated at the time of collection. They are internally mixed with organic materials, metal sulfates, and solid particles of various compositions. Ammoniation and internal mixing of result in freezing at higher temperature than in pure H2SO4 aerosols. K- and S-bearing organic particles and Si-Al-rich particles are common throughout. Sea salt and mineral dust were incorporated into the convective systems from the cloud bases and worked as ice nuclei while being vertically transported. The nonsulfate particles originated from the lower troposphere and were transported to the upper troposphere and lower stratosphere.

Buseck, Peter R.↗
NASA NTRS1999

Role of Dynamic Nucleation at Moving Boundaries in Phase and Microstructure Selection

Solidification microstructures that form under steady-state growth conditions (cells, dendrites, regular eutectics, etc.) are reasonably well understood in comparison to other, more complex microstructures, which form under intrinsically non-steady-state growth conditions due to the competition between the nucleation and growth of several phases. Some important practical examples in this latter class include microstructures forming in peritectic systems in highly undercooled droplets, and in strip cast stainless steels. Prediction of phase and microstructure selection in these systems has been traditionally based on (1) heterogeneous nucleation on a static interface, and (2) comparing the relative growth rate of different phase/microstructures under steady-state growth conditions. The formation of new phases, however, occurs via nucleation on, or ahead of, a moving boundary. In addition, the actual selection process is controlled by a complex interaction between the nucleation process and the growth competition between the nuclei and the pre-existing phase under non-steady-state conditions. As a result, it is often difficult to predict which microstructure will form and which phases will be selected under prescribed processing conditions. This research addresses this critical role of nucleation at moving boundaries in the selection of phases and solidification microstructures through quantitative experiments and numerical modeling in peritectic systems. In order to create a well characterized system in which to study this problem, we focus on the directional solidification of hypo- and hyper-peritectic alloys in the two-phase region, imposing a large enough ratio of temperature gradient/growth rate (G/V(sub p)) to suppress the morphological instability of both the parent (alpha) and peritectic (Beta) phases, i.e. each phase alone would grow as a planar front. Our combined experimental and theoretical results show that, already in this simplified case, the growth competition of these two phases leads to a rich variety of microstructures that depend sensitively upon the relative importance of nucleation, diffusion, and convection.

Karma, Alain↗
DOE OSTI2024

Cloud Processing of Aerosol during SAIL Field Campaign Report

Globally, on average, the release rate of aerosols from clouds is estimated to be about 6,000 Tg/yr and an aerosol particle is estimated to experience about three cloud cycles. Cloud processing of aerosol produces aerosols that have dramatically different physicochemical properties compared to their original form. Cloud processing may transform particles to efficient cloud condensation nuclei (CCN) or ice nucleating particles (INP) that can further participate in cloud formation. We investigated cloud processing of aerosol during the U.S. Department of Energy (DOE)’s Atmospheric Radiation Measurement (ARM) Surface Atmosphere Integrated Field Laboratory (SAIL) field campaign using multi-modal offline analysis techniques available at DOE’s Environmental Molecular Sciences Laboratory (EMSL). The main scientific aim of this project was to understand the processes that transform aerosols (chemically, and physically), and influence aerosol-cloud interactions. Aerosol particles undergo significant modifications due to warm (cloud droplets) and cold cloud (ice crystals) processing. Cloud processing of aerosol has important effects on the atmospheric aerosol number and mass concentration, size distribution, phase separation, and chemical composition.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1981

The formation and growth of sulfate aerosols in the stratosphere

The critical compositions, critical radii, and nucleation rates of sulfuric acid droplets formed through homogeneous heteromolecular nucleation process in the stratosphere under a variety of ambient conditions are calculated. Results are plotted as a function of H2SO4 concentration and H2O concentration so that characteristics of sulfate aerosols can be quickly estimated whenever environmental conditions are known. The effect of the uncertainty in the saturated vapor pressure of H2SO4 on the estimated properties of sulfate aerosols is elucidated. Plottings are presented that illustrate the relative importance of new particle formation by homogeneous nucleation vs growth by heteromolecular condensation on pre-existing nuclei in the stratosphere. The effects of ambient conditions, such as the concentrations of H2SO4 and H2O, the average stratospheric particle radius, and the number concentration of pre-existing nuclei on the relative importance of these two competing processes are discussed.

