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At least 19 records

Formation of a Tropopause Cirrus Layer Observed over Florida during CRYSTAL-FACE

On July 13, 2002 a widespread, subvisible tropopause cirrus layer occurred over the Florida region. This cloud was observed in great detail with the NASA Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) instrumentation, including in situ measurements with the WB-57 aircraft. In this paper, we use the 13 July cloud as a case study to evaluate the physical processes controlling the formation and evolution of tropopause cirrus layers. Microphysics measurements indicate that ice crystal diameters in the cloud layer ranged from about 7 to 50 microns, and the peak number mode was about 10-25 microns. In situ water vapor and temperature measurements in the cloud indicated supersaturation with respect to ice throughout, with ice saturation ratios as large as 1.8. Even when the ice surface area density was as high as about 500 sq microns/cu cm, ice supersaturations of 20-30% were observed. Trajectory analysis shows that the air sampled near the tropopause on this day generally came from the north and cooled considerably during the previous few days. Examination of infrared satellite imagery along air parcel back trajectories from the WB-57 flight track indicates that the tropopause cloud layer formation was, in general, not simply left over ice from recently generated anvil cirrus. Simulations of cloud formation using time-height curtains of temperature along the trajectory paths show that the cloud could have formed in situ near the tropopause as the air was advected into the south Florida region and cooled to unusually low temperatures. If we assume a high threshold for ice nucleation via homogeneous freezing of aqueous sulfate aerosols, the model reproduces the observed cloud structure, ice crystal size distributions, and ice supersaturation statistics. Inclusion of observed gravity wave temperature perturbations in the simulations is essential to reproduce the observed cloud properties. Without waves, crystal number densities are too low, crystal sizes are too large, and the crystals fall out too fast, leaving very little cloud persisting at the end of the simulations. In the cloud simulations, coincidence of high supersaturations and high surface areas can be produced by either recent nucleation or sedimentation of crystals into supersaturated layers. The agreement between model results and observed supersaturations is improved somewhat if we assume that the steady state relative humidity within cirrus at T<200 K is enhanced by about 30%. The WB-57 measurements and the model results suggest that the cloud layer irreversibly dehydrated air near the tropopause.

Jensen, Eric↗

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↗

Homogeneous Aerosol Freezing in the Tops of High-Altitude Tropical Cumulonimbus Clouds

Numerical simulations of deep, intense continental tropical convection indicate that when the cloud tops extend more than a few kilometers above the liquid water homogeneous freezing level, ice nucleation due to freezing of entrained aqueous sulfate aerosols generates large concentrations of small crystals (diameters less than approx. equal to 20 micrometers). The small crystals produced by aerosol freezing have the largest impact on cloud-top ice concentration for convective clouds with strong updrafts but relatively low aerosol concentrations. An implication of this result is that cloud-top ice concentrations in high anvil cirrus can be controlled primarily by updraft speeds in the tops of convective plumes and to a lesser extent by aerosol concentrations in the uppermost troposphere. While larger crystals precipitate out and sublimate in subsaturated air below, the population of small crystals can persist in the saturated uppermost troposphere for many hours, thereby prolonging the lifetime of remnants from anvil cirrus in the tropical tropopause layer.

