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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS1997

Ice Nucleation Processes in Upper Tropospheric Wave-Clouds Observed During SUCCESS

We have compared in situ measurements near the leading-edges of wave-clouds observed during the SUCCESS experiment with numerical modeling of ice nucleation. Observations of high supersaturations with respect to ice (\geq 150\%) near the leading edge of a very cold wave cloud (T < --60^\circC) are consistent with recent theoretical and laboratory studies suggesting that large supersaturations are required to homogeneously freeze sulfate aerosols. Also, the peak ice crystal number densities observed in this cloud (about 4cm -3/sup>) are consistent with the number densities calculated in our model. The consistency between model results (using homogeneous freezing and the observations indicates that the number density of effective heterogeneous ice nuclei must be no more than about 2 cm -3 . In the warmer wave-cloud (T (approx.)eq --37^\circC) relatively large ice number densities were observed (20--40 cm -3 . Our model calculations suggest that these large number densities are only possible if liquid droplets were activated at the cloud leading-edge, followed by subsequent homogeneous freezing. If sulfate aerosols had frozen before liquid droplets could be activated, then the peak ice crystal number density should have been less than 10 cm -3 .

Jensen, E. J.↗
NASA NTRS2012

A FIRE-ACE/SHEBA Case Study of Mixed-Phase Arctic Boundary Layer Clouds: Entrainment Rate Limitations on Rapid Primary Ice Nucleation Processes

Observations of long-lived mixed-phase Arctic boundary layer clouds on 7 May 1998 during the First International Satellite Cloud Climatology Project (ISCCP) Regional Experiment (FIRE)Arctic Cloud Experiment (ACE)Surface Heat Budget of the Arctic Ocean (SHEBA) campaign provide a unique opportunity to test understanding of cloud ice formation. Under the microphysically simple conditions observed (apparently negligible ice aggregation, sublimation, and multiplication), the only expected source of new ice crystals is activation of heterogeneous ice nuclei (IN) and the only sink is sedimentation. Large-eddy simulations with size-resolved microphysics are initialized with IN number concentration N(sub IN) measured above cloud top, but details of IN activation behavior are unknown. If activated rapidly (in deposition, condensation, or immersion modes), as commonly assumed, IN are depleted from the well-mixed boundary layer within minutes. Quasi-equilibrium ice number concentration N(sub i) is then limited to a small fraction of overlying N(sub IN) that is determined by the cloud-top entrainment rate w(sub e) divided by the number-weighted ice fall speed at the surface v(sub f). Because w(sub c)< 1 cm/s and v(sub f)> 10 cm/s, N(sub i)/N(sub IN)<< 1. Such conditions may be common for this cloud type, which has implications for modeling IN diagnostically, interpreting measurements, and quantifying sensitivity to increasing N(sub IN) (when w(sub e)/v(sub f)< 1, entrainment rate limitations serve to buffer cloud system response). To reproduce observed ice crystal size distributions and cloud radar reflectivities with rapidly consumed IN in this case, the measured above-cloud N(sub IN) must be multiplied by approximately 30. However, results are sensitive to assumed ice crystal properties not constrained by measurements. In addition, simulations do not reproduce the pronounced mesoscale heterogeneity in radar reflectivity that is observed.

Fridlin, Ann↗
NASA NTRS2018

Cirrus Susceptibility to Changes in Ice Nuclei: Physical Processes, Model Uncertainties, and Measurement Needs