Yue, G. K.↗
DOE OSTI2026

Final report: Insights from ARM observations into aerosol processing and transport by extratropical cyclones and aerosol effects on cyclone clouds

This project advanced understanding of aerosol–cloud interactions in extratropical cyclones using observations from the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) observatory and ACE-ENA field campaigns, along with satellite datasets and numerical modeling. We have quantified the susceptibility of frontal clouds to aerosols, showing that this susceptibility is similar to that in non-frontal clouds despite substantial (factor 2) differences in droplet concentrations between these cloud types, and also significant differences in cloud albedo. A key finding was that Aitken-mode (here, 60-100nm diameter) aerosols play a disproportionately important role in droplet activation in frontal clouds, and concentrations of these particles are frequently strongly biased in climate models. Activation of aerosols depends strongly on updraft speeds, and via collaboration with Argonne National Laboratory we contributed to quantifying these better with the ARM radar wind profiler at the ENA site. Our studies in the North Atlantic have analogs in the Southern Ocean, and to draw these out we examined data from the MARCUS and SOCRATES field campaigns. We identified new particle formation within extratropical cyclones as a potentially important source of cloud condensation nuclei in these pristine marine environments. By combining ARM observations with perturbed parameter ensemble simulations, we demonstrated that surface observations can effectively constrain aerosol–cloud adjustments and reduce uncertainty in simulated cloud liquid water path responses by approximately 15%, yielding stronger constraints on historical aerosol cooling effects. The work further established precipitation processes as a dominant control on aerosol–cloud interactions and Earth system predictability.

Gordon, Hamish [Department of Chemical Engineering↗
NASA NTRS2003

Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols

NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.

Ackerman, A.↗
DOE OSTI2020

Constraining the Twomey effect from satellite observations: issues and perspectives

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

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1994

Microphysical modeling of cirrus. 2: Sensitivity studies

The one-dimensional cirrus model described in part 1 of this issue has been used to study the sensitivity of simulated cirrus microphysical and radiative properties to poorly known model parameters, poorly understood physical processes, and environmental conditions. Model parameters and physical processes investigated include nucleation rate, mode of nucleation (e.g., homogeneous freezing of aerosols and liquid droplets or heterogeneous deposition), ice crystal shape, and coagulation. These studies suggest that the leading sources of uncertainty in the model are the phase change (liquid-solid) energy barrier and the ice-water surface energy which dominate the homogeneous freezing nucleation rate and the coagulation sticking efficiency at low temperatures which controls the production of large ice crystals (radii greater than 100 mcirons). Environmental conditions considered in sensitivity tests were CN size distribution, vertical wind speed, and cloud height. We found that (unlike stratus clouds) variations in the total number of condensation nuclei (NC) have little effect on cirrus microphysical and radiative properties, since nucleation occurs only on the largest CN at the tail of the size distribution. The total number of ice crystals which nucleate has little or no relationship to the number of CN present and depends primarily on the temperature and the cooling rate. Stronger updrafts (more rapid cooling) generate higher ice number densities, ice water content, cloud optical depth, and net radiative forcing. Increasing the height of the clouds in the model leads to an increase in ice number density, a decrease in effective radius, and a decrease in ice water content. The most prominent effect of increasing cloud height was a rapid increase in the net cloud radiative forcing which can be attributed to the change in cloud temperature as well as change in cloud ice size distributions. It has long been recognized that changes in cloud height or cloud area have the greatest potential for causing feedbacks on climate change. Our results suggest that variations in vertical velocity or cloud microphysical changes associatd with cloud height changes may also be important.

Jensen, Eric J.↗
NASA NTRS2020

Constraining the Twomey effect from satellite observations: Issues and perspectives

The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (ΔNd,ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol–cloud interactions which also comprises rapid adjustments. These adjustments are essentially the responses of cloud fraction and liquid water path to ΔNd,ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large scale (hundreds of kilometres) ΔNd,ant remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and vertical wind and by droplet sink processes. These operate at scales on the order of 10s of metres at which only localized observations are available and at which no approach exists yet to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are three key uncertainties in determining ΔNd,ant, namely the quantification (i) of the cloud-active aerosol – the cloud condensation nuclei concentrations (CCN) at or above cloud base –, (ii) of Nd, as well as (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data. A fourth uncertainty, the anthropogenic perturbation to CCN concentrations, is also not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: In terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, the non-direct relation to the concentration of aerosols, the impossibility to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilizing colocated polarimeter and lidar instruments, ideally including high spectral resolution lidar capability at two wavelengths to maximize vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity, and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd – to – CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect.