Jensen, E. J.↗

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↗

On the Ice Nucleation Spectrum

This work presents a novel formulation of the ice nucleation spectrum, i.e. the function relating the ice crystal concentration to cloud formation conditions and aerosol properties. The new formulation is physically-based and explicitly accounts for the dependency of the ice crystal concentration on temperature, supersaturation, cooling rate, and particle size, surface area and composition. This is achieved by introducing the concepts of ice nucleation coefficient (the number of ice germs present in a particle) and nucleation probability dispersion function (the distribution of ice nucleation coefficients within the aerosol population). The new formulation is used to generate ice nucleation parameterizations for the homogeneous freezing of cloud droplets and the heterogeneous deposition ice nucleation on dust and soot ice nuclei. For homogeneous freezing, it was found that by increasing the dispersion in the droplet volume distribution the fraction of supercooled droplets in the population increases. For heterogeneous ice nucleation the new formulation consistently describes singular and stochastic behavior within a single framework. Using a fundamentally stochastic approach, both cooling rate independence and constancy of the ice nucleation fraction over time, features typically associated with singular behavior, were reproduced. Analysis of the temporal dependency of the ice nucleation spectrum suggested that experimental methods that measure the ice nucleation fraction over few seconds would tend to underestimate the ice nuclei concentration. It is shown that inferring the aerosol heterogeneous ice nucleation properties from measurements of the onset supersaturation and temperature may carry significant error as the variability in ice nucleation properties within the aerosol population is not accounted for. This work provides a simple and rigorous ice nucleation framework where theoretical predictions, laboratory measurements and field campaign data can be reconciled, and that is suitable for application in atmospheric modeling studies.

Barahona, D.↗

Ice Nucleation in the Tropical Tropopause Layer: Implications for Cirrus Occurrence, Cirrus Microphysical Properties, and Dehydration of Air Entering the Stratosphere

Recent laboratory experiments have advanced our understanding of the physical properties and ice nucleating abilities of aerosol particles atlow temperatures. In particular, aerosols containing organics will transition to a glassy state at low temperatures, and these glassy aerosols are moderately effective as ice nuclei. These results have implications for ice nucleation in the cold Tropical Tropopause Layer (TTL; 13-19 km). We have developed a detailed cloud microphysical model that includes heterogeneous nucleation on a variety of aerosol types and homogeneous freezing of aqueous aerosols. This model has been incorporated into one-dimensional simulations of cirrus and water vapor driven by meteorological analysis temperature and wind fields. The model includes scavenging of ice nuclei by sedimenting ice crystals. The model is evaluated by comparing the simulated cloud properties and water vapor concentrations with aircraft and satellite measurements. In this presentation, I will discuss the relative importance of homogeneous and heterogeneous ice nucleation, the impact of ice nuclei scavenging as air slowly ascends through the TTL, and the implications for the final dehydration of air parcels crossing the tropical cold-point tropopause and entering the tropical stratosphere.

tropopause↗

Aerosol–Ice Formation Closure: A Southern Great Plains Field Campaign

Prediction of ice formation in clouds presents one of the grand challenges in the atmospheric sciences. Immersion freezing initiated by ice-nucleating particles (INPs) is the dominant pathway of primary ice crystal formation in mixed-phase clouds, where supercooled water droplets and ice crystals coexist, with important implications for the hydrological cycle and climate. However, derivation of INP number concentrations from an ambient aerosol population in cloud-resolving and climate models remains highly uncertain. We conducted an aerosol-ice formation closure pilot study using a field-observational approach to evaluate the predictive capability of immersion freezing INPs. The closure study relies on co-located measurements of the ambient size-resolved and single-particle composition and INP number concentrations. The acquired particle data serve as input in several immersion freezing parameterizations, that are employed in cloud-resolving and climate models, for prediction of INP number concentrations. We discuss in detail one closure case study in which a front passed through the measurement site, resulting in a change of ambient particle and INP populations. We achieved closure in some circumstances within uncertainties, but we emphasize the need for freezing parameterization of potentially missing INP types and evaluation of the choice of parameterization to be employed. Overall, this closure pilot study aims to assess the level of parameter details and measurement strategies needed to achieve aerosol-ice formation closure. The closure approach is designed to accurately guide immersion freezing schemes in models, and ultimately identify the leading causes for climate model bias in INP predictions.

ice formation↗

Anvil Glaciation in a Deep Cumulus Updraught over Florida Simulated with the Explicit Microphysics Model. I: Impact of Various Nucleation Processes

