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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
NASA NTRS1972

Dissociative excitation of vacuum ultraviolet emission features by electron impact on molecular gases. 3: CO2

Vacuum ultraviolet multiplets of C I, C II, and O I were produced by electron impact of CO2. Absolute emission cross sections for these multiplets were measured from threshold to 350 eV. The electrostatically focussed electron gun used in this series of experiments is described in detail. The atomic multiplets which were produced by dissociative excitation of CO2 and the cross sections at 100 eV are given. The dependence of the excitation functions on electron energy shows that these multiplets are produced by electric-dipole-allowed transitions in CO2.

Mumma, M. J.↗
DOE OSTI2021

Parabolic oxidation kinetics of a plutonium alloy at room temperature

Auger electron spectroscopy (AES) was used to characterize the oxide scale formed on an ~0.5 wt. % Ga plutonium metal alloy. Analysis of changes to the characteristic Auger transitions for Pu and O during sputter depth profiles were used in combination with previously measured sputter yields to determine the thickness of the oxide scale and provide insight into its chemistry. From this data, the parabolic kinetics for the Pu-Ga alloy were determined as a function of relative humidity, RH = 14–92%, and oxygen partial pressure, p(O 2 ) = 31–157 Torr, at 25°C. For each relative humidity investigated, the parabolic rate constant was found to be independent of oxygen partial pressure. Furthermore, power-law fits to the relative humidity effect on the rate constant was found to have a power of n = 1.265, indicating the diffusion species which rate-limits the reaction isn’t molecular water, which subsequent dissociates at the oxide-metal interface, or hydroxyl from dissociation at the gas-surface interface.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Employing a Narrow-Band-Gap Mediator in Ternary Solar Cells for Enhanced Photovoltaic Performance

Ternary organic solar cells (OSCs) provide a convenient and effective means to further improve the power conversion efficiency (PCE) of binary ones via composition control. However, the role of the third component remains to be explored in specific binary systems. Herein, we report ternary blend solar cells by adding the narrow-band-gap donor PCE10 as the mediator into the PBDB-T:IDTT-T binary blend system. The extended absorption, efficient fluorescence resonance energy transfer, enhanced charge dissociation, and induced tighter molecular packing of the ternary blend films enhance the photovoltaic properties of devices and deliver a champion PCE of 10.73% with an impressively high open-circuit voltage (VOC) of 1.03 V. Good miscibility and similar molecular packing behavior of the components guarantee the desired morphology in the ternary blend films, leading to solar cell devices with over 10% PCEs at a range of compositions. Our results suggest that ternary systems with properly aligned energy levels and overlapping absorption among the components hold great promises to further enhance the performance of corresponding binary ones.

14 SOLAR ENERGY↗
DOE OSTI2021

High-level coupled-cluster energetics by merging moment expansions with selected configuration interaction

Inspired by our earlier semi-stochastic work aimed at converging high-level coupled-cluster (CC) energetics, we propose a novel form of the CC(P; Q) theory in which the stochastic Quantum Monte Carlo propagations, used to identify dominant higher-than-doubly excited determinants, are replaced by the selected configuration interaction (CI) approach using the perturbative selection made iteratively (CIPSI) algorithm. The advantages of the resulting CIPSI-driven CC(P; Q) methodology are illustrated by a few molecular examples, including the dissociation of F 2 and the automerization of cyclobutadiene, where we recover the electronic energies corresponding to the CC calculations with a full treatment of singles, doubles, and triples based on the information extracted from compact CI wave functions originating from relatively inexpensive Hamiltonian diagonalizations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1978

Transport properties of monatomic carbon

Transport collision integrals for each of the 18 molecular C2 states that dissociate into ground state carbon atoms are presented. The integrals are obtained by fitting two-body semiempirical interaction potentials, for which the collision integrals are tabulated, to experimental and/or accurate theoretical calculations for each of these states. The collision integrals are applied to calculate the diffusion coefficient, viscosity, and translational contribution to the thermal conductivity of monatomic carbon at 1-atm pressure from 1000 K to 25,000 K. Because of ablation injection, monatomic carbon is an important flow field constituent of ablative flow during planetary entry, and knowledge of the transport properties for carbon species is required for calculating the flow field properties and surface heating.

