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Results for “atomic and molecular collision processes”

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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Anomalous ellipticity dependence of the generation of near-threshold harmonics in noble gases

We measured the ellipticity dependence of the harmonic yield of He, Ne, Ar, Kr, and Xe. It is found that the harmonic yield in general decreases monotonically with increasing laser ellipticity but anomalous dependence does occur for each atom for some harmonic orders. Additionally, we found that the degree of anomaly is weakest in helium but is stronger for the heavier atoms. The anomaly also depends on laser intensity. To explain these features, we developed a quantum trajectory Monte Carlo (QTMC) model based on the quantum path integral theory to study high-order harmonic generation (HHG). The model includes the effect of Coulomb potential from the target ion, thus it is capable of calculating near-threshold harmonics quantitatively. This model reveals that the presence of Coulomb potential would generate orbiting trajectories which are responsible for the anomalous ellipticity dependence near the threshold.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Retrieval of target structure information from laser-induced photoelectrons by few-cycle bicircular laser fields

By analyzing theoretical results from a numerical solution of the time-dependent Schrödinger equation for atoms in few-cycle bicircular laser pulses, we show that high-energy photoelectron momentum spectra can be used to extract accurate elastic scattering differential cross sections of the target ion with free electrons. We find that the retrieval range for a scattering angle with bicircular pulses is wider than with linearly polarized pulses, although the retrieval method has to be modified to account for different returning directions of the electron in the continuum. Overall, this result can be used to extend the range of applicability of ultrafast imaging techniques such as laser-induced electron diffraction and for the accurate characterization of laser pulses.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Nonunique and nonuniform mapping in few-body Coulomb-explosion imaging

Much of our knowledge of molecular geometry and interaction dynamics comes from indirect measurements of the molecular fragments following breakup. This technique—Coulomb-explosion imaging (CEI), i.e., determining the initial molecular configuration of a system from the momenta of the resulting fragments using knowledge of the particle interactions—is one of the fundamental tools of molecular physics. Moreover, CEI has been a staple of molecular studies for decades. Here we show that one often cannot assign a unique initial configuration to the few-body breakup of a polyatomic molecule given the measurement of the resulting fragments' momenta. Specifically, multiple initial configurations can result in identical momenta for a molecule breaking into three or more parts. Finally, the nonunique and nonuniform mapping from the initial configuration to the measured momenta also significantly complicates the determination of molecular alignment at the time of breakup.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2016

Nonsequential double ionization with mid-infrared laser fields

Using a full-dimensional Monte Carlo classical ensemble method, we present a theoretical study of atomic nonsequential double ionization (NSDI) with mid-infrared laser fields, and compare with results from near-infrared laser fields. Unlike single-electron strong-field processes, double ionization shows complex and unexpected interplays between the returning electron and its parent ion core. As a result of these interplays, NSDI for mid-IR fields is dominated by second-returning electron trajectories, instead of first-returning trajectories for near-IR fields. Here, some complex NSDI channels commonly happen with near-IR fields, such as the recollision-excitation-with-subsequent-ionization (RESI) channel, are virtually shut down by mid-IR fields. Besides, the final energies of the two electrons can be extremely unequal, leading to novel e-e momentum correlation spectra that can be measured experimentally.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Measurement of interaction between antiprotons

In this paper, one of the primary goals of nuclear physics is to understand the force between nucleons, which is a necessary step for understanding the structure of nuclei and how nuclei interact with each other. Rutherford discovered the atomic nucleus in 1911, and the large body of knowledge about the nuclear force that has since been acquired was derived from studies made on nucleons or nuclei. Although antinuclei up to antihelium-4 have been discovered and their masses measured, little is known directly about the nuclear force between antinucleons. Here, we study antiproton pair correlations among data collected by the STAR experiment at the Relativistic Heavy Ion Collider (RHIC), where gold ions are collided with a centre-of-mass energy of 200 gigaelectronvolts per nucleon pair. Antiprotons are abundantly produced in such collisions, thus making it feasible to study details of the antiproton–antiproton interaction. By applying a technique similar to Hanbury Brown and Twiss intensity interferometry, we show that the force between two antiprotons is attractive. In addition, we report two key parameters that characterize the corresponding strong interaction: the scattering length and the effective range of the interaction. Our measured parameters are consistent within errors with the corresponding values for proton–proton interactions. Our results provide direct information on the interaction between two antiprotons, one of the simplest systems of antinucleons, and so are fundamental to understanding the structure of more-complex antinuclei and their properties.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Differential electron emission from polycyclic aromatic hydrocarbon molecules under fast ion impact

