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Experiment 5: Science and Technology of Surface Controlled Oscillations: Report on USML-2 Results

Minuscule amounts (e.g., 1 part in 10,000) of a surface-active material in a liquid can drastically affect the surface behavior of the liquid, influencing how the material flows and mixes with other liquid and solid materials. In many respects, the science of surfactants has been empirical, with trial and error dominating over the ability to predict how surfactant type and concentration influence surface behavior. A program for the modeling of surfactant behavior has been established at Yale. This program combines experimental work performed both on the ground and in space, and theoretical and numerical modeling. By levitating a drop of liquid in air, away from solid container surfaces, and by manipulating the drop with acoustic radiation forces, we have been able to establish idealized conditions for surface behavior studies. The primary experiments involve the study of the free oscillations of initially deformed drops. In STS-73, the USML-2 mission of the Space Shuttle, we performed the following measurements: 1) the oscillation of a spherical drop in its quadrupole mode; 2) the oscillation of a drop about a deformed (oblate) shape; 3) the slow static squeezing of the drop from spherical to nearly flat; and 4) the superoscillations of drops when the radiation forces maintaining the drop in a flattened state are suddenly reduced. Analytic and numerical studies have enabled us to understand the physics of these oscillations and to extract material properties such as the dynamic surface tension and the surface viscosities (shear and dilatational). The relation to ground-based studies is essential, because the knowledge and understanding gleaned from our space studies enable us to interpret ground-based data.

Apfel, Robert E.↗

Low-Energy Sputtering Studies of Boron Nitride with Xenon Ions

Sputtering of boron nitride with xenon ions was investigated using secondary ion (SIMS) and secondary neutral (SNMS) mass spectrometry. The ions generated from the ion gun were incident on the target at an angle of 50' with respect to the surface'normal. The energy of ions ranged from 100 eV to 3 keV. A flood electron gun was used to neutralize the positive charge build-up on the target surface. The intensities of sputtered neutral and charged particles, including single atoms, molecules, and clusters, were measured as a function of ion energy. Positive SIMS spectra were dominated by the two boron isotopes whereas BN- and B- were the two major constituents of the negative SIMS spectra. Nitrogen could be detected only in the SNMS spectra. The intensity-energy curves of the sputtered particles were similar in shape. The knees in P-SIMS and SNMS intensity-energy curves appear at around I keV which is significantly higher that 100 to 200 eV energy range at which knees appear in the sputtering of medium and heavy elements by ions of argon and xenon. This difference in the position of the sputter yield knee between boron nitride and heavier targets is due to the reduced ion energy differences. The isotopic composition of secondary ions of boron were measured by bombarding boron nitride with xenon ions at energies ranging from 100 eV to 1.5 keV using a quadrupole mass spectrometer. An ion gun was used to generate the ion beam. A flood electron gun was used to neutralize the positive charge buildup on the target surface. The secondary ion flux was found to be enriched in heavy isotopes at lower incident ion energies. The heavy isotope enrichment was observed to decrease with increasing primary ion energy. Beyond 350 eV, light isotopes were sputtered preferentially with the enrichment increasing to an asymptotic value of 1.27 at 1.5 keV. The trend is similar to that of the isotopic enrichment observed earlier when copper was sputtered with xenon ions in the same energy range.

Ray, P. K.↗

A Multipole Expansion Method for Analyzing Lightning Field Changes

Changes in the surface electric field are frequently used to infer the locations and magnitudes of lightning-caused changes in thundercloud charge distributions. The traditional procedure is to assume that the charges that are effectively deposited by the flash can be modeled either as a single point charge (the Q model) or a point dipole (the P model). The Q model has four unknown parameters and provides a good description of many cloud-to-ground (CG) flashes. The P model has six unknown parameters and describes many intracloud (IC) discharges. In this paper we introduce a new analysis method that assumes that the change in the cloud charge can be described by a truncated multipole expansion, i.e., there are both monopole and dipole terms in the unknown source distribution, and both terms are applied simultaneously. This method can be used to analyze CG flashes that are accompanied by large changes in the cloud dipole moment and complex IC discharges. If there is enough information content in the measurements, the model can also be generalized to include quadrupole and higher order terms. The parameters of the charge moments are determined using a dme-dimensional grid search in combination with a linear inversion, and because of this, local minima in the error function and the associated solution ambiguities are avoided. The multipole method has been tested on computer-simulated sources and on natural lightning at the NASA Kennedy Space Center and U.S. Air Force Eastern Range.

