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NASA NTRS2004

Investigation of Polar Stratospheric Cloud Solid Particle Formation Mechanisms Using ILAS and AVHRR Observations in the Arctic

Satellite observations of denitrification and ice clouds in the Arctic lower stratosphere in February 1997 are used with Lagrangian microphysical box model calculations to evaluate nucleation mechanisms of solid polar stratospheric cloud (PSC) particles. The occurrences of ice clouds are not correlated in time and space with the locations of back trajectories of denitrified air masses, indicating that ice particle surfaces are not always a prerequisite for the formation of solid PSCs that lead to denitrification. In contrast, the model calculations incorporating a pseudoheterogeneous freezing process occurring at the vapor-liquid interface can quantitatively explain most of the observed denitrification when the nucleation activation free energy for nitric acid dihydrate formation is raised by only approx.10% relative to the current published values. Once nucleated, the conversion of nitric acid dihydrate to the stable trihydrate phase brings the computed levels of denitrification closer to the measurements. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Sb~lctureC: loud physics and chemistry; 0340 Atmospheric Composition and Structure: Middle atmosphere-composition and chemistry

Irie, H.↗

NASA NTRS2008

Understanding Ice Supersaturation, Particle Growth, and Number Concentration in Cirrus Clouds

Many factors control the ice supersaturation and microphysical properties in cirrus clouds. We explore the effects of dynamic forcing, ice nucleation mechanisms, and ice crystal growth rate on the evolution and distribution of water vapor and cloud properties in nighttime cirrus clouds using a one-dimensional cloud model with bin microphysics and remote sensing measurements obtained at the Department of Energy's Atmospheric Radiation Measurement (ARM) Climate Research Facility located near Lamont, OK. We forced the model using both large-scale vertical ascent and, for the first time, mean mesoscale velocity derived from radar Doppler velocity measurements. Both heterogeneous and homogeneous nucleation processes are explored, where a classical theory heterogeneous scheme is compared with empirical representations. We evaluated model simulations by examining both bulk cloud properties and distributions of measured radar reflectivity, lidar extinction, and water vapor profiles, as well as retrieved cloud microphysical properties. Our results suggest that mesoscale variability is the primary mechanism needed to reproduce observed quantities. Model sensitivity to the ice growth rate is also investigated. The most realistic simulations as compared with observations are forced using mesoscale waves, include fast ice crystal growth, and initiate ice by either homogeneous or heterogeneous nucleation. Simulated ice crystal number concentrations (tens to hundreds particles per liter) are typically two orders of magnitude smaller than previously published results based on aircraft measurements in cirrus clouds, although higher concentrations are possible in isolated pockets within the nucleation zone.

Comstock, Jennifer M.↗

NASA NTRS1993

Three dimensional modeling of cirrus during the 1991 FIRE IFO 2: Detailed process study

A three-dimensional model of cirrus cloud formation and evolution, including microphysical, dynamical, and radiative processes, was used to simulate cirrus observed in the FIRE Phase 2 Cirrus field program (13 Nov. - 7 Dec. 1991). 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 of solution drops, growth by water vapor deposition, evaporation, aggregation, and vertical transport. Visible and infrared radiative fluxes, and radiative heating rates are calculated using the two-stream algorithm described by Toon et al. Wind velocities, diffusion coefficients, and temperatures were taken from the MAPS analyses and the MM4 mesoscale model simulations. Within the model, moisture is transported and converted to liquid or vapor by the microphysical processes. The simulated cloud bulk and microphysical properties are shown in detail for the Nov. 26 and Dec. 5 case studies. Comparisons with lidar, radar, and in situ data are used to determine how well the simulations reproduced the observed cirrus. The roles played by various processes in the model are described in detail. The potential modes of nucleation are evaluated, and the importance of small-scale variations in temperature and humidity are discussed. The importance of competing ice crystal growth mechanisms (water vapor deposition and aggregation) are evaluated based on model simulations. Finally, the importance of ice crystal shape for crystal growth and vertical transport of ice are discussed.

Jensen, Eric J.↗

NASA NTRS1981

A molecular model for ice nucleation and growth, attachment 2

The central field empirical pair potential model is applied to studying the effects of kinks, ledges, and vacancies on the absorption of water molecules from the vapor. Molecular dynamics simulations indicate that cluster and/or surface modes play a primary role in the absorption process, the flexibility of the hydrogen bond serves to decrease the energy required for structural interconversion, and the rapid distribution of added energy in a hydrogen bonded system lead to aggregate stability which greatly exceeds that predicted by static energy calculations.