Twomey effect↗
NASA NTRS2016

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200-300 over the next 50-100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were 50 smaller than in background clouds. Based on the relationship between cloud droplet number (N(liq))/ and various biomass burning tracers (BBt/ across the multi-campaign dataset, we calculated the magnitude of subarctic and Arctic smoke aerosol-cloud interactions (ACI, where ACI = (1/3) x dln(N(liq))/dln(BBt)) to be 0.12 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (0.02 gm/ cu m) and very high aerosol concentrations (2000-3000 cu m) in the most polluted clouds, the estimated ACI value was only 0.06. In this case, competition for water vapor by the high concentration of CCN strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease shortwave radiative flux by 2 and 4 W/sq or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic. We lastly show evidence to suggest that numerous northern latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei. However, the influence of background particles on smoke-driven indirect effects is currently unclear.

Arctic↗
DOE OSTI2021

Southern Ocean Cloud Properties Derived From CAPRICORN and MARCUS Data

The properties of Southern Ocean (SO) liquid phase non precipitating clouds (hereafter clouds) are examined using shipborne data collected during the Measurements of Aerosols, Radiation and Clouds over the Southern Ocean and the Clouds Aerosols Precipitation Radiation and atmospheric Composition Over the SoutheRN ocean I and II campaigns that took place south of Australia during Autumn 2016 and Summer 2017–2018. Cloud properties are derived using data from W-band radars, lidars, and microwave radiometers using an optimal estimation algorithm. The SO clouds tended to have larger liquid water paths (LWP, 115 ± 117 g m -2 ), smaller effective radii (re, 8.7 ± 3 μm), and higher number concentrations (N d , 90 ± 107 cm-3) than typical values of eastern ocean basin stratocumulus. The clouds demonstrated a tendency for the LWP to increase with Nd presumably due to precipitation suppression up to Nd of approximately 100 cm -3 when mean LWP decreased with increasing Nd. Due to higher optical depth, cloud albedos were less susceptible to changes in Nd compared to subtropical stratocumulus. The highest latitude clouds of the datasets, observed along and near the Antarctic coast, presented a distinctly bimodal character. One mode had the properties of marine clouds further north. Additionally, the other mode occurred in an aerosol environment characterized by high cloud condensation nuclei concentrations and elevated sulfate aerosol without obvious continental aerosol markers. These regions of higher cloud condensation nuclei tended to have higher Nd, smaller re and higher LWP suggesting sensitivity of cloud properties to seasonal biogenic aerosol production in the high latitude SO.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Above-cloud concentrations of cloud condensation nuclei help to sustain some Arctic low-level clouds

Abstract. Previous studies have found that low-level Arctic clouds often persist for long periods even in the face of very low surface cloud condensation nuclei (CCN) concentrations. Here, we investigate whether these conditions could occur due to continuous entrainment of aerosol particles from the free troposphere (FT). We use an idealized large eddy simulation (LES) modeling framework, where aerosol concentrations are low in the boundary layer (BL) but increased up to 50× in the free troposphere. We find that the tests with higher tropospheric aerosol concentrations simulated clouds, which persisted for longer and maintained higher liquid water paths (LWPs). This is due to direct entrainment of the tropospheric aerosol into the cloud layer, which results in a precipitation suppression from the increase in cloud droplet number and in stronger cloud-top radiative cooling, which causes stronger circulations maintaining the cloud in the absence of surface forcing. Together, these two responses result in a more well-mixed boundary layer with a top that remains in contact with the tropospheric aerosol reservoir and can maintain entrainment of those aerosol particles. The surface aerosol concentrations, however, remained low in all simulations. The free-tropospheric aerosol concentration necessary to maintain the clouds is consistent with concentrations that are frequently seen in observations.

