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Theory of atomic additivity in molecular hyperpolizabilities

Hyperpolarizability is a function of frequency. This is called dispersion. Because of the Kramers-Kronig relations, researchers expect that a material that is dispersing light is also absorbing it. Where there is both dispersion and absorption, the molecular polarizabilities are complex functions of the frequency. This led researchers to consider atomic additivity in both the real and imaginary parts of the ordinary and hyperpolarizabilities. This effort is desirable not only from a theoretical point of view, but also because of the existence of a large body of complex refractive index data, which may be used to test the additivity principle with the complex valued ordinary dipole polarizability.

Baird, James K.↗

Comparison of theory with atomic oxygen 130.4 nm radiation data from the Bow Shock ultraviolet 2 rocket flight

Comparison is made between the results obtained from a state-of-the-art flow and radiative model and bow shock vacuum ultraviolet (VUV) data obtained the recent Bow Shock 2 Flight Experiment. An extensive data set was obtained from onboard rocket measurements at a reentry speed of 5 km/sec between the altitudes of approximately 65-85 km. A description of the NO photoionization cell used, the data, and the interpretation of the data will be presented. The primary purpose of the analyses is to assess the utility of the data and to propose a radiation model appropriate to the flight conditions of Bow Shock 2. Theoretical predictions based on flow modeling discussed in earlier work and a new radiation model are compared with data.

Levin, Deborah A.↗

Scattering and Diffraction of Electromagnetic Radiation: An Effective Probe to Material Structure

Scattered electromagnetic waves from material bodies of different forms contain, in an intricate way, precise information on the intrinsic, geometrical and physical properties of the objects. Scattering theories, ever deepening, aim to provide dependable interpretation and prediction to the complicated interaction of electromagnetic radiation with matter. There are well-established multiple-scattering formulations based on classical electromagnetic theories. An example is the Generalized Multi-particle Mie-solution (GMM), which has recently been extended to a special version ̶ the GMM-PA approach, applicable to finite periodic arrays consisting of a huge number (e.g., >>106) of identical scattering centers [1]. The framework of the GMM-PA is nearly complete. When the size of the constituent unit scatterers becomes considerably small in comparison with incident wavelength, an appropriate array of such small element volumes may well be a satisfactory representation of a material entity having an arbitrary structure. X-ray diffraction is a powerful characterization tool used in a variety of scientific and technical fields, including material science. A diffraction pattern is nothing more than the spatial distribution of scattered intensity, determined by the distribution of scattering matter by way of its Fourier transform [1]. Since all linear dimensions entered into Maxwell's equations are normalized by wavelength, an analogy exists between optical and X-ray diffraction patterns. A large set of optical diffraction patterns experimentally obtained can be found in the literature [e.g., 2,3]. Theoretical results from the GMM-PA have been scrutinized using a large collection of publically accessible, experimentally obtained Fraunhofer diffraction patterns. As far as characteristic structures of the patterns are concerned, theoretical and experimental results are in uniform agreement; no exception has been found so far. Closely connected with the spatial distribution of scattered intensities are cross sections, such as for extinction, scattering, absorption, and radiation pressure, as a critical type of key quantity addressed in most theoretical and experimental studies of radiative scattering. Cross sections predicted from different scattering theories are supposed to be in general agreement. For objects of irregular shape, the GMM-PA solutions can be compared with the highly flexible Discrete Dipole Approximation (DDA) [4,5] when dividing a target to no more than ~106 unit cells. Also, there are different ways to calculate the cross sections in the GMM-PA, providing an additional means to examine the accuracy of the numerical solutions and to unveil potential issues concerning the theoretical formulations and numerical aspects. To solve multiple scattering by an assembly of material volumes through classical theories such as the GMM-PA, the radiative properties of the component scatterers, the complex refractive index in particular, must be provided as input parameters. When using a PA to characterize a material body, this involves the use of an adequate theoretical tool, an effective medium theory, to connect Maxwell's phenomenogical theory with the atomistic theory of matter. In the atomic theory, one regards matter as composed of interacting particles (atoms and molecules) embedded in the vacuum [6]. However, the radiative properties of atomic-scaled particles are known to be substantially different from bulk materials. Intensive research efforts in the fields of cluster science and nanoscience attempt to bridge the gap between bulk and atom and to understand the transition from classical to quantum physics. The GMM-PA calculations, which place virtually no restriction on the component-particle size, might help to gain certain insight into the transition.