One of the proposed concepts for mitigating the warming effect of increasing greenhouse gases is seeding cirrus cloud with ice nuclei (IN) in order to reduce the lifetime and coverage of cold cirrus that have a net warming impact on the earth's surface. Global model simulations of the net impact of changing upper tropospheric IN have given widely disparate results, partly as a result of poor understanding of ice nucleation processes in the current atmosphere, and partly as a result of poor representation of these processes in global models. Here, we present detailed process-model simulations of tropical tropopause layer (TTL) transport and cirrus formation with ice nuclei properties based on recent laboratory nucleation experiments and field measurements of aerosol composition. The model is used to assess the sensitivity of TTL cirrus occurrence frequency and microphysical properties to the abundance and efficacy of ice nuclei. The simulated cloud properties compared with recent high-altitude aircraft measurements of TTL cirrus and ice supersaturation. We find that abundant effective IN (either from glassy organic aerosols or crystalline ammonium sulfate with concentrations greater than about 100/L) prevent the occurrences of large ice concentration and large ice supersaturations, both of which are clearly indicated by the in situ observations. We find that concentrations of effective ice nuclei larger than about 50/L can drive significant changes in cirrus microphysical properties and occurrence frequency. However, the cloud occurrence frequency can either increase or decrease, depending on the efficacy and abundance of IN added to the TTL. We suggest that our lack of information about ice nuclei properties in the current atmosphere, as well as uncertainties in ice nucleation processes and their representations in global models, preclude meaningful estimates of climate impacts associated with addition of ice nuclei in the upper troposphere. We will briefly discuss the key field measurements needed to constrain ice nucleation processes.

Jensen, Eric↗
NASA NTRS2014

Sensitivity of Cirrus Properties to Ice Nuclei Abundance

The relative importance of heterogeneous and homogeneous ice nucleation for cirrus formation remains an active area of debate in the cloud physics community. From a theoretical perspective, a number of modeling studies have investigated the sensitivity of ice number concentration to the nucleation mechanism and the abundance of ice nuclei. However, these studies typically only addressed ice concentration immediately after ice nucleation. Recent modeling work has shown that the high ice concentrations produced by homogeneous freezing may not persist very long, which is consistent with the low frequency of occurrence of high ice concentrations indicated by cirrus measurements. Here, I use idealized simulations to investigate the impact of ice nucleation mechanism and ice nuclei abundance on the full lifecycle of cirrus clouds. The primary modeling framework used includes different modes of ice nucleation, deposition growth/sublimation, aggregation, sedimentation, and radiation. A limited number of cloud-resolving simulations that treat radiation/dynamics interactions will also been presented. I will show that for typical synoptic situations with mesoscale waves present, the time-averaged cirrus ice crystal size distributions and bulk cloud properties are less sensitive to ice nucleation processes than might be expected from the earlier simple ice nucleation calculations. I will evaluate the magnitude of the ice nuclei impact on cirrus for a range of temperatures and mesoscale wave specifications, and I will discuss the implications for cirrus aerosol indirect effects in general.

Nuclei↗
NASA NTRS2002

Surface Crystallization of Supercooled Water in Clouds

The process by which liquid cloud droplets homogeneously crystallize into ice is still not well-understood. The ice nucleation process based on the standard and classical theory of homogeneous freezing, initiates within the interior volume of a cloud droplet. Current experimental data on homogeneous freezing rates of ice in droplets of supercooled water, both in air and emulsion oil samples, show considerable scatter. For example, at -33 C, the reported volume-based freezing rates of ice in supercooled water vary by as much as 5 orders of magnitude, which is well outside the range of measurement uncertainties. Here, we show that the process of ice nucleus formation at the air (or oil)-liquid water interface may help to explain why experimental results on ice nucleation rates yield different results in different ambient phases. Our results also suggest that surface crystallization of ice in cloud droplets can explain why low amounts of supercooled water have been observed in the atmosphere near -40 C.

