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New AFM Techniques for Investigating Molecular Growth Mechanisms of Protein Crystals

Atomic Force Microscopy (AFM) has emerged as a powerful technique for investigating protein crystal growth. Earlier AFM studies were among the first to demonstrate that these crystals grew by dislocation and 2D nucleation growth mechanisms [1]. These investigations were restricted to the micron range where only surface features, such as dislocation hillocks and 2D islands are visible. Most AFM instruments can scan at higher resolutions and have the potential to resolve individual protein molecules at nanometer ranges. Such scans are essential for determining the molecular packing arrangements on crystal faces and for probing the growth process at the molecular level. However, at this resolution the AFM tip influences the image produced, with the resulting image being a convolution of the tip shape and the surface morphology [2]. In most studies this problem is resolved by deconvoluting the image to obtain the true surface morphology. Although deconvolution routines work reasonably well for simple one- dimensional shapes, for complex surfaces this approach does not produce accurate results. In this study we devised a new approach which takes advantage of the precise molecular order of crystal surfaces, combined with the knowledge of individual molecular shapes from the crystallographic data of the protein and the AFM tip shape. This information is used to construct expected theoretical AFM images by convoluting the tip shape with the constructed crystal surface shape for a given surface packing arrangement. By comparing the images from actual AFM scans with the constructed ones for different possible surface packing arrangements, the correct packing arrangement can be conclusively determined. This approach was used in this study to determine the correct one from two possible packing arrangements on (I 10) faces of tetragonal lysozyme crystals. Another novel AFM technique was also devised to measure the dimension of individual growth units of the crystal faces. Measuring these units was not attempted before and most studies have assumed that the growth unit consisted of individual protein molecules. The linescan mode of AFM instruments allows the crystal surface to be scanned along a single line. By scanning across a growth step an image showing the motion of the step is obtained. Normally such an image shows a straight line for continuous and constant step velocity. In this study by increasing the scan rate and by decreasing the step velocity (by decreasing the supersaturation), we were able to capture images of individual growth events, shown by jump discontinuities in the step line. By suitable integration of the image the growth unit dimension in the scanned direction can be obtained. Since multiple units can be involved in the growth process it is necessary to collect a statistically relevant sample before drawing conclusions about the growth mechanism. This technique was successfully employed to obtain the dimensions of growth units for the (110) face, showing that they consisted of various aggregates corresponding to the 43 helices in the crystal structure.

Li, Huayu↗

Towards a Model Climatology of Relative Humidity in the Upper Troposphere for Estimation of Contrail and Contrail-Induced Cirrus

The formation of contrails and contrail cirrus is very sensitive to the relative humidity of the upper troposphere. To reduce uncertainty in an estimate of the radiative impact of aviation-induced cirrus, a model must therefore be able to reproduce the observed background moisture fields with reasonable and quantifiable fidelity. Here we present an upper tropospheric moisture climatology from a 26-year ensemble of simulations using the GEOS CCM. We compare this free-running model's moisture fields to those obtained from the MLS and AIRS satellite instruments, our most comprehensive observational databases for upper tropospheric water vapor. Published comparisons have shown a substantial wet bias in GEOS-5 assimilated fields with respect to MLS water vapor and ice water content. This tendency is clear as well in the GEOS CCM simulations. The GEOS-5 moist physics in the GEOS CCM uses a saturation adjustment that prevents supersaturation, which is unrealistic when compared to in situ moisture observations from MOZAIC aircraft and balloon sondes as we will show. Further, the large-scale satellite datasets also consistently underestimate super-saturation when compared to the in-situ observations. We place these results in the context of estimates of contrail and contrail cirrus frequency.

Selkirk, Henry B.↗

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↗

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↗

Protein crystal growth in low gravity

This research involved (1) using the Atomic Force Microscope (AFM) in a study on the growth of lysozyme crystals and (2) refinement of the design of the Thermonucleator which controls the supersaturation required for the nucleation and growth of protein crystals separately. AFM studies of the (110) tetragonal face confirmed that lysozyme crystals grow by step propagation. There appears to be very little step pile up in the growth regimes which we studied. The step height was measured at = 54A which was equal to the (110) interpane spacing. The AFM images showed areas of step retardation and the formation of pits. These defects ranged in size from 0.1 to 0.4 mu. The source of these defects was not determined. The redesign of the Thermonucleator produced an instrument based on thermoelectric technology which is both easier to use and more amenable to use in a mu g environment. The use of thermoelectric technology resulted in a considerable size reduction which will allow for the design of a multi-unit growth apparatus. The performance of the new apparatus was demonstrated to be the same as the original design.