Hale, B. N.↗

NASA NTRS1988

Evolution of polar stratospheric clouds during the Antarctic winter

The occurrence of Polar Stratospheric Clouds (PSCs), initially inferred from satellite measurements of solar extinction, have now also been noted by the recent scientific expeditions in the Antarctic. The presence of such clouds in the Antarctic has been postulated to play a significant role in the depletion of ozone during the transition from winter to spring. The mechanisms suggested involve both dynamical and chemical processes which, explicity or implicitly, are associated with the ice particles constituting the PSCs. It is, thus, both timely and necessary to investigate the evolution of these clouds and ascertain the nature and magnitude of their influences on the state of the Antarctic stratosphere. To achieve these objectives, a detailed microphysical model of the processes governing the growth and sublimation of ice particles in the polar stratosphere was developed, based on the investigations of Ramaswamy and Detwiler. The present studies focus on the physical processes that occur at temperatures below those required for the onset of ice deposition from the vapor phase. Once these low temperatures are attained, the deposition of water vapor onto nucleation particles becomes extremely significant. First, the factors governing the magnitude of growth and the growth rate of ice particles at various altitudes are examined. Second, the ice phase mechanisms are examined in the context of a column model with altitudes ranging from 100 to 5 mb pressure levels. The column microphysical model was used to perform simulations of the cloud evolution, using the observed daily temperatures. The effect due to the growth of the particles on the radiation fields are also investigated using a one dimensional radiative transfer model. Specifically, the perturbations in the longwave cooling and that in the shortwave heating for the late winter/early spring time period are analyzed.

Ramaswamy, V.↗

NASA NTRS1994

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.↗

NASA NTRS2021

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

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

Marine cold air outbreaks↗

NASA NTRS1992

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.↗

NASA NTRS1997

Turbulent Distortion of Condensate Accretion

When a simple model for the relationship between the density-temperature fluctuation correlation and mean values is used, we determine that the rate of change of turbulent intensity can influence directly the accretion rate of droplets. Considerable interest exists in the accretion rate for condensates in nonequilibrium flow with icing and the potential role which reactant accretion can play in nonequilibrium exothermic reactant processes. Turbulence is thought to play an important role in such flows. It has already been experimentally determined that turbulence influences the sizes of droplets in the heterogeneous nucleation of supersaturated vapors. This paper addresses the issue of the possible influence of turbulence on the accretion rate of droplets.

Hazoume, R.↗

NASA NTRS2016

The South Residual CO2 Cap on Mars: Investigations with a Mars Global Climate Model

The CO2 cycle is one of the three controlling climate cycles on Mars. One aspect of the CO2 cycle that is not yet fully understood is the existence of a residual CO2 ice cap that is offset from the south pole. Previous investigations suggest that the atmosphere could control the placement of the south residual cap (e.g., Colaprete et al., 2005). These investigations show that topographically forced stationary eddies in the south during southern hemisphere winter produce colder atmospheric temperatures and increased CO2 snowfall over the hemisphere where the residual cap resides. Since precipitated CO2 ice produces higher surface albedos than directly deposited CO2 ice, it is plausible that CO2 snowfall resulting from the zonally asymmetric atmospheric circulation produces surface ice albedos high enough to maintain a residual cap only in one hemisphere. Our current work builds on these initial investigations with a version of the NASA Ames Mars Global Climate Model (GCM) that includes a sophisticated CO2 cloud microphysical scheme. Processes of cloud nucleation, growth, sedimentation, and radiative effects are accounted for. Simulated results thus far agree well with the Colaprete et al. study—the zonally asymmetric nature of the atmospheric circulation produces enhanced snowfall over the residual cap hemisphere throughout much of the winter season. However, the predicted snowfall patterns vary significantly with season throughout the cap growth and recession phases. We will present a detailed analysis of the seasonal evolution of the predicted atmospheric circulation and snowfall patterns to more fully evaluate the hypothesis that the atmosphere controls the placement of the south residual cap.

climate cycles on Mars↗

NASA NTRS1989

Physical processes in polar stratospheric ice clouds

The formulation and evolution of polar stratospheric ice clouds are simulated using a one-dimensional model of cloud microphysics. It is found that the optical thickness and particle size of ice clouds depend on the cooling rate of the air in which the cloud formed. It is necessary that there be an energy barrier to ice nucleation upon the preexisting aerosols in order to account for the cooling rate dependence of the cloud properties.

