SEARCH · Search NASA
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Collision induced disassociations of 2000 ev diatomic O, N, CO and NO positive molecular ions as function of reactant ion internal energy
Cold wall and multibody collision effects on reflection of imploding shock waves using Monte Carlo method and molecular dynamics
The project involved the study of ultraviolet (UV) and visible emission mechanisms in astrophysical and atmospheric environments. In many situations, the emission is a direct consequence of a charge transferring collision of an ion with a neutral with capture of an electron to an excited state of the product ion. The process is also important in establishing the ionization and thermal balance of an astrophysical plasma. As little of the necessary collision data are available, the main thrust of the project was the calculation of total and state-selective charge transfer cross sections and rate coefficients for a very large number of collision systems. The data was computed using modern explicit techniques including the molecular-orbital close-coupling (MOCC), classical trajectory Monte Carlo (CTMC), and continuum distorted wave (CDW) methods. Estimates were also made in some instances using the multichannel Landau-Zener (MCLZ) and classical over-the-barrier (COB) models. Much of the data which has been computed has been formatted for inclusion in a charge transfer database on the World Wide Web (cfadc.phy.ornl.gov/astro/ps/data/). A considerable amount of data has been generated during the lifetime of the grant. Some of it has not been analyzed, but it will be as soon as possible, the data placed on our website, and papers ultimately written.
Most of the important chemical reactions which occur in the very high temperature air produced around space vehicles as they enter the atmosphere were investigated both experimentally and theoretically, to some extent at least. One remaining reaction about which little is known, and which could be quite important at the extremely high temperatures that will be produced by the class of space vehicles now contemplated - such as the AOTV - is the excitation of bound electron states due to collisions between heavy gas particles. Rates of electronic excitation due to free electron collisions are known to be very rapid, but because these collisions quickly equilibrate the free and bound electron energy, the approach to full equilibrium with the heavy particle kinetic energy will depend primarily on the much slower process of bound electron excitation in heavy particle collisions and the subsequent rapid transfer to free electron energy. This may be the dominant mechanism leading to full equilibrium in the gas once the dissociation process has depleted the molecular states so the transfer between molecular vibrational energy and free electron energy is no longer available as a channel for equilibration of free electron and heavy particle kinetic energies. Two mechanisms seem probable in electronic excitation by heavy particle impact. One of these is the collision excitation and deexcitation of higher electronic states which are Rydberg like. A report, entitled 'Semi-Classical Theory of Electronic Excitation Rates', was submitted previously. This presented analytic expressions for the transition probabilities, assuming that the interaction potential is an exponential repulsion with a perturbation ripple due to the dipole-induced dipole effect in the case of neutral-neutral collisions, and to the ion-dipole interaction in the case of ion-neutral collisions. However the above may be, there is little doubt that excitation of ground state species by collision occurs at the point where the initial and final potentials cross, or at least come very close. Therefore, this mechanism would be applicable to the case where a gas is initially at very low temperature suddenly subjected to high energy heavy particle bombardment. This situation would model the measurement of excitation cross section by molecular beam techniques, for example. The purpose is to report values of cross sections and rate coefficients for collision excitation of ground state atoms estimated with the Landau-Zener transition theory and to compare results with measurement of excitation cross sections for a beam of Hydrogen atoms impacting Argon atom targets. Some very dubious approximations are used, and the comparison with measurement is found less than ideal, but results are at least consistent within order of magnitude. The same model is then applied to the case of N-N atom collisions, even though the approximations then become even more doubtful. Still the rate coefficients obtained are at least plausible in both magnitude and functional form, and as far as I am aware these are the only estimates available for such rate coefficients.
Classical trajectory calculations of the cross sections for vibrational and rotational energy exchange in direct and reactive collisions of hydrogen atoms and hydrogen molecules have been carried out. To test the sensitivity, three potential energy surfaces have been used. For the exchange transitions which occur at small internuclear distances, the rate coefficients for the three surfaces agree quite well. For the direct transitions, there are significant differences for the pure rotational transitions from j=0 to 2 and from j=1 to j=3 in which there is no change in vibration. For higher j the differences tend to disappear, suggesting that the rotational angular momentum can couple to the orbital angular momentum to overcome the centrifugal barrier. Complete numerically exact quantum mechanical calculations for the process in which vJ changes have been performed. Dr. M. A'Hearn has provided data on the fluorescent population of the NH rotational and fine-structure levels from which we should be able to predict accurate photodissociation lifetimes. The distribution rate of C2 is being investigated. A review of H3(+) in terrestrial and extraterrestrial environments was prepared for a volume of Advances in Atomic, Molecular and Optical Physics.
