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At least 379 records · Page 21

Highly Supercooled Riming and Unusual Triple-Frequency Radar Signatures Over McMurdo Station, Antarctica

Riming of ice crystals by supercooled water droplets is an efficient ice growth process, but its basic properties are still poorly known. While it has been shown to contribute significantly to surface precipitation at mid-latitudes, little is known about its occurrence at high latitudes. In Antarctica, two competing effects can influence the occurrence of riming: (i) the scarcity of supercooled liquid water clouds due to the extremely low tropospheric temperatures and (ii) the low aerosol concentration, which may lead to the formation of fewer and larger supercooled drops potentially resulting in an enhanced riming efficiency. In this work, by exploiting the deployment of an unprecedented number of multiwavelength remote sensing systems (including triple-frequency radar measurements) in West Antarctica, during the Atmospheric Radiation Measurements West Antarctic Radiation Experiment (AWARE) field campaign, we evaluate the riming incidence at McMurdo Station and find that riming occurs at much lower temperatures when compared to previous results in the mid-latitudes. This suggests the possible occurrence of a common atmospheric state over Antarctica that includes a rather stable atmosphere inhibiting turbulent mixing, and a high riming efficiency driven by large cloud droplets. We then focus on a peculiar case study featuring a persistent layer with a particularly pronounced riming signature in triple-frequency radar data but only a relatively modest amount of supercooled liquid water. In-depth analysis of the radar observations suggests that such signatures can only be explained by the combined effects of moderately rimed aggregates or similarly shaped florid polycrystals and a narrow particle size distribution (PSD). Simulations of this case study performed with a one-dimensional bin model indicate that similar triple-frequency radar observations can be reproduced when narrow PSDs are simulated. Such narrow PSDs can in turn be explained by two key factors: (i) the presence of a shallow homogeneous droplet or humidified aerosol freezing layer aloft seeding an underlying supercooled liquid layer, and (ii) the absence of turbulent mixing throughout a stable polar atmosphere that sustains narrow PSDs, as hydrometeors grow from the nucleation region aloft to ice particles of several millimeters in size, by vapor deposition and then riming.

Riming↗

Ice Dusty Plasma (Final Report)

The NSF/DOE funding described in this final report was for constructing a substantial upgrade that would enable operation at variable and much lower cryogenic temperatures than was available in a previous experiment that operated from 2013 to 2019. Components for the upgraded experiment were designed and ordered from August to December 2019 and assembly began in early 2020. However, COVID-19 halted all lab work for much of 2020 and then when lab work resumed, numerous restrictions on lab access and in-lab time further impeded progress. Because of these delays, first plasma was obtained in late 2021 and a normal work pace resumed only in mid-2022. A no-cost extension was requested because the COVID-19 delays prevented work from being done at the anticipated rate. Constructing a water-ice experiment was a significant gamble because the parameter regime differs substantially from conventional laboratory plasmas and injecting water vapor into a plasma goes very much against convention as one normally goes to great lengths to avoid water vapor. This experiment opens a new frontier, namely the study of how charged ice grains form, grow, and interact with a plasma environment. The just-completed upgrade was a further gamble because it combines technology never previously used together (cryocoolers, plasma, and ice).

36 MATERIALS SCIENCE↗

Homogeneous freezing nucleation of stratospheric solution droplets

The classical theory of homogeneous nucleation was used to calculate the freezing rate of sulfuric acid solution aerosols under stratospheric conditions. The freezing of stratospheric aerosols would be important for the nucleation of nitric acid trihydrate particles in the Arctic and Antarctic stratospheres. In addition, the rate of heterogeneous chemical reactions on stratospheric aerosols may be very sensitive to their state. The calculations indicate that homogeneous freezing nucleation of pure water ice in the stratospheric solution droplets would occur at temperatures below about 192 K. However, the physical properties of H2SO4 solution at such low temperatures are not well known, and it is possible that sulfuric acid aerosols will freeze out at temperatures ranging from about 180 to 195 K. It is also shown that the temperature at which the aerosols freeze is nearly independent of their size.

Jensen, Eric J.↗

Controlling nucleation in protein solutions

A simple one-step technique for controlling the nucleation stage in protein solutions without the use of a seed crystal was developed using a specially designed apparatus in which the nucleation and growth processes can be separated. The method can be applied only to species that have a temperature-dependent solubility. The effectiveness of this 'thermonucleating' device was demonstrated with the nucleation and growth of ice, Rochelle salt, and lysozyme.

