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DOE OSTI2022

Environmental effects on aerosol–cloud interaction in non-precipitating marine boundary layer (MBL) clouds over the eastern North Atlantic

Abstract. Over the eastern North Atlantic (ENA) ocean, a total of 20 non-precipitating single-layer marine boundary layer (MBL) stratus and stratocumulus cloud cases are selected to investigate the impacts of the environmental variables on the aerosol–cloud interaction (ACIr) using the ground-based measurements from the Department of Energy Atmospheric Radiation Measurement (ARM) facility at the ENA site during 2016–2018. The ACIr represents the relative change in cloud droplet effective radius re with respect to the relative change in cloud condensation nuclei (CCN) number concentration at 0.2 % supersaturation (NCCN,0.2 %) in the stratified water vapor environment. The ACIr values vary from −0.01 to 0.22 with increasing sub-cloud boundary layer precipitable water vapor (PWVBL) conditions, indicating that re is more sensitive to the CCN loading under sufficient water vapor supply, owing to the combined effect of enhanced condensational growth and coalescence processes associated with higher Nc and PWVBL. The principal component analysis shows that the most pronounced pattern during the selected cases is the co-variations in the MBL conditions characterized by the vertical component of turbulence kinetic energy (TKEw), the decoupling index (Di), and PWVBL. The environmental effects on ACIr emerge after the data are stratified into different TKEw regimes. The ACIr values, under both lower and higher PWVBL conditions, more than double from the low-TKEw to high-TKEw regime. This can be explained by the fact that stronger boundary layer turbulence maintains a well-mixed MBL, strengthening the connection between cloud microphysical properties and the below-cloud CCN and moisture sources. With sufficient water vapor and low CCN loading, the active coalescence process broadens the cloud droplet size spectra and consequently results in an enlargement of re. The enhanced activation of CCN and the cloud droplet condensational growth induced by the higher below-cloud CCN loading can effectively decrease re, which jointly presents as the increased ACIr. This study examines the importance of environmental effects on the ACIr assessments and provides observational constraints to future model evaluations of aerosol–cloud interactions.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2011

Remote Sensing the Vertical Profile of Cloud Droplet Effective Radius, Thermodynamic Phase, and Temperature

Cloud-aerosol interaction is a key issue in the climate system, affecting the water cycle, the weather, and the total energy balance including the spatial and temporal distribution of latent heat release. Information on the vertical distribution of cloud droplet microphysics and thermodynamic phase as a function of temperature or height, can be correlated with details of the aerosol field to provide insight on how these particles are affecting cloud properties and their consequences to cloud lifetime, precipitation, water cycle, and general energy balance. Unfortunately, today's experimental methods still lack the observational tools that can characterize the true evolution of the cloud microphysical, spatial and temporal structure in the cloud droplet scale, and then link these characteristics to environmental factors and properties of the cloud condensation nuclei. Here we propose and demonstrate a new experimental approach (the cloud scanner instrument) that provides the microphysical information missed in current experiments and remote sensing options. Cloud scanner measurements can be performed from aircraft, ground, or satellite by scanning the side of the clouds from the base to the top, providing us with the unique opportunity of obtaining snapshots of the cloud droplet microphysical and thermodynamic states as a function of height and brightness temperature in clouds at several development stages. The brightness temperature profile of the cloud side can be directly associated with the thermodynamic phase of the droplets to provide information on the glaciation temperature as a function of different ambient conditions, aerosol concentration, and type. An aircraft prototype of the cloud scanner was built and flew in a field campaign in Brazil.