Tabazadeh, Azadeh↗
NASA NTRS1997

SUCCESS Evidence for Cirrus Cloud Ice Nucleation Mechanisms

During the SUCCESS mission, several measurements were made which should improve our understanding of ice nucleation processes in cirrus clouds. Temperature and water vapor concentration were made with a variety of instruments on the NASA DC-8. These observations should provide accurate upper tropospheric humidities. In particular, we will evaluate what humidities are required for ice nucleation. Preliminary results suggest that substantial supersaturations frequently exist in the upper troposphere. The leading-edge region of wave-clouds (where ice nucleation occurs) was sampled extensively at temperatures near -40 and -60C. These observations should give precise information about conditions required for ice nucleation. In addition, we will relate the observed aerosol composition and size distributions to the ice formation observed to evaluate the role of soot or mineral particles on ice nucleation. As an alternative technique for determining what particles act as ice nuclei, numerous samples of aerosols inside ice crystals were taken. In some cases, large numbers of aerosols were detected in each crystal, indicating that efficient scavenging occurred. Analysis of aerosols in ice crystals when only one particle per crystal was detected should help with the ice nucleation issue. Direct measurements of the ice nucleating activity of ambient aerosols drawn into airborne cloud chambers were also made. Finally, measurements of aerosols and ice crystals in contrails should indicate whether aircraft exhaust soot particles are effective ice nuclei.

Jensen, Eric↗
NASA NTRS1975

Conference on Cloud Physics, Tucson, Ariz., October 21-24, 1974, Proceedings

Condensation and ice nucleation processes are considered, taking into account measurements of cloud nuclei and aerosol size spectra in the semiarid Southwest, the formation of sulfates and the enhancement of cloud condensation nuclei in clouds, biogenic sources of atmospheric ice nuclei, and the experimental determination of the deposition coefficient of water vapor onto ice. Other topics discussed are related to precipitation growth processes, the role of ice in cloud systems, cloud modeling, measurements in Colorado hailstorms during the national hail research experiment, cloud measurements, and measurement techniques. Attention is also given to cloud electrification, zero-gravity experiments, and the control of cloud development by larger scale motions. Individual items are announced in this issue.

Source record↗
NASA NTRS2001

Ice Nucleation in Deep Convection

The processes controlling production of ice crystals in deep, rapidly ascending convective columns are poorly understood due to the difficulties involved with either modeling or in situ sampling of these violent clouds. A large number of ice crystals are no doubt generated when droplets freeze at about -40 C. However, at higher levels, these crystals are likely depleted due to precipitation and detrainment. As the ice surface area decreases, the relative humidity can increase well above ice saturation, resulting in bursts of ice nucleation. We will present simulations of these processes using a large-eddy simulation model with detailed microphysics. Size bins are included for aerosols, liquid droplets, ice crystals, and mixed-phase (ice/liquid) hydrometers. Microphysical processes simulated include droplet activation, freezing, melting, homogeneous freezing of sulfate aerosols, and heterogeneous ice nucleation. We are focusing on the importance of ice nucleation events in the upper part of the cloud at temperatures below -40 C. We will show that the ultimate evolution of the cloud in this region (and the anvil produced by the convection) is sensitive to these ice nucleation events, and hence to the composition of upper tropospheric aerosols that get entrained into the convective column.

Jensen, Eric↗
NASA NTRS2012

Climate Impacts of Ice Nucleation

Several different ice nucleation parameterizations in two different General Circulation Models (GCMs) are used to understand the effects of ice nucleation on the mean climate state, and the Aerosol Indirect Effects (AIE) of cirrus clouds on climate. Simulations have a range of ice microphysical states that are consistent with the spread of observations, but many simulations have higher present-day ice crystal number concentrations than in-situ observations. These different states result from different parameterizations of ice cloud nucleation processes, and feature different balances of homogeneous and heterogeneous nucleation. Black carbon aerosols have a small (0.06 Wm(exp-2) and not statistically significant AIE when included as ice nuclei, for nucleation efficiencies within the range of laboratory measurements. Indirect effects of anthropogenic aerosols on cirrus clouds occur as a consequence of increasing anthropogenic sulfur emissions with different mechanisms important in different models. In one model this is due to increases in homogeneous nucleation fraction, and in the other due to increases in heterogeneous nucleation with coated dust. The magnitude of the effect is the same however. The resulting ice AIE does not seem strongly dependent on the balance between homogeneous and heterogeneous ice nucleation. Regional effects can reach several Wm2. Indirect effects are slightly larger for those states with less homogeneous nucleation and lower ice number concentration in the base state. The total ice AIE is estimated at 0.27 +/- 0.10 Wm(exp-2) (1 sigma uncertainty). This represents a 20% offset of the simulated total shortwave AIE for ice and liquid clouds of 1.6 Wm(sup-2).