Biolsi, L.↗
NASA NTRS1984

Plasma in Saturn's magnetosphere

The spatial and compositional distribution of the thermal plasma in the magnetosphere of Saturn is described in the light of the Voyager encounters. Theoretical considerations are applied to the elucidation of the structure, including two external and two internal boundaries. The outer boundary is a magnetohydrodynamic entity, while the inner boundary of locally created thermal plasma is a result of the dissociative recombination of corotating molecular ions. The internal boundaries, which separate plasmas of different composition, are explained as a charge exchange quasi-resonance phenomenon.

Eviatar, A.↗
NASA NTRS1984

An analysis of the annual cycle in upper stratospheric ozone

The mid-latitude upper stratospheric ozone profiles obtained by the solar backscatter ultraviolet instrument on the Nimbus 7 satellite show a clear annual cycle both in the absolute ozone amounts between 0.98 and 15.6 mbar and in the magnitude of disturbances that reveal themselves as longitudinal structure. At the lowest pressure analyzed a winter maximum in ozone exists, but as one progresses downward in altitude a shift in the temporal phase of the annual cycle occurs in the vicinity of 3 to 4 mbar. Comparison of the observed behavior with the predictions of a one-dimensional photochemical model shows a systematic tendency for calculated ozone amount to be 20-27 percent below the data for pressures less than 7.8 mbar. The chemical model successfully predicts the change in phase of the annual cycle, although at a pressure greater than observed. Diagnosis of model results shows the observed shift to be closely coupled to the magnitude of the ozone column density near 3-4 mbar. The wavelength-dependent attenuation of the solar radiation field by ozone alters the relative magnitude of the molecular oxygen and ozone dissociation rates, leading to a change in the temporal phase of the annual cycle.

Frederick, J. E.↗
NASA NTRS1987

The production of low-energy neutral oxygen beams by grazing-incidence neutralization

The Vanderbilt University neutral oxygen facility produces beams of low-energy neutral oxygen atoms by means of grazing-incidence collisions between ion beams and metal surfaces. Residual ions are reflected by applied electric fields. This method can utilize initial ion beams of either O(+) or O2(+) since a very large percentage of molecular oxygen ions are dissociated when they undergo grazing-incidence neutralization. The method of neutralization is applicable to low-energy beams and to all ions. Particular emphasis is on O and N2 beams for simulation of the low Earth orbit space environment. Since the beam is a pure O-neutral beam and since measurements of the interaction of the beam with solid surfaces are made spectroscopically, absolute reaction rates can be determined. The technique permits the beams to be used in conjunction with electron and photon irradiation for studies of synergistic effects. Comparisons of optical spectra of Kapton excited by 2.5-keV O, O(+), and O2(+) show significant differences. Optical spectra of Kapton excited by neutral oxygen beams of less than 1 keV have been recorded.

Albridge, R. G.↗
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 NTRS1993

Centrifugally driven winds from protostellar disks. I - Wind model and thermal structure

The thermal structure of a wind that is centrifugally driven from the surface of a protostellar disk is studied. A generalized version of the Blandford and Payne self-similar wind model is introduced, and the temperature and ionization distributions in the outflow are investigated. For the evolution of atomic winds, the heat equation and the rate equations that describe the ionization and excitation state of hydrogen are solved self-consistently. Ambipolar diffusion is found to be a robust mechanism for heating the gas. In the more powerful outflows, molecular hydrogen is collisionally dissociated close to the disk surface, and hydrogen is mainly atomic within a few astronomical units from the central source. It is also demonstrated that these outflows have enough momentum to lift dust grains from the disk surface.