Martins, J. V.↗

DOE OSTI2022

Invisible ship tracks show large cloud sensitivity to aerosol

Cloud reflectivity is sensitive to atmospheric aerosol concentrations because aerosols provide the condensation nuclei on which water condenses. Increased aerosol concentrations due to human activity affect droplet number concentration, liquid water and cloud fraction, but these changes are subject to large uncertainties. Ship tracks, long lines of polluted clouds that are visible in satellite images, are one of the main tools for quantifying aerosol–cloud interactions. However, only a small fraction of the clouds polluted by shipping show ship tracks. Here we show that even when no ship tracks are visible in satellite images, aerosol emissions change cloud properties substantially. We develop a new method to quantify the effect of shipping on all clouds, showing a cloud droplet number increase and a more positive liquid water response when there are no visible tracks. We directly detect shipping-induced cloud property changes in the trade cumulus regions of the Atlantic, which are known to display almost no visible tracks. Our results indicate that previous studies of ship tracks were suffering from selection biases by focusing only on visible tracks from satellite imagery. The strong liquid water path response we find translates to a larger aerosol cooling effect on the climate, potentially masking a higher climate sensitivity than observed temperature trends would otherwise suggest.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Surface Observations From Atmospheric Radiation Measurement Sites Constrain the Anthropogenic Contribution to Cloud Droplet Number

Uncertainty in anthropogenic forcing driven by aerosol-cloud interactions (aci) limits our ability to infer the sensitivity of the Earth system to forcing from historical records. The driver of aci is the change in cloud droplet number concentration (N d ) due to changes in aerosol serving as cloud condensation nuclei (CCN). Here, we combine a perturbed parameter ensemble run in a global Earth system model with observations of CCN and single-layer-cloud N d at surface sites in the Azores, the Southern Great Plains, and Ascension Island to provide a constraint on the anthropogenic contribution to present-day N d . These observational lines of evidence constrain the preindustrial to present-day change in N d to be between 11 and 43 cm −3 . This is consistent with the upper end of some previous estimates but has a higher minimum perturbation, pointing to a stronger historical aerosol cooling.

ARM↗

NASA NTRS1990

Microphysical fundamentals governing cirrus cloud growth: Modeling studies

For application to Global Climate Models, large scale numerical models of cirrus cloud formation and maintenance need to be refined to more reliably simulate the effects and feedbacks of high level clouds. A key aspect is how ice crystal growth is initiated in cirrus, which has started a cloud microphysical controversy between camps either believing that heterogeneous or homogeneous drop freezing is predominantly responsible for cold cirrus ice crystal nucleation. In view of convincing evidence for the existence of highly supercooled cloud droplets in the middle and upper troposphere, however, it is concluded that active ice nuclei are rather scarce at cirrus cloud altitudes, and so a new understanding of cirrus cloud formation is needed. This understanding is sought through an examination of cirrus cloud growth models.

Sassen, Kenneth↗

NASA NTRS1989

Cirrus crystal nucleation by homogeneous freezing of solution droplets

A numerical model consisting of a system of differential equations is used to study cirrus crystal nucleation in a rising parcel containing a distribution of cloud condensation nuclei. The evolution of the particle population and the thermodynamic variables in the parcel are examined. The results suggest that, if homogeneous freezing is not considered, liquid water should be detected below -40 C. If homogeneous freezing is considered, the rapid growth of ice crystals and vapor depletion prevent water saturation from being reached. It is shown that the likelihood of a droplet being frozen is increased by lower temperatures, larger droplet diameter, or lower solution density.

Heymsfield, Andrew J.↗

DOE OSTI2026

Beta-Delayed Neutron Emission of 𝑁=84 132Cd

Using the time-of-flight technique, we measured the beta-delayed neutron emission of 132 Cd . From our large-scale shell model (LSSM) calculation using the N3⁢LO interaction [, Phys. Rev. Lett. 131, 022501 (2023)], we suggest the decay is dominated by the transformation of a neutron in the 𝑔7/2 orbital, deep below the Fermi surface, into a proton in the 𝑔9/2 orbital. We compare the beta-decay half-lives and neutron branching ratios of nuclei with 𝑍<50 and 𝑁 ≥82 obtained with our LSSM with those of leading “global” models such as finite-range droplet model (FRDM). Our calculations match known half-lives and neutron branching ratios well and suggest that current leading models overestimate the yet-to-be-measured half-lives. Our model, backed by the 132 Cd decay data presented here, offers robust predictive power for nuclei of astrophysical interest such as 𝑟-process waiting points.

