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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS1988

Two-photon ionization of atomic hydrogen with elliptically polarized light

The theory of two-photon ionization of a hydrogenic state in the nonrelativistic dipole approximation is generalized for elliptically polarized light. An application to the metastable 2S state of atomic hydrogen is made. Significant differences in the angular distribution of the outgoing electrons are found depending upon the polarization of the photons. It is claimed that two-photon ionization employing elliptically polarized photons from lasers may provide an additional test for the theories of multiphoton ionization.

Kassaee, A.↗
DOE OSTI2025

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↗
DOE OSTI2026

Bond Dissociation Energy, Ionization Energy, and Electronic Structure of Thorium Dimer

Diatomic thorium, Th 2 , has been investigated using a laser ablation, supersonic expansion source to produce the molecule and resonant two-photon ionization spectroscopy to measure its bond dissociation energy (BDE) and ionization energy (IE). The molecule has a high density of states in the vicinity of its bond dissociation energy, leading to rapid predissociation as soon as this energy is exceeded. The BDE is identified from this predissociation threshold as D 0 (Th 2 ) = 2.857(7) eV, where the assigned error limit is provided in parentheses in units of the last quoted digit. Similarly, the one-photon ionization threshold has been measured, providing the ionization energy IE(Th 2 ) = 5.042(4) eV. Together with a thermochemical cycle and the atomic ionization energy, these values provide the BDE of the cation, giving D 0 (Th 2 + ) = 4.122(8) eV. Computations show that Th 2 has three nearly degenerate low-lying electronic states (1 3 Σ u + , 1 1 Σ g + , and 1 3 Δ g ) with bonding dominated by 7s and 6d orbitals, indicating predominantly transition-metal-like behavior. The 1 3 Σ u + state exhibits a triple bond, whereas the 1 1 Σ g + and 1 3 Δ g states possess quadruple-bond character and correspondingly shorter bonds. Although 1 3 Σ u + is predicted to be the lowest state without spin–orbit coupling, the large spin–orbit stabilization of the 1 3 Δ g state makes its Ω = 1 g component the ground state. Furthermore, the calculated dissociation energy (2.840 eV) and ionization energy of Th 2 (5.098 eV) are both in excellent agreement with experiment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Bond Dissociation Energies and Electronic Calculations on the Actinide Halides ThX and UX (X = Cl, Br, I)

Resonant two-photon ionization spectroscopy has been used to locate predissociation thresholds in the spectra of the actinide halides ThX and UX, where X = Cl, Br, and I. These predissociation thresholds are identified as the bond dissociation energies (BDEs) of the molecules. The resulting values show very similar BDEs for the corresponding ThX and UX species, with the thorium molecules being slightly more strongly bound: D 0 (ThCl) = 5.077(6) eV, D 0 (ThBr) = 4.391(4) eV, D 0 (ThI) = 3.537(8) eV, D 0 (UCl) = 4.989(3) eV, D 0 (UBr) = 4.313(3) eV, and D 0 (UI) = 3.449(8) eV. Here, the estimated error limit is given in parentheses in units of the last reported digit. Spinor-based coupled cluster calculations have also been carried out on the halides of this work, including also ThF and UF. Here, the final D 0 values after including contributions due to basis set incompleteness, outer-core-correlation, picture-change, and QED effects are within 0.04 eV of the present experimental values in each case.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Thorium Monosilicide, ThSi: An Experimental and Theoretical Study

The present theoretical and experimental combination study investigates the ThSi molecule in detail. Computationally, we utilized high-level multireference and coupled-cluster levels of theory conjoined with large correlation consistent basis sets to study a series of electronic and spin–orbit states of ThSi. Here, we report potential energy curves (PECs), electron configurations at equilibrium distances, spectroscopic constants, energetics, and spin–orbit coupling effects for 16 electronic states of ThSi. The studied 16 electronic states are arranged tightly within 0.9 eV, highlighting the complexity of the electronic spectrum of ThSi. The ground electronic state of ThSi is a single-reference 1 1 Σ + state that derives from the 1σ 2 2σ 2 1π 4 electronic configuration. The Ω = 0 + spin–orbit ground state of ThSi is composed of 1 1 Σ + (47%) and 13Π (44%) electronic states. Our measured bond energy (D0) of ThSi, obtained using resonant two-photon ionization (R2PI) spectroscopy is 3.146(4) eV, where the assigned error limit is given in parentheses in units of the last quoted digits. The computed D0 of ThSi (Ω = 0 + ) at the CBS-C-CCSD(T)-δT(Q)-δDK-δSO level (3.181 eV) is in good agreement with the experimental value. Our derived enthalpy of formation for ThSi, Δ f H 0K o (ThSi(g)), is 971.8(6.0) kJ/mol. Finally, we have performed density functional theory (DFT) calculations for ThSi(1 1 Σ + ) using 16 exchange correlation functionals that span multiple rungs of “Jacob’s ladder” of density functional approximation (DFA) to assess the DFT errors on D 0 , r e , and ω e of ThSi with respect to experimental and ab initio coupled-cluster values.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1973

