A hybrid data, modeling and deep learning approach for prediction of the small-scale dynamics of the upper troposphere
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Ice Clouds↗
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An airborne, miniaturized cloud condensation nuclei counter: SBIR Phase I Final Report
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47 OTHER INSTRUMENTATION↗
Dynamic compression effects of H 2 O in a dynamic diamond anvil cell: Origin of metastable ice VII and its crystal growth kinetics
We report on the structural verification of metastable ice VII solidifying in the phase space of ice VI at 1.80 GPa at room temperature. Using time-resolved (TR) x-ray diffraction and TR ruby luminescence paired with high-speed microphotography utilizing a dynamic diamond anvil cell, an initial compression rate range from 0.12 to 95.84 GPa/s was explored. The solidification pressure of metastable ice VII has a potential sigmoidal dependence upon compression rate with a turnover compression rate of ∼80 GPa/s. The preferred crystallization of ice VII in the stability field of ice VI is due to the increased nucleation rate of ice VII over ice VI at 1.77 GPa that is driven by the surface energy difference between the liquid and solid phases along with the change in Gibbs free energy of solidification. The dynamic pressure-volume–compression behaviors of ice phases (VI and VII) show a lattice stiffening in both phases, especially during the compression loading. It is also found that the compression rate greatly affects the solid-solid phase transition between ice VI and VII but does not affect the liquid-solid transition between water and ice VI as much. Lastly, a third phase transition was found to occur after metastable ice VII transforms into high-density amorphous (HDA) ice, which could be a disordered hydrogen-bonded network configuration of ice VII forming out of HDA ice facilitated by the decoupling of the oxygen movement and reorientation of the H 2 O molecule. These results demonstrate the complexity of a seemingly simple molecule H 2 O, how it can readily change its static properties with the modification of (de)compression rate, and highlight the need to use multiple TR structural and spectroscopic probes at higher time resolutions to realize the most comprehensive understanding.
Chemical bonding↗
Microphysics and Radiative Properties of Cirrus: Instrumentation and Analysis
Work under this grant has involved further development of a new aircraft instrument (the cloudscope) for real time characterization of atmospheric particulates together with field observations of such particulates, both in the form of ice and also as nuclei responsible for nucleation of both ice and water cloud particles. Part of the work involving assessment of the frequency of ice crystal shapes has been carried out in collaboration with the Meteorological Service of Canada; part of the work in a field program with the NCAR C-130. Part of the work has been interpreted in terms of laboratory simulation of ice crystal growth under a wide variety of conditions carried out under a grant from Physical Meteorology Program, National Science Foundation.
Hallett, John↗
TPSAS-NF1676L-13393-DND
In the two plus decades since it became evident that polar stratospheric clouds (PSCs) play a major role in the springtime depletion of polar ozone, the detailed composition and morphology of PSCs has been an area of interest. Although our PSC knowledge base is substantial, there is still considerable uncertainty in specific key areas related to their composition and formation. Probably the least well understood of these is the nucleation process responsible for the formation of nitric acid trihydrate (NAT) particles and the circumstances under which NAT formation and growth leads to stratospheric denitrification. CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) is an excellent instrument for observing PSCs and has already produced an extensive set of PSC observations with unprecedented spatial and temporal resolution covering five winters. These observations are providing new insight into the key remaining questions regarding PSC composition and formation mechanisms. In this paper, we examine the CALIOP PSC observations in combination with a microphysical model in attempt to better understand the underlying physical mechanisms for NAT nucleation. Of particular interest is the early phase of the 2009-2010 Arctic winter when CALIOP frequently observed extended regions of tenuous NAT clouds, clearly before ice was present in the polar vortex. This provides unprecedented large-scale evidence that ice particles are not the only nuclei on which NAT may form. Microphysical model calculations along backward trajectories from these CALIOP NAT cloud observations are used to investigate possible ice-independent, heterogeneous NAT nucleation mechanisms. These analyses will then be expanded to other winters to assess the overall significance of an ice-independent nucleation mechanism for NAT PSCs.