Madurga, M [Department of Physics and Astronomy, U↗

DOE OSTI2023

Aerosol Hygroscopic Growth, Mixing State, and Cloud Condensation Nuclei Activity during TRACER (Field Campaign Report)

Convective clouds play a critical role in the Earth’s climate system. Recent research has shown that a realistic representation of convective processes is critical to constraining climate sensitivity in global climate models. Theoretical and modeling studies showed that aerosols could have strong dynamic feedback to convection in warm and humid environments through enhancing ice-related processes and condensational growth. A few observation-based studies also suggested the influence of aerosols on convective cloud and precipitation properties. However, robust observational quantification of an aerosol effect on convective clouds isolated from other factors remains elusive. Understanding the impact of aerosol on convective clouds requires knowledge of the cloud condensation nuclei (CCN) spectrum, which represents the number of particles that uptake water and form cloud droplets as a function of supersaturation. The water uptake by aerosol is also of critical importance for the direct interaction of aerosol with radiation (i.e., aerosol direct effect) due to light scattering and absorption by aerosol. While both droplet activation under supersaturated conditions (i.e., relative humidity RH > 100%) and the hygroscopic growth under sub-saturated conditions (i.e., RH < 100%) are strongly influenced by particle hygroscopicity, the thermodynamic regimes and measurement methods are quite different. Aerosol particles, especially organic particles, can exhibit higher hygroscopicity for droplet activation than that for hygroscopic growth. In the subsaturated regime, the hygroscopicity of organic particles can also vary strongly with RH. However, global climate models usually treat organic species in aerosols with a constant hygroscopicity, potentially introducing substantial uncertainties in the quantification of aerosol radiative effects.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Cloud condensation nuclei concentrations derived from the CAMS reanalysis

Determining number concentrations of cloud condensation nuclei (CCN) is one of the first steps in the chain in analysis of cloud droplet formation, the direct microphysical link between aerosols and cloud droplets, and a process key for aerosol–cloud interactions (ACI). However, due to sparse coverage of in situ measurements and difficulties associated with retrievals from satellites, a global exploration of their magnitude, source as well as temporal and spatial distribution cannot be easily obtained. Thus, a better representation of CCN numbers is one of the goals for quantifying ACI processes and achieving uncertainty-reduced estimates of their associated radiative forcing. Here, we introduce a new CCN dataset which is derived based on aerosol mass mixing ratios from the latest Copernicus Atmosphere Monitoring Service reanalysis (CAMSRA) in a diagnostic model that uses CAMSRA aerosol properties and a simplified kappa-Köhler framework suitable for global models. The emitted aerosols in CAMSRA are not only based on input from emission inventories using aerosol observations, they also have a strong tie to satellite-retrieved aerosol optical depth (AOD) as this is assimilated as a constraining factor in the reanalysis. Furthermore, the reanalysis interpolates for cases of poor or missing retrievals and thus allows for a full spatiotemporal quantification of CCN numbers. The derived CCN dataset captures the general trend and spatial and temporal distribution of total CCN number concentrations and CCN from different aerosol species. A brief evaluation with ground-based in situ measurements demonstrates the improvement of the modelled CCN over the sole use of AOD as a proxy for CCN as the overall correlation coefficient improved from 0.37 to 0.71. However, we find the modelled CCN from CAMSRA to be generally high biased and find a particular erroneous overestimation at one heavily polluted site which emphasises the need for further validation. The CCN dataset (https://doi.org/10.26050/WDCC/QUAERERE_CCNCAMS_v1, Block, 2023), which is now freely available to users, features 3-D CCN number concentrations of global coverage for various supersaturations and aerosol species covering the years 2003–2021 with daily frequency. This dataset is one of its kind as it offers lots of opportunities to be used for evaluation in models and in ACI studies.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1978

Airborne measurements of cloud-forming nuclei and aerosol particles in stabilized ground clouds produced by solid rocket booster firings

Airborne measurements of cloud volumes, ice nuclei and cloud condensation nuclei, liquid particles, and aerosol particles were obtained from stabilized ground clouds (SGCs) produced by Titan 3 launches at Kennedy Space Center, 20 August and 5 September 1977. The SGCs were bright, white, cumulus clouds early in their life and contained up to 3.5 g/m3 of liquid in micron to millimeter size droplets. The measured cloud volumes were 40 to 60 cu km five hours after launch. The SGCs contained high concentrations of cloud condensation nuclei active at 0.2%, 0.5%, and 1.0% supersaturation for periods of three to five hours. The SGCs also contained high concentrations of submicron particles. Three modes existed in the particle population: a 0.05 to 0.1 micron mode composed of aluminum-containing particles, a 0.2 to 0.8 micron mode, and a 2.0 to 10 micron mode composed of particles that contained primarily aluminum.