Koshak, William J.↗

Research on Spectroscopy, Opacity, and Atmospheres

A web site has been set up to make the calculations accessible; (i.e., cfakus.harvard.edu) This data can also be accessed by FTP. It has all of the atomic and diatomic molecular data, tables of distribution function opacities, grids of model atmospheres, colors, fluxes, etc, programs that are ready for distribution, and most of recent papers developed during this grant. Atlases and computed spectra will be added as they are completed. New atomic and molecular calculations will be added as they are completed. The atomic programs that had been running on a Cray at the San Diego Supercomputer Center can now run on the Vaxes and Alpha. The work started with Ni and Co because there were new laboratory analyses that included isotopic and hyperfine splitting. Those calculations are described in the appended abstract for the 6th Atomic Spectroscopy and oscillator Strengths meeting in Victoria last summer. A surprising finding is that quadrupole transitions have been grossly in error because mixing with higher levels has not been included. All levels up through n=9 for Fe I and II, the spectra for which the most information is available, are now included. After Fe I and Fe II, all other spectra are "easy". ATLAS12, the opacity sampling program for computing models with arbitrary abundances, has been put on the web server. A new distribution function opacity program for workstations that replaces the one used on the Cray at the San Diego Supercomputer Center has been written. Each set of abundances would take 100 Cray hours costing $100,000.

Kurucz, Robert L.↗

The Dynamics of Ultrasonically Levitated Drops in an Electric Field

Ultrasonic and electrostatic levitation techniques have allowed the experimental investigation of the nonlinear oscillatory dynamics of free droplets with diameter between 0.1 and 0.4 cm. The measurement of the resonance frequencies of the first three normal modes of large amplitude shape oscillations in an electric field of varying magnitude has been carried out with and without surface charges for weakly conducting liquids in air. These oscillations of nonspherical levitated drops have been driven by either modulating the ultrasonic field or by using a time-varying electric field, and the free decay from the oscillatory state has been recorded. A decrease in the resonance frequency of the driven fundamental quadrupole mode has been measured for increasing oblate deformation in the absence of an electric field. Similarly, a decrease in this frequency has also been found for increasing DC electric field magnitude. A soft nonlinearity exists in the amplitude dependence of the resonant mode frequencies for freely decaying as well as ultrasonically and electrically driven uncharged drops. This decrease in resonance frequency is accentuated by the presence of free surface charge on the drop. Subharmonic resonance excitation has been observed for drops in a time-varying electric field, and hysteresis exists for resonant modes driven to large amplitude. Mode coupling from lower-order resonances to higher-order modes has been found to be very weak, even for fairly large amplitude shape oscillations. Most of these results are in general agreement with predictions from recent analytical and numerical investigations.

Trinh, E. H.↗

Computer Simulation of the far Infrared Collision Induced Absorption Spectra of Gaseous CO2

Far infrared collision induced absorption spectra of gaseous CO2 were computed using molecular dynamics simulations. The quadrupole and hexadecapole multipolar induction, through the trace, and the anisotropy of the molecular polarizability were found to be insufficient to represent properly the dipole induction mechanism. For a detailed analysis of the induction process the spectra obtained were decomposed into components resulting from different terms of the induced dipole. Based on this decomposition, all additional overlap contribution for each term was proposed. When spectra were recomputed including such overlap, good agreement between experiment and simulation was achieved over the temperature range at which measurements exist (233-400 K). The use of an anisotropic intermolecular potential was found to be of critical importance for obtaining the right shape of the far wings of the spectra.