M C Pitts↗
Demonstration of neutron radiation-induced nucleation of supercooled water
In this study, we present direct evidence for neutrons causing nucleation of supercooled water. Highly purified water (20 nm filtration) is cooled to well below freezing (as low as −20 °C) with a radioactive calibration source of neutrons/gamma-rays either present or removed during each of many control cooling runs for the same volume of water. When it is primarily neutrons irradiating the sample bulk, the non-equilibrium freezing point (also known as the “supercooling point”) is, on average, +0.7 °C warmer than the control equivalent, with a statistical significance of greater than 5 Sigma, with systematic uncertainty included. This effect is not observed with water in the presence of gamma-rays instead of neutrons. While these neutrons should have theoretically had sufficient energy to mount the energy barrier, corroborating our results, their raising of supercooling temperature has never been reported experimentally to the best of our knowledge. The potential to use deeply supercooled solutions, not only water, as metastable detectors for radiation and perhaps dark matter or neutrino physics presents now a new avenue for exploration.
Szydagis, Matthew↗
Characterizing Surface Ice-Philicity Using Molecular Simulations and Enhanced Sampling
The formation of ice, which plays an important role in diverse contexts ranging from cryopreservation to atmospheric science, is often mediated by solid surfaces. Although surfaces that interact favorably with ice (relative to liquid water) can facilitate ice formation by lowering nucleation barriers, the molecular characteristics that confer ice-philicity to a surface are complex and incompletely understood. To address this challenge, here we introduce a robust and computationally efficient method for characterizing surface ice-philicity that combines molecular simulations and enhanced sampling techniques to quantify the free energetic cost of increasing surface–ice contact at the expense of surface–water contact. Using this method to characterize the ice-philicity of a family of model surfaces that are lattice matched with ice but vary in their polarity, we find that the nonpolar surfaces are moderately ice-phobic, whereas the polar surfaces are highly ice-philic. In contrast, for surfaces that display no complementarity to the ice lattice, we find that ice-philicity is independent of surface polarity and that both nonpolar and polar surfaces are moderately ice-phobic. Furthermore, our work thus provides a prescription for quantitatively characterizing surface ice-philicity and sheds light on how ice-philicity is influenced by lattice matching and polarity.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Attendee Response to Guiding Questions of the September 2014 DOE Workshop on North Slope of Alaska Priorities
We advocate for several modeling approaches suitable to prove understanding of and capability to model aerosol behavior in nucleating droplets and ice and to model regional cloud systems at the mesoscale. The full complement of data that is ideal for particular study types is increasingly well understood; the ASR ISDAC Science Plan provides an excellent example of listing the data required for each study type targeted by that campaign. Whereas discussion here focused on the microscale and mesoscale, other studies should obviously focus on the regional, seasonal and global scale. When considering ice microphysics alone, laser focus on unconstrained model components could be usefully intensified (e.g., collision-coalescence kernels). Similarly, a focus on boundary layer structure would be deeply valuable to a wide range of model types. The expense of observations motivates efficient planning for observational data sets to support specific study approaches; the concept of closure is often useful (e.g., the surface energy budget).
nucleation↗
The Structural Properties of Vapor Deposited Water Ice and Astrophysical Implications
Films of vapor deposited water ice at low temperature (T<30 K) show a number of interesting structural changes during a gradual warmup. We would like to talk about the structure of the low temperature high density amorphous form of water ice, the process of crystallization, and some recent work on the morphological changes of water ice films at high temperature. The studies of the high density amorphous form are from in-situ electron microscopy as well as numerical simulations of molecular dynamics and have lead to new insights into the physical distinction between this high density amorphous form and the low density amorphous form. For the process of crystallization, we propose a model that describes the crystallization of water ice from the amorphous phase to cubic ice in terms of the nucleation of small domains in the ice. This model agrees well with the behavior of water ice in our electron microscopy studies and finds that pure water above the glass transition is a strong liquid. In more recent work, we have concentrated on temperatures above the crystallization temperature and we find interesting morphological changes related to the decrease in viscosity of the amorphous component in the cubic crystalline regime. Given enough time, we would like to put these results in an astrophysical context and discuss some observed features of the frost on interstellar grains and the bulk ice in comets.
Jenniskens, P.↗
Ice crystal growth in a dynamic thermal diffusion chamber
Ice crystals were grown in a supersaturated environment produced by a dynamic thermal diffusion chamber, which employed two horizontal plates separated by a distance of 2.5 cm. Air was circulated between and along the 1.2 m length of the plates past ice crystals which nucleated and grew from a fiber suspended vertically between the two plates. A zoom stereo microscope with a magnification which ranged from 3X to 80X and both 35 mm still photographs and 16 mm time lapse cine films taken through the microscope were used to study the variation of the shape and linear growth rate of ice crystals as a function of the ambient temperature, the ambient supersaturation, and the forced ventilation velocity. The ambient growth conditions were varied over the range of temperature 0 to -40 C, over the range of supersaturation 4% to 50% with respect to ice, and over the range of forced ventilation velocities 0 cm/s to 20 cm/s.
