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NASA NTRS2002

D-Wave Resonances in Positronium Hydride

The problem of calculating the position and width of the lowest-lying (L = 0, 1) resonances in the Ps + H scattering system has recently been re-examined by the authors [1]. In the model used, resonances axe assumed generated by bound Rydberg states in the closed re-arranged channel [e(+) + H(-)]. This infinite series of Coulomb bound states are shifted somewhat by the coupling with the open scattering channel [Ps + H]. Estimates using this approach, first carried out by one of the authors [2] using a simple form of scattering wavefunction, indicated an anticipated small shift of resonance away from the Rydberg energy in the S-wave (L = 0). More recent results by Ho and Yan [3] using the complex-rotation method showed unexpected significant shifting in the P (L = 1) and D (L = 2)-wave resonance energies from their respective unperturbed values. Our re-calculation of the resonances [I I for L = 0 and I indicates that, in each case, reasonably consistent resonance energies are obtained by coupling the two lowest lying states (IS and 2S for L = 0 and 2P and 3P for L = 1). For each L it is the higher state (2S and 3P, respectively) that produces the resonance. The lower state (1S and 2P, respectively) is effective only in increasing the non-resonant phase shift. In this work we extend the model to L = 2 (D-waves). Our results show that, unlike the S and P-waves, the 313-state alone produces a resonant energy that is very close to the result of Yan and Ho [3]. Inclusion of the 4D-state produces a second resonance in the scattering system shifted up slightly from its unperturbed Rydberg energy.

Drachman, Richard J.↗
NASA NTRS2001

Polarizabilities and Other Properties of the td Muons Molecular Ion

Wavefunctions of Hylleraas type were used earlier to calculate energy levels of muonic systems. Recently, we found in the case of the molecular ions H2+, D2+ and HD+ that it was necessary to include high powers of the internuclear distance in the Hylleraas functions to localize the nuclear motion when treating the ions as three-body systems without invoking the Born-Oppenheimer approximation. We try the same approach in a muonic system, td(mu-). Improved convergence is obtained for J = 0 and 1 states for shorter expansions when we use this type of generalized Hylleraas function, but as the expansion length increases the high powers are no longer useful. We obtain good energy values for the two lowest J = 0 and J = 1 states and compare them with the best 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 of the ground state is then calculated using second-order perturbation theory with intermediate J = 1 pseudostates. It should be possible to measure the polarizability by observing Rydberg states of atoms with td(mu-) acting as the nucleus.

Bhatia, A. K.↗
NASA NTRS1993

Optically thick cascade to the O I 3s 3S state in the Earth's thermosphere

The electron impact excitation cross section for the O I (1304 A) emission is enhanced in the terrestrial thermosphere owing to an optically thick cascade mechanism. Values for the contribution of the cascade have been calculated and deduced from measured 1304-A airglow emissions to between o and 200%. We have developed a model to calculate a large portion of the optically thick cascade contribution, including contributions from the radiative entrapment of the O I (1040, 1027, and 989 A) lines. High-resolution spectroscopic data from a sounding rocket experiment are analyzed using this model. The optically thick cascade contribution for the three lower lying states was evaluated to be 24.5% and compares well with recent calculations. The data, however, support a total contribution of 40%. The 15.5% difference is likely due to the contribution from higher Rydberg states.

