Variability of Ice Supersaturation, Nucleation, and Cirrus in TTL Vertical Layers
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DiGangi, Joshua P,↗
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Lidar Measurements of Relative Humidity and Ice Supersaturation in the Upper Troposphere
We compute upper tropospheric relative humidity profiles using water vapor profiles measured by an airborne DIAL and a ground-based Raman lidar.
LASE↗
Bluntness and Supersaturation Effects on the Second Mode Instability in Mach 10 Flow
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Hypersonics↗
Improved Cloud Condensation Nucleus Spectrometer
An improved thermal-gradient cloud condensation nucleus spectrometer (CCNS) has been designed to provide several enhancements over prior thermal- gradient counters, including fast response and high-sensitivity detection covering a wide range of supersaturations. CCNSs are used in laboratory research on the relationships among aerosols, supersaturation of air, and the formation of clouds. The operational characteristics of prior counters are such that it takes long times to determine aerosol critical supersaturations. Hence, there is a need for a CCNS capable of rapid scanning through a wide range of supersaturations. The present improved CCNS satisfies this need. The improved thermal-gradient CCNS (see Figure 1) incorporates the following notable features: a) The main chamber is bounded on the top and bottom by parallel thick copper plates, which are joined by a thermally conductive vertical wall on one side and a thermally nonconductive wall on the opposite side. b) To establish a temperature gradient needed to establish a supersaturation gradient, water at two different regulated temperatures is pumped through tubes along the edges of the copper plates at the thermally-nonconductive-wall side. Figure 2 presents an example of temperature and supersaturation gradients for one combination of regulated temperatures at the thermally-nonconductive-wall edges of the copper plates. c) To enable measurement of the temperature gradient, ten thermocouples are cemented to the external surfaces of the copper plates (five on the top plate and five on the bottom plate), spaced at equal intervals along the width axis of the main chamber near the outlet end. d) Pieces of filter paper or cotton felt are cemented onto the interior surfaces of the copper plates and, prior to each experimental run, are saturated with water to establish a supersaturation field inside the main chamber. e) A flow of monodisperse aerosol and a dilution flow of humid air are introduced into the main chamber at the inlet end. The inlet assembly is designed to offer improved (relative to prior such assemblies) laminar-flow performance within the main chamber. Dry aerosols are subjected to activation and growth in the supersaturation field. f) After aerosol activation, at the outlet end of the main chamber, a polished stainless-steel probe is used to sample droplets into a laser particle counter. The probe features an improved design for efficient sampling. The counter has six channels with size bins in the range of 0.5- to 5.0-micron diameter. g) To enable efficient sampling, the probe is scanned along the width axis of the main chamber (thereby effecting scanning along the temperature gradient and thereby, further, effecting scanning along the supersaturation gradient) by means of a computer-controlled translation stage.