Keller, V. W.↗
Measurements of the aerosol and ice crystal populations in tropical stratospheric cumulonimbus anvils
A pair of particle size spectrometers was flown aboard the NASA U-2 operating from the Canal Zone to make measurements of the aerosol and ice crystal budgets in cirrus produced by thunderstorms in the tropics. Measurements indicate that fairly large crystals up to 1 mm in size are injected into the stratosphere during cumulonimbus activity. Ice water contents range from a few thousandths to a few hundredths of a gram per cubic meter. Because the ambient temperature is typically around -80 C the mass of the larger crystals largely returns to lower altitudes before evaporating. Aerosol size distributions indicate a curious narrow growth mode between 0.15 and 0.2 micron in cirrus anvils which is absent outside these clouds. The presence of this narrow mode is attributed to near water saturation produced at cloud top. Nucleation of new ice crystals as well as aerosol is hypothesized
Knollenberg, R. G.↗
The Mars Dust Cycle: Investigating the Effects of Radiatively Active Water Ice Clouds on Surface Stresses and Dust Lifting Potential with the NASA Ames Mars General Circulation Model
The dust cycle is a critically important component of Mars' current climate system. Dust is present in the atmosphere of Mars year-round but the dust loading varies with season in a generally repeatable manner. Dust has a significant influence on the thermal structure of the atmosphere and thus greatly affects atmospheric circulation. The dust cycle is the most difficult of the three climate cycles (CO2, water, and dust) to model realistically with general circulation models. Until recently, numerical modeling investigations of the dust cycle have typically not included the effects of couplings to the water cycle through cloud formation. In the Martian atmosphere, dust particles likely provide the seed nuclei for heterogeneous nucleation of water ice clouds. As ice coats atmospheric dust grains, the newly formed cloud particles exhibit different physical and radiative characteristics. Thus, the coupling between the dust and water cycles likely affects the distributions of dust, water vapor and water ice, and thus atmospheric heating and cooling and the resulting circulations. We use the NASA Ames Mars GCM to investigate the effects of radiatively active water ice clouds on surface stress and the potential for dust lifting. The model includes a state-of-the-art water ice cloud microphysics package and a radiative transfer scheme that accounts for the radiative effects of CO2 gas, dust, and water ice clouds. We focus on simulations that are radiatively forced by a prescribed dust map, and we compare simulations that do and do not include radiatively active clouds. Preliminary results suggest that the magnitude and spatial patterns of surface stress (and thus dust lifting potential) are substantial influenced by the radiative effects of water ice clouds.
Kahre, Melinda A.↗
A study of mesospheric rocket contrails and clouds produced by liquid-fueled rockets
Changes in the atmospheric composition, particularly through the condensation of rocket vehicle exhaust, caused by the flights of 400 heavy lift launch vehicles (HLLV) to carry crews and materials into space to build a satellite solar power system (SPS) were examined. Attention was given to the formation of mesospheric contrails and clouds. A one-dimensional model was used to formulate the photochemistry and vertical transport of water vapor, its nucleation into an ice cloud, and the microphysical development of the cloud. Considering one HLLV launch per day for a decade, it is projected that the upper atmosphere water vapor concentration would be increased by 10-20%, thereby augmenting the size and opacity of natural noctilucent clouds by 50%. No climatological consequences are foreseen from the clouds, although spectacular noctiluminescent cloud displays are thought to be possible.
Turco, R. P.↗
Antarctic NAT PSC Belt of June 2003: Observational Validation of the Mountain Wave Seeding Hypothesis
Satellite observations of polar stratospheric clouds (PSCs) over Antarctica in June 2003 revealed small nitric acid trihydrate (NAT) particles forming suddenly along the vortex edge. Models suggest the trigger was mountain waves over the Antarctic Peninsula (AP) forming ice for NAT nucleation. We test this hypothesis by analyzing perturbations in stratospheric radiances from the Atmospheric Infrared Sounder (AIRS). AIRS data show mountain waves over the AP on 10-14 June, with no resolved wave activity before or after. Peak wave temperature amplitudes derived from independent 40 hPa channels all return values of 10-12 K, in agreement with values used to model this NAT event. These observations support a NAT wake from a small region of mountain wave activity over the AP as the source of this circumpolar NAT outbreak.