Xu, Yu-Lin↗

Physics through the 1990s: Atomic, molecular and optical physics

The volume presents a program of research initiatives in atomic, molecular, and optical physics. The current state of atomic, molecular, and optical physics in the US is examined with respect to demographics, education patterns, applications, and the US economy. Recommendations are made for each field, with discussions of their histories and the relevance of the research to government agencies. The section on atomic physics includes atomic theory, structure, and dynamics; accelerator-based atomic physics; and large facilities. The section on molecular physics includes spectroscopy, scattering theory and experiment, and the dynamics of chemical reactions. The section on optical physics discusses lasers, laser spectroscopy, and quantum optics and coherence. A section elucidates interfaces between the three fields and astrophysics, condensed matter physics, surface science, plasma physics, atmospheric physics, and nuclear physics. Another section shows applications of the three fields in ultra-precise measurements, fusion, national security, materials, medicine, and other topics.

Source record↗

Theory of direct scattering of neutral and charged atoms

The theory for direct elastic and inelastic collisions between composite atomic systems formulated within the framework of the Glauber approximation is presented. It is shown that the phase-shift function is the sum of a point Coulomb contribution and of an expression in terms of the known electron-hydrogen-atom and proton-hydrogen-atom phase shift function. The scattering amplitude is reexpressed, the pure Coulomb scattering in the case of elastic collisions between ions is isolated, and the exact optical profile function is approximated by a first-order expansion in Glauber theory which takes into account some multiple collisions. The approximate optical profile function terms corresponding to interactions involving one and two electrons are obtained in forms of Meijer G functions and as a one-dimensional integral, and for collisions involving one or two neutral atoms, the scattering amplitude is further reduced to a simple closed-form expression.

Franco, V.↗

Scattered-light scanner measurements of cryogenic liquid-jet breakup

The effect of highly turbulent Mach 1 gas flow and high thermal gradients on drop size measurements was investigated with a scattered light scanner. The instrument, developed at NASA-Lewis, was used to measure characteristic drop diameters or cyrogenic liquid sprays. By correcting for gas turbulence and thermal gradient affects, it was possible to obtain good reproducible data with the scattered light scanner. Tests were conducted primarily in the aerodynamic-stripping regime of liquid atomization and it was found that the loss of small droplets due to vaporization and dispersion had a marketed effect on drop size measurements. The nitrogen gas flow rate exponent of 1.33 is the same as that predicted by atomization theory for liquid jet breakup in high velocity gas flow. However, when the sprays were sampled farther downstream of the atomizer, at axial distances of 2.5 and 4.5 cm, the exponent for W sub n decreased 1.2 and 0.9, respectively. This was attributed to the loss of small droplets due to vaporization when values of downstream axial distances exceeded 1.3 cm.

Ingebo, Robert D.↗

Gas-phase flowrate effect on disintegrating cryogenic liquid-jets

Two phase liquid and gaseous nitrogen flow in a pneumatic two fluid atomizer was investigated. Characteristic dropsize for cryogenic sprays were measured with a scattered light scanning instrument developed at NASA-Lewis. Tests were conducted primarily in the aerodynamic stripping regime of liquid jet atomization. At a sampling distance of bar-x=1.3 cm, the Sauter mean, D(sub 32), and volume median, D(sub v.5), drop diameters were measured and correlated with nitrogen gas flowrate, W(sub n), to give the following expressions: D sub 32 to the -1=210W(sub n) to the -1.33 and D(sub v.5) to the -1=150 W(sub n to the -1.33, where reciprocal diameters and gas flowrate are in cm (-1) and g/sec, respectively. The exponent 1.33 for nitrogrn gas flowrate, W(sub n), is the same as that predicted by atomization theory for liquid-jet breakup in high velocity gasflow. When the spray was sampled at axial distances of bar-x=2.5 and 4.5 cm downstream of the atomizer, the exponent decreased to 1.2 and 0.9, respectively. This was attributed to the loss of small droplets due to their rapid vaporization.

