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At least 109 records · Page 6

Reconstruction of the complex angle-dependent photoionization transition dipole from a laser-dressed streaking experiment

We study the retrieval of the angular dependence of the photoionization transition dipole phase of an attosecond XUV pulse in order to reconstruct the whole photoelectron wave packet after the photoemission process. Using a one-electron model Ar atom, we show that the full electron wave packet can be reconstructed from IR-free photoelectron angular distributions and the streaking electron spectra in an IR-dressed XUV photoionization, with photoelectrons along the common polarization direction of the two pulses. The method relies on the validity of the strong-field approximation so it is valid only for higher energy photoelectrons. Here, we also point out that a single photoionization group time delay is not enough to represent a photoemission process; instead, a complete characterization of the electron wave packet requires the retrieval of the spectral phase over the whole bandwidth of the wave packet.

74 ATOMIC AND MOLECULAR PHYSICS↗

Attosecond photoionization delays in the vicinity of molecular Feshbach resonances

Temporal delays extracted from photoionization phases are currently determined with attosecond resolution by using interferometric methods. Such methods require special care when photoionization occurs near Feshbach resonances due to the interference between direct ionization and autoionization. Although theory can accurately handle these interferences in atoms, in molecules, it has to face an additional, so far insurmountable problem: Autoionization is slow, and nuclei move substantially while it happens, i.e., electronic and nuclear motions are coupled. Here, we present a theoretical framework to account for this effect and apply it to evaluate time-resolved and vibrationally resolved photoelectron spectra and photoionization phases of N 2 irradiated by a combination of an extreme ultraviolet (XUV) attosecond pulse train and an infrared pulse. We show that Feshbach resonances lead to unusual non–Franck-Condon vibrational progressions and to ionization phases that strongly vary with photoelectron energy irrespective of the vibrational state of the remaining molecular cation.

74 ATOMIC AND MOLECULAR PHYSICS↗

Vacuum Ultraviolet Photoionization of Complex Chemical Systems

Tunable vacuum ultraviolet (VUV) radiation coupled to mass spectrometry is applied to the study of complex chemical systems in this paper. The identification of novel reactive intermediates and radicals is revealed in flame, pulsed photolysis, and pyrolysis reactors, leading to the elucidation of spectroscopy, reaction mechanisms, and kinetics. Mass-resolved threshold photoelectron photoion coincidence measurements provide unprecedented access to vibrationally resolved spectra of free radicals present in high-temperature reactors. Photoionization measurements in water clusters, nucleic acid base dimers, and their complexes with water provide signatures of proton transfer in hydrogen-bonded and π-stacked systems. Experimental and theoretical methods to track ion–molecule reactions and fragmentation pathways in intermolecular and intramolecular hydrogen-bonded systems in sugars and alcohols are described. Photoionization of laser-ablated molecules, clusters, and their reaction products inform thermodynamics and spectroscopy that are relevant to astrochemistry and catalysis. Finally, new directions in coupling VUV radiation to interrogate complex chemical systems are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Radon Photoionization: Project Technical Report

In most low-background physics experiments, radon is a significant and problematic source of background radiation because it is inert and sufficiently long-lived to pervade laboratory spaces. It may be possible to manipulate (and thus mitigate) radon electromagnetically by taking advantage of its relatively low first ionization energy. When considering ambient-temperature gas phases, only iodine is comparable. The other noble gases, and the most important constituents of breathable air (nitrogen and oxygen), all have higher ionization energies; so it may be possible to selectively manipulate radon in a variety of gas streams by ionizing it with an appropriately low-energy source of photons. Radon’s first ionization energy is in the vacuum UV part of the electromagnetic spectrum, which can be produced using a deuterium lamp. In this report, we present our attempts to manipulate radon via UV photoionization in a laboratory setting. This approach has the potential to increase radon removal efficiency from gases and/or to improve the efficiency of radon detectors. Unfortunately, our experiments suggest that either the life-time of a photoionized radon ion (before it re-neutralizes) is too short to be of much practical use and/or that our low-cost UV-photon source was not sufficiently energetic for efficient photoionization of radon.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Catastrophic Cooling in Superwinds. III. Nonequilibrium Photoionization

Observations of some starburst-driven galactic superwinds suggest that strong radiative cooling could play a key role in the nature of feedback and the formation of stars and molecular gas in star-forming galaxies. These catastrophically cooling superwinds are not adequately described by adiabatic fluid models, but they can be reproduced by incorporating nonequilibrium radiative cooling functions into the fluid model. In this work, we have employed the atomic and cooling module maihem implemented in the framework of the flash hydrodynamics code to simulate the formation of radiatively cooling superwinds as well as their corresponding nonequilibrium ionization (NEI) states for various outflow parameters, gas metallicities, and ambient densities. We employ the photoionization program cloudy to predict radiation- and density-bounded photoionization for these radiatively cooling superwinds, and we predict UV and optical line emission. Our nonequilibrium photoionization models built with the NEI states demonstrate the enhancement of C iv, especially in metal-rich, catastrophically cooling outflows, and O vi in metal-poor ones.

Cooling flows↗

Vibrational intensity distributions for continuum photoionization of oxygen

Results from measurements of vibrational intensity distributions for continuum photoionization of O2 are reported. Measurements were made using the 584 and 304 A He lines. The photoionization cross section of O2 shows a substantial dip in magnitude over a 20 A band centered about 590 A; thus the possibility exists that a 584 A photoelectron spectrum of O2 includes an autoionized contribution and the vibrational intensity distributions may not correspond to those of continuum ionization. Oxygen photoionization cross section shows no structure around 304 A and purley continuum ionization is expected.