Gettelman, Andrew↗
NASA NTRS1994

Ice nucleation in the upper troposphere: Sensitivity to aerosol number density, temperature, and cooling rate

We have investigated the processes that control ice crystal nucleation in the upper troposphere using a numerical model. Nucleation of ice resulting from cooling was simulated for a range of aerosol number densities, initial temperatures, and cooling rates. In contrast to observations of stratus clouds, we find that the number of ice crystals that nucleate in cirrus is relatively insensitive to the number of aerosols present. The ice crystal size distribution at the end of the nucleation process is unaffected by the assumed initial aerosol number density. Essentially, nucleation continues until enough ice crystals are present such that their deposition growth rapidly depletes the vapor and shuts off any further nucleation. However, the number of ice crystals nucleated increases rapidly with decreasing initial temperature and increasing cooling rate. This temperature dependence alone could explain the large ice crystal number density observed in very cold tropical cirrus.

Jensen, E. J.↗
NASA NTRS2015

Thermodynamic Derivation of the Activation Energy for Ice Nucleation

Cirrus clouds play a key role in the radiative and hydrological balance of the upper troposphere. Their correct representation in atmospheric models requires an understanding of the microscopic processes leading to ice nucleation. A key parameter in the theoretical description of ice nucleation is the activation energy, which controls the flux of water molecules from the bulk of the liquid to the solid during the early stages of ice formation. In most studies it is estimated by direct association with the bulk properties of water, typically viscosity and self-diffusivity. As the environment in the ice-liquid interface may differ from that of the bulk, this approach may introduce bias in calculated nucleation rates. In this work a theoretical model is proposed to describe the transfer of water molecules across the ice-liquid interface. Within this framework the activation energy naturally emerges from the combination of the energy required to break hydrogen bonds in the liquid, i.e., the bulk diffusion process, and the work dissipated from the molecular rearrangement of water molecules within the ice-liquid interface. The new expression is introduced into a generalized form of classical nucleation theory. Even though no nucleation rate measurements are used to fit any of the parameters of the theory the predicted nucleation rate is in good agreement with experimental results, even at temperature as low as 190 K, where it tends to be underestimated by most models. It is shown that the activation energy has a strong dependency on temperature and a weak dependency on water activity. Such dependencies are masked by thermodynamic effects at temperatures typical of homogeneous freezing of cloud droplets; however, they may affect the formation of ice in haze aerosol particles. The new model provides an independent estimation of the activation energy and the homogeneous ice nucleation rate, and it may help to improve the interpretation of experimental results and the development of parameterizations for cloud formation.

Cirrus clouds↗
NASA NTRS1994

A study of Type I polar stratospheric cloud formation

Mechanisms for the formation of Type I (nitric acid-based) polar stratospheric clouds (PSCs) are discussed. If the pre-existing sulfate aerosols are liquid prior to PSC formation, then nitric acid particles (Type Ib) form by HNO3 dissolution in aqueous H2SO4 solution droplets. This process does not require a nucleation step for the formation of HNO3 aerosols, so most pre-existing aerosols grow to become relatively small HNO3-containing particles. At significantly lower temperatures, the resulting supercooled solutions (Type Ib) may freeze to form HNO3 ice particles (Type Ia). If the pre-existing sulfate aerosols are initially solid before PSC formation, then HNO3 vapor can be deposited directly on the frozen sulfate particles. However, because an energy barrier to the condensation exists a nucleation mechanism is involved. Here, we suggest a unique nucleation mechanism that involves formation of HNO3/H20 solutions on the sulfate ice particles. These nucleation processes may be highly selective, resulting in the formation of relatively small number of large particles.