Leu, Ming-Taun↗
Modeling the Growth Rates of Tetragonal Lysozyme Crystal Faces
The measured macroscopic growth rates of the (110) and (101) faces of tetragonal lysozyme show an unexpectedly complex dependence on the supersaturation. The growth rates decay asymptotically to zero when the supersaturation is lowered to zero and increase rapidly when the supersaturation is increased. When supersaturations are increased still further the growth rates attain a maximum before starting to decrease. However, growth of these crystals is known to proceed by the classical dislocation and 2D nucleation growth mechanisms. This anomaly can be explained if growth is assumed to occur not by monomer units but by lysozyme aggregates. Analysis of the molecular packing of these crystals revealed that they were constructed of strongly bonded 4(sub 3) helices, while weaker bonds were responsible for binding the helices to each other. It follows that during crystal growth the stronger bonds are formed before the weaker ones. Thus, the growth of these crystals could be viewed as a two step process: aggregate growth units corresponding to the 4(sub 3) helix are first formed in the bulk solution by stronger intermolecular bonds and then attached to the crystal face by weaker bonds on dislocation hillocks or 2D islands. This will lead to a distribution of aggregates in the solution with monomers and lower order aggregates being predominant at low supersaturations and higher order aggregates being predominant at high supersaturations. If the crystal grows mostly by higher order aggregates, such as tetramers and octamers, it would explain the anomalous dependence of the growth rates on the supersaturation. Besides the analysis of molecular packing, a comprehensive analysis of the measured (110) and (101) growth rates was also undertaken in this study. The distribution of aggregates in lysozyme nutrient solutions at various solution conditions were determined from reversible aggregation reactions at equilibrium. The supersaturation was defined for each aggregate species with respect to its concentration at saturation in order to apply growth rate models to this process. The measured growth rates were then compared with the predicted ones from several dislocation and 2D nucleation growth models, employing tetramer and octamer growth units in polydisperse solutions and monomer units in monodisperse solutions. For the (110) face, the calculations consistently showed that the measured growth rates followed the expected model relations with octamer growth units. For the (101) face, it is not possible to obtain a clear agreement between the predicted and measured growth rates for a single growth unit as done for the (110) face. However, the calculations do indicate that the average size of the growth unit is between a tetramer and an octamer. This suggests that tetramers, octamers and other intermediate size growth units all participate in the growth process for this face. These calculations show that it is possible to model the macroscopic protein crystal growth rates if the molecular level processes can be account for, particularly protein aggregation processes in the bulk solution. Our recent investigations of tetragonal lysozyme crystals employing high resolution atomic force microscopy scans have further confirmed the growth of these crystals by aggregate growth units corresponding to 4(sub 3) helices.
Li, Meirong↗
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↗
Growth of (101) Faces of Tetragonal Lysozyme Crystals: Measured Growth Rate Trends
Earlier extensive measurements of the growth rates of the (110) face of tetragonal lysozyme crystals had shown unexpected dependencies on the supersaturation. In this study similar growth rate measurements were done for the (101) faces of the crystals. The data show a similar dependence on the supersaturation, becoming appreciable only at high supersaturations, reaching a maximum value and then decreasing. As reported in earlier studies, the (101) growth rates are larger at low supersaturations than the (110) growth rates at the same conditions, and smaller at high supersaturations. These trends suggest that the growth mechanism of the (101) is similar to that of the (110) face, involving the addition of lysozyme aggregates formed in solution, but with a growth unit smaller than that of the (110) face.
Forsythe, Elizabeth L.↗
Growth of (101) faces of tetragonal lysozyme crystals: measured growth-rate trends
Previous extensive measurements of the growth rates of the (110) face of tetragonal lysozyme crystals have shown unexpected dependencies on the supersaturation. In this study, similar growth-rate measurements were performed for the (101) faces of the crystals. The data show a similar dependence on the supersaturation, becoming appreciable only at high supersaturations, reaching a maximum value and then decreasing. The (101) growth rates are larger at low supersaturations than the (110) growth rates under the same conditions and are smaller at high supersaturations. These trends suggest that the growth mechanism of the (101) face is similar to that of the (110) face: both processes involve the addition of multimeric growth units formed in solution, but the average size of the units for the (101) face is likely to be smaller than for the (110) face.
Egg Proteins/chemistry↗
Measurable characteristics of lysozyme crystal growth
The behavior of protein crystal growth is estimated from measurements performed at both the microscopic and molecular levels. In the absence of solutal flow, it was determined that a model that balances the macromolecular flux toward the crystal surface with the flux of the crystal surface well characterizes crystal growth observed using microscopic methods. Namely, it was determined that the model provides accurate estimates for the crystal-growth velocities upon evaluation of crystal-growth measurements obtained in time. Growth velocities thus determined as a function of solution supersaturation were further interpreted using established deterministic models. From analyses of crystal-growth velocities, it was found that the mode of crystal growth varies with respect to increasing solution supersaturation, possibly owing to kinetic roughening. To verify further the hypothesis of kinetic roughening, crystal growth at the molecular level was examined using atomic force microscopy (AFM). From the AFM measurements, it was found that the magnitude of surface-height fluctuations, h(x), increases with increasing solution supersaturation. In contrast, the estimated characteristic length, xi, decreases rapidly upon increasing solution supersaturation. It was conjectured that the magnitude of both h(x) and xi could possibly determine the mode of crystal growth. Although the data precede any exact theory, the non-critical divergence of h(x) and xi with respect to increasing solution supersaturation was nevertheless preliminarily established. Moreover, approximate models to account for behavior of both h(x) and xi are also presented.