Feigelson, Robert S.↗

Analysis of Ice Nucleating Aerosol Measurements during SUCCESS: April, May 1996

This section describes our research activities during year three of this effort. In the second year, preliminary archive data sets were submitted to the SUCCESS archive. After additional analyses, final versions were prepared and submitted. These are included on the SUCCESS CD-ROM data editions that were recently released by NASA Ames. Over the range of temperature and supersaturation conditions of our measurements (15 to -40 C, and from ice saturation to approximately 15% water supersaturation), IN concentrations ranged from less than 0.1 to approximately 500 per liter, being generally greater at colder temperatures and higher supersaturations. To estimate the potential of aircraft exhaust as a source of IN, we examined data from six days of the field project when the DC-8 was following closely behind other humidity conditions of our measurements. In April 1997, a microphysical workshop was convened at NCAR to select cases for in depth analyses and to address questions about the consistency of cloud ice crystal measurements (size distributions and mass concentrations) and aerosol size distributions. We attended this meeting and contributed to the discussions. A particular concern was identified in the CN measurements. On the DC-8, CN measurements were obtained by four different investigator groups, using commercially available instrumentation. The DC-8 SUCCESS CN data showed long periods where the measurements were in substantial agreement, but there were also periods with large discrepancies. Several possible factors were identified that could help explain these discrepancies, including minimum detectable particle size, response at reduced pressures, and location of sample inlet on the aircraft.

Rogers, D. C.↗

Inclusion of Linearized Moist Physics in Nasa's Goddard Earth Observing System Data Assimilation Tools

Inclusion of moist physics in the linearized version of a weather forecast model is beneficial in terms of variational data assimilation. Further, it improves the capability of important tools, such as adjoint-based observation impacts and sensitivity studies. A linearized version of the relaxed Arakawa-Schubert (RAS) convection scheme has been developed and tested in NASA's Goddard Earth Observing System data assimilation tools. A previous study of the RAS scheme showed it to exhibit reasonable linearity and stability. This motivates the development of a linearization of a near-exact version of the RAS scheme. Linearized large-scale condensation is included through simple conversion of supersaturation into precipitation. The linearization of moist physics is validated against the full nonlinear model for 6- and 24-h intervals, relevant to variational data assimilation and observation impacts, respectively. For a small number of profiles, sudden large growth in the perturbation trajectory is encountered. Efficient filtering of these profiles is achieved by diagnosis of steep gradients in a reduced version of the operator of the tangent linear model. With filtering turned on, the inclusion of linearized moist physics increases the correlation between the nonlinear perturbation trajectory and the linear approximation of the perturbation trajectory. A month-long observation impact experiment is performed and the effect of including moist physics on the impacts is discussed. Impacts from moist-sensitive instruments and channels are increased. The effect of including moist physics is examined for adjoint sensitivity studies. A case study examining an intensifying Northern Hemisphere Atlantic storm is presented. The results show a significant sensitivity with respect to moisture.

Convection↗

Overview of the NASA Airborne Tropical TRopopause EXperiment (ATTREX)

The NASA Airborne Tropical TRopopause EXperiment (ATTREX) is a series of airborne campaigns focused on understanding physical processes in the Tropical Tropopause Layer (TTL) and their role in atmospheric chemistry and climate. ATTREX is using the high-altitude, long-duration NASA Global Hawk Unmanned Air System to make in situ and remote-sensing measurements spanning the Pacific. A particular ATTREX emphasis is to better understand the dehydration of air as it passes through the cold tropical tropopause region. The ATTREX payload contains 12 in situ and remote sensing instruments that measure water vapor, clouds, multiple gaseous tracers (CO, CO2, CH4, NMHC, SF6, CFCs, N2O), reactive chemical compounds (O3, BrO, NO2), meteorological parameters, and radiative fluxes.ATTREX flight series have been conducted in the fall of 2011 from Armstrong Flight Research Center (AFRC) in California, in the winter of 2013 from AFRC, and in the winterspring of 2014 from Guam. The first two flight series provided extensive sampling of the central and eastern Pacific, whereas the last flight series permitted sampling in the western Pacific. The sampling strategy has primarily involved repeated ascents and descents through the depth of the TTL (about 13-19 km). Over 100 TTL profiles were obtained on each flight series. The ATTREX dataset includes TTL water vapor measurements with unprecedented accuracy, ice crystal size distributions and habits. The cloud and water measurements provide unique information about TTL cloud formation, the persistence of supersaturation with respect to ice, and dehydration. The plethora of tracers measured on the Global Hawk flights are providing unique information about TTL transport pathways and time scales. The meteorological measurements are revealing dynamical phenomena controlling the TTL thermal structure, and the radiation measurements are providing information about heating rates associated with TTL clouds and water vapor.This presentation will provide an overview of the ATTREX flights, examples of measurements from the flights, and plans for modelinganalysis of the ATTREX dataset.