Environmental Sciences & Ecology↗
DOE OSTI2025

Aerosol Microphysics and Chemical Measurements at Mt. Soledad and Scripps Pier during the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) from February 2023 to February 2024 UCSD Library Collection

This dataset includes guest instrument measurements and other PI products for aerosol microphysics and chemical measurements collected at Mt. Soledad and Scripps Pier during the Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) from February 2023 to February 2024. The measurements include the following instruments at Mt. Soledad: High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS, Aerodyne), Scanning Electrical Mobility Spectrometer (SEMS, Brechtel Manufacturing Inc.), Aerodynamic Particle Sizer (APS, Droplet Measurements Technologies), Single Particle Soot Photometer (SP2, Drople Measurements Technologies), Meteorological Station (WXT520, Vaisala), Ozone (Teco), and trace gas proxies (Teledyne). In addition, the analyses of particle filters collected at Mt. Soledad for three dry-diameter size cuts (<1 micron, <0.5 micron, <0.18 micron) and at Scripps Pier for one dry-diameter size cut (<1 micron) by Fourier Transform Infrared (FTIR) and X-ray Fluorescence (XRF) are reported. A differential mobility analyzer operated as a scanning mobility particle sizer (SMPS, TSI Inc.), a printed particle optical spectrometer (POPS, Grimm), and a continuous flow diffusion cloud condensation nuclei (CCN, DMT) counter provide the mobility aerosol size distribution (30-360 nm), optical size distribution (150 - 6000 nm), size-resolved CCN distribution (30-360 nm) at 0.2, 0.4, 0.6, 0.8, and 1.0% supersaturation. Measurements are reported for both sampling from an isokinetic aerosol inlet and from a Counterflow Virtual Impactor (CVI, Brechtel Manufacturing Inc.). The data are available at the following link: https://library.ucsd.edu/dc/collection/bb0898306q

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Maritime Aerosol and CCN Profiles Derived From Ship₋Based Measurements Over Eastern North Pacific During MAGIC

Atmospheric aerosols are widely recognized to give rise to a substantial radiative forcing to the climate by scattering and absorbing radiation and by modifying the microphysical, lifetime, and radiative properties of clouds. During the Marine ARM GPCI Investigation of Clouds (MAGIC) over the Eastern North Pacific (ENP), the ship-based measured cloud condensation nuclei (CCN) concentration at 0.2% supersaturation (N CCN,0.2 ) and condensation nuclei concentration (N CN ) had mean values of 116.7 and 219.4 cm ⁻3 , with the highest concentrations found closest to LA due to an increase in aerosol sources. Moving westward, both N CCN,0.2 and N CN gradually decreased until stabilizing near 100 cm ⁻3 and 200 cm ⁻3 , respectively. Using the methods proposed by Ghan and Collins (2004), https://doi.org/10.1175/1520-0426(2004)021<0387:uoisdt>2.0.co;2 and Ghan et al. (2006), https://doi.org/10.1029/2004jd005752, N CCN,0.2 profiles are retrieved using the surface measured N CCN,0.2 as a constraint. For coupled conditions, correlations between the retrieved N CCN,0.2 profiles and cloud-droplet number concentration (N C ) increase from 0.26 at the surface to 0.38 near cloud base, particularly true for non-drizzling clouds. Although the correlations are lower than expected, the percentage increase (46.2%) is encouraging. Finally, the relationships between cloud breakup (CB) and the stratocumulus to cumulus transition (SCT) with environmental conditions and associated aerosols are also studied. The decreased N CN trend east of CB is mainly caused by precipitation scavenging, while the increased N CN trend west of CB is strongly associated with the increased surface wind speed and fewer drizzle events. A further study is needed using high-resolution models to simulate these events.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2021

Preconditioning of overcast-to-broken cloud transitions by riming in marine cold air outbreaks