Interaction between polycyclic aromatic hydrocarbon (PAH) molecule and energetic ion is a subject of interest in different areas of modern physics. Here, we present measurements of energy and angular distributions of absolute double differential electron emission cross section for coronene (C 24 H 12 ) and fluorene (C 13 H 10 ) molecules under fast bare oxygen ion impact. For coronene, the angular distributions of the low energy electrons are quite different from that of simpler targets like Ne or CH 4 , which is not the case for fluorene. The behaviour of the higher electron energy distributions for both the targets are similar to that for simple targets. In case of coronene, a clear signature of plasmon resonance is observed in the analysis of forward-backward angular asymmetry of low energy electron emission. For fluorene, such signature is not identified probably due to lower oscillator strength of plasmon compared to the coronene. The theoretical calculation based on the first-order Born approximation with correct boundary conditions (CB1), in general, reproduced the experimental observations qualitatively, for both the molecules, except in the low energy region for coronene, which again indicates the role of collective excitation. Single differential and total cross sections are also deduced. An overall comparative study is presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

A combined experimental and computational study on the reaction dynamics of the 1-propynyl (CH 3 CC, X 2 A 1 ) – propylene (CH 3 CHCH 2 , X 1 A') system: formation of 1,3-dimethylvinylacetylene (CH 3 CCCHCHCH 3 , X 1 A') under single collision conditions

The reaction of the 1-propynyl radical (CH 3 CC; X 2 A 1 ) with propylene (CH 3 CHCH 2 ; X 1 A') was studied in a crossed molecular beam machine at a collision energy of 37 ± 1 kJ mol –1 . Experimental data combined with high-level electronic structure (CCSD(T)-F12/cc-pVTZ-F12//ωB97X-D/6-311G(d,p)) and RRKM calculations reveal the reaction mechanism. Here, the overall barrierless and exoergic reaction involves indirect reaction dynamics and commences preferentially with addition of 1-propynyl with its radical centre to the carbon–carbon double bond at the terminal carbon atom of propylene. This work focuses on molecular mass growth process (hydrogen loss channels) although theory suggests methyl loss as a prevalent channel. In these processes, the C6H9 collision complexes either emit atomic hydrogen or undergo isomerisation followed by atomic hydrogen loss to preferentially yield the cis/trans isomers of 1,3-dimethylvinylacetylene (2-hexen-4-yne) as the primary product. Analysis of reaction dynamics of 1-propynyl and ethynyl radicals with propylene along with their fractional abundance in deep space suggests formation of methyl- and dimethyl derivatives of vinylacetylene in cold molecular clouds. Once formed they may engage in fundamental molecular mass growth processes via the barrierless Hydrogen Abstraction Vinylacetylene Addition mechanism that leads to the formation of methyl- and dimethylnaphthalenes thus providing a versatile route to methyl-substituted PAHs in interstellar medium.

1-propynyl↗
NASA NTRS1984

Laboratory studies of atomic collision processes of importance in planetary atmospheres

Progress in the following research supported under NSG 7386 is reported: (1) measurement of differential cross sections for atomic and molecular collisions relevant to analysis and modeling of data from Pioneer 11, Pioneer 12, Voyager 1, and Voyager 2; (2) analysis of measured differential cross section results to provide scattering data in forms that are easy to apply to atmospheric modeling work; (3) analysis of the data to give basic information on the molecular potentials involved in the scattering process; and (4) development and initial use of apparatus to study dissociative processes in neutral molecules.

Stebbings, R. F.↗
NASA NTRS1984

Molecular processes in a high temperature shock layer

Models of the shock layer encountered by an Aeroassisted Orbital Transfer Vehicle require as input accurate cross sections and rate constants for the atomic and molecular processes that characterize the shock radiation. From the estimated atomic and molecular densities in the shock layer and the expected residence time of 1 m/s, it can be expected that electron-ion collision processes will be important in the shock model. Electron capture by molecular ions followed by dissociation, e.g., O2(+) + e(-) yields 0 + 0, can be expected to be of major importance since these processes are known to have high rates (e.g., 10 to the -7th power cu/cm/sec) at room temperature. However, there have been no experimental measurements of dissociative recombination (DR) at temperatures ( 12000K) that are expected to characterize the shock layer. Indeed, even at room temperature, it is often difficult to perform experiments that determine the dependence of the translational energy and quantum yields of the product atoms on the electronic and vibrational state of the reactant molecular ions. Presented are ab initio quantum chemical studies of DR for molecular ions that are likely to be important in the atmospheric shock layer.