Muramidase/chemistry↗
Description of the NRL isothermal haze chamber
In the IHC the critical supersaturation is inferred from the measurement of the size of particles which have grown to their equilibrium size at exactly 100 percent RH. The largest size channel corresponds to a critical supersaturation of 0.014 percent. The growth time required for particles of this size to reach their equilibrium size exceeds the 110 second residence time in the IHC. Since the supersaturation spectrum is always very steep in this region, the contribution of these larger particles which have not yet attained their equilibrium size to smaller size channels is negligible. However, failure of these particles to reach their equilibrium size could result in a significant lowering of the count in the size channel corresponding to the smaller critical supersaturation.
Hoppel, W. A.↗
A new method to measure homogeneous nucleation rates in shock tubes
The centered expansion wave of a shock tube is utilized to expand and supersaturate a condensable vapor in small concentration in an inert carrier gas. The supersaturated state, located at the rear of the expansion wave, is preserved for a controlled period and then terminated by a recompressing shock wave. During the period of supersaturation, condensation nuclei are formed homogeneously. The nucleation rate is measured as a function of supersaturation by a Mie-light scattering technique. The method is tested using water and the results are compared with classical nucleation theory.
Peters, F.↗
Homogeneous nucleation kinetics
Homogeneous nucleation kinetics are rederived in a manner fundamentally similar to the approach of classical nucleation theory with the following modifications and improvements. First, the cluster is a parent phase cluster and does not require energization to the parent state. Second, the thermodynamic potential used to describe phase stability is a continuous function along the pathway of phase decomposition. Third, the kinetics of clustering corresponds directly to the diffusional flux of monomers through the cluster distribution and are formally similar to classical theory with the resulting kinetic equation modified by two terms in the preexponential factor. These terms correct for the influence of a supersaturation dependent clustering within the parent phase and for the influence of an asymmetrical cluster concentration as a function of cluster size at the critical cluster size. Fourth, the supersaturation dependence of the nucleation rate is of the same form as that given by classical nucleation theory. This supersaturation dependence must however be interpreted in terms of a size dependent surface tension. Finally, there are two scaling laws which describe supersaturation to either constant nucleation rate or to the thermodynamically determined physical spinodal.
Rasmussen, D. H.↗
Protein crystal growth in low gravity
This Final Technical Report for NASA Grant NAG8-774 covers the period from April 27, 1989 through December 31, 1992. It covers five main topics: fluid flow studies, the influence of growth conditions on the morphology of isocitrate lyase crystals, control of nucleation, the growth of lysozyme by the temperature gradient method and graphoepitaxy of protein crystals. The section on fluid flow discusses the limits of detectability in the Schlieren imaging of fluid flows around protein crystals. The isocitrate lyase study compares crystals grown terrestrially under a variety of conditions with those grown in space. The controlling factor governing the morphology of the crystals is the supersaturation. The lack of flow in the interface between the drop and the atmosphere in microgravity causes protein precipitation in the boundary layer and a lowering of the supersaturation in the drop. This lowered supersaturation leads to improved crystal morphology. Preliminary experiments with lysozyme indicated that localized temperature gradients could be used to nucleate crystals in a controlled manner. An apparatus (thermonucleator) was designed to study the controlled nucleation of protein crystals. This apparatus has been used to nucleate crystals of materials with both normal (ice-water, Rochelle salt and lysozyme) and retrograde (horse serum albumin and alpha chymotrypsinogen A) solubility. These studies have lead to the design of an new apparatus that small and more compatible with use in microgravity. Lysozyme crystals were grown by transporting nutrient from a source (lysozyme powder) to the crystal in a temperature gradient. The influence of path length and cross section on the growth rate was demonstrated. This technique can be combined with the thermonucleator to control both nucleation and growth. Graphoepitaxy utilizes a patterned substrate to orient growing crystals. In this study, silicon substrates with 10 micron grooves were used to grow crystals of catalase, lysozyme and canavalin. In all cases, the crystals grew oriented to the substrate. The supersaturation needed for nucleation and growth was lower on the patterned substrates. In some cases, isolated, large crystals were grown.