Tabazadeh, A.↗
NASA NTRS2016

On the Importance of High Frequency Gravity Waves for Ice Nucleation in the Tropical Tropopause Layer

Recent investigations of the influence of atmospheric waves on ice nucleation in cirrus have identified a number of key processes and sensitivities: (1) ice concentrations produced by homogeneous freezing are strongly dependent on cooling rates, with gravity waves dominating upper tropospheric cooling rates; (2) rapid cooling driven by high-frequency waves are likely responsible for the rare occurrences of very high ice concentrations in cirrus; (3) sedimentation and entrainment tend to decrease ice concentrations as cirrus age; and (4) in some situations, changes in temperature tendency driven by high-frequency waves can quench ice nucleation events and limit ice concentrations. Here we use parcel-model simulations of ice nucleation driven by long-duration, constant-pressure balloon temperature time series, along with an extensive dataset of cold cirrus microphysical properties from the recent ATTREX high-altitude aircraft campaign, to statistically examine the importance of high-frequency waves as well as the consistency between our theoretical understanding of ice nucleation and observed ice concentrations. The parcel-model simulations indicate common occurrence of peak ice concentrations exceeding several hundred per liter. Sedimentation and entrainment would reduce ice concentrations as clouds age, but 1-D simulations using a wave parameterization (which underestimates rapid cooling events) still produce ice concentrations higher than indicated by observations. We find that quenching of nucleation events by high-frequency waves occurs infrequently and does not prevent occurrences of large ice concentrations in parcel simulations of homogeneous freezing. In fact, the high-frequency variability in the balloon temperature data is entirely responsible for production of these high ice concentrations in the simulations.

simulation↗
NASA NTRS2017

Cirrus Susceptibility to Changes in Ice Nuclei: Physical Processes, Model Uncertainties, and Measurement Needs

In this talk, I will begin by discussing the physical processes that govern the competition between heterogeneous and homogeneous ice nucleation in upper tropospheric cirrus clouds. Next, I will review the current knowledge of low-temperature ice nucleation from laboratory experiments and field measurements. I will then discuss the uncertainties and deficiencies in representations of cirrus processes in global models used to estimate the climate impacts of changes in cirrus clouds. Lastly, I will review the critical field measurements needed to advance our understanding of cirrus and their susceptibility to changes in aerosol properties.

Jensen, Eric↗
NASA NTRS2023

A 1D Model for Nucleation of Ice From Aerosol Particles: An Application to a Mixed-Phase Arctic Stratus Cloud Layer

Mixed-phase clouds (MPCs) have been identified as significant contributors to uncertainties in climate projections, attributable to model representation of processes controlling the formation and loss of supercooled water droplets and ice particles from the atmosphere. Arctic MPCs are commonly widespread and long-lived, with sustained ice crystal formation processes that challenge current understanding. This study examines the ice-nucleating particle (INP) reservoir dynamics governing immersion-mode heterogeneous freezing in an observed case of Arctic MPCs using a simplified 1D aerosol-cloud model. The model setup includes prescribed dynamical forcings and thermodynamic profiles, and represents INPs as multicomponent and polydisperse particle size distributions. Diagnostic and prognostic approaches to immersion freezing parameterization are compared, including time-independent (singular) number- and surface area-based descriptions and a time-dependent description following classical nucleation theory (CNT). The choice of freezing parameterization defines the size of the INP reservoir. The CNT-based description yields an orders of magnitude larger INP reservoir than the singular parameterizations, which is the dominant factor for sustained ice crystal formation. The efficiency of the freezing process and cloud cooling are of secondary importance. A diagnostic treatment neglecting INP loss is only accurate when the INP reservoir size is large and INP depletion weak. Since a larger INP reservoir sustains ice crystal formation substantially longer, and ice water path scales with ice crystal concentrations for the conditions considered, resolving the source of differences in INP reservoir dynamics due to model implementation is a high priority for advancing climate model physics.

