Measurements of recombination of electrons with HCO+ ions.
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Leu, M. T.↗
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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↗
Plasma decay in hydrocarbons and hydrocarbon- and H 2 O-containing mixtures excited by high-voltage nanosecond discharge at elevated gas temperatures
Plasma decay after a high-voltage nanosecond discharge was experimentally and numerically studied in pure hydrocarbons (C 2 H 6 and C 3 H 8 ), and H 2 O:N 2 and C 3 H 8 :O 2 mixtures for pressures in the range 2–4 Torr and gas temperatures from 300 to 600 K. In a stoichiometric C 3 H 8 :O 2 mixture, plasma decay was also studied in a repetitively pulsed discharge for varing numbers of discharge pulses (varying degrees of fuel oxidation). The rate of plasma decay was determined from the temporal evolution of electron density measured using the microwave interferometer. It was observed that gas heating to 600 K leads to a decrease in the rate of plasma decay in all cases. The effect of heating on plasma decay was most profound in the H 2 O:N 2 mixture (after a single discharge pulse) and in the C 3 H 8 :O 2 mixture for high degrees of fuel oxidation. A kinetic scheme was developed to numerically simulate the plasma decay in hydrocarbons and combustible mixtures. Numerical analysis showed that, under the conditions studied, plasma decay was controlled by dissociative electron recombination with simple molecular and cluster ions. Gas heating led to a decrease in the rate of the electron-ion recombination and the rate of conversion of molecular ions to cluster ions. As a result, the gas temperature increase caused a decrease in the fraction of cluster ions for which the recombination coefficients are an order of magnitude higher than the recombination coefficients for molecular ions. The influence of gas heating on the decrease of the amount of cluster ions was more important when the ion composition was dominated by hydrated H 3 O + (H 2 O) k ions. The rates of the formation of these ions are extremely sensitive to any variations in gas temperature. A result, in agreement with our observations, gas heating led to an anomalous decrease in the rates of plasma decay in the H 2 O:N 2 mixture, as well as in the C 3 H 8 :O 2 mixture when H 2 O molecules were produced due to fuel oxidation.
20 FOSSIL-FUELED POWER PLANTS↗
Cooling and recombination processes in cometary plasma
The ion electron plasma in comets is examined for cooling processes which result from its interactions with the neutral coma. A cometary coma model is formulated that is composed predominantly of H2O and its decomposition products where electrons are cooled in a variety of processes at rates varying with energy. It is shown that solar plasma plus accumulated cometary ions and electrons is affected very strongly as it flows into the coma. The electrons are rapidly cooled and all but some 10% of the ions undergo charge exchange. Photodissociation of H2O is assumed where ion electron recombination is the dominant loss process.
Wallis, M. K.↗
Dielectronic recombination rates, ionization equilibrium, and radiative emission rates for calcium and nickel ions in low-density high-temperature plasmas
The total dielectronic recombination rates for Ca and Ni ions were calculated taking into account autoionization to excited states of the recombining ion and stabilizing radiative transitions of the recombining electron. Radiative transitions of the recombining ion are found to be the dominant stabilizing processes, and the relative importance of Delta n = 0 and Delta n not equal to 0 transitions in the relevant temperature region is determined for each ion. The relative importance of the Delta n = 0 and Delta n not equal to 0 contributions is significantly altered for some ions by the inclusion of autoionization to excited levels. The relative abundance of the various ionization stages has been determined by using a corona equilibrium model in which collisional ionization and inner-shell excitation followed by autoionization are balanced by direct radiative and dielectronic recombination.
Jacobs, V. L.↗
(abstract) Experimental and Modeling Studies of the Exchange Current at the Alkali Beta'-Alumina/Porous Electrode/Alkali Metal Vapor Three Phase Boundary
The microscopic mechanism of the alkali ion-electron recombination reaction at the three phase boundary zone formed by a porous metal electrode in the alkali vapor on the surface of an alkali beta'-alumina solid electrolyte (BASE) ceramic has been studied by comparison of the expected rates for the three simplest reaction mechanisms with known temperature dependent rate data; and the physical parameters of typical porous metal electrode/BASE/alkali metal vapor reaction zones. The three simplest reactions are tunneling of electrons from the alkali coated electrode to a surface bound alkali metal ion; emission of an electron from the electrode with subsequent capture by a surface bound alkali metal ion; and thermal emission of an alkali cation from the BASE and its capture on the porous metal electrode surface where it may recombine with an electron. Only the first reaction adequately accounts for both the high observed rate and its temperature dependence. New results include crude modeling of simple, one step, three phase, solid/solid/gas electrochemical reaction.
conversion↗
Concerning sources of O/1D/ in Aurora - Electron impact and dissociative recombination
The present investigation is concerned with two questions. One is related to the possibility that the O(1D) level is produced by an as yet unidentified process in aurora. The second question is concerned with the need for an additional source and the altitude over which it is required. The data base of the AE satellite (AE-D in particular) was examined for this study. It is found that dissociative recombination and electron impact are inadequate sources of O(1D) in aurora. Nearly 90% of the source function is unidentified below 200 km and about 55% is missing above 250 km. The possibility that thermal electron impact could provide the missing source above 250 km was examined. Calculations showed that the missing source above 250 km could be explained by thermal electron impact if the electron temperatures were approximately 2900 K.