Guberman, S. L.↗
DOE OSTI2019

Radiative Association of Atomic and Ionic Carbon

We present calculated cross sections and rate coefficients for the formation of the dicarbon cation (C$^+_2$) by the radiative association process in collisions of a C( 3 $P$) atom and a C + ( 2 $P$ o ) ion. Molecular structure calculations for a number of low-lying doublet and quartet states of C$^+_2$ are used to obtain the potential energy surfaces and transition dipole moments coupling the states of interest, substantially increasing the available molecular data for C$^+_2$ . Using a quantum-mechanical method, we explore a number of allowed transitions and determine those contributing to the radiative association process. The calculations extend the available data for this process down to the temperature of 100 K, where the rate coefficient is found to be about 2 Χ 10 -18 cm 3 s -1 . We provide analytical fits suitable for incorporation into astrochemical reaction databases.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Multi-fluid and kinetic models of partially ionized magnetic reconnection

Magnetic reconnection in partially ionized plasmas is a ubiquitous and important phenomenon in both laboratory and astrophysical systems. Here, simulations of partially ionized magnetic reconnection with well-matched initial conditions are performed using both multi-fluid and fully-kinetic approaches. Despite similar initial conditions, the time-dependent evolution differs between the two models. In multi-fluid models, the reconnection rate locally obeys either a decoupled Sweet–Parker scaling, where neutrals are unimportant, or a fully coupled Sweet–Parker scaling, where neutrals and ions are strongly coupled, depending on the resistivity. In contrast, kinetic models show a faster reconnection rate that is proportional to the fully-coupled, bulk Alfvén speed, $v^*_A$. In this work, these differences are interpreted as the result of operating in different collisional regimes. Multi-fluid simulations are found to maintain $ν_{ni}L/v^*_A$ ≳1, where $ν_{ni}$ is the neutral–ion collision frequency and L is the time-dependent current sheet half-length. This strongly couples neutrals to the reconnection outflow, while kinetic simulations evolve to allow $ν_{ni}L/v^*_A$ <1, decoupling neutrals from the reconnection outflow. Differences in the way reconnection is triggered may explain these discrepancies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS2002

Charge Transfer Calculations and Database for Astrophysics

A variety of theoretical approaches, having different but overlapping energy ranges of applicability, are applied to investigate charge transfer processes for collisions of atomic ions with atoms and molecules. The methods include quantal molecular-orbital close-coupling, classical trajectory Monte Carlo, and continuum distorted wave methods. Recent collision systems studied include S(+4) + H, S(+4) + He, N(+7) + He, H2O, CO, and CO2, O(+q)(q = 1 - 8) + H, H2, and S(+q)(q = 1 - 16) + H2. The database effort is concentrating on astrophysically important reactions of atomic ions X(+q)(X=H-Zn, q=1-4, and selected higher charges) with H, He, various metal atoms, H2, and other selected molecular targets. Existing data, much of it produced by us, has been compiled and critically evaluated. Data for many reactions missing in the literature are estimated using the multichannel Landau-Zener approximation. Fits to cross sections and rate coefficients using standard functions are provided as well as tabulations of the raw data. The database is available on the World Wide Web at cfadc.phy.ornl.gov/astro/ps/data.

Wang, J. G.↗
DOE OSTI2017

Influence of coupling on thermal forces and dynamic friction in plasmas with multiple ion species

The recently proposed effective potential theory is used to investigate the influence of coupling on inter-ion-species diffusion and momentum exchange in multi-component plasmas. Thermo-diffusion and the thermal force are found to diminish rapidly as strong coupling onsets. We found that for the same coupling parameters, the dynamic friction coefficient there tends to be unity. Our results provide an impetus for addressing the role of coupling on diffusive processes in inertial confinement fusion experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1999

Laser Optogalvanic Spectroscopy pf Neon and Argon in a Discharge Plasma and its Significance for Microgravity Combustion