Ingebo, Robert D.↗

Gas-phase flowrate effect on disintegrating cryogenic liquid-jets

Two phase liquid and gaseous nitrogen flow in a pneumatic two fluid atomizer was investigated. Characteristic dropsize for cryogenic sprays were measured with a scattered light scanning instrument developed at NASA-Lewis. Tests were conducted primarily in the aerodynamic stripping regime of liquid jet atomization. At a sampling distance of bar-x =1.3 cm, the Sauter mean, D(sub 32), and volume median, D(sub v.5), drop diameters were measured and correlated with nitrogen gas flowrate, W(sub n), to give the following expressions: D sub 32 to the -1=210W(sub n) to the -1.33 and D(sub v.5) to the -1=150 W(sub n to the -1.33, where reciprocal diameters and gas flowrate are in cm (-1) and g/sec, respectively. The exponent 1.33 for nitrogen gas flowrate, W(sub n), is the same as that predicted by atomization theory for liquid-jet breakup in high velocity gasflow. When the spray was sampled at axial distances of bar-x=2.5 and 4.5 cm downstream of the atomizer, the exponent decreased to 1.2 and 0.9, respectively. This was attributed to the loss of small droplets due to their rapid vaporization.

Ingebo, Robert D.↗

Asymptotic Energies and QED Shifts for Rydberg States of Helium

This paper reviews progress that has been made in obtaining essentially exact solutions to the nonrelativistic three-body problem for helium by a combination of variational and asymptotic expansion methods. The calculation of relativistic and quantum electrodynamic corrections by perturbation theory is discussed, and in particular, methods for the accurate calculation of the Bethe logarithm part of the electron self energy are presented. As an example, the results are applied to the calculation of isotope shifts for the short-lived 'halo' nucleus He-6 relative to He-4 in order to determine the nuclear charge radius of He-6 from high precision spectroscopic measurements carried out at the Argonne National Laboratory. The results demonstrate that the high precision that is now available from atomic theory is creating new opportunities to create novel measurement tools, and helium, along with hydrogen, can be regarded as a fundamental atomic system whose spectrum is well understood for all practical purposes.

Drake, G.W.F.↗

Hot hydrogen atom reactions moderated by H2 and He

Photolysis experiments were performed on the H2-CD4-NH3 and He-CD4-NH3 systems. The photolysis (1849 A) involved only NH3. Mixtures of H2:CD4:NH3 included all combinations of the ratios (200,400,800):(10,20,40):4. Two He:CD4:NH3 mixtures were examined where the ratios equalled the combinations 100:(10,20):4. Abstraction of a D from CD4 by the photolytically produced hot hydrogen from ammonia was monitored by mass spectrometric determination of HD. Both experiment and semiempirical hot-atom theory show that H2 is a very poor thermalizer of hot hydrogens with excess kinetic energy of about 2 eV. Applications of the hard-sphere collision model to the H2-CD4-NH3 system resulted in predicted ratios of net HD production to NH3 decomposition that were two orders of magnitude smaller than the experimental ratios. On the other hand, helium is found to be a very efficient thermalizer; here, the classical model yields reasonable agreement with experiments. Application of a semiempirical hot-atom program gave quantitative agreement with experiment for either system.

Aronowitz, S.↗

Low-temperature Positron Annihilation

For a satisfactory understanding of astrophysical annihilation radiation, especially that observed from the galactic center direction, the interaction of positrons with the ambient medium must be carefully investigated. Although hot, ionized regions may be important sources of annihilation radiation, the simpler processes occurring in low-temperature neutral hydrogen gas are mainly addressed. The goal is to set limits on conditions in the annihilation region by using the predictions of atomic theory compared with the observed gamma-ray line width, continuum strength and time dependence.

Drachman, R. J.↗

Low-temperature positron annihilation

For a satisfactory understanding of astrophysical annihilation radiation, especially that observed from the Galactic center direction, the interaction of positrons with the ambient medium must be carefully investigated. Although hot, ionized regions may be important sources of annihilation radiation, the simpler processes occurring in low-temperature neutral hydrogen gas are mainly addressed. The goal is to set limits on conditions in the annihilation region by using the predictions of atomic theory compared with the observed gamma-ray line width, continuum strength and time dependence.

Drachman, R. J.↗

Effect of mass-velocity on liquid jet atomization in Mach 1 gasflow

Interacting two-phase flow in four differently sized pneumatic two-fluid atomizers was investigated to determine the effect of gas mass-velocity on the Sauter mean diameter of sprays produced by small diameter liquid jets breaking up in high velocity gas flow. Tests were conducted primarily in the acceleration-wave regime for liquid jet atomization, where it was found that the loss of droplets due to vaporization had a marked effect on drop size measurements. A scattered-light scanner, developed at NASA Lewis Research Center, was used to measure the Sauter mean diameter, D sub 32, which was correlated with nitrogen gas mass-velocity to give the following expression: D (sup -1)(sub 32) = 11.7(rho (sub n) V (sub n)) (sup 1.33). The exponent 1.33 for the gas mass-velocity is identical to that predicted by atomization theory for liquid jet breakup in the acceleration-wave regime.

