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All sourcesNASA NTRSDOE OSTI
NASA NTRS2005

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↗
NASA NTRS1991

Doppler indices of gas phase formation in hypobaric environments: Time-intensity analysis

A semi-quantitative method to analyze decompression data is described. It possesses the advantage that it allows a graded response to decompression rather than the dichotomous response generally employed. A generalized critical volume (C-V), or stoichiometric time-dependent equilibrium model is examined that relates the constant of the equation P sub i equals m P sub f plus b to variable tissue supersaturation and gas washout terms. The effects of the tissue ratio on gas phase formation indicate that a decreased ratio yields fewer individuals with Doppler detectable gas bubbles, but those individuals still present with Spencer Grade 3 or 4. This might indicate a local collapse of tissue saturation. The individuals with Grade 3 or 4 could be at risk for type 2 decompression sickness by transpulmonic arterialization. The primary regulator of the problems of decompression sickness is the reduction of local supersaturation, presumably governed by the presence and number of gas micronuclei. It is postulated that a reduction in these nuclei will favor a low incidence of decompression sickness in microgravity secondary to hypokinesia and adynamia.

Powell, Michael R.↗
DOE OSTI2025

Autonomous Infrared and Small (Wide) Angle X-Ray Scattering (IR-S(W)AXS) Capability

Thin water films are 2-D, nanoconfined layers that form on solid surfaces exposed to humid atmospheres—environments ubiquitous across catalysis, corrosion science, soil science, and subsurface geochemistry. At relative humidity (RH) values below saturation, these films are Å–nm thick and exhibit properties that differ sharply from bulk water, including disrupted H-bonding and impeded mass transport. Owing to their high surface-to-volume ratio, dissolution of the solid can rapidly drive strong supersaturation with respect to secondary phases. Reactivity in thin water films is highly sensitive to film thickness, and critically, thickness evolves during reaction because the hygroscopicity of the interfacial system changes as ions accumulate or diminish in the film and as reaction products transform. To accurately probe and control these dynamics, a capability is needed that can measure and automatically maintain a constant water-film thickness while simultaneously monitoring solid dissolution, nucleation, and growth. This project developed an autonomous Infrared/Small Angle X-ray Scattering-Wide Angle X-ray Scattering (IR/(W)SAXS) for investigating reactivity in thin water films on solid surfaces exposed to humidified gases. The capability consists of an IR spectrometer, a (W)SAXS instrument, and a mass flow controller system for generating variably humidified gas flows to a custom reaction cell. Progress on each of the major components of the capability are detailed below.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2004

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

On July 13, 2002, a widespread, thin tropopause cirrus layer occurred over the Florida region. This cloud was observed in great detail with the CRYSTAL-FACE instrumentation, including in-situ measurements with the WB-57 aircraft. We use this cloud case study to evaluate the physical processes controlling the formation and evolution of tropopause cirrus layers. Microphysics indicate ice crystal diameters in the cloud layer ranged from about 7 to 40 um, and the peak number mode was about 10-25 um. 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. TRajectory analysis shows that the air sampled near the tropopause on this day generally came from the north and cooled considerable during the previous days.Examination of visible satellite imagery indicates that the cloud layer formation was, in general, not simply left over ice from convectively generated anvil cirrus.

Jensen, Eric↗
NASA NTRS2008

Formation of Large (Approximately 100 micrometers) Ice Crystals Near the Tropical Tropopause