Simulations of a cumulonimbus cloud observed in the Cirrus regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) with an advanced version of the Explicit Microphysics Model (EMM) are presented. The EMM has size-resolved aerosols and predicts the time evolution of sizes, bulk densities and axial ratios of ice particles. Observations by multiple aircraft in the troposphere provide inputs to the model, including observations of the ice nuclei and of the entire size distribution of condensation nuclei. Homogeneous droplet freezing is found to be the source of almost all of the ice crystals in the anvil updraught of this particular model cloud. Most of the simulated droplets that freeze to form anvil crystals appear to be nucleated by activation of aerosols far above cloud base in the interior of the cloud ("secondary" or "in cloud" droplet nucleation). This is partly because primary droplets formed at cloud base are invariably depleted by accretion before they can reach the anvil base in the updraught, which promotes an increase with height of the average supersaturation in the updraught aloft. More than half of these aerosols, activated far above cloud base, are entrained into the updraught of this model cloud from the lateral environment above about 5 km above mean sea level. This confirms the importance of remote sources of atmospheric aerosol for anvil glaciation. Other nucleation processes impinge indirectly upon the anvil glaciation by modifying the concentration of supercooled droplets in the upper levels of the mixed-phase region. For instance, the warm-rain process produces a massive indirect impact on the anvil crystal concentration, because it determines the mass of precipitation forming in the updraught. It competes with homogeneous freezing as a sink for cloud droplets. The effects from turbulent enhancement of the warm-rain process and from the nucleation processes on the anvil ice properties are assessed.

Phillips, Vaughan T. J.↗

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↗

Implications of Observed High Supersaturation for TTL Cloud Formation and Dehydration

In situ measurements of water vapor concentration made during the CRYSTAL-FACE and Pre-AVE missions indicate higher than expected supersaturations in both clear and cloudy air near the cold tropical tropopause: (1) steady-state ice supersaturations of 20-30% were measured within cirrus at T < 200 K; (2) supersaturations exceeding 100% (near water saturation) were observed under cloud-free conditions near 187 K. The in-cloud measurements challenge the conventional belief that any water vapor in excess of ice saturation should be depleted by crystal growth given sufficient time. The high clear-sky supersaturations imply that thresholds for ice nucleation due to homogeneous freezing of aerosols (or any other mechanism) are much higher than those inferred from laboratory measurements. We will use simulations of Tropical Tropopause Layer (TTL) transport and cloud formation throughout the tropics to show that these effects have important implications for TTL cloud frequency and freeze-drying of air crossing the tropical tropopause cold trap.

Jensen, Eric↗

African Dust Aerosols as Atmospheric Ice Nuclei

Measurements of the ice nucleating ability of aerosol particles in air masses over Florida having sources from North Africa support the potential importance of dust aerosols for indirectly affecting cloud properties and climate. The concentrations of ice nuclei within dust layers at particle sizes below 1 pn exceeded 1/cu cm; the highest ever reported with our device at temperatures warmer than homogeneous freezing conditions. These measurements add to previous direct and indirect evidence of the ice nucleation efficiency of desert dust aerosols, but also confirm their contribution to ice nuclei populations at great distances from source regions.

DeMott, Paul J.↗

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↗

On the Susceptibility of Cold Tropical Cirrus to Ice Nuclei Abundance

Numerical simulations of cirrus formation in the tropical tropopause layer (TTL) are used to evaluate the impact heterogeneous ice nuclei (IN) abundance on cold cloud microphysical properties. The model includes homogeneous and heterogeneous ice nucleation, deposition growthsublimation, and sedimentation. Reanalysis temperature and wind fields are used to force the simulations, with addition of high-frequency wave temperature variability based on in situ measurements. The model results are constrained by recent in situ observations of TTL cirrus and relative humidity, as well as satellite measurements of cirrus bulk properties and occurrence frequencies. Temperature variability driven by high-frequency waves has a dominant influence on TTL cirrus microphysical properties and occurrence frequencies, and inclusion of these waves is required to produce agreement between the simulated and observed cloud properties as well as the abundance of TTL cirrus. With a composition-independent supersaturation threshold for homogeneous freezing of aqueous aerosols, the model produces excessive ice concentrations compared with in situ observations. Inclusion of relatively numerous heterogeneous nuclei ( 100L) in the simulations improves the agreement with observed ice concentrations. However, when IN contribute significantly to TTL cirrus ice nucleation, the occurrence frequency of large supersaturations with respect to ice is less than indicated by in situ measurements. The simulated TTL cirrus extinction statistics agree with observations (within uncertainties) from both in situ and remote-sensing measurements. We find that the sensitivity of TTL cirrus extinction and ice water content statistics to heterogeneous ice nuclei abundance is relatively weak. Likewise, the simulated occurrence frequencies of TTL cirrus are insensitive to ice nuclei abundance, both in terms of cloud frequency height distribution and regional distribution throughout the tropics.