Toon, Owen B.↗

NASA NTRS2020

The Prevalence of Precipitation from Polar Supercooled Clouds

Supercooled clouds substantially impact polar surface energy budgets but large-scale models often underestimate their occurrence, which motivates accurately establishing metrics of basic processes. An analysis of long-term measurements at Utqiaġvik, Alaska, and McMurdo Station, Antarctica, combines lidar-validated use of soundings to identify supercooled cloud layers and colocated ground-based profiling radar measurements to quantify cloud base precipitation. We find that more than 85 % (75 %) of sampled supercooled layers are precipitating over the Arctic (Antarctic) site, with more than 75 % (50 %) precipitating continuously to the surface. Such high frequencies can be reconciled with substantially lesser spaceborne estimates by considering differences in radar hydrometeor detection sensitivity. While ice precipitation into supercooled clouds from aloft is common, we also find that the great majority of supercooled cloud layers without ice falling into them are themselves continuously generating precipitation. Such sustained primary ice formation is consistent with continuous activation of immersion-mode ice nucleating particles (INPs), suggesting that supercooled cloud formation is a principal gateway to ice formation at temperatures greater than ~ −38 °C over polar regions. The prevalence of weak precipitation fluxes is also consistent with supercooled cloud longevity, and with well-observed and widely simulated case studies. An analysis of colocated microwave radiometer retrievals suggests that weak precipitation fluxes can be nonetheless consequential to moisture budgets for supercooled clouds owing to small liquid water paths. Finally, we suggest that these ground-based precipitation rate statistics offer valuable guidance for improving the representation of polar cloud processes in large-scale models.

Polar clouds↗

NASA NTRS2013

Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations

An extratropical cyclone that crossed the United States on 9-11 April 2009 was successfully simulated at high resolution (3-km horizontal grid spacing) using the Colorado State University Regional Atmospheric Modeling System. The sensitivity of the associated warm front to increasing pollution levels was then explored by conducting the same experiment with three different background profiles of cloud-nucleating aerosol concentration. To the authors' knowledge, no study has examined the indirect effects of aerosols on warm fronts. The budgets of ice, cloud water, and rain in the simulation with the lowest aerosol concentrations were examined. The ice mass was found to be produced in equal amounts through vapor deposition and riming, and the melting of ice produced approximately 75% of the total rain. Conversion of cloud water to rain accounted for the other 25%. When cloud-nucleating aerosol concentrations were increased, significant changes were seen in the budget terms, but total precipitation remained relatively constant. Vapor deposition onto ice increased, but riming of cloud water decreased such that there was only a small change in the total ice production and hence there was no significant change in melting. These responses can be understood in terms of a buffering effect in which smaller cloud droplets in the mixed-phase region lead to both an enhanced vapor deposition and decreased riming efficiency with increasing aerosol concentrations. Overall, while large changes were seen in the microphysical structure of the frontal cloud, cloud-nucleating aerosols had little impact on the precipitation production of the warm front.

ice↗

NASA NTRS2021

The Prevalence of Precipitation From Polar Supercooled Clouds

Supercooled clouds substantially impact polar surface energy budgets, but large-scale models often underestimate their occurrence, which motivates accurately establishing metrics of basic processes. An analysis of long-term measurements at Utqiaġvik, Alaska, and McMurdo Station, Antarctica, combines lidar-validated use of soundings to identify supercooled cloud layers and colocated ground-based profiling radar measurements to quantify cloud base precipitation. We find that more than 85 % (75 %) of sampled supercooled layers are precipitating over the Arctic (Antarctic) site, with more than 75 % (50 %) precipitating continuously to the surface. Such high frequencies can be reconciled with substantially lesser spaceborne estimates by considering differences in radar hydrometeor detection sensitivity. While ice precipitation into supercooled clouds from aloft is common, we also find that the great majority of supercooled cloud layers without ice falling into them are themselves continuously generating precipitation. Such sustained primary ice formation is consistent with continuous activation of immersion-mode ice-nucleating particles (INPs), suggesting that supercooled cloud formation is a principal gateway to ice formation at temperatures greater than ∼−38 ∘C over polar regions. The prevalence of weak precipitation fluxes is also consistent with supercooled cloud longevity and with well-observed and widely simulated case studies. An analysis of colocated microwave radiometer retrievals suggests that weak precipitation fluxes can be nonetheless consequential to moisture budgets for supercooled clouds owing to small liquid water paths. The results here also demonstrate that the observed abundance of mixed-phase clouds can vary substantially with instrument sensitivity and methodology. Finally, we suggest that these ground-based precipitation rate statistics offer valuable guidance for improving the representation of polar cloud processes in large-scale models.

Supercooled clouds↗

NASA NTRSDate not supplied

TPSAS-NF1676L-10947-DND

There are large uncertainties in quantifying dust effects on the climate because of the limitations on the measurements and observations of dust-cloud-precipitation-dynamics interactions. As a major terrestrial source of atmospheric aerosols, dusts may serve as a significant climate forcing for the changing climate due to its effect on solar and thermal radiation as well as on clouds and precipitation processes. Latest satellites measurements enable us to determine dust loadings and cloud distributions and can potentially be used to reduce the uncertainties in the estimations of aerosol effects on climate. This study uses sensors on various satellites to investigate the impact of mineral dust on cloud microphysical and precipitation processes in convective systems. A trans-Atlantic dust outbreak of Saharan origin occurring in early March 2004 is considered. For the observed convective systems under a given convective strength, small hydrometeors were found more prevalent in the dusty stratiform regions than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust regions, particularly at altitudes where heterogeneous nucleation of mineral dust prevails, further supports the observed changes of clouds and precipitation. These microphysical effects of the dusts on clouds are to shift the size spectrum of precipitation-sized hydrometeors from heavy precipitation to light precipitation and ultimately to suppress precipitation and increase the lifecycle of cloud systems, especially for stratiform clouds.