Demattei, R. C.↗

Sensitivity of Boreal-Summer Circulation and Precipitation to Atmospheric Aerosols in Selected Regions: The Americas - Part 2

Aerosol perturbations over selected land regions are imposed in Version-4 of the Goddard Earth Observing System (GEOS-4) general circulation model (GCM) to assess the influence of increasing aerosol concentrations on regional circulation patterns and precipitation in four selected regions: India, Africa, and North and South America. Part 1 of this paper addresses the responses to aerosol perturbations in India and Africa. This paper presents the same for aerosol perturbations over the Americas. GEOS-4 is forced with prescribed aerosols based on climatological data, which interact with clouds using a prognostic scheme for cloud microphysics including aerosol nucleation of water and ice cloud hydrometeors. In clear-sky conditions the aerosols interact with radiation. Thus the model includes comprehensive physics describing the aerosol direct and indirect effects on climate (hereafter ADE and AIE respectively). Each simulation is started from analyzed initial conditions for 1 May and was integrated through June-July-August of each of the six years: 1982 1987 to provide a 6-ensemble set. Results are presented for the difference between simulations with double the climatological aerosol concentration and one-half the climatological aerosol concentration for three experiments: two where the ADE and AIE are applied separately and one in which both the ADE and AIE are applied. The ADE and AIE both yield reductions in net radiation at the top of the atmosphere and surface while the direct absorption of shortwave radiation contributes a net radiative heating in the atmosphere. A large net heating of the atmosphere is also apparent over the subtropical North Atlantic Ocean that is attributable to the large aerosol perturbation imposed over Africa. This atmospheric warming and the depression of the surface pressure over North America contribute to a northward shift of the inter-Tropical Convergence Zone over northern America, an increase in precipitation over Central America and the Caribbean, and an enhancement of convergence in the North American monsoon region.

Wilcox, E. M.↗

TPSAS-NF1676L-20101-DND

Aerosols influence climate through their direct and indirect effects. The aerosol indirect effect is based on the way they interact with surrounding clouds. During cloud formation and development, aerosols act as cloud nucleation nuclei (CCN) or ice nuclei, which modifies cloud micro-, macro-physical and radiative properties, and hence helps to shape the Earth's radiation budget. Dominant sources of ocean-derived aerosols that may serve as CCN include sea spray and biogenic aerosol. In this study, we used 10-years global observations from the A-Train satellites to show seasonal variations of cloud droplet number concentrations (CDNC), ocean chlorophyll concentrations, aerosol angstrom parameter, and rainfall. Potential cloud-aerosol interactions are further discussed based on seasonal and spatial correlations between microphysics of clouds and aerosols. Emphasis for this study is placed on the southern ocean and tropical Pacific.

Shan Zeng↗

Real-time latent heat emission during dynamic-compression freezing of water

Abstract Dynamic compression studies have been used to study the nucleation kinetics of water to ice VII for decades. Diagnostics such as photon Doppler velocimetry, transmission loss, and imaging have been used to measure pressure/density, and phase fraction, while temperature has remained the difficult thermodynamic property to quantify. In this work, we measured pressure/density and implemented a diagnostic to measure the temperature. In doing so the temperature shows quasi-isentropically compressed liquid water forms ice at pressures below the previously defined metastable limit, and the liquid phase is not hypercoooled as previously thought above that limit. Instead, the latent heat raises the temperature to the liquid-ice-VII melt line, where it remains with increasing pressure. We propose a hypothesis to corroborate these results with previous work on dynamic compression freezing. These results provide constraints for nucleation models, and suggest this technique be used to investigate phase transitions in other materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Microphysical modeling of cirrus. 1: Comparison with 1986 FIRE IFO measurements