Gruszka, Marcin↗

A Multipole Expansion Method for Analyzing Lightning Field Changes

Changes in the surface electric field are frequently used to infer the locations and magnitudes of lightning-caused changes in thundercloud charge distributions. The traditional procedure is to assume that the charges that are effectively deposited by the flash can be modeled either as a single point charge (the Q-model) or a point dipole (the P-model). The Q-model has 4 unknown parameters and provides a good description of many cloud-to-ground (CG) flashes. The P-model has 6 unknown parameters and describes many intracloud (IC) discharges. In this paper, we introduce a new analysis method that assumes that the change in the cloud charge can be described by a truncated multipole expansion, i.e., there are both monopole and dipole terms in the unknown source distribution, and both terms are applied simultaneously. This method can be used to analyze CG flashes that are accompanied by large changes in the cloud dipole moment and complex IC discharges. If there is enough information content in the measurements, the model can also be generalized to include quadrupole and higher order terms. The parameters of the charge moments are determined using a 3-dimensional grid search in combination with a linear inversion, and because of this, local minima in the error function and the associated solution ambiguities are avoided. The multipole method has been tested on computer simulated sources and on natural lightning at the NASA Kennedy Space Center and USAF Eastern Range.

Koshak, William J.↗

Recent Results from a Laboratory Study of Charging Mechanisms in a Dusty Plasma

A laboratory investigation has been developed to experimentally study the interaction of micron sized particles with plasmas and electromagnetic radiation. The intent is to investigate under what conditions particles of various compositions and sizes become charged, or discharged, while exposed to an electron beam and UV radiation. This investigation uses a unique laboratory technique known as electrodynamic suspension of particles. Here, a single charged micron size particle is suspended in a quadrupole trap and then subjected to a controlled environment. In this paper, we will discuss recent results from this experiment in which different materials including polystyrene and aluminum oxide, and sizes ranging from 10 microns to 1 micron have been used to determine charge to mass ratios and then subjected to an electron beam and /or UV radiation. In each instance, the particle's charge as well as beam current flux and radiation intensity flux is measured. These results will be compared with initial results using salt crystals. It was found that a negatively charged salt crystal exposed for 30 minutes to a 500 eV electron beam with primary electron beam current of -3.06 x 10(exp -5) picoamps yielded a secondary electron current of 3.23 x 10(exp -5) picoamps. Additionally, the particle was observed to be steadily losing charge over this time interval. By studying the microphysics of one particle, a better understanding of theoretical models and other laboratory results associated with particle charging mechanisms can be achieved.

Venturini, Catherine C.↗

Applications of Bayesian Statistics to Problems in Gamma-Ray Bursts

This presentation will describe two applications of Bayesian statistics to Gamma Ray Bursts (GRBS). The first attempts to quantify the evidence for a cosmological versus galactic origin of GRBs using only the observations of the dipole and quadrupole moments of the angular distribution of bursts. The cosmological hypothesis predicts isotropy, while the galactic hypothesis is assumed to produce a uniform probability distribution over positive values for these moments. The observed isotropic distribution indicates that the Bayes factor for the cosmological hypothesis over the galactic hypothesis is about 300. Another application of Bayesian statistics is in the estimation of chance associations of optical counterparts with galaxies. The Bayesian approach is preferred to frequentist techniques here because the Bayesian approach easily accounts for galaxy mass distributions and because one can incorporate three disjoint hypotheses: (1) bursts come from galactic centers, (2) bursts come from galaxies in proportion to luminosity, and (3) bursts do not come from external galaxies. This technique was used in the analysis of the optical counterpart to GRB970228.

Meegan, Charles A.↗

A Laboratory Study of the Charging/Discharging Mechanisms of a Dust Particle Exposed to an Electron Beam

The interaction of micron sized particles or "dust particles" with different space and planetary environments has become an important area of research. One particular area of interest is how dust particles interact with plasmas. Studies have shown that charged dust particles immersed in plasmas can alter plasma characteristics, while ions and electrons in plasmas can affect a particle's potential and thereby, its interaction with other particles. The basis for understanding these phenomena is the charging mechanisms of the dust particle, specifically, how the particle's charge and characteristics are affected when exposed to ions and electrons. At NASA Marshall Space Flight Center, a laboratory experiment has been developed to study the interaction of dust particles with electrons. Using a unique laboratory technique known as electrodynamic suspension, a single charged particle is suspended in a modified quadrupole trap. Once suspended, the particle is then exposed to an electron beam to study the charging/discharging mechanisms due to collisions of energetic electrons. The change in the particle's charge, approximations of the charging/discharging currents, and the charging/discharging yield are calculated.