Polarization phenomena in multiphoton ionization of atoms

The theory of multiphoton ionization for an atomic system of arbitrary complexity is developed using a density matrix formalism. An expression is obtained which determines the differential N-photon ionization cross section as a function of the polarization states of the target atom and the incident radiation. The parameters which characterize the photoelectron angular distribution are related to the general reduced matrix elements for the N-photon transition. Two-photon ionization of unpolarized atoms is treated as an illustration of the use of the theory. The dependence of the multiphoton ionization cross section on the polarization state of the incident radiation, which has been observed in two- and three-photon ionization of Cs, is accounted for by the theory. Finally, the photoelectron spin polarization produced by the multiphoton ionization of unpolarized atoms, like the analogous polarization resulting from single-photon ionization, is found to depend on the circular polarization of the incident radiation.

Jacobs, V. L.↗
NASA NTRS1973

Polarization phenomena in multiphoton ionization of atoms.

The theory of multiphoton ionization for an atomic system of arbitrary complexity is developed using a density matrix formalism. An expression is obtained which determines the differential N-photon ionization cross section as a function of the polarization states of the target atom and the incident radiation. The parameters which characterize the photo-electron angular distribution are related to the general reduced matrix elements for the N-photon transition. Two-photon ionization of unpolarized atoms is treated as an illustration of the use of the theory. The dependence of the multiphoton ionization cross section on the polarization state of the incident radiation, which has been observed in two- and three-photon ionization of Cs, is accounted for by the theory. Finally, the photoelectron spin polarization produced by the multiphoton ionization of unpolarized atoms, like the analogous polarization resulting from single-photon ionization, is found to depend on the circular polarization of the incident radiation.

Jacobs, V. L.↗
NASA NTRS1984

Identification of the SiCC radical toward IC +10216 - The first molecular ring in an astronomical source

In the radio spectrum of the envelope of the evolved carbon star IRC +10216, the fraction of lines from exotic molecules seldom or never observed in the terrestrial laboratory is exceptionally high. At least 20 lines have not been identified, and it is not known whether one, two, or a number of new molecules are involved. It is shown in the present investigation that nine of the previously unidentified lines in IRC +10216 are produced by SiCC, a radical long known to exist in stellar atmospheres. The true ground-state geometry of this radical has only been obtained recently on the basis of an elegant two-photon ionization experiment in a supersonic molecular beam. Information regarding the molecular geometry and lower rotational levels of SiCC is presented in a graph. The intensities of the SiCC lines confirm the assignments, yield new data on the temperature and density in the envelope of IRC +10216, and indicate that the amount of SiCC there is substantial.

Thaddeus, P.↗
NASA NTRS1986

The nature of the bonding in the transition metal trimers

The electronic structure of the transition metal (TM) trimers was studied by comparing the bonding in the Ca3, Sc3, and Cu3 molecules. The complete active space SCF/externally contracted configuration interaction (CI) ratio for the low-lying states of Sc3 and Sc3(+) and the SCF/CI ratio for Ca3 and Cu3 trimers, all for near equilateral triangle geometries, were calculated. In addition, vertical excitation energies for Cu3 were computed, leading to a new assignment of the upper state in the resonant two-photon ionization spectrum. Based on these studies, bonding in other TM trimers was discussed.

Walch, Stephen P.↗
DOE OSTI2026

New correlated numerical methods for attosecond molecular single and double ionization

This project resulted in the development of ASTRA, a new molecular ionization code capable of describing single and double ionization processes in polyatomic molecules with correlated electrons and time-dependent fields. Key achievements include: (i) the development of the PRISM hybrid-integral library enabling core-ionization and high-angular-momentum convergence; (ii) implementation of time-dependent Schrödinger equation solvers for pump–probe spectroscopies; (iii) validation against experimental and theoretical benchmarks for atoms and molecules; and (iv) extension to two-photon double ionization using the finite-pulse virtual-sequential model. These developments establish ASTRA as a versatile platform for attosecond molecular dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1976

Radiative cooling of a low-density plasma

The paper extends and improves the radiative cooling coefficient calculations of Cox and Tucker (1969) and Cox and Daltabuit (1971) for a low-density optically thin plasma with no molecules or dust, of cosmic abundances in the range from 10,000 to 100,000,000 K. Earlier rates applied to a plasma containing H, He, C, N, O, Ne, Mg, Si, and S; the present study added Ca, Fe, and Ni. For the elements included, many individual lines are calculated which previously has been averaged together. The cooling processes considered are permitted, forbidden, and semiforbidden line transitions, including contributions from dielectronic recombination and bremsstrahlung, radiative recombination, and two-photon continua. The ionization balance is calculated in collisional equilibrium using an approximate auto-ionization following inner-shell excitation and the low-density limit for the dielectronic recombination rate. Cooling in various observational bands in the soft X-ray region is determined.