Hindman, E. E., II↗

DOE OSTI2023

Retrieved Number Concentration of Cloud Condensation Nuclei (RNCCN) Profile Value-Added Product Report

The cloud condensation nuclei (CCN) concentration at cloud base is the most relevant measure of the aerosol that influences droplet formation in clouds. Since the CCN concentration depends on supersaturation, a more general measure of the CCN concentration is the CCN spectrum (values at multiple supersaturations). The CCN spectrum is now measured at the surface at several U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility observatories and by the ARM Mobile Facility (AMF) but is not measured at the cloud base. Rather than rely on expensive aircraft measurements for all studies of aerosol effects on clouds, a way to project CCN observations made at the surface to cloud base is needed. Remote sensing of aerosol extinction provides information about the vertical profile of the aerosol but cannot be directly related to the CCN concentration because the aerosol extinction is strongly influenced by humidification, particularly near cloud base. Ghan and Collins (2004) and Ghan et al. (2006) propose a method to remove the influence of humidification from the extinction profiles and tie the “dry extinction” retrieval to the surface CCN concentration, thus estimating the CCN profile. This methodology has been implemented as ARM’s Retrieved Number Concentration of CCN (RNCCN) Profile Value-Added Product (VAP).

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1982

Crystal nucleation in Pd-Si alloys

A study of the crystal phase nucleation in undercooled droplets of Pd-Si alloys with composition near the Pd(84.5)Si(15.5) eutectic composition is reported. Molten droplets are released at the top of a drop tube and solidify (to either a crystalline or glassy state) during descent. This provides a containerless (and nearly gravity free) environment so that nucleation due to container walls or vibrations is eliminated. It is found that crystallization, due to homogeneous nucleation, is bypassed in droplets of 1 mm diameter when cooled at 760 K/sec. From this an upper limit of the homogeneous nucleation rate is estimated. Results are compared with a previously published study of nucleation in 0.06 mm to 0.33 mm diameter droplets, which indicated that nucleation results from heterogeneous surface nucleation and that the number of these nuclei is dependent on the atmosphere in the drop tube.

Drehman, A. J.↗

DOE OSTI2023

Enhancements in Cloud Condensation Nuclei Activity From Turbulent Fluctuations in Supersaturation

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

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Are turbulence effects on droplet collision–coalescence a key to understanding observed rain formation in clouds?

Rain formation is a critical factor governing the lifecycle and radiative forcing of clouds and therefore it is a key element of weather and climate. Cloud microphysics–turbulence interactions occur across a wide range of scales and are challenging to represent in atmospheric models with limited resolution. Based on past experiments and idealized numerical simulations, it has been postulated that cloud turbulence accelerates rain formation by enhancing drop collision–coalescence. We provide substantial evidence for significant impacts of turbulence on the evolution of cloud droplet size distributions and rain formation by comparing high-resolution observations of cumulus congestus clouds with state-of-the-art large-eddy simulations coupled with a Lagrangian particle-based microphysics scheme. Turbulent coalescence must be included in the model to accurately represent the observed drop size distributions, especially for drizzle drop sizes at lower heights in the cloud. Turbulence causes earlier rain formation and greater rain accumulation compared to simulations with gravitational coalescence only. The observed rain size distribution tail just above cloud base follows a power law scaling that deviates from theoretical scalings considering either a purely gravitation collision kernel or a turbulent kernel neglecting droplet inertial effects, providing additional evidence for turbulent coalescence in clouds. In contrast, large aerosols acting as cloud condensation nuclei (“giant CCN”) do not significantly impact rain formation owing to their long timescale to reach equilibrium wet size relative to the lifetime of rising cumulus thermals. Overall, turbulent drop coalescence exerts a dominant influence on rain initiation in warm cumulus clouds, with limited impacts of giant CCN.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1976