Venturini, C. C.↗

Static Properties and Stark Effect of the Ground State of the HD Molecular Ion

We have calculated static properties of the ground state of the HD(+) ion and its lowest-lying P-state without making use of the Born-Oppenheimer approximation, as was done in the case of H2(+) and D2(+) [Phys. Rev. A 58, 2787 (1998)]. The ion is treated as a three-body system whose ground state is spherically symmetric. The wavefunction is of generalized Hylleraas type, but it is necessary to include high powers of the internuclear distance to localize the nuclear motion. We obtain good values of the energies of the ground S-state and lowest P-state and compare them with earlier calculations. Expectation values are obtained for various operators, the Fermi contact parameters, and the permanent quadrupole moment. The cusp conditions are also calculated. The polarizability was then calculated using second-order perturbation theory with intermediate P pseudostates. Since the nuclei in HD(+) are not of equal mass there is dipole coupling between the lowest two rotational states, which are almost degenerate. This situation is carefully analyzed, and the Stark shift is calculated variationally as a function of the applied electric field.

Bhatia, A. K.↗

Dark Matter in the Universe and in the Galaxy

During the past four years, Prof. Kamionkowski and collaborators have made progress in research on the nature and distribution of dark-matter in the Universe and in the Galaxy, and on related topics in astrophysics and cosmology. We have made progress on research on the cosmic microwave background, large-scale structure, issues related to particle dark matter, and the gamma-ray-burst enigma. A significant fraction of the research supported by this ATP has been on the cosmic microwave background (CMB). Prof. Kamionkowski and collaborators showed how the polarization of the CMB could be used to detect long-wavelength gravitational waves, such as those produced by inflation. With Kosowsky, Prof. Kamionkowski calculated the amplitude of a stochastic gravitational-wave background that could be detected for a satellite experiment of a given sensitivity and angular resolution. They showed that polarization should improve the sensitivity oa MAP to these gravity waves, and that the Planck Surveyor should do even better. Prof. Kamionkowski, Caldwell, and a student calculated and illustrated the CMB temperature/polarization pattern produced by a single plane-wave gravitational wave. They calculated the amplitude of such a wave that would be detectable with MAP and Planck, and compared that with the sensitivity of traditional gravitational-wave detectors like LIGO and LISA. With Lue and Wang, the PI showed how parity violation from new high-energy physics could conceivably give rise to an observable signature in the CMB polarization. With Loeb, Prof. Kamionkowski showed how measurement of the polarization of CMB photons scattered by hot gas in a cluster could be used to determine the quadrupole moment of the CMB incident on that cluster. Prof. Kamionkowski and Jaffe calculated the amplitude of secondary anisotropies produced by scattering of CMB photons from reionized regions. Research has also been carried out on probing the large-scale distribution of mass in the Universe today, and on structure-formation theories. They investigated the possibility of determining the large-scale distribution of mass in the Universe via measurement of ellipticity-ellipticity correlations in the FIRST radio survey induced by weak gravitational lensing due to mass inhomogeneities along the line of sight. Dr. Summers, Prof. Kamionkowski, and a student investigated the distribution of protogalactic masses and angular momenta in an effort to understand how the luminosity function and angular-momentum distribution of disk galaxies arises from an initial power spectrum of density perturbations. Several projects related to the distribution and possible detection of dark matter in our Galactic halo were studied. The PI was involved in several projects involving the calculation of nuclear-reaction rates needed for stellar evolution and for predictions of solar-neutrino fluxes.