Safier, Pedro N.↗
NASA NTRS1993

Performance assessment of low pressure nuclear thermal propulsion

A low pressure nuclear thermal propulsion (LPNTP) system, which takes advantage of hydrogen dissociation/recombination, was proposed as a means of increasing engine specific impulse (Isp). The effect of hydrogen dissociation/recombination on LPNTP Isp is examined. A two-dimensional computer model was used to show that the optimum chamber pressure is approximately 100 psia (at a chamber temperature of 3,000 K), with an Isp approximately 15 s higher than at 1,000 psia. At high chamber temperatures and low chamber pressures, the increase in Isp is due to both lower average molecular weights caused by dissociation and added kinetic energy from monatomic hydrogen recombination. Monatomic hydrogen recombination increases the Isp more then hydrogen dissociation. Variations in the mole fraction of monatomic hydrogen are similar to variations in static pressure along the axial nozzle position. Most recombination occurs close to the nozzle throat. Practical variations in nozzle geometry have minimal impact on recombination. Other models which can simulate a wider range of nozzle designs should be used in the future. The uncertainty of the hydrogen kinetic reaction rates at high temperatures (approximately 3,000 K) affects the accuracy of the analysis and should be verified with simple bench tests.

Gerrish, H. P., Jr.↗
DOE OSTI2022

On the Dynamics of the Carbon–Bromine Bond Dissociation in the 1-Bromo-2-Methylnaphthalene Radical Anion

This paper studies the mechanism of electrochemically induced carbon–bromine dissociation in 1-Br-2-methylnaphalene in the reduction regime. In particular, the bond dissociation of the relevant radical anion is disassembled at a molecular level, exploiting quantum mechanical calculations including steady-state, equilibrium and dissociation dynamics via dynamic reaction coordinate (DRC) calculations. DRC is a molecular-dynamic-based calculation relying on an ab initio potential surface. This is to achieve a detailed picture of the dissociation process in an elementary molecular detail. From a thermodynamic point of view, all the reaction paths examined are energetically feasible. The obtained results suggest that the carbon halogen bond dissociates following the first electron uptake follow a stepwise mechanism. Indeed, the formation of the bromide anion and an organic radical occurs. The latter reacts to form a binaphthalene intrinsically chiral dimer. This paper is respectfully dedicated to Professors Anny Jutand and Christian Amatore for their outstanding contribution in the field of electrochemical catalysis and electrosynthesis.

1-bromo-2-methylnaphthalene↗
NASA NTRS1971

Dissociative excitation of vacuum-ultraviolet emission features by electron impact on molecular gases. II.

Atomic-nitrogen multiplets have been excited. The excitation cross sections have been measured over the energy range from threshold to 350 eV. The transition arrays, mean wavelengths, and cross sections for dissociative excitation of the multiplets at 100 eV are presented. The experiment featured a monoenergetic electron beam which was incident on a quasi-static gas target. Vacuum-ultraviolet emission features were isolated by a normal-incidence monochromator, and multiscaling pulse-counting techniques were used.

Mumma, M. J.↗
DOE OSTI2021

Modeling dissociation of ionic liquids with electrolyte NRTL model

Dissociation of ionic liquids (ILs) is critical to electrochemical process performance by affecting ionic conductivity. Prior studies of thermodynamic modeling either assumed no dissociation or complete dissociation that were not consistent with experimental observations. This work presented an eNRTL model for three aqueous imidazolium-based IL systems: [Emim][EtSO 4 ], [Emim][TFA], and [Emim][TfO]. The model accurately correlates the IL dissociation and VLE data in the entire concentration range from pure IL to infinite dilution aqueous solution. The system non-ideality is dominated by the dissociation chemistry. Dissociation behavior is driven by strong short-range interaction of the molecular IL-water pair relative to the dissociated IL-water pair, consistent with prior studies indicating that molecular IL and water can form an energetically favorable complex. The interaction energy parameters calculated in this work qualitatively agrees with the hydrogen bonding ability of the anions previously reported. This research not only provides a model that well describes the IL dissociation but also demonstrates the physical significance of eNRTL model.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1992

