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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 253 records · Page 14
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DOE OSTI2015

Dissociative double-photoionization of butadiene in the 25-45 eV energy range using 3-D multi-coincidence ion momentum imaging spectrometry

Dissociative double-photoionization of butadiene in the 25-45 eV energy range has been studied with tunable synchrotron radiation using full three-dimensional ion momentum imaging. Using ab initio calculations, the electronic states of the molecular dication below 33 eV are identified. The results of the measurement and calculation show that double ionization from π orbitals selectively triggers twisting about the terminal or central C–C bonds. We show that this conformational rearrangement depends upon the dication electronic state, which effectively acts as a gateway for the dissociation reaction pathway. For photon energies above 33 eV, three-body dissociation channels where neutral H-atom evaporation precedes C–C charge-separation in the dication species appear in the correlation map. The fragment angular distributions support a model where the dication species is initially aligned with the molecular backbone parallel to the polarization vector of the light, indicating a high probability for double-ionization to the “gateway states” for molecules with this orientation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Correlated proton-electron hole dynamics in protonated water clusters upon extreme ultraviolet photoionization

The ultrafast nuclear and electronic dynamics of protonated water clusters H+(H2O)n after extreme ultraviolet photoionization is investigated. In particular, we focus on cluster cations with n = 3, 6, and 21. Upon ionization, two positive charges are present in the cluster related to the excess proton and the missing electron, respectively. A correlation is found between the cluster's geometrical conformation and initial electronic energy with the size of the final fragments produced. As a result, for situations in which the electron hole and proton are initially spatially close, the two entities become correlated and separate in a time-scale of 20 to 40 fs driven by strong non-adiabatic effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Double photoionization of halogenated benzene

We have experimentally investigated the double-photoionization process in C{sub 6}BrF{sub 5} using monochromatized synchrotron radiation. We compare our results with previously published data for partially deuterated benzene (C{sub 6}H{sub 3}D{sub 3}) over a wide range of photon energies from threshold to 270 eV. A broad resonance in the ratio of doubly to singly charged parent ions at about 65 eV appears shifted in energy compared to benzene data. This shift is due to the difference in the bond lengths in two molecules. A simple model can explain the shape of this resonance. At higher photon energies, we observe another broad resonance that can be explained as a second harmonic of the first resonance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Fine- and hyperfine-structure effects in molecular photoionization. II. Resonance-enhanced multiphoton ionization and hyperfine-selective generation of molecular cations

Resonance-enhanced multiphoton ionization (REMPI) is a widely used technique for studying molecular photoionization and producing molecular cations for spectroscopy and dynamics studies. Here, we present a model for describing hyperfine-structure effects in the REMPI process and for predicting hyperfine populations in molecular ions produced by this method. This model is a generalization of our model for fine- and hyperfine-structure effects in one-photon ionization of molecules presented in Paper I [M. Germann and S. Willitsch, J. Chem. Phys. 145, 044314 (2016)]. This generalization is achieved by covering two main aspects: (1) treatment of the neutral bound-bound transition including the hyperfine structure that makes up the first step of the REMPI process and (2) modification of our ionization model to account for anisotropic populations resulting from this first excitation step. Our findings may be used for analyzing results from experiments with molecular ions produced by REMPI and may serve as a theoretical background for hyperfine-selective ionization experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

A simple photoionization scheme for characterizing electron and ion spectrometers

We present a simple diode laser-based photoionization scheme for generating electrons and ions with well-defined spatial and energetic (≲2 eV) structures. This scheme can easily be implemented in ion or electron imaging spectrometers for the purpose of off-line characterization and calibration. The low laser power ∼1 mW needed from a passively stabilized diode laser and the low flux of potassium atoms in an effusive beam make our scheme a versatile source of ions and electrons for applications in research and education.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Distinguishing resonance symmetries with energy-resolved photoion angular distributions from ion-pair formation in O 2 following two-photon absorption of a 9.3 eV femtosecond pulse

We present a combined experimental and theoretical study on the photodissociation dynamics of ion-pair formation in O 2 following resonant two-photon absorption of a 9.3 eV femtosecond pulse, where the resulting O + ions are detected using 3-D momentum imaging. Ion-pair formation states of $^3\Sigma^-_g$ and $^3\Pi_g$ symmetry are accessed through predissociation of optically dark continuum Rydberg states converging to the B $^2\Sigma^-_g$ ionic state, which are resonantly populated via a mixture of both parallel-parallel and parallel-perpendicular two-photon transitions. This mixture is evident in the angular distribution of the dissociation relative to the light polarization, and varies with the kinetic energy release (KER) of the fragmenting ion-pair. The KER-dependent photoion angular distribution reveals the underlying two-photon absorption dynamics involved in the ion-pair production mechanism and indicates the existence of two nearly degenerate continuum resonances possessing different symmetries, which can both decay by coupling to ion-pair states of the same total symmetry through internal conversion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