Recent high-altitude aircraft measurements with in situ imaging instruments indicated the presence of relatively large (approx.100 microns length), thin (aspect ratios of approx.6:1 or larger) hexagonal plate ice crystals near the tropical tropopause in very low concentrations (<0.01/L). These crystals were not produced by deep convection or aggregation. We use simple growth-sedimentation calculations as well as detailed cloud simulations to evaluate the conditions required to grow the large crystals. Uncertainties in crystal aspect ratio leave a range of possibilities, which could be constrained by knowledge of the water vapor concentration in the air where the crystal growth occurred. Unfortunately, water vapor measurements made in the cloud formation region near the tropopause with different instruments ranged from <2 ppmv to approx.3.5 ppmv. The higher water vapor concentrations correspond to very large ice supersaturations (relative humidities with respect to ice of about 200%). If the aspect ratios of the hexagonal plate crystals are as small as the image analysis suggests (6:1, see companion paper (Lawson et al., 2008)) then growth of the large crystals before they sediment out of the supersaturated layer would only be possible if the water vapor concentration were on the high end of the range indicated by the different measurements (>3 ppmv). On the other hand, if the crystal aspect ratios are quite a bit larger (approx.10:1), then H2O concentrations toward the low end of the measurement range (approx.2-2.5 ppmv) would suffice to grow the large crystals. Gravity-wave driven temperature and vertical wind perturbations only slightly modify the H2O concentrations needed to grow the crystals. We find that it would not be possible to grow the large crystals with water concentrations less than 2 ppmv, even with assumptions of a very high aspect ratio of 15 and steady upward motion of 2 cm/s to loft the crystals in the tropopause region. These calculations would seem to imply that the measurements indicating water vapor concentrations less than 2ppmv are implausible, but we cannot rule out the possibility that higher humidity prevailed upstream of the aircraft measurements and the air was dehydrated by the cloud formation. Simulations of the cloud formation with a detailed model indicate that homogeneous freezing should generate ice concentrations larger than the observed concentrations (20/L), and even concentrations as low as 20/L should have depleted the vapor in excess of saturation and prevented growth of large crystals. It seems likely that the large crystals resulted from ice nucleation on effective heterogeneous nuclei at low ice supersaturations. Improvements in our understanding of detailed cloud microphysical processes require resolution of the water vapor measurement discrepancies in these very cold, dry regions of the atmosphere.

Jensen, E. J.↗
NASA NTRS1988

Observations of condensation nuclei in the 1987 airborne Antarctic ozone experiment

The condensation nucleus counter (CNC) flown of the NASA ER-2 in the Airborne Antarctic Ozone Experiment provides a measurement of the number mixing ratio of particles which can be grown by exposure to supersaturated n-butyl alcohol vapor to diameters of a few microns. Such particles are referred to as condensation nuclei (CN). The ER-2 CNC was calibrated with aerosols of known size and concentration and was found to provide an accurate measure of the number concentration of particles larger than about 0.02 micron. Since the number distribution of stratospheric aerosols is usually dominated by particles less than a few tenths of micron in diameter, the upper cutoff of the ER-2 CNC has not been determined experimentally. However, theory suggests that the sampling and counting efficiency should remain near one for particles as large as 1 micron in diameter. Thus, the CN mixing ratio is usually a good measure of the mixing ratio of submicron particles.

Wilson, J. C.↗
DOE OSTI2026

Dependence of CCN closure relationship with organic fraction from two airborne field campaigns over mid-latitude land and ocean

This study investigates the relationship between measured and calculated cloud condensation nuclei (CCN) number concentration and its dependence with organic fraction utilizing aircraft observations from The Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA, 2017–2018) and The Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE, 2016) campaigns, which represent midlatitude marine and continental environments, respectively. For the ACE-ENA marine region, aerosol and CCN concentrations were significantly higher in summer than in winter, whereas at continental site for HI-SCALE, aerosol and CCN concentrations showed no pronounced differences between spring and autumn. Using aerosol chemical composition and number size distribution data, CCN concentrations at various supersaturations are calculated based on Köhler theory and then compared with observations from CCN counter. The results show that CCN closure performs well at both sites with a slight overestimation, with mean closure ratio (CR) of 1.13 and 1.17, respectively. Further investigation reveals that CR at lower supersaturation perform better than that at higher supersaturation. The dependence of CR on organic mass fraction (MForg) varies by environment: for marine aerosols, CR decreases with increasing organic fraction at lower supersaturations, whereas continental aerosols exhibit a consistent overestimation, with CR decreasing as organic fraction increases at higher supersaturations. This study provides key insights into CCN characteristics over midlatitude marine and continental environments, emphasizing the necessity of incorporating size-resolved chemical composition and mixing states into future model parameterizations, and contributing to a better understanding of aerosol–cloud interactions.

ACE-ENA field campaign↗
NASA NTRS1986

Occultation determination of Neptune's oblateness and stratospheric methane mixing ratio

The occultation of a star by Neptune on August 20, 1985 was observed at 2.2 micron wavelength with telescopes at the European Southern Observatory (ESO) and the Cerro Tololo Inter-American Observatory (CTIO). The detection of a 'central flash' midway between immersion and emersion has allowed the determination of Neptune's oblateness and the atmospheric extinction at 2.2 microns, which is related to the stratospheric methane mixing ratio. An oblateness of (2.08 +0.19 or -0.18) x 10 to the 2nd is found and, assuming a stratospheric temperature of 120 K, a value of 0.6 percent is inferred (with an uncertainty of a factor of 10) for the methane mixing ratio (CH4/H2) at 0.3 mbar. The latter value may indicate supersaturation of methane in Neptune's stratosphere.