We have used a one-dimensional model of cirrus formation to study the development of cirrus clouds during the 1986 First ISCCP (International Satellite Cloud Climatology Project) Regional Experiment (FIRE) intensive field observations (IFO). The cirrus model includes microphysical, dynamical, and radiative processes. Sulfate aerosols, solution drops, ice crystals, and water vapor are all treated as interactive elements in the model. Ice crystal size distributions are fully resolved based on calculations of homogeneous freezing nucleation, growth by water vapor deposition, evaporation, coagulation, and vertical transport. We have focused on the cirrus observed on November 1, 1986. Vertical wind speed for the one-dimensional simulation is taken from a mesoscale model simulation for the appropriate time period. The mesoscale model simulation suggested that strong upward motions over Wyoming and subsequent horizontal transport of upper level moisture were responsible for the cirrus observed over Wisconsin on this date. We assumed that our one-dimensional model could be used to represent a vertical column moving from Wyoming to Wisconsin over a period of several hours. Ice crystal nucleation occurs in our model in the 8 to 10-km region as a result of the strong updrafts (and cooling) early in the simulation. Growth, coagulation, and sedimentation of these ice crystals result in a broad cloud region (5-10 km thick) with an optical depth of 1-2 after a few hours, in agreement with the FIRE measurements. Comparison with aircraft microphysical measurements made over Wisconsin indicates that the simulation generated reasonable ice water content, but the predicted ice number densities are too low, especially for radii less than about 50 microns. Sensitivity tests suggest that better agreement between simulated and observed microphysical properties is achieved if the nucleation rate is higher or stronger vertical mixing (perhaps associated with multidimensional motions) is present.

Jensen, Eric J.↗

A Laboratory Study on the Phase Transition for Polar Stratospheric Cloud Particles

The nucleation and growth of different phases of simulated polar stratospheric cloud (PSC) particles were investigated in the laboratory. Solutions and mixtures of solutions at concentrations 1 to 5 m (molality) of ammonium sulfate, ammonium bisulfate, sodium chloride, sulfuric acid, and nitric acid were supercooled to prescribed temperatures below their equilibrium melting point. These solutions were contained in small diameter glass tubing of volumes ranging from 2.6 to 0.04 ml. Samples were nucleated by insertion of an ice crystal, or in some cases by a liquid nitrogen cooled wire. Crystallization velocities were determined by timing the crystal growth front passages along the glass tubing. Solution mixtures containing aircraft exhaust (soot) were also examined. Crystallization rates increased as deltaT2, where deltaT is the supercooling for weak solutions (2 m or less). The higher concentrated solutions (greater than 3 m) showed rates significantly less than deltaT2. This reduced rate suggested an onset of a glass phase. Results were applied to the nucleation of highly concentrated solutions at various stages of polar stratospheric cloud development within the polar stratosphere.

Teets, Edward H., Jr.↗

Predicting the Mineral Composition of Dust Aerosols: Representing Key Processes - Part 1

Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the model extensions result in better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

aerosols↗

Systematic Relationships Between Lidar Observables and Sizes And Mineral Composition Of Dust Aerosols

The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

Dust↗

High concentrations of ice: Investigations using polarimetric radar observations combined with in situ measurements and cloud modeling (Final Report)