Cotton, Daniel M.↗
NASA NTRS1996

Products of Dissociative Recombination in the Ionosphere

SRI International undertook a novel experimental measurement of the product states formed by dissociative recombination (DR) of O2(+), NO(+), and N2(+) as a function of both electron energy and reactant ion vibrational level. For these measurements we used a recently developed experimental technique for measuring dissociation product distributions that allows both the branching ratios to be accurately determined and the electronic and rovibrational state composition of the reactant ions to be specified. DR is the dominant electron loss mechanism in all regions of the ionosphere. In this process, electron attachment to the molecular ion produces an unstable neutral molecule that rapidly dissociates. For a molecular ion such as O2(+), the dissociation recombination reaction is (1) O2(+) + e yields O + O + W. The atomic products of this reaction, in this case two oxygen atoms, can be produced in a variety of excited states and with a variety of kinetic energies, as represented by W in Eq. (1). These atoms are not only active in the neutral chemistry of the ionosphere, but are also especially important because their optical emissions are often used to infer in situ concentrations of the parent molecular ion and ambient electron densities. Many laboratory measurements have been made of DR reaction rates under a wide range of electron temperatures, but very little is known about the actual distributions among the final states of the atomic products. This lack of knowledge seriously limits the validity and effectiveness of efforts to model both natural and man-made ionospheric disturbances. Bates recently identified major deficiencies in the currently accepted branching ratios for O2(+) as they relate to blue and green line emission measurements in the nocturnal F-region. During our two-year effort, we partially satisfied our ambitious goals. We constructed and operated a variable pressure, electron-impact ion source and a high pressure, hollow-cathode discharge ion source for O2(+), NO(+), and N2(+) beams. Translational spectroscopy of the products of dissociative charge transfer in Cs vapor was used to accurately assay the composition of the O2(+) and NO(+) beams and to develop a methodology for the vibrationally controlled preparation of the ground state ion beams. Attempts to assay the N2(+) beam revealed a novel two-electron process in the charge transfer reactions. A coaxial electron gun for the DR measurements was constructed following an extensive numerical design of the fields. Tests of the gun, however, found substantial perturbations of the magnetic fields by the soft iron (CMI-C) assembly containing the Langmuir probe that locates the electron beam. Hydrogen annealing of the iron failed to eliminate the field perturbations, necessitating the removal of the probe assembly. During this work on the coaxial electron gun, we discovered that predissociated high Rydberg states of O2 could be produced by subjecting the molecules to a sudden perturbation by an electromagnetic field. This technique allowed a measurement of the product branching to the atomic limits for the lowest seven vibrational levels of O2(+).

Cosby, Philip↗
NASA NTRS1974

Dissociation of CH4 by electron impact: Production of metastable hydrogen and carbon fragments

Metastable fragments produced by electron impact excitation of CH4 have been investigated for incident electron energies from threshold to 300 eV. Only metastable hydrogen and carbon atoms were observed. Onset energies for the production of metastable hydrogen atoms were observed at electron impact energies of 22.0 + or - .5 eV, 25.5 + or - .6 eV, 36.7 + or - .6 eV and 66 + or - 3 eV, and at 26.6 + or - .6 eV for the production of metastable carbon atoms. Most of the fragments appear to have been formed in high-lying Rydberg states. The total metastable hydrogen cross section reaches a maximum value of approximately 1 X 10 to the minus 18th power sq cm at 100 eV. At the same energy, the metastable carbon cross section is 2 x 10 to the minus 19th power sq cm.

Finn, T. G.↗
NASA NTRS1981

Lyman-alpha fluorescence from hydrogen photofragments of CH4 and H2O

The process of H-Lyman-alpha fluorescence produced through photodissociation of CH4 and H2O provides an example for the usefulness of the detection of fluorescence of dissociation fragments as an aid in identifying some high lying Rydberg states. In the first experiment reported, an electron storage ring synchrotron radiation source was used. The fluorescence produced was detected with a solar blind photomultiplier and a Cs photocathode with a spectral sensitivity in the wavelength range from 1050 to 1950 A. In the second experiment considered, an intense atomic line source was employed.

Wu, C. Y. R.↗
NASA NTRS1982

Fluorescence yields from photodissociation of SO2 at 1060-1330 A

The absorption and fluorescence cross sections of SO2 were measured in the 1060-1330 A region using synchrotron radiation as the light source. Several absorption bands were observed and assigned tentatively to the Rydberg states converging to the SO2(+) states. It is shown that the apparent quantum yields for excitation wavelengths longer than 1200 A are small, and are presumably emitted from the O(1S) and S(1S) metastable species. At shorter excitation wavelengths, the fluorescence cross sections increase at the threshold wavelengths of possible SO2 dissociation processes.

Suto, M.↗
NASA NTRS1982

Photodissociation yields of CS2 at 1060-1520 A

Photoabsorption and fluorescence cross sections of CS2 were measured in the 1060-1520 A region using synchrotron radiation in order to provide information needed for modeling the CS abundance in the interstellar medium. The absorption in the 1060-1200 A region is smooth and continuous, except for the presence of a strong absorption band at 1117 A, while for wavelengths longer than 1200 A, the absorption spectrum shows the structure of Rydberg states. The fluorescence in the 1900-3000 A region begins to appear at 1335 A, and is mainly the CS(A 1Pi-Chi 1Sigma +) transition in the 2400-2800 A region. The fluorescence in the 1900-8000 A region begins to appear at 1490 A, and, in addition to the previous transition, is composed of the transitions of S(1S0-3P1) at 4589 A and of CS(d 3 Delta, a-prime 3Sigma +, and a 3Pi-Chi 1Sigma +) at 3000-4000 A. The quantum yields for the production of fluorescence are determined to have maxima of 13 and 7.5% at 1235 A for the fluorescence in the 1900-8000 and 1900-3000 A regions, respectively.