Rotational relaxation of molecular H2 at moderate temperatures

A coupled rotation-vibration-dissociation model is used to compute the rotational relaxation times for molecular hydrogen as a function of final temperatures (500-5000 K) in a hypothetical scenario of sudden compression. The theoretical model is based on a master equation solver. The bound-bound and bound-free transition rates have been computed using a quasi-classical trajectory method. A review of the available experimental data on the rotational relaxation of hydrogen is presented, with a critical overview of the method of measurements and data reduction, including the sources of errors. The experimental data are compared with the computed results.

Sharma, S. P.↗
NASA NTRS1983

Ion bombardment and adsorption studies on ilmenite (FeTiO3) by X-ray photoelectron spectroscopy

The effects of 5 KeV argon and oxygen ion bombardment on FeTiO3 (ilmenite) at low temperatures have been studied using X-ray photoelectron spectroscopy (XPS). Also, using this same technique, the adsorption of O2, NO, N2O, and CO at 300 K and the adsorption of O2 and D2O at 150K have been studied. Argon and oxygen ion bombardment of ilmenite have confirmed earlier studies on metal oxides that argon ions generally reduce the anion species while oxygen ions generally oxidize the anion species. The two iron states involved were Fe sup +2 and Fe sup O. The reduction of Ti sup +4 was not verified although a significant shift in the Ti(2p1,3) binding energies toward the metallic state was observed after oxygen ion bombardment at low temperatures. At temperatures above 150K, O2 adsorbs dissociatively on ilmenite while D2O adsorbs molecularly below 170K. Above 300 K No, N2O, and CO do not appear to adsorb dissociatively. Low temperature adsorption of D2O was found to be inhibited by predosing the ilmenite with O2.

Schulze, P. D.↗
DOE OSTI2020

Nonadiabatic molecular dynamics simulation of C2H22+ in a strong laser field*

We investigate the alignment dependence of the strong laser dissociation dynamics of molecule C 2 H 2 2 + in the frame of real-time and real-space time-dependent density function theory coupled with nonadiabatic quantum molecular dynamics (TDDFT-MD) simulation. This work is based on a recent experiment study “ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene” [Wolter et al , Science 354 , 308–312 (2016)]. Our simulations are in excellent agreement with the experimental data and the analysis confirms that the alignment dependence of the proton dissociation dynamics comes from the electron response of the driving laser pulse. Our results validate the ability of the TDDFT-MD method to reveal the underlying mechanism of experimentally observed and control molecular dissociation dynamics.

Physics↗
DOE OSTI2022

Formation and dissociation of shear-induced high-energy dislocations: insight from molecular dynamics simulations

Solid-phase processing (SPP) allows one to create complex microstructures, not achievable via thermal processing alone. The resulting structures exhibit a rich palette of defects, both thermal and non-thermal, including defect substructures, such as dislocation networks. It is essential to understand the mechanisms of deformation and defect structure formation to guide SPP towards achieving desired microstructures and material properties. In this study, large-scale molecular dynamics simulations are used to investigate the effects of inhomogeneous strain distribution, that mimics deformation conditions of tribological tests, on the evolution of defects under severe shear deformation in polycrystalline Al. Analysis of defect nucleation and reaction pathways reveals that strong geometric constraints suppress the nucleation and slide of low energy dislocation 1/2$\langle110\rangle${111} but promote the nucleation and slide of high energy dislocations, such as [$1\bar1$0] (001) and 1/2 [$1\bar1$$\bar2$]($1\bar1$1). Further, a rough contact surface, characteristic to tribological tests, imposes an inhomogeneous stress field leading to inhomogeneous defect substructures due to location-dependent activation of slip systems. The results suggest that high-energy dislocations can dominate the evolution of grain structures in highly constrained environments, which should be considered in modeling plastic deformation and grain refinement during SPP.

42 ENGINEERING↗