Helium afterglow discussing stability of collisional-radiative recombination of ions with electrons and neutral particles
Molecular dynamics calculations of the scattering of D2O from the glycerol surface at different collision energies are reported. The results for the trapping probabilities and energy transfer are in good agreement with experiments. The calculations demonstrate that the strong attractive forces between these two strongly hydrogen bonding molecules have only a minor effect on the initial collision dynamics. The trapping probability is influenced to a significant extent by the repulsive hard sphere-like initial encounter with the corrugated surface and, only at a later stage, by the efficiency of energy flow in the multiple interactions between the water and the surface molecules.
Polycyclic Aromatic Hydrocarbons (PAHs) are an important and ubiquitous component of carbon-bearing materials in space. PAHs are the best-known candidates to account for the IR emission bands (UIR bands) and PAH spectral features are now being used as new probes of the ISM. PAHs are also thought to be among the carriers of the diffuse interstellar absorption bands (DIBs). In the model dealing with the interstellar spectral features, PAHs are present as a mixture of radicals, ions and neutral species. PAH ionization states reflect the ionization balance of the medium while PAH size, composition, and structure reflect the energetic and chemical history of the medium. A major challenge for laboratory astrophysics is to reproduce (in a realistic way) the physical conditions that exist in the emission and/or absorption interstellar zones. An extensive laboratory program has been developed at NASA Ames to assess the physical and chemical properties of PAHs in such environments and to describe how they influence the radiation and energy balance in space and the interstellar chemistry. In particular, laboratory experiments provide measurements of the spectral characteristics of interstellar PAH analogs from the ultraviolet and visible range to the infrared range for comparison with astronomical data. This paper will focus on the recent progress made in the laboratory to measure the direct absorption spectra of neutral and ionized PAHs in the gas phase in the near-UV and visible range in astrophysically relevant environments. These measurements provide data on PAHs and nanometer-sized particles that can now be directly compared to astronomical observations. The harsh physical conditions of the IS medium - characterized by a low temperature, an absence of collisions and strong VUV radiation fields - are simulated in the laboratory by associating a molecular beam with an ionizing discharge to generate a cold plasma expansion. PAH ions are formed from the neutral precursors in an isolated environment at low temperature (of the order of 100 K). The spectra of neutral and ionized PAHs are measured using the high sensitivity methods of cavity ring down spectroscopy (CRDS). These experiments provide unique information on the spectra of free, cold large carbon molecules and ions in the gas phase. Intrinsic band profiles and band positions of cold gas-phase PAHs can now be measured with high-sensitivity spectroscopy and directly compared to the astronomical data. The electronic bands measured for ionized PAH are found to be intrinsically broad (about 20 cm(sup -1)) while the bands associated with the neutral precursors are narrower (of the order of 2 - 10 cm(sup -1)). The laboratory data are discussed and compared with recent astronomical spectra of large and narrow DIBs and with the spectra of circumstellar environments of selected carbon stars and the implications for the interstellar PAH population are derived. Preliminary results also show that carbon nanoparticles are formed during the short residence time of the precursors in the plasma.