Kamionkowski, Marc↗

Research on Spectroscopy, Opacity, and Atmospheres

To make my calculations more readily accessible I have set up a web site cfaku5.harvard.edu that can also be accessed by FTP. it has 5 9GB disks that hold all of my atomic and diatomic molecular data, my tables of distribution function opacities, my grids of model atmospheres, colors, fluxes, etc, my program that are ready for distribution, most of my recent papers. Atlases and computed spectra will be added as they are completed. New atomic and molecular calculations will be added as they are completed. I got my atomic programs that had been running on a Cray at the San Diego Supercomputer Center to run on my Vaxes and Alpha. I started with Ni and Co because there were new laboratory analyses that included isotopic and hyperfine splitting. Those calculations are described in the appended abstract for the 6th Atomic Spectroscopy and oscillator Strengths meeting in Victoria last summer. A surprising finding is that quadrupole transitions have been grossly in error because mixing with higher levels has not been included. I now have enough memory in my Alpha to treat 3000 x 3000 matrices. I now include all levels up through n=9 for Fe I and 11, the spectra for which the most information is available. I am finishing those calculations right now. After Fe I and Fe 11, all other spectra are "easy", and I will be in mass production. ATL;LS12, my opacity sampling program for computing models with arbitrary abundances, has been put on the web server. I wrote a new distribution function opacity program for workstations that replaces the one I used on the Cray at the San Diego Supercomputer Center. Each set of abundances would take 100 Cray hours costing $100,000. 1 ran 25 cases. Each of my opacity CDs contains three abundances. I have a new program -iinning on the Alpha that takes about a week. I am going to have to get a faster processor or I will have to dedicate a whole workstation just to opacities.

Kurucz, Robert L.↗

Sulfuric Acid Monohydrate: Formation and Heterogeneous Chemistry in the Stratosphere

We have investigated some thermodynamic properties (i.e., freezing/melting points) and heterogeneous chemistry of sulfuric acid monohydrate (SAM, H2SO4.H2O), using a fast flow reactor coupled to a quadrupole mass spectrometer. The freezing point observations of thin liquid sulfuric acid films show that for acid contents between 75 and 85 wt % the monohydrate crystallizes readily at temperatures between 220 and 240 K on a glass substrate. Once formed, SAM can be thermodynamically stable in the H2O partial pressure range of (1-4) x 10(exp -4) torr and in the temperature range of 220-240 K. For a constant H2O partial pressure, lowering the temperature causes SAM to melt when the temperature and water partial pressure conditions are out of its stability regime. The reaction probability measurements indicate that the hydrolysis of N2O5 is significantly suppressed owing to the formation of crystalline SAM: The reaction probability on water-rich SAM (with higher relative humidity, or RH) is of the order of 10(exp -3) at 210 K and decreases by more than an order of magnitude for the acid-rich form (with lower RH). The hydrolysis rate of ClONO2 on water-rich SAM is even smaller, of the order of 10(exp -4) at 195 K. These reported values on crystalline SAM are much smaller than those on liquid solutions. No enhancement of these reactions is observed in the presence of HCl vapor at the stratospheric concentrations. In addition, Brunauer, Emmett, and Teller analysis of gas adsorption isotherms and photomicrography have been performed to characterize the surface roughness and porosities of the SAM substrate. The results suggest the possible formation of SAM in some regions of the middle- or low-latitude stratosphere and, consequently, much slower heterogeneous reactions on the frozen aerosols.

Zhang, Renyi↗

Heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(s)

The heterogeneous reactions of HNO3(g) + NaCl(s) yields HCl(g) + NaNO3(s) (eq 1) and N2O5(g) + NaCl(s) yields ClNO2(g) + NaNO3(S) (eq 2) were investigated over the temperature range 223-296 K in a flow-tube reactor coupled to a quadrupole mass spectrometer. Either a chemical ionization mass spectrometer (CIMS) or an electron-impact ionization mass spectrometer (EIMS) was used to provide suitable detection sensitivity and selectivity. In order to mimic atmospheric conditions, partial pressures of HNO3 and N2O5 in the range 6 x 10(exp -8) - 2 x 10(exp -6) Torr were used. Granule sizes and surface roughness of the solid NaCl substrates were determined by using a scanning electron microscope. For dry NaCl substrates, decay rates of HNO3 were used to obtain gamma(1) = 0.013 +/- 0.004 (1sigma) at 296 K and > 0.008 at 223 K, respectively. The error quoted is the statistical error. After all corrections were made, the overall error, including systematic error, was estimated to be about a factor of 2. HCl was found to be the sole gas-phase product of reaction 1. The mechanism changed from heterogeneous reaction to predominantly physical adsorption when the reactor was cooled from 296 to 223 K. For reaction 2 using dry salts, gamma(2) was found to be less than 1.0 x 10(exp -4) at both 223 and 296 K. The gas-phase reaction product was identified as ClNO2 in previous studies using an infrared spectrometer. An enhancement in reaction probability was observed if water was not completely removed from salt surfaces, probably due to the reaction of N2O5(g) + H2O(s) yields 2HNO3(g). Our results are compared with previous literature values obtained using different experimental techniques and conditions. The implications of the present results for the enhancement of the hydrogen chloride column density in the lower stratosphere after the El Chichon volcanic eruption and for the chemistry of HCl and HNO3 in the marine troposphere are discussed.