Sharp, W. E.↗
Electron-temperature dependence of the recombination of HCO(+) ions with electrons
A microwave-afterglow mass-spectrometer apparatus employing microwave heating of the electrons has been used to determine the dependence on Te of the recombination coefficient of electrons with HCO(+) ions. By comparison of the observed electron-density decays to the computed behavior of a recombination- and ambipolar-diffusion-controlled afterglow, it is found that the Te dependence of the recombination coefficients follows a power law with an index of -0.69 + or - 0.07 over the range Te = 293-5500 K. The magnitude of the recombination coefficient is similar to that observed and calculated for simple diatomic ions, while the temperature dependence is somewhat stronger than the Te exp -0.5 dependence predicted by a simplified theory for diatomic ions.
Ganguli, B.↗
Shock-tube studies of N sup plus and O sup plus recombination radiation in the vacuum ultraviolet Final report
Shock tube spectral measurements of electron recombinations with nitrogen and oxygen ions in far UV radiation range
Marrone, P. V.↗
Tracking structural solvent reorganization and recombination dynamics following e – photoabstraction from aqueous I – with femtosecond x-ray spectroscopy and scattering
Here we present a sub-picosecond resolved investigation of the structural solvent reorganization and geminate recombination dynamics following 400 nm two-photon excitation and photodetachment of a valence p electron from the aqueous atomic solute, I–(aq). The measurements utilized time-resolved X-ray Absorption Near Edge Structure (TR-XANES) spectroscopy and X-ray Solution Scattering (TR-XSS) at the Linac Coherent Light Source x-ray free electron laser in a laser pump/x-ray probe experiment. The XANES measurements around the L 1 -edge of the generated nascent iodine atoms (I 0 ) yield an average electron ejection distance from the iodine parent of 7.4 ± 1.5 Å with an excitation yield of about 1/3 of the 0.1M NaI aqueous solution. The kinetic traces of the XANES measurement are in agreement with a purely diffusion-driven geminate iodine–electron recombination model without the need for a long-lived (I 0 :e–) contact pair. Nonequilibrium classical molecular dynamics simulations indicate a delayed response of the caging H 2 O solvent shell and this is supported by the structural analysis of the XSS data: We identify a two-step process exhibiting a 0.1 ps delayed solvent shell reorganization time within the tight H-bond network and a 0.3 ps time constant for the mean iodine–oxygen distance changes. The results indicate that most of the reorganization can be explained classically by a transition from a hydrophilic cavity with a well-ordered first solvation shell (hydrogens pointing toward I–) to an expanded cavity around I 0 with a more random orientation of the H 2 O molecules in a broadened first solvation shell.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Time-dependent study of the emitted light and electron density in a low-pressure helium afterglow.
Excited state populations time dependence resulting from ion-electron recombination in He afterglow studied by emitted light relation to electron density
Collins, C. B.↗
Photoionization of seeded combustion products as a method of enhancing the efficiency of magnetohydrodynamic power generators
Here, in this study, we performed an experimental and computational investigation into the feasibility of utilizing photoionization to enhance the electrical conductivity of seeded oxy-fuel combustion products and improve the performance of magnetohydrodynamic (MHD) power generators. We applied a variety of optical and microwave diagnostics to study the ionization and recombination processes of potassium excited by an excimer laser in a high-velocity oxy-fuel free jet. Computational fluid dynamic (CFD) simulations were performed to model the thermophysical properties and species densities of the free jet. The CFD results were validated with position-dependent potassium concentration measurements. Electron recombination exponential lifetimes were measured through time-resolved microwave transmission. The experimental electron lifetimes were compared with lifetimes calculated from CFD-predicted species densities and literature recombination rates. It was determined that K + or O 2 are the most likely recombination partners for photoionized electrons. Time-resolved fluorescence measurements provided evidence of an ionization pathway involving a two-photon ionization of KOH . Finally, a zero-dimensional chemical kinetic model was developed to assess the fundamental viability of inducing a non-equilibrium electron population to provide a net energy return in combustion-driven MHD power generators. We determined that a high energy return is feasible for targeting electrode boundary layers with ultraviolet photoionization. We also found that photoionization could potentially lower the required temperature of the bulk gas flow.