NASA Laboratory Astrophysics Workshop 2006, is the fourth in a series of workshops held at four year intervals, to assess the laboratory needs of NASA's astrophysics missions - past, current and future. Investigators who need laboratory data to interpret their observations from space missions, theorists and modelers, experimentalists who produce the data, and scientists who compile databases have an opportunity to exchange ideas and understand each other's needs and limitations. The multi-wavelength character of these workshops allows cross-fertilization of ideas, raises awareness in the scientific community of the rapid advances in other fields, and the challenges it faces in prioritizing its laboratory needs in a tight budget environment. Currently, we are in the golden age of Space Astronomy, with three of NASA s Great Observatories, Hubble Space Telescope (HST), Chandra X-Ray Observatory (CXO), and Spitzer Space Telescope (SST), in operation and providing astronomers and opportunity to perform synergistic observations. In addition, the Far Ultraviolet Spectroscopic Explorer (FUSE), XMM-Newton, HETE-2, Galaxy Evolution Explorer (GALEX), INTEGRAL and Wilkinson Microwave Anisotropy Probe (WMAP), are operating in an extended phase, while Swift and Suzaku are in their prime phase of operations. The wealth of data from these missions is stretching the Laboratory Astrophysics program to its limits. Missions in the future, which also need such data include the James Webb Space Telescope (JWST), Space Interferometry Mission (SIM), Constellation-X (Con-X), Herschel, and Planck. The interpretation of spectroscopic data from these missions requires knowledge of atomic and molecular parameters such as transition probabilities, f-values, oscillator strengths, excitation cross sections, collision strengths, which have either to be measured in the laboratory by simulating space plasma and interactions therein, or by theoretical calculations and modeling. Once the laboratory data are obtained, a key step to making them available to the observer is the creation and maintenance of critically compiled databases. Other areas of study, that are important for understanding planet formation, and for detection of molecules that are indicators of life, are also supported by the Laboratory Astrophysics program. Some examples are: studies of ices and dust grains in a space environment; nature and evolution of interstellar carbon-rich dust; and polycyclic aromatic hydrocarbons. In addition, the program provides an opportunity for the investigation of novel ideas, such as simulating radiative shock instabilities in plasmas, in order to understand jets observed in space. A snapshot of the currently funded program, mission needs, and relevance of laboratory data to interpreting observations, will be obtained at this workshop through invited and contributed talks and poster papers. These will form the basis for discussions in splinter groups. The Science Organization Committee will integrate the results of the discussions into a coherent White Paper, which will provide guidance to NASA in structuring the Laboratory Astrophysics program in subsequent years, and also to the scientific community in submitting research proposals to NASA for funding.
Carbon molecules and ions play an important role in space. Polycyclic Aromatic Hydrocarbons (PAHs) are the best-known candidates to account for the infrared emission bands (UIR bands) and PAH spectral features are now being used as probes of the interstellar medium in Galactic and extra-galactic environments. PAHs are also thought to be among the carriers of the diffuse interstellar absorption bands (DIBs). In the model dealing with the interstellar spectral features, PAHs are present as a mixture of radicals, ions and neutral species. PAH ionization states reflect the ionization balance of the medium while PAH size, composition, and structure reflect the energetic and chemical history of the medium. A major challenge for laboratory Astrochemistry is to reproduce (in a realistic way) the physical conditions that exist in the emission and absorption interstellar zones. An extensive laboratory program has been developed in various laboratories to characterize the physical and chemical properties of PAHs in astrophysical environments and to describe how they influence the radiation and energy balance in space and the interstellar chemistry. In particular, laboratory experiments provide measurements of the spectral characteristics of interstellar PAH analogs from the ultraviolet and visible range to the infrared range for comparison with astronomical data. The harsh physical conditions of the interstellar medium - characterized by a low temperature, an absence of collisions and strong ultraviolet radiation fields - are simulated in the laboratory by associating a molecular beam with an ionizing discharge to generate a cold plasma expansion. PAH ions are formed from the neutral precursors in an isolated environment at low temperature (of the order of 100 K). The spectra of neutral and ionized PAHs are measured using the high sensitivity methods of cavity ring down spectroscopy (CRDS). These experiments provide unique information on the spectra of free, cold large carbon molecules and ions in the gas phase.