Day, R. L.↗
NASA NTRS1983

Atomic nitrogen emissions from photodissociation of N2

Cross sections for the production of N I emissions at 1412, 1493, and 1743 A and the undispersed fluorescence in the range 1050-1800 A produced through photodissociative excitation of N2 have been determined at selected intense atomic emission lines and throughout the synchrotron radiation continuum from 500 to 620 A. The neutral excited atomic nitrogen fragments are produced through direct dissociation processes as well as predissociation from the well-known two-electron excited Rydberg states. The yield for photodissociative excitation processes is found to have the same magnitude as that for photodissociative ionization processes reported by other investigators. The Doppler shifts of the excited atomic fragments have been calculated, and the relevance to atmospheric observations is discussed.

Wu, C. Y. R.↗
NASA NTRS1984

Study of the sulphur-containing molecules in the EUV region. IV - The dissociation processes of SO2 in the 760 A region

The fluoresence throughout the VUV and violet regions has been observed from photoexcitation of SO2, and the absolute fluorescence cross sections of the VUV emissions have been measured at selected atomic emission lines and in the synchrotron radiation continuum from 550 to 760 A. Emissions from the O I 1304 A and several S I lines account for the fluorescence observed in the VUV region, while the fluorescence observed in the UV and violet regions is due to excited SO and, also, possibly to excited SO2(+) and SO(+). Structure in the VUV fluorescence excitation function is attributed to predissociation of Rydberg states. The VUV fluorescence resulting from an O2 elimination process, SO2 + h times nu yielding metastable S + O2, has been observed in the present work although the threshold for this process has not been determined. The threshold corresponding to the total dissociation process, SO2 + h times nu yielding metastable S + 2O, has been measured and found to agree reasonably with the expected value calculated from thermochemical data. The processes for the formation of S(+) are also discussed.

Wu, C. Y. R.↗
NASA NTRS1986

Quantitative photoabsorption and fluorescence study of H2O and D2O at 50-190 nm

The photoabsorption cross sections and the fluorescence quantum yields of H2O and D2O were measured in the 50-190 nm region using synchrotron radiation as a light source. The oscillator strengths for the Rydberg states of H2O and D2O were determined from the absorption cross sections measured. The processes for the production of fluorescence from the excited species H(asterisk) (n greater than 2), D(asterisk) (n greater than 2), OH(asterisk) (A) and OD(asterisk) (A) are discussed. The upper limit for the dissociation energy of D(D-OD) was determined, from the threshold of the OD(A-X) fluorescence, to be 5.14 + or - 0.01 eV. The upper limit for the cross section of visible fluorescence from the excited H2O(+) ions was determined to be 2 x 10 to the -19th sq cm. A comparison between the photoexcitation spectra of H2O and D2O is made.

Lee, L. C.↗
NASA NTRS1989

Introduction to dissociative recombination

Dissociative recombination (DR) of molecular ions with electrons has important consequences in many areas of physical science. Ab-initio calculations coupled with resonant scattering theory and multichannel quantum defect studies have produced detailed results illuminating the role of ion vibrational excitation, the quantum yields of the DR products, and the role of Rydberg states. The theoretical and experimental results are discussed.

Guberman, Steven L.↗
NASA NTRS1989

Ab initio studies of dissociative recombination

Quantum chemical calculations of the dissociative recombination of O2(+) and N2(+) are reported. An approach for calculating autoionization widths from high-principal-quantum-number Rydberg states is summarized, and an example is presented for the lowest dissociative state of O2. For O2(+), the 1Sigma(+)u state is the sole source of O(1S) from the lowest 10 vibrational levels of the ion. Rate coefficients for generating O(1S) and O(1D) at ionospheric temperatures are reported.