Feigelson, Robert S.↗
Measurements of cloud condensation nuclei spectra within maritime cumulus cloud droplets: Implications for mixing processes
In a cloud formed during adiabatic expansion, the droplet size distribution will be systematically related to the critical supersaturation of the cloud condensation nuclei (CNN), but this relationship can be complicated in entraining clouds. Useful information about cloud processes, such as mixing, can be obtained from direct measurements of the CNN involved in droplet nucleation. This was accomplished by interfacing two instruments for a series of flights in maritime cumulus clouds. One instrument, the counterflow virtual impactor, collected cloud droplets, and the nonvolatile residual nuclei of the droplets was then passed to a CCN spectrometer, which measured the critical supersaturation (S(sub c)) spectrum of the droplet nuclei. The measured S(sub c) spectra of the droplet nuclei were compared with the S(sub c) spectra of ambient aerosol particles in order to identify which CCN were actually incorporated into droplets and to determine when mixing processes were active at different cloud levels. The droplet nuclei nearly always exhibited lower median S(sub c)'s than the ambient aerosol, as expected since droplets nucleate perferentially on particles with lower critical supersaturations. Critical supersaturation spectra from nuclei of droplets near cloud base were similar to those predicted for cloud regions formed adiabatically, but spectra of droplet nuclei from middle cloud levels showed some evidence that mixing had occurred. Near cloud top, the greatest variation in the spectra of the droplet nuclei was observed, and nuclei with high S(sub c)'s were sometimes present even within relatively large droplets. This suggests that the extent of mixing increases with height in cumulus clouds and that inhomogeneous mixing may be important near cloud top. These promising initial results suggest improvements to the experimental technique that will permit more quantitative results in future experiments.
Twohy, Cynthia H.↗
Metastable Solution Thermodynamic Properties and Crystal Growth Kinetics
The crystal growth rates of NH4H2PO4, KH2PO4, (NH4)2SO4, KAl(SO4)2 central dot 12H2O, NaCl, and glycine and the nucleation rates of KBr, KCl, NaBr central dot 2H2O, (NH4)2Cl, and (NH4)2SO4 were expressed in terms of the fundamental driving force of crystallization calculated from the activity of supersaturated solutions. The kinetic parameters were compared with those from the commonly used kinetic expression based on the concentration difference. From the viewpoint of thermodynamics, rate expressions based on the chemical potential difference provide accurate kinetic representation over a broad range of supersaturation. The rates estimated using the expression based on the concentration difference coincide with the true rates of crystallization only in the concentration range of low supersaturation and deviate from the true kinetics as the supersaturation increases.