TIME-DEPENDENT PHOTOIONIZATION OF GASEOUS NEBULAE: THE PURE HYDROGEN CASE

We study the problem of time-dependent photoionization of low density gaseous nebulae subjected to sudden changes in the intensity of ionizing radiation. To this end, we write a computer code that solves the full time-dependent energy balance, ionization balance, and radiation transfer equations in a self-consistent fashion for a simplified pure hydrogen case. It is shown that changes in the ionizing radiation yield ionization/thermal fronts that propagate through the cloud, but the propagation times and response times to such fronts vary widely and nonlinearly from the illuminated face of the cloud to the ionization front (IF). IF/thermal fronts are often supersonic, and in slabs initially in pressure equilibrium such fronts yield large pressure imbalances that are likely to produce important dynamical effects in the cloud. Further, we studied the case of periodic variations in the ionizing flux. It is found that the physical conditions of the plasma have complex behaviors that differ from any steady-state solution. Moreover, even the time average of ionization and temperature is different from any steady-state case. This time average is characterized by overionization and a broader IF with respect to the steady-state solution for a mean value of the radiation flux. Around the time average of physical conditions there is a large dispersion in instantaneous conditions, particularly across the IF, which increases with the period of radiation flux variations. Moreover, the variations in physical conditions are asynchronous along the slab due to the combination of nonlinear propagation times for thermal fronts/IFs and equilibration times.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Photoionization heating of nova ejecta by the post-outburst supersoft source

The expanding ejecta from a classical nova remains hot enough (∼10{sup 4} K) to be detected in thermal radio emission for up to years after the cessation of mass loss triggered by a thermonuclear instability on the underlying white dwarf (WD). Nebular spectroscopy of nova remnants confirms the hot temperatures observed in radio observations. During this same period, the unstable thermonuclear burning transitions to a prolonged period of stable burning of the remnant hydrogen-rich envelope, causing the WD to become, temporarily, a super-soft X-ray source. We show that photoionization heating of the expanding ejecta by the hot WD maintains the observed nearly constant temperature of (1−4) × 10{sup 4} K for up to a year before an eventual decline in temperature due to either the cessation of the supersoft phase or the onset of a predominantly adiabatic expansion. We simulate the expanding ejecta using a one-zone model as well as the Cloudy spectral synthesis code, both incorporating the time-dependent WD effective temperatures for a range of masses from 0.60 M{sub ⊙} to 1.10 M{sub ⊙}. We show that the duration of the nearly isothermal phase depends most strongly on the velocity and mass of the ejecta and that the ejecta temperature depends on the WD’s effective temperature, and hence its mass.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

On the size and mass of photoionized clouds in extended spiral galaxy halos

The size and mass of two circumgalactic medium (CGM) clouds in the halo (impact parameter = 65 kpc) of a nearby late-type galaxy, MGC-01-04-005 (cz=1865 km s{sup −1}), are investigated using a close triplet of QSO sight lines (the “LBQS Triplet”). Far ultraviolet spectra obtained with the Cosmic Origins Spectrograph on board the Hubble Space Telescope find two velocity components in Lyα at ∼1830 and 1900 km s{sup −1} in two of these sight lines, requiring minimum transverse cloud sizes of ⩾10 kpc. A plausible, but not conclusive, detection of C iv 1548 Å absorption at the higher velocity in the third sight line suggests an even larger lower limit of ⩾23 kpc for that cloud. Using various combinations of constraints, including photoionization modeling for one absorber, lower limits on masses of these two clouds of ≳10{sup 6}M{sub ⊙} are obtained. Ground-based imaging and long-slit spectroscopy of MCG-01-04-005 obtained at the Apache Point Observatory 3.5 m telescope find it to be a relatively normal late-type galaxy with a current star formation rate (SFR) of ∼0.01M{sub ⊙} yr{sup −1}. GALEX photometry finds an SFR only a few times higher over the last 10{sup 8} years. We conclude that the CGM clouds probed by these spectra are typical because they are at impact parameters of 0.4–0.5 R{sub vir} from a rather typical, non-starbursting late-type galaxy; thus, these size and mass results should be generic for this class. Therefore, at least some CGM clouds are exceptionally large and massive.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2012