Ingebo, Robert D.↗

Small-droplet spray measurements with a scattered-light scanner

Interacting two-phase flow through pneumatic two-fluid nozzles was investigated to determine the effect of nitrogen gas mass-velocity on the Sauter mean diameter of water sprays produced by the breakup of small diameter liquid-jets in high velocity gas streams. Tests were conducted primarily in the aerodynamic-stripping regime of liquid-jet atomization. It was found that the loss of droplets due to vaporization and dispersion had a marked effect on drop size measurements. A scattered-light scanner, developed at NASA Lewis Research Center was used to measure Sauter mean diameters, D sub 32, as small as 5 microns, which were correlated with nitrogen gas mass-velocity to give the following expression: D(sup -1)(sub 32) = 11.7(rho (sub n) V(sub n))(sup 1.33) where D sub 32 and p(sub n)V(sub n) are given in centimeters and g/sq cm-sec, respectively. The exponent 1.33 is the same as that predicted by atomizing theory for liquid-jet breakup in high velocity gas streams.

Ingebo, Robert D.↗

Gas density effect on dropsize of simulated fuel sprays

Two-phase flow in pneumatic two-fluid fuel nozzles was investigated experimentally to determine the effect of atomizing-gas density and gas mass-flux on liquid-jet breakup in sonic-velocity gas-flow. Dropsize data were obtained for the following atomizing-gases: nitrogen; argon; carbon dioxide; and helium. They were selected to cover a gas molecular-weight range of 4 to 44. Atomizing-gas mass-flux ranged from 6 to 50 g/sq cm-sec and four differently sized two-fluid fuel nozzles were used having orifice diameters that varied from 0.32 to 0.56 cm. The ratio of liquid-jet diameter to SMD, D sub o/D sub 32, was correlated with aerodynamic and liquid-surface forces based on the product of the Weber and Reynolds number, We*Re, and gas-to-liquid density ratio, rho sub g/rho sub l. To correlate spray dropsize with breakup forces produced by using different atomizing-gases, a new molecular-scale dimensionless group was derived. The derived dimensionless group was used to obtain an expression for the ratio of liquid-jet diameter to SMD, D sub o/D sub 32. The mathematical expression of this phenomenon incorporates the product of the Weber and Reynolds number, liquid viscosity, surface tension, acoustic gas velocity, the RMS velocity of gas molecules, the acceleration of gas molecules due to gravity, and gas viscosity. The mathematical expression encompassing these parameters agrees well with the atomization theory for liquid-jet breakup in high velocity gas flow. Also, it was found that at the same gas mass-flux, helium was considerably more effective than nitrogen in producing small droplet sprays with SMD's in the order of 5 micrometers.

Ingebo, Robert D.↗

Gas density effect on dropsize of simulated fuel sprays

Two-phase flow in pneumatic two-fluid fuel nozzles was investigated experimentally to determine the effect of atomizing-gas density and gas mass-flux on liquid-jet breakup in sonic-velocity gas-flow. Dropsize data were obtained for the following atomizing-gases: nitrogen; argon; carbon dioxide; and helium. They were selected to cover a gas molecular-weight range of 4 to 44. Atomizing-gas mass-flux ranged from 6 to 50 g/sq cm-sec and four differently sized two-fluid fuel nozzles were used having orifice diameters that varied from 0.32 to 0.56 cm. The ratio of liquid-jet diameter to SMD, D sub o/D sub 32, was correlated with aerodynamic and liquid-surface forces based on the product of the Weber and Reynolds number, and gas-to-liquid density ratio, rho sub g/rho sub 1. To correlate spray dropsize with breakup forces produced by using different atomizing-gases, a new molecular-scale dimensionless group was derived. The derived dimensionless group was used to obtain an expression for the ratio of liquid-jet diameter to SMD, D sub o/D sub 32. The mathematical expression of this phenomenon incorporates the product of the Weber and Reynolds number, liquid viscosity, surface tension, acoustic gas velocity, the RMS velocity of gas molecules, the acceleration of gas molecules due to gravity, and gas viscosity. The mathematical expression encompassing these parameters agrees well with the atomization theory for liquid-jet breakup in high velocity gas flow. Also, it was found that at the same gas mass-flux, helium was considerably more effective than nitrogen in producing small droplet sprays with SMD's in the order of 5 micrometers.

Ingebo, Robert D.↗