Jensen, Eric J.↗

Overview of the Airborne Tropical TRopopause EX

The NASA Airborne Tropical TRopopause EXperiment (ATTREX) is a series of airborne campaigns focused on understanding physical processes in the Tropical Tropopause Layer (TTL) and their role in atmospheric chemistry and climate. ATTREX is using the high-altitude, long-duration NASA Global Hawk Unmanned Air System to make in situ and remote-sensing measurements spanning the Pacific. A particular ATIREX emphasis is to better understand the dehydration of air as it passes through the cold tropical tropopause region. The ATTREX payload contains 12 in situ and remote sensing instruments that measure water vapor, clouds, multiple gaseous tracers (CO, CO2, CH4, NMHC, SF6, CFCs, N2O), reactive chemical compounds (O3, BrO, NO2), meteorological parameters, and radiative fluxes. ATTREX flight series have been conducted in the fall of 2011 from Armstrong Flight Research Center (AFRC) in California, in the winter of 2013 from AFRC, and in the winter/spring of 2014 from Guam. The first two f light series provided extensive sampling of the central and eastern Pacific, whereas the last flight series permitted sampling in the western Pacific. The sampling strategy has primarily involved repeated ascents and descents through the depth of the TTL (about 13-19 km). Over 100 TTL profiles were obtained on each flight series. The ATTREX dataset includes TTL water vapor measurements with unprecedented accuracy, ice crystal size distributions and habits. The cloud and water measurements provide unique information about TTL cloud formation, the persistence of supersaturation with respect to ice, and dehydration. The plethora of tracers measured on the Global Hawk flights are providing unique information about TTL transport pathways and time scales. The meteorological measurements are revealing dynamical phenomena controlling the TTL thermal structure, and the radiation measurements are providing information about heating rates associated with TTL clouds and water vapor. This presentation will provide an overview of the ATTREX flights, examples of measurements from the flights, and plans for modeling/analysis of the ATTREX dataset.

Airborne↗

Balloon-Borne Measurements of Total Reactive Nitrogen, Nitric Acid, and Aerosol in the Cold Arctic Stratosphere

Total reactive nitrogen (NO(Y)) between 15 and 29 km was measured for the first time on board a balloon within the Arctic cold vortex. Observations of HNO3, aerosol, and ozone were made by instruments on the same balloon gondola which was launched from Esrange, Sweden (68 deg N, 20 deg E) on January 23, 1989. The NO(y) mixing ratio was observed to increase very rapidly from 6 ppbv at 18 km altitude to a maximum of 21 ppbv at 21 km, forming a sharp layer with a thickness of about 2 km. A minimum in the NO(y) mixing ratio of 5 ppbv was found at 27 km. The measured HNO3 profile shows broad similarities to that of NO(y). This observation, together with the observed very low column amount of NO2, shows that NO(x) had been almost totally converted to HNO3, and that NO(y) was composed mainly of HNO3. The enhanced aerosol concentration between 19 and 22 km suggests that the maximum abundance of HNO3 trapped in the form of nitric acid trihydrate (NAT) was about 6 ppbv at 21 km. The sampled air parcels were highly supersaturated with respect to NAT. Although extensive denitrification throughout the stratosphere did not prevail, an indication of denitrification was found at altitudes of 27 and 22 km, and between 18 and 15 km.

