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DOE OSTI2020

Backpropagated frame transformation theory: A reformulation

In this work, the energy-dependent frame transformation theory of Gao and Greene [H. Gao and C. H. Greene, Phys. Rev. A 42, 6946 (1990)] is extended to yield a quantitatively accurate description of the dissociative recombination process. Evidence is presented to show that direct application of the original theory leads to inaccurate cross sections. A major revision, based on an interaction-free backpropagation of the Born-Oppenheimer solutions, markedly improves the frame transformation theory, reducing its average error by orders of magnitude. The original theory and its extension are tested on the previously explored two-dimensional (2D) model that is tailored to describe the singlet ungerade states of molecular hydrogen. The 2D model can be solved exactly (within the numerical accuracy) without implementing the Born-Oppenheimer approximation. These exact results then serve as a benchmark for the frame transformation theory developed in this paper.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1972

Lifetime and quenching of CO /a super 3 pi/ produced by recombination of CO2 ions in a helium afterglow.

Demonstration that rapid dissociative recombination of CO2(+) in a flowing, helium afterglow is an efficient source of CO in the a super 3 pi metastable state. Ions produced by mixing CO2 with He(2 super 3 S) recombine to produce a CO metastable afterglow with a number density as great as 10 to the 9th per sq cm. Monitoring of the (a super 3 pi-X super 1 sigma) Cameron transition in CO was used to study the lifetime and quenching of CO (a super 3 pi) by CO2, N2, NO, and He. Recombination of CO2(+) also produces CO in the d super 3 delta and a' super 3 sigma states.

Wauchop, T. S.↗
NASA NTRS1976

The O I /5577-A wavelength/ airglow - Observations and excitation mechanisms

Analysis of the O I /5577-A wavelength/ airglow observations conducted on board the Atmosphere Explorer C satellite yields the following results when combined with simultaneous measurements of ion and neutral composition. A volume emission rate profile derived after sunset requires the production of an O(1S) atom in 8% of the O2(+) recombinations. Photoelectric impact on atomic oxygen and the dissociative recombination of O2(+) are important sources of O(1S) in the dayglow; however, the airglow measurements require a large additional production of O(1S) below 200 km in addition to these. The reaction N + O2(+) yielding NO(+) + O(1S) can provide the missing O(1S) source if the rate coefficient is near 2.5 times 10 to the minus 11th cu cm per sec.

Frederick, J. E.↗
NASA NTRS1979

Recombination of NO/+/ in the mid-latitude trough and the polar ionization hole

The dissociative recombination of NO(+) with electrons is further examined using a sample of Atmosphere Explorer data from the midlatitude ionization trough. The electron temperature for this data sample covered a range of 2500 K, thus allowing an accurate determination of the temperature dependence of the rate coefficient. The results confirm earlier determinations which were made from a large data base, and the rate coefficient alpha is found to be inversely proportional to the electron temperature. The possibility of a neglected process in the NO(+) chemistry is investigated which, if it were included, might result in a smaller temperature dependence of alpha. Such a source would require a direct dependence on electron temperature. A possible candidate is associative recombination of energetic N(D-2) with O. The results confirm recent measurements which find that this process cannot be significant. The NO(+) chemistry is a very sensitive indicator of chemical equilibrium conditions. By using measurements of the relevant parameters made in the polar ionization hole it is found that horizontal drifts do not appear to be significant in this region.

Torr, M. R.↗
NASA NTRS1989

Recombination measurements in microwave plasma afterglows

The physical implications of problems arising during afterglow-plasma dissociative recombination experiments are discussed, summarizing recent results. Typical numerical data are compiled in tables, and particular attention is given to (1) microwave heating of electrons in afterglow plasmas, (2) the role of vibrationally excited ions in afterglows, (3) electron-ion recombination at high ambient gas densities, and (4) ion-ion recombination.

Johnsen, Rainer↗
NASA NTRS1984

Recombination of electrons with H3(+) and H5(+) ions

A microwave afterglow-mass spectrometer apparatus is used to determine the dissociative recombination coefficients for capture of electrons by H3(+) and H5(+) ions as a function of electron temperature. At an ion and neutral temperature of 240 K, the coefficient for H3(+) is found to vary slowly with the electron temperature at first, decreasing from 1.6 x 10 to the -7th cu cm/s at an electron temperature of 240 K to 1.2 x 10 to the -7th cu cm/s at an electron temperature of 500 K; at electron temperatures ranging from 500 to 3000 K, the coefficient falls as the reciprocal of the electron temperature. It is noted that the results, which have an uncertainty of + or - 20 percent, agree satisfactorily over the common energy range (0.03-0.36 eV) with the recombination cross sections determined in merged beam measurements by Auerbach et al. (1977). Attention is also given to the implication of the results for modeling planetary atmospheres and interstellar clouds.