This DOE-funded joint project had the over-arching goal of understanding the reasons for observed size distributions of ice particles in cold clouds. Its approach involves the use of cloud models and field observations by radar and aircraft of real storms. The project addresses three major research objectives: (1) Utilize a novel polarimetric radar technique to retrieve size distributions and amounts of ice from radar data collected during the previous DOE ARM field campaigns; (2) Evaluate the results of ice microphysical retrievals using available in situ aircraft measurements and other remote sensors (e.g., vertically pointing cloud radars and wind profilers); (3) Improve the treatment of microphysical processes leading to cloud glaciation and ice multiplication in numerical cloud models. The study was performed by three research organizations: University of Oklahoma, The Hebrew University of Jerusalem, Israel, and Lund University, Sweden. The Israel and Swedish partners were funded by the sub-awards from the University of Oklahoma. Cloud modeling studies have been performed by the research teams at The Hebrew University of Jerusalem (HUJ) and Lund University to identify the origins of high concentrations of cloud ice in areas of high ice water content (HIWC). The Hebrew University Cloud Model (HUCM) with full spectral bin microphysics and the Lund University aerosol-cloud (AC) model with a hybrid bin / bulk microphysics scheme complementing HUCM were utilized for simulations. Both research teams had particular focus on secondary ice production (SIP) as one of the possible sources of enhanced ice concentration. The HUJ group suggested a novel concept of ice multiplication during droplet freezing. It is assumed that splintering and droplet fragmentation during droplet freezing takes place because of dendritic growth within a supercooled drop. The resulting simulations of SIP generated small ice in concentrations exceeding hundreds per liter similar to what was observed in the HIWC regions of the tropical storms. The Lund team explored the SIP mechanisms such as breakup of ice particles due to ice-ice collisions and ice sublimation that are expected to dominate the continental storms. They also quantified the impact of homogeneous nucleation of cloud droplets on the total number concentration of ice at very low temperatures near the tops of the clouds. Additionally, the Lund AC model is able to simulate the effect of aerosols of various types (including biological) on the cloud life cycle and the corresponding ice production. The HUCM / AC model was used to simulate one of the “golden” cases of the DOE MC3E campaign on 20 May 2011. The model output was converted into the fields of polarimetric radar variables using the polarimetric radar forward operator developed at the University of Oklahoma and compared with radar observations and in situ microphysical measurements onboard research aircraft. It was demonstrated that specific differential phase KDP is the best radar parameter to identify the HIWC areas and quantify the corresponding ice parameters. For the first time, the shape of the vertical profile of KDP was realistically reproduced by the cloud model with the KDP maximum in the dendritic growth layer (DGL) centered at the -15°C isotherm. The University of Oklahoma team has developed a methodology for polarimetric radar retrievals of such microphysical parameters of ice as ice water content (IWC), mean volume diameter (Dm), and total number concentration (Nt) of ice particles. These retrievals have been validated using in situ aircraft measurements during 6 field campaigns and proved to be quite robust and reliable. This allowed to build the first climatology of the vertical profiles of polarimetric radar variables and retrieved microphysical parameters for the three types of weather systems: continental MCSs, maritime MCSs, and tropical cyclones / hurricanes (Hu and Ryzhkov 2022). The data were collected by a multitude of the WSR-88D radars in 13 continental and 10 maritime MCSs and 11 landfalling hurricanes. The HIWC areas were identified within the examined storms and the corresponding “HIWC statistics” was compared with the “background” one without HIWC. An overarching conclusion of the study is that maritime tropical storms (MCSs and hurricanes) are characterized by smaller size ice in higher concentration compared to the continental MCSs. High ice water content in the HIWC areas is primarily caused by a strong jump in a number concentration of ice particles rather than the increase of their size compared to the “background” environment. This may point to the homogeneous nucleation of excessive amounts of supercooled droplets and / or secondary ice production as the possible origins of HIWC. Such a climatology provides a good observational reference for the modelers to evaluate the performance of their models. As an example, the in-depth analysis of the 20 May 2011 MC3E case shows that the advanced cloud models developed in the course of this study still tend to underestimate the number concentration of ice in the HIWC areas although they succeed in reproducing realistically looking vertical profiles of IWC and Nt. The results of the project research are summarized in 13 journal papers.

54 ENVIRONMENTAL SCIENCES↗

Dynamical States of Low Temperature Cirrus

Low ice crystal concentration and sustained in-cloud supersaturation, commonly found in cloud observations at low temperature, challenge our understanding of cirrus formation. Heterogeneous freezing from effloresced ammonium sulfate, glassy aerosol, dust and black carbon are proposed to cause these phenomena; this requires low updrafts for cirrus characteristics to agree with observations and is at odds with the gravity wave spectrum in the upper troposphere. Background temperature fluctuations however can establish a dynamical equilibrium between ice production and sedimentation loss (as opposed to ice crystal formation during the first stages of cloud evolution and subsequent slow cloud decay) that explains low temperature cirrus properties. This newly-discovered state is favored at low temperatures and does not require heterogeneous nucleation to occur (the presence of ice nuclei can however facilitate its onset). Our understanding of cirrus clouds and their role in anthropogenic climate change is reshaped, as the type of dynamical forcing will set these clouds in one of two preferred microphysical regimes with very different susceptibility to aerosol.

Barahona, D.↗

CO2 Snow on Mars and Early Earth: Experimental Constraints

Greenhouse warming due to carbon dioxide atmospheres may be responsible for maintaining the early Earth's surface temperature above freezing and may even have allowed for liquid water on early Mars. However, the high levels of CO2 required for such warming should have also resulted in the formation of CO2 clouds. These clouds, depending on their particle size, could lead to either warming or cooling. The particle size in turn is determined by the nucleation and growth conditions. Here we present laboratory studies of the nucleation and growth of carbon dioxide on water ice under Martian atmospheric conditions. We find that a critical saturation, S = 1.34, is required for nucleation, corresponding to a contact parameter between solid water and solid carbon dioxide of m = 0.95. We also find that after nucleation occurs, growth of CO2 is very rapid and proceeds without a surface kinetic barrier. Because growth would be expected to continue until the CO2 pressure is lowered to its vapor pressure, we expect particles larger than those being currently suggested for the present and past Martian atmospheres. Using this information in a microphysical model described in a companion paper, we find that CO2 clouds are best described as "snow", having a relatively small number of large particles.