Lellouch, E.↗
DOE OSTI2026

Reaction Diffusion Modelling of 3D Pillar Electrodes in Single-Catalyst CO 2 Reduction Cascades

Effective electrochemical CO 2 reduction to liquid fuels requires that the local catalytic environment facilitates the desired reactivity, yet a microscopic understanding of this environment is difficult to achieve from experiment alone. In this work, a 3D reaction-diffusion model was developed to explore the effects of electrode surface area and local geometry on the performance of a heterogeneous catalyst that performs a two-step CO 2 reduction cascade reaction to CO and then CH 3 OH under aqueous conditions. Kinetic parameters for the model were inspired by experimental results using a cobalt phthalocyanine (CoPc) catalyst. Three-dimensional architectures composed of arrays of square pillars with varying dimensions and either smooth or periodically modulated surfaces were tested, revealing the extent to which geometry modulates the performance of the cascade reactions. Although structural variations modulate local concentration gradients, we find that electrochemically active surface area predominantly governs the overall cascade reaction. Moreover, the results suggest that supersaturation of CO, with concentrations up to ten-fold higher than the equilibrium solubility limit, might be critical for more efficient conversion to CH 3 OH. For any given geometry, the spatially averaged ratio of [CO] to [CO 2 ] is dictated by the electrochemically active surface area and determines the yield of CH 3 OH. For a fixed surface area, geometries that spatially confine the electrolyte yield moderate local [CO] to [CO 2 ] ratios within small volumes. In contrast, less confining geometries result in a broader distribution of local ratios spread over larger volumes, with both configurations yielding the same spatially averaged [CO] to [CO 2 ] ratio. These insights provide valuable design principles—highlighting the critical importance of surface area and possibly CO supersaturation—for engineering advanced electrode architectures that leverage intermediate trapping and CO supersaturation to enhance overall performance in tandem CO 2 reduction systems.

COMSOL↗
NASA NTRS1999

The Effect of Temperature and Solution pH on the Nucleation of Tetragonal Lysozyme Crystals

Part of the challenge of macromolecular crystal growth for structure determination is obtaining crystals with a volume suitable for x-ray analysis. In this respect an understanding of the effect of solution conditions on macromolecule nucleation rates is advantageous. This study investigated the effects of supersaturation, temperature, and pH on the nucleation rate of tetragonal lysozyme crystals. Batch crystallization plates were prepared at given solution concentrations and incubated at set temperatures over 1 week. The number of crystals per well with their size and axial ratios were recorded and correlated with solution conditions. Crystal numbers were found to increase with increasing supersaturation and temperature. The most significant variable, however, was pH; crystal numbers changed by two orders of magnitude over the pH range 4.0-5.2. Crystal size also varied with solution conditions, with the largest crystals obtained at pH 5.2. Having optimized the crystallization conditions, we prepared a batch of crystals under the same initial conditions, and 50 of these crystals were analyzed by x-ray diffraction techniques. The results indicate that even under the same crystallization conditions, a marked variation in crystal properties exists.

Judge, Russell A.↗
NASA NTRS2000

Quantifying Main Trends in Lysozyme Nucleation: The Effect of Precipitant Concentration and Impurities

Full factorial experiment design incorporating multi-linear regression analysis of the experimental data allows the main trends and effects to be quickly identified while using only a limited number of experiments. These techniques were used to identify the effect of precipitant concentration and the presence of an impurity, the physiological lysozyme dimer, on the nucleation rate and crystal dimensions of the tetragonal form of chicken egg white lysozyme. Increasing precipitant concentration was found to decrease crystal numbers, the magnitude of this effect also depending on the supersaturation. The presence of the dimer generally increased nucleation. The crystal axial ratio decreased with increasing precipitant concentration independent of impurity.

Burke, Michael W.↗
NASA NTRS2000

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 water vapor and MTP temperature profiles acquired from the NASA DC-8 aircraft during the recent Pacific Exploratory Mission Tropics B (PEM Tropics B) field mission in the tropical Pacific and the SAGE-III Ozone Loss and Validation Experiment (SOLVE) in the Arctic as well as water vapor profiles derived from the ground-based DOE ARM Southern Great Plains (SGP) CART Raman lidar are used. Comparisons of the lidar water vapor measurements with available in situ measurements show reasonable agreement for water vapor mixing ratios above 0.05 g/kg. Relative humidity frequency distributions computed using LASE data indicate that ice supersaturation occurred about 5-11% of the time when temperatures were below -35 C. While a higher frequency of ice supersaturation was observed during SOLVE, higher peak values of relative humidity were observed during PEM Tropics B. The relative humidity fields associated with cirrus clouds are also examined.