Macdonald, J. A.↗
NASA NTRS1977

The structure of cometary ionospheres. II - CO-rich comets

The structure of the ionosphere of a CO-rich comet is computed using two different models. The first one, the photochemical model, assumes that the dissociation and ionization of cometary neutrals and ions are due to photoionization, and photodissociation by solar UV radiation together with dissociative recombinations and ion-neutral reactions. The second one, the internal source model, also incorporates the ionization and dissociation effects of an electric current discharging through the inner coma. The generation of this current has been discussed in earlier papers. It is concluded that the internal source model can explain qualitatively the basic morphology of the ionospheres of CO-rich comets such as Humason (1962, VIII) and Morehouse (1908, III), whereas the photochemical model cannot. The main aim of this paper is not so much to provide accurate numerical estimates as to draw attention to a process which may very well dominate the structures of cometary ionospheres.

Ip, W.-H.↗
NASA NTRS1986

Mass and energy balance of the cold Io torus

A new model of the cold Io torus is described. Ions and energy are injected into the system by independent processes so that the mass balance is isolated from the energy balance. The primary source of energy is local ionization and acceleration of hot pickup ions resulting from charge exchange between thermal ions and an extended cloud of Iogenic sulfur and oxygen atoms. The primary energy loss mechanism of the plasma is collisionally excited line emission at optical wavelengths. The primary ion source is radial diffusion inward from the hot torus on a time scale of 140-710 days. The primary ion loss mechanism is a novel two-step enhanced recombination mechanism involving charge exchange between thermal ions and an extended cloud of neutral SO2 molecules, followed by rapid dissociative recombination of the resultant molecular ion. The model provides a self-consistent solution which reconciles a number of diverse observations with known physical processes.

Moreno, M. A.↗
NASA NTRS1997

Mechanism for the Green Glow of the Upper Ionosphere

The generation of the green line of atomic oxygen by dissociative recombination of 02 plus occurs by the capture of an electron into a repulsive state of 02 followed by dissociation along another state of a different electronic symmetry. The two states are coupled together by mixed symmetry Rydberg states. Quantum chemical calculations give a rate coefficient at room temperature of (0.39 (+ 0.31 or -0.19)) x 10 exp -8 cubic centimeters per second. The quantum yield of excited oxygen is within the range deduced from ground, rocket, and satellite observations. The rate coefficients and yields are needed in models of the optical emission, chemistry, and energy balance of planetary ionospheres.

Guberman, Steven L.↗
NASA NTRS1990

Theoretical studies of important processes in planetary and comet atmospheres

Dissociative recombination (DR) reactions in planetary and comet atmospheres are discussed. A computer program was developed which determines DR cross sections and rates using potential curves and electronic capture widths. It uses Multi-Channel Quantum Defect Theory (MQDT) to include excited Rydberg resonance levels in the DR cross section and rate calculations. Each vibrational level of a molecular ion is the limit for an infinite series of Rydberg states. Above each ion vibrational level are Rydberg vibrational levels having higher ion levels as their series limit. These Rydberg vibrational levels are resonances, i.e., neutral states which are imbedded in the electron-molecular ion continuum. The process in which the Rydberg level causes an abrupt perturbation in the cross section for DR (because of interference between capture into the Rydberg level and capture into the repulsive dissociative state) is referred to as indirect recombination. The process in which the Rydberg levels are excluded and recombination goes from the entrance channel to the repulsive state is called direct recombination. The full DR process, i.e., both direct and indirect recombination, is the process of importance for planetary atmospheres. These ideas are illustrated with the new results for DR from excited ion vibrational levels of O2(+) into the dissociative state which leads to O(1S) + O(1D).

Guberman, Steven L.↗
NASA NTRS1996

Electron-Ion Recombination Rate Coefficient Measurements in a Flowing Afterglow Plasma

The flowing-afterglow technique in conjunction with computer modeling of the flowing plasma has been used to determine accurate dissociative-recombination rate coefficients alpha for the ions O2(+), HCO(+), CH5(+), C2H5(+), H3O(+), CO2(+), HCO2(+), HN2O(+), and N2O(+) at 295 K. We find that the simple form of data analysis that was employed in earlier experiments was adequate and we largely confirm earlier results. In the case of HCO(+) ions, published coefficients range from 1.1 X 10(exp -7) to 2.8 x 10(exp -7) cu cm/S, while our measurements give a value of 1.9 x 10(exp -7) cu cm/S.