aerosol↗
NASA NTRS2018

Thermodynamic and Dynamic Aspects of Ice Nucleation

It is known that ice nucleating particles (INP) immersed within supercooled droplets promote the formation of ice. Common theoretical models used to represent this process assume that the immersed particle lowers the work of ice nucleation without significantly affecting the dynamics of water in the vicinity of the particle. This is contrary to evidence showing that immersed surfaces significantly affect the viscosity and diffusivity of vicinal water. To study how this may affect ice formation this work introduces a model linking the ice nucleation rate to the modification of the dynamics and thermodynamics of vicinal water by immersed particles. It is shown that INP that significantly reduce the work of ice nucleation also pose strong limitations to the growth of the nascent ice germs. This leads to the onset of a new ice nucleation regime, called spinodal ice nucleation, where the dynamics of ice germ growth instead of the ice germ size determines the nucleation rate. Nucleation in this regime is characterized by an enhanced sensitivity to particle area and cooling rate. Comparison of the predicted ice nucleation rate against experimental measurements for a diverse set of species relevant to cloud formation suggests that spinodal ice nucleation may be common in nature.

Barahona, Donifan↗
NASA NTRS2023

Importance of Ice Nucleation and Precipitation on Climate With the Parameterization of Unified Microphysics Across Scales Version 1 (PUMASv1)

Cloud microphysics is critical for weather and climate prediction. In this work, we document updates and corrections to the cloud microphysical scheme used in the Community Earth System Model (CESM) and other models. These updates include a new nomenclature for the scheme, now called Parameterization of Unified Microphysics Across Scales (PUMAS), and the ability to run the scheme on graphics processing units (GPUs). The main science changes include refactoring an ice number limiter and associated changes to ice nucleation, adding vapor deposition onto snow, and introducing an implicit numerical treatment for sedimentation. We also detail the improvements in computational performance that can be achieved with GPU acceleration. We then show the impact of these scheme changes on the (a) mean state climate, (b) cloud feedback response to warming, and (c) aerosol forcing. We find that corrections are needed to the immersion freezing parameterization and that ice nucleation has important impacts on climate. We also find that the revised scheme produces less cloud liquid and ice but that this can be adjusted by changing the loss process for cloud liquid (autoconversion). Furthermore, there are few discernible effects of the PUMAS changes on cloud feedbacks but some reductions in the magnitude of aerosol–cloud interactions (ACIs). Small cloud feedback changes appear to be related to the implicit sedimentation scheme, with a number of factors affecting ACIs.

Clouds↗
NASA NTRS2000

GCSS Cirrus Parcel Model Comparison Project

The Cirrus Parcel Model Comparison Project, a project of GCSS Working Group on Cirrus Cloud Systems (WG2), involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. The goal of this project is to document and understand the factors resulting in significant inter-model differences. The intent is to foment research leading to model improvement and validation. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (-40 C) and "cold" (-60 C) cirrus subject to updrafts of 4, 20 and 100 cm/s, respectively. Five models participated. These models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze drops) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found for the homogeneous-nucleation-only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, non-negligible quantitative differences are found. Detailed analysis reveals that the homogeneous nucleation formulation, aerosol size, ice crystal growth rate (particularly the deposition coefficient), and water vapor uptake rate are critical components that lead to differences in predicted microphysics. Systematic bias exists between results based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies, but each includes assumptions that can only be justified by further laboratory data. Consequently, it is not yet clear if the two approaches can be made consistent. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 cm/s) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice nucleation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of ice number concentration and ice crystal diffusional growth rate, which is sensitive to the deposition coefficient when ice particles are small, partially controls the peak nucleation rate achieved in an air parcel and the duration of the active nucleation time period. The effects of heterogeneous nucleation are most pronounced in weak updraft situations. Vapor competition by the nucleated (heterogeneous) ice crystals limits the achieved ice supersaturation and thus suppresses the contribution of homogeneous nucleation. Correspondingly, ice crystal number density is markedly reduced. Definitive laboratory and atmospheric benchmark data are needed for the heterogeneous nucleation process. Inter-model differences are correspondingly greater than in the case of the homogeneous nucleation process acting alone.

Lin, Ruei-Fong↗