Kim, Soojin↗
The Effect of Solution Conditions on the Nucleation Kinetics of Tetragonal Lysozyme Crystals
An understanding of protein crystal nucleation rates and the effect of solution conditions upon them, is fundamental to the preparation of protein crystals of the desired size and shape for X-ray diffraction analysis. The ability to predict the effect of supersaturation, temperature, pH and precipitant concentration on the number and size of crystals formed is of great benefit in the pursuit of protein structure analysis. In this study we experimentally examine the effect of supersaturation, temperature, pH and sodium chloride concentration on the nucleation rate of tetragonal chicken egg white lysozyme crystals. In order to do this batch crystallization plates were prepared at given solution concentrations and incubated at three different temperatures over the period of one week. The number of crystals per well with their size and dimensions were recorded and correlated against solution conditions. Duplicate experiments indicate the reproducibility of the technique. Although it is well known that crystal numbers increase with increasing supersaturation, large changes in crystal number were also correlated against solution conditions of temperature, pH and salt concentration over the same supersaturation ranges. Analysis of these results enhance our understanding of the effect of solution conditions such as the dramatic effect that small changes in charge and ionic strength can have on the number of tetragonal lysozyme crystals that form and grow in solution.
Judge, Russell A.↗
Tropospheric Lapse Rate and Methane on Titan
We have reanalyzed the Voyager radio occultation data for Titan with two alternative approaches to methane condensation. In one approach, methane condensation is enhanced by the presence of nitrogen. In the other approach, methane condensation does not occur. As pointed out by Thompson, nitrogen lowers the condensation level for a methane/nitrogen Mixture and we find that the upper limit on surface relative humidity of methane obtained from the Voyager occultation data is lowered from 0.7 to 0.6. However, 140% supersaturation of methane in the troposphere, suggested by Courtin et al., allows all surface humidities to be consistent with the Voyager occultation data and the upper limit is set by other considerations. We conclude that if supersaturation is not included then the surface relative humidity of methane is between 0.08 and 0.6, with values close to 0.6 indicated. If supersaturation is included then the surface relative humidity of methane is between 0.08 and 0.85, again, with values close to 0.6 indicated. The tropospheric lapse rate on Titan appears to be determined by radiative equilibrium. It is everywhere stable against dry convection but is unstable to moist convection. This is consistent with a supersaturated atmosphere in which condensation - and hence moist convection - is inhibited. The absence of dry convection in the troposphere of Titan can be explained by a simple grey model which shows that the radiative profile of any gas for which the ratio of the gas constant to the specific heat at constant pressure is greater than 0.25 never becomes unstable to dry convection.
McKay, C. P.↗
Ice Cloud Formation and Dehydration in the Tropical Tropopause Layer
Stratospheric water vapor is important not only for its greenhouse forcing, but also because it plays a significant role in stratospheric chemistry. several recent studies have focused on the potential for dehydration due to ice cloud formation in air rising slowly through the tropical tropopause layer. Holton and Gettelman showed that temperature variations associated with horizontal transport of air in the tropopause layer can drive ice cloud formation and dehydration, and Gettelman et al. recently examined the cloud formation and dehydration along kinematic trajectories using simple assumptions about the cloud properties. In this study, we use a Lagrangian, one-dimensional cloud model to further investigate cloud formation and dehydration as air is transported horizontally and vertically through the tropical tropopause layer. Time-height curtains of temperature are extracted from meteorological analyses. The model tracks the growth and sedimentation of individual cloud particles. The regional distribution of clouds simulated in the model is comparable to the subvisible cirrus distribution indicated by SAGE II. The simulated cloud properties depend strongly on the assumed ice supersaturation threshold for ice nucleation. with effective nuclei present (low supersaturation threshold), ice number densities are high (0.1--10 cm(circumflex)-3), and ice crystals do not grow large enough to fall very far, resulting in limited dehydration. With higher supersaturation thresholds, ice number densities are much lower (less than 0.01 cm(circumflex)-3), and ice crystals grow large enough to fall substantially; however, supersaturated air often crosses the tropopause without cloud formation. The clouds typically do not dehydrate the air along trajectories down to the temperature minimum saturation mixing ratio. Rather the water vapor mixing ratio crossing the tropopause along trajectories is typically 10-50% larger than the saturation mixing ratio.
Jensen, Eric↗