COOLING AND HEATING FUNCTIONS OF PHOTOIONIZED GAS

Cooling and heating functions of cosmic gas are crucial ingredients for any study of gas dynamics and thermodynamics in the interstellar and intergalactic media. As such, they have been studied extensively in the past under the assumption of collisional ionization equilibrium. However, for a wide range of applications, the local radiation field introduces a non-negligible, often dominant, modification to the cooling and heating functions. In the most general case, these modifications cannot be described in simple terms and would require a detailed calculation with a large set of chemical species using a radiative transfer code (the well-known code Cloudy, for example). We show, however, that for a sufficiently general variation in the spectral shape and intensity of the incident radiation field, the cooling and heating functions can be approximated as depending only on several photoionization rates, which can be thought of as representative samples of the overall radiation field. This dependence is easy to tabulate and implement in cosmological or galactic-scale simulations, thus economically accounting for an important but rarely included factor in the evolution of cosmic gas. We also show a few examples where the radiation environment has a large effect, the most spectacular of which is a quasar that suppresses gas cooling in its host halo without any mechanical or non-radiative thermal feedback.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Benchmark of few-level quantum theory vs ab initio numerical solutions for the strong-field Autler–Townes effect in photoionization of hydrogen

Abstract The temporal and spectral consequences of an intermediate resonance en route to photoionization are investigated theoretically in two ways: by solving few-level model equations and by ab initio numerical solution of the time-dependent Schrödinger equation, in both cases for hydrogen in three dimensions. The model consists of atomic states resonantly field-dressed in a three-level reduction of the hydrogen atom that consists of the 2 p –3 d (Balmer) transition and one energetically-distant continuum state. The model’s level occupation probabilities are derived from three Schrödinger amplitude equations and are benchmarked against an ab initio numerical solution for the hydrogen electron’s wavefunction under the same field. We examine contrasts between the results of the two approaches with a particular focus on Autler–Townes doublets that appear in the photoelectron spectrum.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Wigner time delay in photoionization: a 1D model study

Abstract In scattering theory, the Wigner–Smith time delay, calculated through a phaseshift derivative or its multichannel generalization, has been demonstrated to measure the amount of delay or advance experienced by colliding particles during their interaction with the scattering potential. Fetic, Becker, and Milosevic argue that this concept cannot be extended to include photoionization, viewed as a half-scattering experiment. Their argument is based on the lack of information about scattering phaseshifts in the part of the wavefunction (satisfying the ingoing-wave boundary condition) going to the detector. This article aims to test this claim by examining a photodetachment process in a simple 1D model with a short-range symmetrical potential. Using time-dependent perturbation theory with a dipole interaction, the relevant wavepacket of the outgoing particle is analyzed and compared to the free wavepacket as a reference. Our findings confirm that, indeed, a time delay arises in the liberated fragmentation wavepacket, which is expressed as an energy derivative of the scattering phaseshift. Our study highlights that the source of the phaseshift content in the wavepacket arriving at the detector is the dipole matrix element, which is a direct consequence of imposing the ingoing-wave boundary condition. We illustrate our results through numerical simulations of both the non-free and free wavepackets. The amount of the observed time delay is found to be half of that appearing in a typical scattering experiment.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Density functional study of the variants of inter-Coulombic decay resonances in the photoionization of Cl@C 60

Inter-Coulombic decay (ICD) resonances in the photoionization of Cl@C 60 endofullerene molecule are calculated using a perturbative density functional theory (DFT) method. This is the first ICD study of an open shell atom in a fullerene cage. Here, three classes of resonances are probed: (i) Cl inner vacancies decaying through C 60 outer continua, (ii) C 60 inner vacancies decaying through Cl outer continua, and (iii) inner vacancies of either system decaying through the continua of Cl-C 60 hybrid levels, the hybrid Auger-ICD resonances. Comparisons with Ar@C 60 results reveal that the properties of hybrid Auger-ICD resonances are affected by the extent of level hybridization.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Photoionization of endohedral molecules: N 2 @C 60