Ferrare, Richard A.↗
NASA NTRS2001

Precipitation Efficiency in the Tropical Deep Convective Regime

Precipitation efficiency in the tropical deep convective regime is analyzed based on a 2-D cloud resolving simulation. The cloud resolving model is forced by the large-scale vertical velocity and zonal wind and large-scale horizontal advections derived from TOGA COARE for a 20-day period. Precipitation efficiency may be defined as a ratio of surface rain rate to sum of surface evaporation and moisture convergence (LSPE) or a ratio of surface rain rate to sum of condensation and deposition rates of supersaturated vapor (CMPE). Moisture budget shows that the atmosphere is moistened (dryed) when the LSPE is less (more) than 100 %. The LSPE could be larger than 100 % for strong convection. This indicates that the drying processes should be included in cumulus parameterization to avoid moisture bias. Statistical analysis shows that the sum of the condensation and deposition rates is bout 80 % of the sum of the surface evaporation rate and moisture convergence, which ads to proportional relation between the two efficiencies when both efficiencies are less han 100 %. The CMPE increases with increasing mass-weighted mean temperature and creasing surface rain rate. This suggests that precipitation is more efficient for warm environment and strong convection. Approximate balance of rates among the condensation, deposition, rain, and the raindrop evaporation is used to derive an analytical solution of the CMPE.

Li, Xiaofan↗
NASA NTRS1998

Dissolved gases in perennially ice-covered lakes of the McMurdo Dry Valleys, Antarctica

Measurements of dissolved N2, O2, Ar, CO2, and CH4 were made in perennially ice-covered Lake Hoare. Results confirm previous reports that O2 concentrations in the upper water column exceed atmospheric equilibrium and that N2 and Ar are supersaturated throughout the water column. The mean supersaturation of N2 was found to be 2.0 (+/- 0.37) and Ar was 3.8 (+/- 1.1). The ratios of N2/Ar (20.3 +/- 13.8), and O2/Ar (22.5 +/- 4.0) at the ice-water interface are consistent with those previously measured, suggesting that bubble formation is the main process for removing gas from the lake. However, the saturations of N2 and Ar greatly exceed those previously predicted for degassing by bubble formation only at the ice-water interface. The data support the hypothesis that removal of gas by bubbles occurs in the water column to a depth of 11 m in Lake Hoare. CO2 concentration increases from near zero at the ice-water interface to 80-100 times saturation at and below the chemocline at c. 28 m. There is considerable variability in the gas concentrations throughout the water column; samples separated in depth by one metre may vary by more than 50% in gas content. It is likely that this phenomenon results from the lack of turbulent mixing in the water column. Methane (c. 2 micrograms l-1) was detected below the chemocline and immediately above the sediment/water interface at a depth of 30 m. Samples from lakes Vanda, Joyce, and Miers, also show supersaturations of O2, N2, and Ar at levels similar to levels found in Lake Hoare.

NASA Discipline Exobiology↗
NASA NTRS1998

The Effect of Temperature and Solution pH on Tetragonal Lysozyme Nucleation Kinetics

Part of the challenge of macromolecular crystal growth for structure determination is obtaining an appropriate number of crystals with a crystal volume suitable for x-ray analysis. In this respect an understanding of the effect of solution conditions on macromolecule nucleation rates is advantageous. This study investigated the effects of supersaturation, temperature and pH on the nucleation rate of tetragonal lysozyme crystals. Batch crystallization plates were prepared at given solution concentrations and incubated at set temperatures over one week. The number of crystals per well with their size and axial ratios were recorded and correlated with solution conditions, Duplicate experiments indicate the reproducibility of the technique, Crystal numbers were found to increase with increasing supersaturation and temperature. The most significant variable however, was pH, where crystal numbers changed by two orders of magnitude over the pH range 4.0 to 5.2. Crystal size varied also with solution conditions, with the largest crystals being obtained at pH 5.2. Having optimized the crystallization conditions, a batch of crystals were prepared under exactly the same conditions and fifty of these crystals were analyzed by x-ray techniques. The results indicate that even under the same crystallization conditions, a marked variation in crystal properties exists.