Marine cold air outbreaks (CAOs) commonly form overcast cloud decks that transition into broken cloud fields downwind, dramatically altering the local radiation budget. In this study, we investigate the impact of frozen hydrometeors on these transitions. We focus on a CAO case in the NW Atlantic, the location of the multi-year flight campaign ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment). We use MERRA-2 (Modern-Era Retrospective analysis for Research and Applications, version 2) reanalysis fields to drive large eddy simulations with mixed-phase two-moment microphysics in a Lagrangian framework. We find that transitions are triggered by substantial rain (rainwater paths >25 g m−2), and only simulations that allow for aerosol depletion result in sustained breakups, as observed. Using a range of diagnostic ice nucleating particle concentrations, Ninp, we find that increasing ice progressively accelerates transitions, thus abbreviating the overcast state. Ice particles affect the cloud-topped boundary layer evolution, primarily through riming-related processes prior to substantial rain, leading to (1) a reduction in cloud liquid water, (2) early consumption of cloud condensation nuclei, and (3) early and light precipitation cooling and moistening below cloud. We refer to these three effects collectively as “preconditioning by riming”. Greater boundary layer aerosol concentrations available as cloud condensation nuclei (CCN) delay the onset of substantial rain. However, cloud breakup and low CCN concentration final stages are found to be inevitable in this case, due, primarily, to liquid water path buildup. An ice-modulated cloud transition speed suggests the possibility of a negative cloud–climate feedback. To address prevailing uncertainties in the model representation of mixed-phase processes, the magnitude of ice formation and riming impacts and, thereby, the strength of an associated negative cloud–climate feedback process, requires further observational evaluation by targeting riming hot spots with in situ imaging probes that allow for both the characterization of ice particles and abundance of supercooled droplets.

Marine cold air outbreaks↗
DOE OSTI2025

Aircraft in-situ measurements from SOCRATES constrain the anthropogenic perturbations of cloud droplet number

Aerosol-cloud interactions (ACI) in warm clouds alter reflected shortwave radiation by influencing cloud microphysical and macrophysical properties. The variable of state controlling ACI is the cloud droplet number concentration (N d ). Here, we examine the perturbations in N d due to anthropogenic aerosols (ΔN d, PD-PI ) using a perturbed parameter ensemble (PPE) hosted in the sixth Community Atmosphere Model (CAM6). Surrogate models are created for the CAM6 PPE outputs and are used to generate 1 million model variants of CAM6 by sampling 45 sources of parameter uncertainty. The range of uncertain physical parameters related to ACI are constrained with observations of aerosol and cloud properties from SOCRATES. The likely range of uncertain parameters and the associated range of ΔN d, PD-PI are more strongly constrained with observations of N d relative to observations of cloud condensation nuclei. We conduct sensitivity tests of how constraints on ΔN d, PD-PI are affected by systematic uncertainties in observations and our limitations in our surrogate models created for CAM6 PPE outputs. Based on this, we provide guidance on the impact of reducing systematic uncertainty in airborne microphysical observations and in surrogate models.

Song, Ci [Univ. of Wyoming, Laramie, WY (United St↗
DOE OSTI2020

Reducing uncertainties in satellite estimates of aerosol–cloud interactions over the subtropical ocean by integrating vertically resolved aerosol observations

Satellite quantification of aerosol effects on clouds relies on aerosol optical depth (AOD) as a proxy for aerosol concentration or cloud condensation nuclei (CCN). However, the lack of error characterization of satellite-based results hampers their use for the evaluation and improvement of global climate models. We show that the use of AOD for assessing aerosol–cloud interactions (ACIs) is inadequate over vast oceanic areas in the subtropics. Instead, we postulate that a more physical approach that consists of matching vertically resolved aerosol data from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite at the cloud-layer height with Moderate Resolution Imaging Spectroradiometer (MODIS) Aqua cloud retrievals reduces uncertainties in satellite-based ACI estimates. Combined aerosol extinction coefficients (σ) below cloud top (σBC) from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and cloud droplet number concentrations (N d ) from MODIS Aqua yield high correlations across a broad range of σBC values, with σBC quartile correlations ≥0.78. In contrast, CALIOP-based AOD yields correlations with MODIS Nd of 0.54–0.62 for the two lower AOD quartiles. Moreover, σBC explains 41% of the spatial variance in MODIS N d , whereas AOD only explains 17%, primarily caused by the lack of spatial covariability in the eastern Pacific. Compared with σBC, near-surface σ weakly correlates in space with MODIS N d , accounting for a 16% variance. It is concluded that the linear regression calculated from ln(N d )–ln(σBC) (the standard method for quantifying ACIs) is more physically meaningful than that derived from the Nd–AOD pair.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