We have used the Long Wavelength Spectrometer (LWS) aboard the Infrared Space Observatory (ISO) to map the far-infrared continuum emission (45-175 micrometer) toward several massive Giant Molecular Cloud (GMC) cores located near the Galactic center. The observed far-infrared and submillimeter spectral energy distributions imply low temperatures (approx. 15 - 22 K) for the bulk of the dust in all the sources, consistent with external heating by the diffuse ISRF and suggest that these GMCs do not harbor high- mass star-formation sites, in spite of their large molecular mass. Observations of FIR atomic fine structure lines of C(sub II) and O(sub I) indicate an ISRF enhancement of approx. 10(exp 3) in the region. Through continuum radiative transfer modeling we show that this radiation field strength is in agreement with the observed FIR and submillimeter spectral energy distributions, assuming primarily external heating of the dust with only limited internal luminosity (approx. 2 x 10(exp 5) solar luminosity). Spectroscopic observations of millimeter-wave transitions of H2CO, CS, and C-34S carried out with the Caltech Submillimeter Observatory (CSO) and the Institut de Radio Astronomie Millimetrique (IRAM) 30-meter telescope indicate a gas temperature of approx. 80 K, significantly higher than the dust temperatures, and density of approx. 1 x 10(exp 5)/cc in GCM0.25 + 0.01, the brightest submillimeter source in the region. We suggest that shocks caused by cloud collisions in the turbulent interstellar medium in the Galactic center region are responsible for heating the molecular gas. This conclusion is supported by the presence of wide-spread emission from molecules such as SiO, SO, and CH3OH, which are considered good shock tracers. We also suggest that the GMCs studied here are representative of the "typical", pre-starforming cloud population in the Galactic center.
Surprisingly strong CO emission has been observed from more than a dozen debris disks around nearby main-sequence stars. The origin of this CO is unclear, in particular whether it is left over from the protoplanetary disk phase or is second-generation material released from collisions between icy bodies like debris dust. The primary unexplored avenue for distinguishing the origin of the material is understanding its molecular composition. Here we present a deep search for five molecules (CN, HCN, HCO+, SiO, and CH3OH) in the debris disk around 49 Ceti. We take advantage of the high sensitivity of the Atacama Large Millimeter/submillimeter Array at Band 7 to integrate for 3.2 hr at modest spatial (1′′) and spectral (0.8 km s−1) resolution. Our search yields stringent upper limits on the flux of all surveyed molecular lines, which imply abundances relative to CO that are orders of magnitude lower than those observed in protoplanetary disks and solar system comets, and also those predicted in outgassing models of second-generation material. However, if CI shielding is responsible for extending the lifetime of any CO produced in second-generation collisions as proposed by Kral et al., then the line ratios do not reflect true ice phase chemical abundances but rather imply that CO is shielded by its own photodissociation product, CI, and other molecules are rapidly photodissociated by the stellar and interstellar radiation field.
Measurement of the cross section of stripping the mass 2 and 4 isotopes from molecular hydrogen in their parent gases at kinetic energies between 50 and 500 eV. The angular dependence of the ions is found to be highly peaked in the forward direction, at energies above 100 eV. Plotted vs incident velocity, the cross sections for H2 and D2 approached the same value at the highest velocities and did diverge toward lower velocities. The behavior of the cross sections is found to be consistent with a theoretical model suggested by Demkov and Komarov (1968).
We present the gas-phase spectroscopy of neutral and ionized polycyclic aromatic hydrocarbons (PAHs) measured in the W-Visible-NIR range in an astrophysically relevant environment. These measurements provide data on PAHs and nanometer sized particles that can now be directly compared to astronomical observations. The harsh physical conditions of the IS medium - characterized by a low temperature, an absence of collisions and strong VUV radiation fields - are simulated in the laborat'ory by associating a molecular beam with an ionizing discharge to generate a cold plasma expansion. PAH ions are formed from the neutral precursors in an isolated environment at low temperature ($\sim lOO$-K). The spectra of neutral and ionized PAHs are measured using the high sensitivity methods of cavity ring down spectroscopy (CRDS) and multiplex integrated cavity output spectroscopy (MICOS). These experiments provide unique information on the spectra of free, cold large carbon molecules and ions in the gas phase. The electronic bands measured for ionized PAH are found to be intrinsically broad ($\geq$20 cm$^{-l}$) while the bands associated with the neutral precursors are narrower (of the order of 2 - 10 cm$^{-l}$). The laboratory data are discussed and compared with recent astronomical spectra of large and narrow DIBs and with the spectra of circumstellar environments of selected carbon stars (see contribution of Cami et al.) and the implications for the interstellar PAH population are derived. Preliminary results also show that carbon nanoparticles are formed during the short residence time of the precursors in the plasma. This finding holds great potential for understanding the formation process of interstellar grains.