Leu, Ming-Taun↗

Pump Effects in Planetary Mass Spectrometers

Mass spectrometers provide a useful tool in solar system exploration since fundamental questions of Solar System formation and evolution may be constrained by models based on the chemical and isotopic data provided by these instruments. For example, comparison of such data between the atmospheres of the terrestrial planets enables an understanding of mechanisms of atmospheric loss to space and production sources such as from planetary outgassing and from infall from objects such as comets. Over the past 25 years, mass spectrometers have been sent to Mars, Venus, Comet Halley, and Jupiter and are presently in transit to the Saturnian system to sample the atmosphere of Saturn's moon Titan. The quality of data derived from a very small, lightweight, and rugged instrument is constrained not only by the mass analyzer itself, but also by the performance of its gas sampling and pumping systems. A comparison of several planetary mass spectrometer experiments is provided with a focus on the demands placed on the gas processing and pumping systems. For example, the figure below is a mass spectrum from deep in the atmosphere of Jupiter obtained from a quadrupole mass spectrometer developed in the early 1980's for the Galileo Probe (Niemann et al., Space Sci. Rev., 60, 111-142 (1992)). Measurements of Jovian noble gases and other species with this system is described.

Mahaffy, Paul↗

Dusty Plasma Experiments Using an Electrodynamic Balance

Knowledge of the formation, distribution, physical, chemical and optical characteristics of interstellar, interplanetary, and planetary dust grains provide valuable information about many issues dealing with the origin and formation of the solar system bodies, interplanetary and interstellar environments as well as various industrial processes. Understanding the microphysics of individual grains and their interaction with the surrounding environment is key to properly model various conditions and interpret existing data. The theory and models of individual dust grains are well developed for environments that vary from dense planetary atmospheres to dusty plasmas to diffuse environments such is interplanetary space. However, experimental investigations of individual dust grains in equilibrium are less common, perhaps due to the difficult of these experiments. Laboratory measurements of dust grains have primarily measured ensemble properties or transient properties of single grains. A technique developed in the 1950's for ion spectroscopy, known as a quadrupole trap or 'Paul Trap', has recently been used to investigate single micron-sized dust grains. This scaled ion trap called an electrodynamic balance has been used for atmospheric aerosol research. A description of this technique is provided. Recent results from experiments to investigate the equilibrium potential of dust grains exposed to far ultraviolet light or to -,in electron or ion beam are presented. This laboratory technique ]ends itself to many applications that relate to planetary atmospheres, heliospheric environments, pre-stellar and pre-planetary conditions, and industrial settings. Several planned experimental approaches are presented. Potential experiments to investigate the interaction of multiple dust grains using an electrodynamic balance are proposed.

Spann, J. F.↗

Influence of Mean-Density Gradient on Small-Scale Turbulence Noise

A physics-based methodology is described to predict jet-mixing noise due to small-scale turbulence. Both self- and shear-noise source teens of Lilley's equation are modeled and the far-field aerodynamic noise is expressed as an integral over the jet volume of the source multiplied by an appropriate Green's function which accounts for source convection and mean-flow refraction. Our primary interest here is to include transverse gradients of the mean density in the source modeling. It is shown that, in addition to the usual quadrupole type sources which scale to the fourth-power of the acoustic wave number, additional dipole and monopole sources are present that scale to lower powers of wave number. Various two-point correlations are modeled and an approximate solution to noise spectra due to multipole sources of various orders is developed. Mean flow and turbulence information is provided through RANS-k(epsilon) solution. Numerical results are presented for a subsonic jet at a range of temperatures and Mach numbers. Predictions indicated a decrease in high frequency noise with added heat, while changes in the low frequency noise depend on jet velocity and observer angle.

Khavaran, Abbas↗