Judge, Russell A.↗
DOE OSTI2024

Droplet Growth or Evaporation Does Not Buffer the Variability in Supersaturation in Clean Clouds

Abstract Water vapor supersaturation in clouds is a random variable that drives activation and growth of cloud droplets. The Pi Convection–Cloud Chamber generates a turbulent cloud with a microphysical steady state that can be varied from clean to polluted by adjusting the aerosol injection rate. The supersaturation distribution and its moments, e.g., mean and variance, are investigated for varying cloud microphysical conditions. High-speed and collocated Eulerian measurements of temperature and water vapor concentration are combined to obtain the temporally resolved supersaturation distribution. This allows quantification of the contributions of variances and covariances between water vapor and temperature. Results are consistent with expectations for a convection chamber, with strong correlation between water vapor and temperature; departures from ideal behavior can be explained as resulting from dry regions on the warm boundary, analogous to entrainment. The saturation ratio distribution is measured under conditions that show monotonic increase of liquid water content and decrease of mean droplet diameter with increasing aerosol injection rate. The change in liquid water content is proportional to the change in water vapor concentration between no-cloud and cloudy conditions. Variability in the supersaturation remains even after cloud droplets are formed, and no significant buffering is observed. Results are interpreted in terms of a cloud microphysical Damköhler number (Da), under conditions corresponding to , i.e., the slow-microphysics regime. This implies that clouds with very clean regions, such that is satisfied, will experience supersaturation fluctuations without them being buffered by cloud droplet growth. Significance Statement The saturation ratio (humidity) in clouds controls the growth rate and formation of cloud droplets. When air in a turbulent cloud mixes, the humidity varies in space and time throughout the cloud. This is important because it means cloud droplets experience different growth histories, thereby resulting in broader size distributions. It is often assumed that growth and evaporation of cloud droplets buffers out some of the humidity variations. Measuring these variations has been difficult, especially in the field. The purpose of this study is to measure the saturation ratio distribution in clouds with a range of conditions. We measure the in-cloud saturation ratio using a convection cloud chamber with clean to polluted cloud properties. We found in clouds with low concentrations of droplets that the variations in the saturation ratio are not suppressed.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Large Aerosol Particles Favor Haze Conditions Through Limitations on Water Budget and Activation Kinetics

Experiments in the Pi Convection‐Cloud Chamber conducted by systematically changing the diameter of injected dry aerosol particles while holding the temperature difference constant demonstrate that dry diameter strongly influences the onset of haze‐dominated conditions. Two factors contribute: the system becomes water‐limited, resulting in reduction of supersaturation by growing aerosol particles to the activation diameter; and the activation process becomes kinetically limited. Dry aerosol diameter exerts a strong influence on activation time, with a power‐law exponent of 9/2. Kinetically limited activation occurs when the ratio of the activation and droplet residence times is greater than unity. The findings demonstrate that a haze‐dominated state, where cloud formation is suppressed, can be achieved not only with weak supersaturation forcing and high aerosol concentration but also with large, hygroscopic aerosol particles. These results have implications for cloud formation in polluted environments, fog development near the ocean, and hygroscopic cloud seeding.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1995

Interactions in Undersaturated and Supersaturated Lysozyme Solutions: Static and Dynamic Light Scattering Results

We have performed multiangle static and dynamic light scattering studies of lysozyme solutions at pH=4.7. The Rayleigh ratio R(sub g) and the collective diffusion coefficient D(sub c) were determined as function of both protein concentration c(sub p) and salt concentration c(sub s) with two different salts. At low salt concentrations, the scattering ratio K(sub c)(sub p)/R(sub theta) and diffusivity increased with protein concentration above the values for a monomeric, ideal solution. With increasing salt concentration this trend was eventually reversed. The hydrodynamic interactions of lysozyme in solution, extracted from the combination of static and dynamic scattering data, decreased significantly with increasing salt concentration. These observations reflect changes in protein interactions, in response to increased salt screening, from net repulsion to net attraction. Both salts had the same qualitative effect, but the quantitative behavior did not scale with the ionic strength of the solution. This indicates the presence of salt specific effects. At low protein concentrations, the slopes of K(sub c)(sub p)/R(sub theta) and D(sub c) vs c(sub p) were obtained. The dependence of the slopes on ionic strength was modeled using a DLVO potential for colloidal interactions of two spheres, with the net protein charge Z(sub e) and Hamaker constant A(sub H) as fitting parameters. The model reproduces the observed variations with ionic strength quite well. Independent fits to the static and dynamic data, however, led to different values of the fitting parameters. These and other shortcomings suggest that colloidal interaction models alone are insufficient to explain protein interactions in solutions.

Muschol, Martin↗