Polycyclic Aromatic Hydrocarbons (PAHs) are an important and ubiquitous component of carbon-bearing materials in space. PAHs are the best-known candidates to account for the IR emission bands (UIR bands) and PAH spectral features are now being used as new probes of the ISM. PAHs are also thought to be among the carriers of the diffuse interstellar absorption bands (DIBs). In the model dealing with the interstellar spectral features, PAHs are present as a mixture of radicals, ions and neutral species. PAH ionization states reflect the ionization balance of the medium while PAH size, composition, and structure reflect the energetic and chemical history of the medium. A major challenge for laboratory astrophysics is to reproduce (in a realistic way) the physical conditions that exist in the emission and/or absorption interstellar zones, An extensive laboratory program has been developed at NASA Ames to characterize the physical and chemical properties of PAHs in astrophysical environments and to describe how they influence the radiation and energy balance in space and the interstellar chemistry. In particular, laboratory experiments provide measurements of the spectral characteristics of interstellar PAH analogs from the ultraviolet and visible range to the infrared range for comparison with astronomical data. This paper will focus on the recent progress made in the laboratory to measure the direct absorption spectra of neutral and ionized PAHs in the gas phase in the near-W and visible range in astrophysically relevant environments. These measurements provide data on PAHs and nanometer-sized particles that can now be directly compared to astronomical observations. The harsh physical conditions of the IS medium - characterized by a low temperature, an absence of collisions and strong V W radiation fields - are simulated in the laboratory by associating a molecular beam with an ionizing discharge to generate a cold plasma expansion. PAH ions are formed from the neutral precursors in an isolated environment at low temperature (of the order of 100 K). The spectra of neutral and ionized PAHs are measured using the high sensitivity methods of cavity ring down spectroscopy (CRDS). These experiments provide unique information on the spectra of free, cold large carbon molecules and ions in the gas phase. Intrinsic band profiles and band positions of cold gas-phase PAHs can now be measured with high- sensitivity spectroscopy and directly compared to the astronomical data. The electronic bands measured for ionized PAH are found to be intrinsically broad (about 20/cm) while the bands associated with the neutral precursors are narrower (of the order of 2 - 10/cm).
Rate coefficients for the reactive processes of ortho-para conversion in which the j = 0 rotational level of molecular hydrogen is excited to the j = 1 and j = 3 level by impacts with hydrogen atoms are calculated for temperatures between 30 K and 1000 K using a fully converged complete close-coupled method. Rate coefficients are also obtained for the excitation from the j = 0 to the j = 2 rotational level and from the j = 1 to the j = 3 rotational level. The interference between the direct and reactive channels is taken into account as is the geometric phase resulting from the adiabatic separation of electronic and nuclear motion that generates the potential energy surface. Convenient analytic representations of the rate coefficients are presented.
The concept of activated recombination of atomic species on surfaces can explain the production of vibrationally and translationally excited desorbed molecular species. Equilibrium statistical mechanics predicts that the molecular quantum state distributions of desorbing molecules is a function of surface temperature only when the adsorption probability is unity and independent of initial collision conditions. In most cases, the adsorption probability is dependent upon initial conditions such as collision energy or internal quantum state distribution of impinging molecules. From detailed balance, such dynamical behavior is reflected in the internal quantum state distribution of the desorbing molecule. This concept, activated recombinative desorption, may offer a common thread in proposed mechanisms of spacecraft glow. Using molecular beam techniques and equipment available at Los Alamos, which includes a high translational energy 0-atom beam source, mass spectrometric detection of desorbed species, chemiluminescence/laser induced fluorescence detection of electronic and vibrationally excited reaction products, and Auger detection of surface adsorbed reaction products, a fundamental study of the gas surface chemistry underlying the glow process is proposed.
Time-dependent perturbation-theory techniques are used to derive a compact expression, valid to arbitrary order and displaying time dependence explicitly, for a quantum-mechanical transition amplitude applicable to the description of resonances. A solution representing a complex-energy generalization of the usual real-energy (nonresonant) amplitude is obtained and generalized to all orders by introducing a complex-energy T matrix. Applications to physical problems such as the extension of the Fermi golden rules to resonances (Norbury and Deutchman, 1984); pion production in relativistic nucleus-nucleus collisions (Norbury et al., 1985); and the determination of resonant cross sections for nuclear, atomic, or molecular processes involving the formation and decay of intermediate discrete or continuum states are indicated.