Gougousi, Theodosia↗
NASA NTRS1974

Measurements of positive ion conversion and removal reactions relating to the Jovian ionosphere

Measured rates are presented for the reaction of He(+) ions with H2 (and D2) molecules to form H(+), H2(+), and HeH(+) ions, as well as for the subsequent reactions of H(+) and HeH(+) ions with H2 to form H3(+). The neutralization of H3(+) /and H5(+)/ ions by dissociative recombination with electrons is shown to be fast. The reaction He(+) + H2 is slow (k 1.1 x 10 to the minus 13th cu cm/sec at 300 K) and produces principally H(+) by the dissociative charge transfer branch. It is concluded that there may be a serious bottleneck in the conversion of two of the primary ions of the upper Jovian ionosphere, H(+) and He(+) (which recombine slowly), to the rapidly recombining H3(+) ion.

Johnsen, R.↗
NASA NTRS1991

Molecular origin of Io's fast sodium

Neutral sodium emissions encircling Jupiter exhibit an intricate and variable structure that is well matched by a simple loss process from Io's atmosphere. These observations imply that fast neutral sodium is created locally in the Io plasma torus, both near Io and as much as 8 hours downstream. Sodium-bearing molecules may be present in Io's upper atmosphere, where thay are ionized by the plasma torus and swept downstream. The molecular ions dissociate and dissociatively recombine on a short time scale, releasing neutral fragments into escape trajectories from Jupiter. This theory explains a diverse set of sodium observations, and it implies that molecular reactions (particularly electron impact ionization and dissociation) are important at the top of Io's atmosphere.

Schneider, Nicholas M.↗
NASA NTRS1976

Abundances of simple oxygen-bearing molecules and ions in interstellar clouds

The abundances of simple oxygen-bearing interstellar molecules in warm (T at least 40 K), diffuse, and moderately thick clouds are calculated on the basis of binary gas-phase reactions. The most important reactions are ion-molecule, charge-exchange, and dissociative-recombination reactions, as suggested mainly by earlier workers. The progenitor of these molecules in diffuse clouds is the cosmic-ray-produced H(+) ion, working through the charge-exchange reaction with O. The ionization of H(+) and He(+) is also discussed. Dissociative charge exchange of He(+) with H2 is an important source of H(+) in regions of large fractional abundance of H2, as well as an important destruction mechanism for He(+) even for small f (at least 0.1). The calculated molecular abundances are consistent with some of the available observational information.

Glassgold, A. E.↗
NASA NTRS1980

The excitation and collisional deactivation of metastable N/2P/ atoms in auroras

The concentration and altitude distribution of metastable N(2P) atoms was measured in a diffuse IBC II(+) auroral arc. The dominant N(2P) source is shown to be the dissociative excitation of N2 by electron impact with a minor contribution from the dissociative recombination of N2(+) ions. The possibility that an ion-molecule process involving atomic oxygen and vibrationally excited N2(+) ions is a significant N(2P) source is examined. Values for the proportional yield of N(+), N(2P), N(2D), and N(4S) atoms from electron-impact dissociation of N2 under optically thick conditions are given.

Zipf, E. C.↗
NASA NTRS1991

Laboratory simulation of the surface of Halley's Comet

In the past year we have developed a model for the dissociation of icy grains in comets. In general, this model does not predict the radical yield that is observed in the jets of comets. To reproduce these yields, the concentration of the radical's precursors will have to be too high to be consistent with the abundance that we expect in comets. We have also constructed a theoretical model for the formation of ions on icy cometary grains. That model shows that only a small number of the cometary ions could be produced as ions in icy grains if the particle has only positively charged ions. If it contains both positive and negative ions then it could have a higher concentration of ions without violating charge neutrality. When such a particle evaporates, it can release ions with both charges into the gas phase. These ions could produce radicals via dissociative recombination with electrons if they are positive ions or by photoattachment of electrons if they are negative electrons. Finally, an avalanche process involving the acceleration of electrons towards charged particles is evaluated. It is shown that this will not lead directly to gas phase ions, but it might lead to additional ionization and dissociation on the grain.

Jackson, William M.↗
NASA NTRS1987

Molecular processes in a high temperature shock layer

Research was completed on several aspects of dissociative recombination (DR) for the molecules NO(+), N2(+), and O2(+). For O2(+), DR with an electron is described by, O2(+) + e(-) yields O + O. Model studies were completed of the windows arising in DR cross section from excited ion vibrational levels and of the variation of the DR cross section with the intersection point of the ion and neutral dissociative state potential curves.

Guberman, Steven L.↗
NASA NTRS1994

Recombination of H(3+) and D(3+) ions with electrons

Flowing-afterglow measurements in decaying H3(+) or D3(+) plasmas suggest that de-ionization does not occur by simple binary recombination of a single ion species. We find that vibrational excitation of the ions fails to provide an explanation for the effect, contrary to an earlier suggestion. Instead, we suggest that collisional stabilization of H3** Rydberg molecules by ambient electrons introduces an additional dependence on electron density. The proposed mechanism would permit plasma de-ionization to occur without the need for dissociative recombination by the mechanism of potential-surface crossings.

Johnsen, R.↗