Studies of the exhaust products from solid propellant rocket motors

This study was undertaken to determine the feasibility of conducting environmental chamber tests on the physical processes which occur when a solid rocket motor exhaust mixes with the ambient atmosphere. Of particular interest was the interaction between hydrogen chloride, aluminum oxide, and water vapor. The program consisted of three phases: (1) building a small rocket motor and using it to provide the exhaust species in a controlled environment; (2) evaluating instruments used to detect and measure HCl concentrations and if possible determining whether the HCl existed in the gaseous state or as an acid aerosol; (3) monitoring a series of 6.4-percent scale space shuttle motor tests and comparing the results to the environmental chamber studies. Eighteen firings were conducted in an environmental chamber with the initial ambient relative humidity set at values from 29 to 100 percent. Two additional firings were made in a large shed, and four were made on an open concrete apron. Six test firings at MSFC were monitored, and the ground level concentrations are reported. Evidence is presented which shows that the larger Al2O3 (5 to 50 micrometers) particles from the rocket motor can act as condensation nuclei. Under appropriate ambient conditions where there is sufficient water vapor this results in the formation of an acid aerosol. Droplets of this acid were detected both in the environmental chamber and in the scaled shuttle engine tests.

Dawbarn, R.↗

NASA NTRS1987

On the prolonged lifetime of the El Chichon sulfuric acid aerosol cloud

The observed decay of the aerosol mixing ratio following the eruption of El Chichon appears to have been 20-30 percent slower than that following the eruption of Fuego in 1974, even though the sulfuric acid droplets were observed to grow to considerably larger sizes after El Chichon. This suggests the possible presence of a condensation nuclei and sulfuric acid vapor source and continued growth phenomena occurring well after the El Chichon eruption. It is proposed that the source of these nuclei and the associated vapor may be derived from annual evaporation and condensation of aerosol in the high polar regions during stratospheric warming events, with subsequent spreading to lower latitudes.

Hofmann, D. J.↗

DOE OSTI2025

Crystalline Organic Compounds as Effective Nuclei in Contact Efflorescence of Ammonium Sulfate

Contact nucleation is believed to play a role in liquid-to-solid phase transitions in the atmosphere including ice nucleation and salt efflorescence. Here, for this work, contact efflorescence of optically levitated ammonium sulfate droplets by collisions with organic particles is probed using a long working-distance optical trap. Two highly viscous water-soluble organic compounds (d-(+)-raffinose and citric acid), and two insoluble highly surface-active organic compounds (stearic acid and cis-pinonic acid) were probed for their ability to induce efflorescence upon contact. While three of the organics showed minimal effectiveness as contact nuclei, cis-pinonic acid showed a remarkable ability to initiate contact efflorescence of ammonium sulfate, occurring near ammonium sulfate’s deliquescence relative humidity. Further analysis of cis-pinonic acid using bright-field microscopy in an electrodynamic balance provided evidence that the cis-pinonic acid particles are crystalline under the laboratory conditions. We suggest that the close lattice match between crystalline ammonium sulfate and crystalline cis-pinonic acid may account for the observed effectiveness in initiating contact efflorescence of ammonium sulfate. In contrast, tests of contact nucleation between cis-pinonic acid and sodium chloride, a pair with a poor lattice match, did not result in efflorescence. These findings suggest that crystalline organic compounds in the atmosphere could act as effective nuclei for contact efflorescence of atmospherically relevant salts, provided they share a compatible lattice structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1995

Origin of condensation nuclei in the springtime polar stratosphere

An enhanced sulfate aerosol layer has been observed near 25 km accompanying springtime ozone depletion in the Antarctic stratosphere. We use a one-dimensional aerosol model that includes photochemistry, particle nucleation, condensational growth, coagulation, and sedimentation to study the origin of the layer. Annual cycles of sunlight, temperature, and ozone are incorporated into the model. Our results indicate that binary homogeneous nucleation leads to the formation of very small droplets of sulfuric acid and water under conditions of low temperature and production of H2SO4 following polar sunrise. Photodissociation of carbonyl sulfide (OCS) alone, however, cannot provide sufficient SO2 to create the observed condensation nuclei (CN) layer. When subsidence of SO2 from very high altitudes in the polar night vortex is incorporated into the model, the CN layer is reasonably reproduced. The model predictions, based on the subsidence in polar vortex, agree with in situ measurements of particle concentration, vertical distribution, and persistence during polar spring.

Zhao, Jingxia↗