20 FOSSIL-FUELED POWER PLANTS↗
Detection of interstellar recombination lines from emitters of intermediate mass.
The 18-cm microwave spectra of Orion B and W3A show evidence of an emission feature to the high-frequency side of the carbon recombination line. Observations at different frequencies establish that this feature results from electronic recombination. In addition, theoretical considerations, results of 21-cm observations, and computer-simulated spectra suggest that the new feature originates in a predominantly neutral hydrogen region and can be explained by a superposition of recombination lines from any or all of the following elements: Mg-24, Si-28, S-32, and Fe-56.
Chaisson, E. J.↗
Electron temperature dependence of recombination of Ne super plus sub 2 ions with electrons
Electron temperature dependence of molecular neon ions recombination with electrons using microwave afterglow/mass spectrometer, obtaining recombination coefficient
Biondi, M. A.↗
Excitons in Hematite Fe 2 O 3 : Short-Time Dynamics from TD-DFT and Non-Adiabatic Dynamics Theories
We present a first-principles study of the short-time dynamics of excitons in hematite Fe 2 O 3 . We used time-dependent density functional theory (TD-DFT) with an underlying DFT+U treatment of electron interactions to characterize the electronic structure of excitons and nonadiabatic molecular dynamics theory (NA-MD) to determine their recombination (electronic ground-state recovery) and relaxation dynamics. Decoherence-corrected trajectory surface hopping approaches in NA-MD simulations yielded recovery times of ~1.1 to 1.8 ns and “higher-lying” exciton relaxation times of ~60 to 70 fs, in accord with experimentally derived lifetimes. With hematite phonons in the range of ~100 to 700 cm –1 , higher-lying excitons relax within one or two oscillations of the phonons before getting trapped into an electron–hole pair Exc-3 structure on the first excited state potential energy surface. This structure resembles already a pair of polarons (electron polaron plus hole polaron) with associated lattice distortions three (3) basal planes away. On longer time scales, the electron–hole bipolaronic pair hops to structures Exc-5, then Exc-7, then Exc-9, ... with the electron polaron and hole polaron separated by 5, 7, 9, ... basal planes in a process of charge separation. The largest frequency phonon ~672 cm –1 for the Exc-3 exciton structure is associated with the electron polaron moiety of the exciton. This phonon is a good candidate for giving rise to the recently observed and reported postexcitation transient IR absorption peak.
36 MATERIALS SCIENCE↗
Field-aligned dynamics of chemically induced perturbations to the ionosphere
Ionospheric modification using photochemically reactive vapors is studied with a one-dimensional, multiion, fluid model of plasma flow along magnetic field lines. The magnitudes of ion and electron density changes are determined by considering both chemical processes (i.e., photoionization, ion-molecule reactions, dissociative recombination, electron attachment) and transport processes (i.e., multispecies diffusion, electric currents, ambipolar electric fields). The numerical treatment in the model is not specific to any type of release or any interaction chemistry. It has been used to simulate releases of Ba, CO2, and CF3Br in the ionosphere, but generalization to other species may be easily accomplished. The results of the calculations are found to be in good agreement with experimental observations. The feasibility of modifying the parallel current paths in the auroral F region is examined.
Bernhardt, P. A.↗
The oxygen emission lines in Wolf-Rayet spectra
The statistical equilibrium of oxygen in the line-emitting regions of WR stars is studied using the one-representative point theory of Castor and van Blerkom (1970) for a wider range of the radiation temperature, electron temperature, and electron density. Radiative processes, collisional processes, and electronic recombination are studied for a 59-level model atom. The level populations depart by large factors from those expected for LTE at the electron temperature and electron density. When the parameters have the values found previously by Bhatia and Underhill to be representative for WR stars, the oxygen atoms are strongly concentrated in the lower levels of O(2+), O(3+), and O(4+). The predicted relative energies in typical lines of O III, O IV, and O V for a solar abundance ratio of O to H are compatible with what is observed in WC and WN spectra.
Bhatia, A. K.↗
Recombination Rates of Electrons with Interstellar PAH Molecules
The goal of this project is to develop a general model for the recombination of electrons with PAH molecules in an interstellar environment. The model is being developed such that it can be applied to a small number of families of PAHs without reference to specific molecular structures. Special attention will be focused on modeling the approximately circular compact PAHs in a way that only depends on the number of carbon atoms.
Ballester, Jorge↗