B Lin↗

NASA NTRS2010

Changes in Stratiform Clouds of Mesoscale Convective Complex Introduced by Dust Aerosols

Aerosols influence the earth s climate through direct, indirect, and semi-direct effects. There are large uncertainties in quantifying these effects due to limited measurements and observations of aerosol-cloud-precipitation interactions. As a major terrestrial source of atmospheric aerosols, dusts may serve as a significant climate forcing for the changing climate because of its effect on solar and thermal radiation as well as on clouds and precipitation processes. Latest satellites measurements enable us to determine dust aerosol loadings and cloud distributions and can potentially be used to reduce the uncertainties in the estimations of aerosol effects on climate. This study uses sensors on various satellites to investigate the impact of mineral dust on cloud microphysical and precipitation processes in mesoscale convective complex (MCC). A trans-Atlantic dust outbreak of Saharan origin occurring in early March 2004 is considered. For the observed MCCs under a given convective strength, small hydrometeors were found more prevalent in the dusty stratiform regions than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust regions, particularly at altitudes where heterogeneous nucleation of mineral dust prevails, further supports the observed changes of clouds and precipitation. The consequences of the microphysical effects of the dust aerosols were to shift the size spectrum of precipitation-sized hydrometeors from heavy precipitation to light precipitation and ultimately to suppress precipitation and increase the lifecycle of cloud systems, especially over stratiform areas.

Lin, B.↗

NASA NTRS2003

Effect of Viscosity on the Crystallization of Undercooled Liquids

There have been numerous studies of glasses indicating that low-gravity processing enhances glass formation. NASA PI s are investigating the effect of low-g processing on the nucleation and crystal growth rates. Dr. Ethridge is investigating a potential mechanism for glass crystallization involving shear thinning of liquids in 1-g. For shear thinning liquids, low-g (low convection) processing will enhance glass formation. The study of the viscosity of glass forming substances at low shear rates is important to understand these new crystallization mechanisms. The temperature dependence of the viscosity of undercooled liquids is also very important for NASA s containerless processing studies. In general, the viscosity of undercooled liquids is not known, yet knowledge of viscosity is required for crystallization calculations. Many researchers have used the Turnbull equation in error. Subsequent nucleation and crystallization calculations can be in error by many orders of magnitude. This demonstrates the requirement for better methods for interpolating and extrapolating the viscosity of undercooled liquids. This is also true for undercooled water. Since amorphous water ice is the predominant form of water in the universe, astrophysicists have modeled the crystallization of amorphous water ice with viscosity relations that may be in error by five orders-of-magnitude.

Source record↗

NASA NTRS2001

Carbon Dioxide Clouds at High Altitude in the Tropics and in an Early Dense Martian Atmosphere

We use a time dependent, microphysical cloud model to study the formation of carbon dioxide clouds in the Martian atmosphere. Laboratory studies by Glandor et al. show that high critical supersaturations are required for cloud particle nucleation and that surface kinetic growth is not limited. These conditions, which are similar to those for cirrus clouds on Earth, lead to the formation of carbon dioxide ice particles with radii greater than 500 micrometers and concentrations of less than 0.1 cm(exp -3) for typical atmospheric conditions. Within the current Martian atmosphere, CO2 cloud formation is possible at the poles during winter and at high altitudes in the tropics during periods of increased atmospheric dust loading. In both cases, temperature perturbations of several degrees below the CO2 saturation temperature are required to nucleate new cloud particles suggesting that dynamical processes are the most common initiators of carbon dioxide clouds rather than diabatic cooling. The microphysical cloud model, coupled to a two-stream radiative transfer model, is used to reexamine the impact of CO2 clouds on the surface temperature within a dense CO2 atmosphere. The formation of carbon dioxide clouds leads to a warmer surface than what would be expected for clear sky conditions. The amount of warming is sensitive to the presence of dust and water vapor in the atmosphere, both of which act to dampen cloud effects. The radiative warming associated with cloud formation, as well as latent heating, work to dissipate the clouds when present. Thus, clouds never last for periods much longer than several days, limiting their overall effectiveness for warming the surface. The time average cloud optical depth is approximately unity leading to a 5-10 K warming, depending on the surface pressure. However, the surface temperature does not rise about the freezing point of liquid water even for pressures as high as 5 bars, at a solar luminosity of 75% the current value.

Colaprete, Anthony↗