Guberman, Steven L.↗
NASA NTRS1991

Induced ClO vacuum ultraviolet fluorescence

Some vibronic transitions of ClO such as G(v-prime = 11 )-X(v-double prime = 10), G(v-prime = 5)-X(v-double prime = 3) and H(v-prime = 4)-X(v-double prime = 2), which promote overtones of X(2pi3/2) to bound Rydberg states, are nearly resonant with the 130.6 nm O-atom emission line and possess sizable Franck-Condon factors. On this basis broadband detection of 'O atom' fluorescence in experiments involving vibrationally excited ClO(X) is ascribed to the radiative decay of ClO(G, H) rather than to the formation of O atoms; these observations raise the probability of monitoring ClO(X; v = 0) by VUV-induced fluorescence.

Colussi, A. J.↗
NASA NTRS1994

NLTE model stellar atmospheres with line blanketing near the series limits

In this paper we study the influence of line-merging regions at the intermediate long-wavelength side of a continuum threshold on the computed model atmosphere structure and predicted spectrum. In order to model these regions sufficiently accurately, we have developed two concepts. First, we have extended the occupation probability formalism of Hummer and Mihalas to non-local thermodynamic equilibrium (non-LTE) plasmas. Second, in order to treat the very complicated opacity in the line merging region, we have generalized the concept of opacity distribution functions to treat non-LTE situations. All Rydberg states are consistently included within this framework, so that no arbitrary cutoff of high (LTE) levels is made. We have calculated several pure hydrogen models atmospheres for two effective temperatures, T(sub eff) = 20000 and 35000 K, and discussed the differences between models calculated with various treatments of the line merging. In particular, we have shown that the error in the predicted profiles of Balmer lines resulting from the neglect of line merging is typically of the order of 3-4%, while the errors in the far-UV portion of the Balmer continuum reaches 15-35%. The errors generally decrease with increasing effective temperature. At the same time, the internal accuracy of the models is shown to be about or below 0.5% for all predicted spectral features. We conclude that for interpreting current high-accuracy spectrophotometric observations models including the line merging are necessary, and that the formalism developed in this paper is capable of providing a sufficiently accurate and robust modeling technique.

Hubeny, I.↗
NASA NTRS1997

High-Resolution Studies of Extreme-Ultraviolet Emission from CO by Electron Impact

We report a high-resolution study (0.0036 nm full width at half maximum) of electron-impact-induced emission spectra of CO at 30-, 75-, and 100-eV electron-impact energies. The spectral features were acquired in optically thin conditions. At the specified resolution, attainable with our 3-m vacuum ultraviolet spectrometer, we observe rotationally resolved emission bands of CO in the extreme ultraviolet, from the vibronic states B (sup 1)sigma(sup +)(0), C (sup 1)sigma(sup+)(0), and E (sup 1)pi(0), to the ground state X (sup 1)sigma(sup +)(0). A simple model of these bands, based on the Honl-London factors and the rotational constants, is constructed and is shown to be in good agreement with the observed spectra. The predissociation yield for the E (sup 1)pi electronic state has been determined, showing that the E state has the largest predissociation cross section of CO for all singlet-state Rydberg series members. The excitation function of the [E (sup 1)pi(0) yields X (sup 1)sigma(sup +)(0)] transition, in the 0-800-eV impact energy range, is measured, permitting determination of the oscillator strength by using a modified Born approximation analytical fit.

Ciocca, Marco↗
NASA NTRS2005

Atomic and Molecular Physics

A symposium on atomic and molecular physics was held on November 18, 2005 at Goddard Space Flight Center. There were a number of talks through the day on various topics such as threshold law of ionization, scattering of electrons from atoms and molecules, muonic physics, positron physics, Rydberg states etc. The conference was attended by a number of physicists from all over the world.

Bhatia, Anand K.↗
NASA NTRS1976

Decomposition of the photoabsorption Schumann-Runge continuum in O2

The photoabsorption Schumann-Runge continuum in O2 has been decomposed into the contribution from states of both valence and Rydberg character. The decomposition of the experimental photoabsorption (or high-energy, zero-angle, electron energy-loss) data contains contributions from three valence states, four Rydberg states, and one state of unknown character. Information on the perturbed valence-state potential-energy curves in the Franck-Condon region obtained by this analysis substantiate the recent theoretical conclusions of strong valence-Rydberg perturbations in the 8-12 eV excitation region. There is presently no unambiguous identification for the state at 8.93 plus or minus 0.04 eV, found in the optical and all the electron energy-loss data.

Cartwright, D. C.↗