Raymond, J. C.↗
NASA NTRS1982

The ultraviolet spectrum of Herbig-Haro object 2H

IUE spectra of Herbig-Haro object 2H are presented. The spectra show a strong 'excess' UV continuum and prominent emission lines of C, N, O, Si, Mg, and possibly Al. The continuum, F(lambda), exhibits a turnover shortward of about 1450 A, confirming for the first time the H0 two-photon nature of the emission source. A possible absorption feature near 1680 A, which could result from a new grain or molecular constituent in these protostellar objects is also noted. Recently computed models of steady shocks into partially ionized gas reproduce the two-photon spectral shape, but its observed intensity relative to H-beta and the Balmer continuum is anomalously high. It is suggested that a range of shock velocities, 70-100 km/s, or nonsteady, 'truncated' shocks may be responsible. Future high-sensitivity UV observations of HH objects may be used to probe grain extinction curves in star-forming regions.

Brugel, E. W.↗
NASA NTRS1972

Research on the properties and interactions of simple atomic and ionic systems

Simple ionic systems were studied, such as metastable autoionizing states of the negative He ion, two-photon decay spectrum of metastable He ion, optical excitation with low energy ions, and lifetime measurements of singly ionized Li and metastable He ion. Simple atomic systems were also investigated. Metastable autoionizing atomic energy levels in alkali elements were included, along with lifetime measurements of Cr-53, group 2A isotopes, and alkali metal atoms using level crossing and optical double resonance spectroscopy.

Novick, R.↗
NASA NTRS1986

Resonance ionization mass spectrometry for isotopic abundance measurements

Resonance ionization mass spectrometry (RIMS) is a relatively new laser-based technique for the determination of isotopic abundances. The resonance ionization process depends upon the stepwise absorption of photons from the laser, promoting atoms of the element of interest through progressively higher electronic states until an ion is formed. Sensitivity arises from the efficiency of the resonant absorption process when coupled with the power available from commercial laser sources. Selectivity derives naturally from the distinct electronic structure of different elements. This isobaric discrimination has provided the major impetus for development of the technique. Resonance ionization mass spectrometry was used for analysis of the isotopic abundances of the rare earth lutetium. Isobaric interferences from ytterbium severely effect the ability to measure small amounts of the neutron-deficient Lu isotopes by conventional mass spectrometric techniques. Resonance ionization for lutetium is performed using a continuous-wave laser operating at 452 nm, through a sequential two-photon process, with one photon exciting the intermediate resonance and the second photon causing ionization. Ion yields for microgram-sized quantities of lutetium lie between 10(6) and 10(7) ions per second, at overall ionization efficiencies approaching 10(-4). Discrimination factors against ytterbium greater than 10(6) have been measured. Resonance ionization for technetium is also being explored, again in response to an isobaric interference, molybdenum. Because of the relatively high ionization potential for Tc, three-photon, two-color RIMS processes are being developed.

Miller, C. M.↗
NASA NTRS1987

Partial redistribution in high-density, highly ionized plasmas

The conditions for which partial redistribution functions must be used for radiation transport in high-Z, high-density, laser-produced plasmas are examined. A previously developed two-photon formalism based on the model microfield method is used to calculate redistribution functions including electron and ion Stark broadening with ion dynamic effects. The competition between the relaxation rates and spontaneous emission is shown to determine the conditions for partial redistribution. The discussion makes use of microfield fluctuation rates and broadening coefficients which can be determined from simulation calculations. The redistribution function for the Ly-alpha transition of Ar XVIII is presented for typical plasma conditions.

Talin, B.↗
NASA NTRS1983

Ultraviolet continuum and H2 fluorescent emission in Herbig-Haro objects 43 and 47

IUE short wavelength spectra are presented for the low excitation Herbig-Haro objects HH 43 and HH 47. In the former, several emission lines in the Lyman band of H2 from an excited state are observed which are due to fluorescence from the H Ly-alpha line pumping a lower state (that is in turn excited by a low-velocity shock wave). No evidence of highly ionized gas emission is found in the UV spectra, and both objects exhibit a UV continuum which peaks in the vicinity of 1500 A and is probably caused by H two-photon emission enhanced by low velocity shock collisional excitation.

Schwartz, R. D.↗