Kondo, Y.↗

The Vertical Structure of Relative Humidity and Ozone in the Tropical Upper Troposphere: Intercomparisons Among In Situ Observations, A-Train Measurements and Large-Scale Models

In situ measurements in the tropics have shown that in regions of active convection, relative humidity with respect to ice in the upper troposphere is typically close to saturation on average, and supersaturations greater than 20% are not uncommon. Balloon soundings with the cryogenic frost point hygrometer (CFH) at Costa Rica during northern summer, for example, show this tendency to be strongest between 11 and 15.5 km (345-360 K potential temperature, or approximately 250-120 hPa). this is the altitude range of deep convective detrainment. Additionally, simultaneous ozonesonde measurements show that stratospheric air (O3 greater than 150 ppbv) can be found as low as approximately 14 km (350 K/150 hPa). In contrast, results from northern winter show a much drier upper troposphere and little penetration of stratospheric air below the tropopause at 17.5 km (approximately 383 K). We show that these results are consistent with in situ measurements from the Measurement of Ozone and water vapor by Airbus In-service airCraft (MOZAIC) program which samples a wider, though still limited, range of tropical locations. To generalize to the tropics as a whole, we compare our insitu results to data from two A-Train satellite instruments, the Atmospheric Infrared Sounder (AIRS) and the Microwave Limb Sounder (MLS) on the Aqua and Aura satellites respectively. Finally, we examine the vertical structure of water vapor, relative humidity and ozone in the NASA Goddard MERRA analysis, an assimilation dataset, and a new version of the GEOS CCM, a free-running chemistry-climate model. We demonstrate that conditional probability distributions of relative humidity and ozone are a sensitive diagnostic for assessing the representation of deep convection and upper troposphere/lower stratosphere mixing processes in large-scale analyses and climate models.

Selkirk, Henry B.↗

Warm fog dispersal

The charged particle generator was further tested after some design modification. The generator performance was measured with additional instrumentation and found to confirm previous measurements. Plans for a field testing were than developed. The overall status of the program and the field test plans were presented to a group of atmospheric scientists and electrostatic experts at the NASA/MSFC sponsored USRA Workshop on Electrostatic Fog Dispersal at NCAR, Boulder, Colorado discussed in previous sections. The recommendations from this workshop are being evaluated as to whether NASA should proceed with the field test or whether further theoretical research on the phenomenon of electrostatic fog dispersal and additional development of the charged particle generator should be carried out. Information obtained from the USRA Workshop clearly identified three physical mechanisms that could possibly influence the fog dispersal process, which heretofore have not been considered, and which may provide additional insight to the direction of further fog dispersal work. These mechanisms are: the effect of corona discharge on the electric field strength at the surface, the influx of fog into the cleared volume by turbulent diffusion, and the increase in supersaturation as liquid water is removed, activating haze particles, and thus generating more fog. Plans are being formulated to investigate these mechanisms.

Frost, W.↗

Vertical Mass, Momentum, Moisture, and Heat Fluxes in Hurricanes above 10 km during CAMEX-3 and CAMEX-4

The third and fourth NASA Convection and Moisture Experiments (CAMEX-3 and CAMEX-4) during the Atlantic hurricane seasons of 1998 and 2001, respectively, have yielded comprehensive multi-aircraft datasets using, both remote and in-situ instrumentation. Among these are high-frequency in-situ measurements of vertical wind, horizontal wind, temperature, and water vapor, made from NASA's DC-8 aircraft in the upper portions of the hurricane (typically above 10 km). Wind and temperature measurements were made at 20 hz by the NASA/Ames Meteorological Measurement System, while water vapor was measured at 1 hz by the NASA/JPL Laser Hygrometer. Fluxes of heat, momentum, and moisture at these levels are important, since modeling studies have shown that ice processes, which are dominant at temperatures below -40C (where the DC-8 flies) are important for hurricane intensification. Also, there are indications from satellite studies that latent heat release at DC-8 levels is significant, perhaps a third of those in the mid-troposphere. Preliminary results show that typical updrafts in the eyewall region are comparable to or higher than previous observations of tropical convection, with several instances of updraft magnitudes of 15 meters per second (the maximum observed was 21 meters per second). They also show significant supersaturations (10-20% or more) in the updrafts, which would enhance the latent heat release at the upper levels of the hurricane. This paper will examine the magnitude and distribution of small and mesoscale vertical fluxes of mass, momentum, moisture, and heat. The goal is to examine the role of these fluxes in the overall budgets of the respective quantities in the upper portions of the hurricane.

Pfister, Leonhard↗