PSC (POLAR STRATOSPHERIC CLOUDS)↗
Study of Ice Particle Formation and Lifetime in Space Environment
The ice particles are formed when liquid and/or humid gases vent to the space. These submicroscopic ice particles are potential contamination sources of the environments during Skylab operations. The critical size of ice particle and its nucleation rate based on the theory of homogeneous and heterogeneous nucleation by sublimation are analyzed. The equations which are pertinent for studying the growth and evaporation of the ice particles are formulated. The mechanisms affecting the lifetime of ice particle are discussed. The gas dynamic techniques for experimental study of ice particle formation are proposed.
Jeng, D.↗
Cirrus cloud model parameterizations: Incorporating realistic ice particle generation
Recent cirrus cloud modeling studies have involved the application of a time-dependent, two dimensional Eulerian model, with generalized cloud microphysical parameterizations drawn from experimental findings. For computing the ice versus vapor phase changes, the ice mass content is linked to the maintenance of a relative humidity with respect to ice (RHI) of 105 percent; ice growth occurs both with regard to the introduction of new particles and the growth of existing particles. In a simplified cloud model designed to investigate the basic role of various physical processes in the growth and maintenance of cirrus clouds, these parametric relations are justifiable. In comparison, the one dimensional cloud microphysical model recently applied to evaluating the nucleation and growth of ice crystals in cirrus clouds explicitly treated populations of haze and cloud droplets, and ice crystals. Although these two modeling approaches are clearly incompatible, the goal of the present numerical study is to develop a parametric treatment of new ice particle generation, on the basis of detailed microphysical model findings, for incorporation into improved cirrus growth models. For example, the relation between temperature and the relative humidity required to generate ice crystals from ammonium sulfate haze droplets, whose probability of freezing through the homogeneous nucleation mode are a combined function of time and droplet molality, volume, and temperature. As an example of this approach, the results of cloud microphysical simulations are presented showing the rather narrow domain in the temperature/humidity field where new ice crystals can be generated. The microphysical simulations point out the need for detailed CCN studies at cirrus altitudes and haze droplet measurements within cirrus clouds, but also suggest that a relatively simple treatment of ice particle generation, which includes cloud chemistry, can be incorporated into cirrus cloud growth.
Sassen, Kenneth↗
Microphysical modeling of cirrus. 2: Sensitivity studies
The one-dimensional cirrus model described in part 1 of this issue has been used to study the sensitivity of simulated cirrus microphysical and radiative properties to poorly known model parameters, poorly understood physical processes, and environmental conditions. Model parameters and physical processes investigated include nucleation rate, mode of nucleation (e.g., homogeneous freezing of aerosols and liquid droplets or heterogeneous deposition), ice crystal shape, and coagulation. These studies suggest that the leading sources of uncertainty in the model are the phase change (liquid-solid) energy barrier and the ice-water surface energy which dominate the homogeneous freezing nucleation rate and the coagulation sticking efficiency at low temperatures which controls the production of large ice crystals (radii greater than 100 mcirons). Environmental conditions considered in sensitivity tests were CN size distribution, vertical wind speed, and cloud height. We found that (unlike stratus clouds) variations in the total number of condensation nuclei (NC) have little effect on cirrus microphysical and radiative properties, since nucleation occurs only on the largest CN at the tail of the size distribution. The total number of ice crystals which nucleate has little or no relationship to the number of CN present and depends primarily on the temperature and the cooling rate. Stronger updrafts (more rapid cooling) generate higher ice number densities, ice water content, cloud optical depth, and net radiative forcing. Increasing the height of the clouds in the model leads to an increase in ice number density, a decrease in effective radius, and a decrease in ice water content. The most prominent effect of increasing cloud height was a rapid increase in the net cloud radiative forcing which can be attributed to the change in cloud temperature as well as change in cloud ice size distributions. It has long been recognized that changes in cloud height or cloud area have the greatest potential for causing feedbacks on climate change. Our results suggest that variations in vertical velocity or cloud microphysical changes associatd with cloud height changes may also be important.
Jensen, Eric J.↗
Highly supercooled riming and unusual triple-frequency radar signatures over McMurdo Station, Antarctica
Abstract. 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.
54 ENVIRONMENTAL SCIENCES↗