Glandorf, David L.↗

Probing the structure of cometary ice

Computer simulations of bulk and vapor deposited amorphous ices are presented. The structure of the bulk low density amorphous ice is in good agreement with experiments on pressure disordered amorphous ice. Both the low density bulk ice and the vapor deposited ices exhibit strong ordering. Vapor deposition of hot (300 K) water molecules onto a cold (77 K) substrate yields less porous ices than deposition of cold (77 K) water molecules onto a cold substrate. Both vapor deposited ices are more porous than the bulk amorphous ice. The structure of bulk high density amorphous ice is only in fair agreement with experimental results. Attempts to simulate high density amorphous ice via vapor deposition were not successful. Electron diffraction results on vapor deposited amorphous ice indicate that the temperature of the nucleation of the cubic phase depends upon the amount of time between the deposition and the onset of crystallization, suggesting that freshly deposited ice layers reconstruct on time of the order of hours. The temperature dependence of the microporosity of the vapor deposited amorphous ices might affect laboratory experiments that are aimed at simulating astrophysical ices in the context of the origin of prebiotic organic material and its transport to the Earth.

Wilson, Michael A.↗

Computational Modeling Approaches to Multiscale Design of Icephobic Surfaces

To aid in the design of surfaces that prevent icing, a model and computational simulation of impact ice formation at the single droplet scale was implemented. The nucleation of a single supercooled droplet impacting on a substrate, in rime ice conditions, was simulated. Open source computational fluid dynamics (CFD) software was used for the simulation. To aid in the design of surfaces that prevent icing, a model of impact ice formation at the single droplet scale was proposed•No existing model simulates simultaneous impact and freezing of a single super-cooled water droplet•For the 10-week project, a low-fidelity feasibility study was the goal.

adhesion↗

Nucleation in Synoptically Forced Cirrostratus

Formation and evolution of cirrostratus in response to weak, uniform and constant synoptic forcing is simulated using a one-dimensional numerical model with explicit microphysics, in which the particle size distribution in each grid box is fully resolved. A series of tests of the model response to nucleation modes (homogeneous-freezing-only/heterogeneous nucleation) and heterogeneous nucleation parameters are performed. In the case studied here, nucleation is first activated in the prescribed moist layer. A continuous cloud-top nucleation zone with a depth depending on the vertical humidity gradient and one of the nucleation parameters is developed afterward. For the heterogeneous nucleation cases, intermittent nucleation zones in the mid-upper portion of the cloud form where the relative humidity is on the rise, because existent ice crystals do not uptake excess water vapor efficiently, and ice nuclei (IN) are available. Vertical resolution as fine as 1 m is required for realistic simulation of the homogeneous-freezing-only scenario, while the model resolution requirement is more relaxed in the cases where heterogeneous nucleation dominates. Bulk microphysical and optical properties are evaluated and compared. Ice particle number flux divergence, which is due to the vertical gradient of the gravity-induced particle sedimentation, is constantly and rapidly changing the local ice number concentration, even in the nucleation zone. When the depth of the nucleation zone is shallow, particle number concentration decreases rapidly as ice particles grow and sediment away from the nucleation zone. When the depth of the nucleation zone is large, a region of high ice number concentration can be sustained. The depth of nucleation zone is an important parameter to be considered in parametric treatments of ice cloud generation.

Lin, R.-F.↗

Physical processes in polar stratospheric ice clouds

A one dimensional model of cloud microphysics was used to simulate the formation and evolution of polar stratospheric ice clouds. Some of the processes which are included in the model are outlined. It is found that the clouds must undergo preferential nucleation upon the existing aerosols just as do tropospheric cirrus clouds. Therefore, there is an energy barrier between stratospheric nitric acid particles and ice particles implying that nitric acid does not form a continuous set of solutions between the trihydrate and ice. The Kelvin barrier is not significant in controlling the rate of formation of ice particles. It was found that the cloud properties are sensitive to the rate at which the air parcels cool. In wave clouds, with cooling rates of hundreds of degrees per day, most of the existing aerosols nucleate and become ice particles. Such clouds have particles with sizes on the order of a few microns, optical depths on order of unity and are probably not efficient at removing materials from the stratosphere. In clouds which form with cooling rates of a few degrees per day or less, only a small fraction of the aerosols become cloud particles. In such clouds the particle radius is larger than 10 microns, the optical depths are low and water vapor is efficiently removed. Seasonal simulations show that the lowest water vapor mixing ratio is determined by the lowest temperature reached, and that the time when clouds disappear is controlled by the time when temperatures begin to rise above the minimum values.

Toon, Owen B.↗