Calculations of the photoionization of the nitrogen $1σ_g$, $1σ_u$, and $2σ_g$, states of the N 2 @C 60 molecule are performed at the density functional theory (DFT) level taking full account of the molecular geometry of both N 2 and the C 60 . In this work, the results show that cross sections are sensitive to the parity of the final channels, with a complex interplay between the native $σ_u$ resonance in free N 2 and confinement resonances. A quite different behavior is obtained for the asymmetry parameters.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2013

RESONANCES IN THE PHOTOIONIZATION CROSS SECTIONS OF ATOMIC NITROGEN SHAPE THE FAR-ULTRAVIOLET SPECTRUM OF THE BRIGHT STAR IN 47 TUCANAE

The far-ultraviolet spectrum of the Bright Star (B8 III) in 47 Tuc (NGC 104) shows a remarkable pattern: it is well fit by local thermodynamic equilibrium models at wavelengths longer than Ly{beta}, but at shorter wavelengths it is fainter than the models by a factor of two. A spectrum of this star obtained with the Far Ultraviolet Spectroscopic Explorer shows broad absorption troughs with sharp edges at 995 and 1010 A and a deep absorption feature at 1072 A; none of which are predicted by the models. We find that these features are caused by resonances in the photoionization cross sections of the first and second excited states of atomic nitrogen (2s {sup 2} 2p {sup 3} {sup 2} D {sup 0} and {sup 2} P {sup 0}). Using cross sections from the Opacity Project, we can reproduce these features, but only if we use the cross sections at their full resolution, rather than the resonance-averaged cross sections usually employed to model stellar atmospheres. These resonances are strongest in stellar atmospheres with enhanced nitrogen and depleted carbon abundances, a pattern typical of post-asymptotic giant branch stars.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Validity of the static-exchange approximation for inner-shell photoionization of polyatomic molecules

The simple single-channel static-exchange approximation completely ignores correlation between the continuum and molecular ion electrons. In molecular systems with symmetry equivalent atoms, the single-channel approximation can seriously fail in core ionization when using delocalized orbitals to represent the core hole states. We present cross sections and molecular frame photoelectron angular distributions with both localized and delocalized core orbitals in CF 4 F (1 s ) ionization. We show that only a full coupled-channel calculation can recover an accurate description of the physics of inner-shell photoionization when using delocalized orbitals, whereas nearly the same result can be obtained from independent single-channel static-exchange calculations when localized core orbitals are used. A grid-based variational method described here makes such single-channel calculations possible on larger systems without local-exchange approximations. Illustrative calculations on the core ionization of SF 6 are presented to illustrate the power of the grid-based method.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Relativistic and correlation effects in the photoionization dynamics of oganesson ( Z = 118): Spin-orbit-interaction-activated interchannel coupling effects

High-Z atoms are excellent laboratories to study the combination of relativistic and many-electron correlation effects in electronic structure and dynamics. In the present work, the relativistic-random-phase approximation at different levels of truncation is employed to explore the final-state correlation effects in the photoelectron dynamics of the heaviest known element in the Periodic Table: oganesson (Og) with Z = 118. Here, the focus of this work is to illustrate the relativistic effects resulting from coupling different photoionization channels arising from spin-orbit split subshells, termed the spin-orbit-interaction-activated interchannel coupling effect. Comparison with the photoelectron dynamics of Rn on a qualitative level is also carried out, since Og is a homologue of Rn. The photoelectron dynamics of 7p, 7s, and 6d subshells are investigated and differences between Og and Rn, due to enhanced relativistic effects, are investigated.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Quantum beats in two-color photoionization to the spin-orbit split continuum of Ar

We report a study of the quantum beats in two-color photoionization of argon. An attosecond extreme ultraviolet pulse train prepares an electronic wave packet of definite odd parity, with total angular momentum J = 1, targeting the states between 14.0 and 14.5 eV from the ground state. Two-photon ionization of this wave packet with a tunable infrared probe pulse makes the constituent states interfere in both continuum channels, corresponding to the core angular momenta j c = 1/2 and 3/2, respectively. We analyze photoelectron spectrograms as a function of the time delay of the probe pulse and identify oscillations due to several pairs of states through Fourier decomposition. We observe phase differences between the corresponding beat signals in the two spin-orbit split continua. Comparison of theoretical simulations with the experimental measurements allows us to interpret the amplitudes and phases of ionization signals. Furthermore, we express the observed phase differences in terms of the off-diagonal elements of the short-range scattering matrix and the dipole matrix elements to the continuum eigenchannels.

74 ATOMIC AND MOLECULAR PHYSICS↗