occurences↗

The impacts of immersion ice nucleation parameterizations on Arctic mixed-phase stratiform cloud properties and the Arctic radiation budget in GEOS-5

The influence of four different immersion freezing parameterizations on Arctic clouds and the top-of-the atmosphere (TOA) and surface radiation fluxes is investigated in the fifth version of the National Aeronautics and Space Administration (NASA) Goddard Earth Observing System (GEOS-5) with sea surface temperature, sea ice fraction and aerosol emissions held fixed. The different parameterizations were derived from a variety of sources, including classical nucleation theory, field and laboratory measurements. Despite the large spread in the ice-nucleating particle (INP) concentrations in the parameterizations, the cloud properties and radiative fluxes had a tendency to form two groups, with the lower INP concentration category producing larger water path and low-level cloud fraction during winter and early spring, whereas the opposite occurred during the summer season. The stability of the lower troposphere was found to strongly correlate with low-cloud fraction, and along with the effect of ice nucleation, ice sedimentation and melting rates, appears to explain the spring-to-summer reversal pattern in the relative magnitude of the cloud properties between the two categories of simulations. The strong modulation effect of the liquid phase on immersion freezing led to the successful simulation of the characteristic Arctic cloud structure, with a layer rich in supercooled water near cloud top and ice and snow at lower levels. Comparison with satellite retrievals and in situ data suggest that simulations with low INP concentrations more realistically represent Arctic clouds and radiation.

Arctic↗

The Role of Composition and Surface Area Variability in Ice Nucleation, and How to Get Rid of It

Ice nucleation active site densities and nucleation rates are commonly determined by measuring the fraction of droplets that freeze at different temperatures. In analysing these experiments it is commonly assumed that variability in the immersed particle surface area and composition within a sample can be neglected, allowing a simple parameterization of ice nucleation efficiencies. Here it is shown that these approximations may result in large error, and translate into a bias in estimated active site densities of about six orders of magnitude. When applied in cloud models it may represent up to 5 K error in cloud glaciation temperature. A solution to this enduring problem is proposed for the first time. It is shown that by performing droplet freezing experiments varying mean particle surface area along with the temperature such a bias can be quantitatively removed. This amounts to differentiating the "freezing rate'' from the ice nucleation coefficient, or, the apparent and the actual active site density of a material. The proposed method will contribute to reduce existing uncertainties in the relative strength of the ice nucleation ability of different aerosol species, and the modeling of mixed-phase clouds.

Barahona, Donifan↗

Cirrus Parcel Model Comparison Phase 2

The Cirrus Parcel Model Comparison (CPMC) project, a project of the GEWEX Cloud System Study Working Group on cirrus clouds (GCSS WG2), is an international effort to advance our knowledge of numerical simulations of cirrus cloud initiation. This project was done in two phases. In Phase 1 of CPMC, the critical components determining the predicted cloud microphysical properties were identified using parcel models in which the aerosol and ice crystal size distributions are explicitly resolved, the formulation of the homogeneous freezing of aqueous solution droplets, especially the gradient of nucleation rate with respect to solution concentration; aerosol growth modeling; and the mass accommodation coefficient of water vapor on ice surface (the deposition coefficient). In Phase 1, all simulations were conducted using a given background aerosol distribution. To complete the comparison study, participant model responses to a range of background aerosol distributions are investigated in Phase 2.

Lin, Ruei-Fong↗

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.↗

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.↗