A detailed study of combustion mechanisms in flames, employing laser-based diagnostics, has provided good knowledge and understanding of the physical phenomena, and led to better characterization of the dynamical and chemical combustion processes, both under low-gravity (in space) and normal gravity (in ground based facilities, e.g. drop towers). Laser induced fluorescence (LIF), laser-induced incandescence (LII) and LIF thermometry have been widely used to perform nonintrusive measurements and to better understand combustion phenomena. Laser optogalvanic (LOG) spectroscopy has well-established applications in ion mobility measurements, atomic and molecular spectroscopy, ionization rates, recombination rates, velocity measurements and as a combustion probe for trace element detection. Absorption spectra of atomic and molecular species in flames can be obtained via LOG spectroscopy by measuring the voltage and current changes induced by laser irradiation. There are different kinds of processes that contribute to a discharge current, namely: (1) electron impact ionization, (2) collisions among the excited atoms of the discharge species and (3) Penning ionization. In general, at higher discharge currents, the mechanism of electron impact ionization dominates over Penning ionization, whereby the latter is hardly noticeable. In a plasma, whenever the wavelength of a laser coincides with the absorption of an atomic or molecular species, the rate of ionization of the species momentarily increases or decreases due to laser-assisted acceleration of collisional ionization. Such a rate of change in the ionization is monitored as a variation in the transient current by inserting a high voltage electrode into the plasma. Optogalvanic spectroscopy in discharges has been useful for characterizing laser line-widths and for providing convenient calibration lines for tunable dye lasers in the ultraviolet, visible and infrared wavelength regions. Different kinds of quantitative information, such as the electron collisional ionization rate, can be extracted from the complex processes occurring within the discharge. In the optogalvanic effect (OGE), there is no problem of overlap from background emissions, and hence even weak signals can be detected with a high signal-to-noise ratio, which makes the optogalvanic effect sensitive enough to resolve vibrational changes in molecular bonds and differences in energy levels brought about by different electron spins. For calibration purposes, neon and argon gaseous discharges have been employed most extensively, because these gases are commonly used as buffer gases within hollow-cathode lamps and provide an acceptable density of calibration lines. In the present work, our main aim has been to understand the dominant physical processes responsible for the production of the OGE signal, based on the extensive time resolved optogalvanic waveforms recorded, and also to extract quantitative information on the rates of excited state collisional processes.

Misra, Prabhakar↗
NASA NTRS1993

Molecular processes in comets

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.

Dalgarno, A.↗
NASA NTRS1995

Model atmospheres for M (sub)dwarf stars. 1: The base model grid

We have calculated a grid of more than 700 model atmospheres valid for a wide range of parameters encompassing the coolest known M dwarfs, M subdwarfs, and brown dwarf candidates: 1500 less than or equal to T(sub eff) less than or equal to 4000 K, 3.5 less than or equal to log g less than or equal to 5.5, and -4.0 less than or equal to (M/H) less than or equal to +0.5. Our equation of state includes 105 molecules and up to 27 ionization stages of 39 elements. In the calculations of the base grid of model atmospheres presented here, we include over 300 molecular bands of four molecules (TiO, VO, CaH, FeH) in the JOLA approximation, the water opacity of Ludwig (1971), collision-induced opacities, b-f and f-f atomic processes, as well as about 2 million spectral lines selected from a list with more than 42 million atomic and 24 million molecular (H2, CH, NH, OH, MgH, SiH, C2, CN, CO, SiO) lines. High-resolution synthetic spectra are obtained using an opacity sampling method. The model atmospheres and spectra are calculated with the generalized stellar atmosphere code PHOENIX, assuming LTE, plane-parallel geometry, energy (radiative plus convective) conservation, and hydrostatic equilibrium. The model spectra give close agreement with observations of M dwarfs across a wide spectral range from the blue to the near-IR, with one notable exception: the fit to the water bands. We discuss several practical applications of our model grid, e.g., broadband colors derived from the synthetic spectra. In light of current efforts to identify genuine brown dwarfs, we also show how low-resolution spectra of cool dwarfs vary with surface gravity, and how the high-regulation line profile of the Li I resonance doublet depends on the Li abundance.

Allard, France↗
NASA NTRS1985

A complex T-matrix derivation of a resonance amplitude

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.

Norbury, J. W.↗
DOE OSTI2021

Eisenbud–Wigner–Smith time delay in atom–laser interactions

We report recent development of ultrafast measurement techniques on the sub-femtosecond time scale has enabled us to see the atom–laser interaction in real time. One of the important observables to study the temporally resolved dynamics is the various time delay in the process. Time delays is an experimentally measurable quantity, where the time is not. Time delays in quantum collisions and in photoionization/photodetachment of atomic and molecular systems is reviewed. The formalisms of time delay in the context of quantum collisions by Eisenbud and Wigner that by Smith and their equivalence is discussed. The time-reversal symmetry between solutions with outgoing and ingoing wave boundary conditions allow us to interpret photoionization/photodetachment as half-scattering. Subsequently, the formalism of Eisenbud–Wigner–Smith time delay is extended in photoionization/photodetachment from collisions. We discuss that the time delay can be written as a self-adjoint quantum operator which depicts its measurability. On the experimental side, the measurement protocols are reviewed for attosecond streaking and RABBITT. Along with the EWS time delay, the measurement introduces an additional (which is negative) time delay. From the measurement of total delay and an analytical/numerical estimate of the measurement induced part, one gets the EWS time delay in the process. A few illustrative examples of studies on time delay are given to get a flavour of the outstanding advances made in this field in the last two decades.

74 ATOMIC AND MOLECULAR PHYSICS↗