Gardner, J. L.↗

Photoionization of barium clouds via the 3D metastable levels

The photoionization of optically thin barium clouds is analyzed and shown to occur primarily by a two-step process involving the 3D metastable term as the intermediate state. The equilibrium populations of the 1D and 3D metastable levels are calculated and found to differ significantly from the values now in the literature. These populations are combined with newly available photoionization data to calculate the resulting photoionization rate in the upper atmosphere.

Carlsten, J. L.↗

Photoionization of atoms and molecules

A literature review on the present state of knowledge in photoionization is presented. Various experimental techniques that have been developed to study photoionization, such as fluorescence and photoelectron spectroscopy, mass spectroscopy, are examined. Various atoms and molecules were chosen to illustrate these techniques, specifically helium and xenon atoms and hydrogen molecules. Specialized photoionization such as in positive and negative ions, excited states, and free radicals is also treated. Absorption cross sections and ionization potentials are also discussed.

Samson, J. A. R.↗

Dissociative and double photoionization of CO2 from threshold to 90 A

The molecular photoionization, dissociative photoionization and double photoionization cross sections for CO2 were measured from their onsets down to 90 A by using various combinations of mass spectrometers (a coincidence time-of-flight mass spectrometer and a magnetic mass spectrometer) and light sources (synchrotron radiation, and glow and spark discharge). It is concluded that the one broad peak and the three shoulders in the total adsorption cross section curve between 640 and 90 A are caused completely by dissociative ionization processes. Several peaks observed in the cross section curve for the total fragmentation CO(+)3, O(+) and C(+) are compared with those in the photoelectron spectrum reported for CO2.

Masuoka, T.↗

Dissociative and double photoionization of CO from threshold to 90 A

Partial cross sections for molecular photoionization (CO(+)), dissociative photoionization (C(+) and O(+)), and dissociative double photoionization (C(2+)) in CO have been measured from their thresholds to 90 A using techniques of mass spectrometry. The results are compared with data reported previously. Several peaks observed in the cross section curves for dissociated fragments are tentatively assigned by comparing with those in the photoelectron spectra reported for CO. It is concluded that the shoulder in the total absorption cross section curve between 400 and 90 A results solely from the dissociative ionization processes.

Masuoka, T.↗

Photoionization in the halo of the Galaxy

The ionizing radiation field in the halo is calculated and found to be dominated in the 13.6-45 eV range by light from O-B stars that escapes the disk, by planetary nebulae at 45-54 eV, by quasars and the Galactic soft X-ray background at 54-2000 eV, and by the extragalactic X-ray background at higher energies. Photoionization models are calculated with this radiation field incident on halo clouds of constant density for a variety of densities, for normal and depleted abundances, and with variations of the incident spectrum. For species at least triply ionized, such as Si IV, C IV, N V, and O VI, the line ratios are determined by intervening gas with the greatest volume, which is not necessarily the greatest mass component. Column densities from doubly ionized species like Si III should be greater than from triply ionized species. The role of photoionized gas in cosmic ray-supported halos and Galactic fountains is discussed. Observational tests of photoionization models are suggested.

Bregman, Joel N.↗

Flash-photoionized nebulae

Under conditions of high radiation intensity and low gas density, recombination may be neglected in determining the ionization state of a photoionized gas. Calculations of the ionization structure of nebulae in this 'flash-photoionized' regime are reported. Very hard spectra of ionizing ultraviolet radiation may be produced by filtration of the ionizing flux through a neutral hydrogen layer which preferentially absorbs photons just above the hydrogen photoionization threshold. Fluxes with these hard spectra produce gas layer in which helium is largely doubly ionized while hydrogen is largely neutral. Such a layer leads to anomalously high ratios of He II to H I recombination line strengths. These results are applied to the problem of the spectrum of the arc in the cluster of galaxies A370. It is found that the spectrum may possibly be reconciled with the light echo model.

Katz, J. I.↗

X-ray spectral signatures of photoionized plasmas

Plasma emission codes have become a standard tool for the analysis of spectroscopic data from cosmic X-ray sources. However, the assumption of collisional equilibrium, typically invoked in these codes, renders them inapplicable to many important astrophysical situations, particularly those involving X-ray photoionized nebulae. This point is illustrated by comparing model spectra which have been calculated under conditions appropriate to both coronal plasmas and X-ray photoionized plasmas. It is shown that the (3s-2p)/(3d-2p) line ratios in the Fe L-shell spectrum can be used to effectively discriminate between these two cases. This diagnostic will be especially useful for data analysis associated with AXAF and XMM, which will carry spectroscopic instrumentation with sufficient sensitivity and resolution to identify X-ray photoionized nebulae in a wide range of astrophysical environments.

Liedahl, Duane A.↗

Photoionization Modeling and the K Lines of Iron

We calculate the efficiency of iron K line emission and iron K absorption in photoionized models using a new set of atomic data. These data are more comprehensive than those previously applied to the modeling of iron K lines from photoionized gases, and allow us to systematically examine the behavior of the properties of line emission and absorption as a function of the ionization parameter, density and column density of model constant density clouds. We show that, for example, the net fluorescence yield for the highly charged ions is sensitive to the level population distribution produced by photoionization, and these yields are generally smaller than those predicted assuming the population is according to statistical weight. We demonstrate that the effects of the many strongly damped resonances below the K ionization thresholds conspire to smear the edge, thereby potentially affecting the astrophysical interpretation of absorption features in the 7-9 keV energy band. We show that the centroid of the ensemble of K(alpha) lines, the K(beta) energy, and the ratio of the K(alpha(sub 1)) to K(alpha(sub 2)) components are all diagnostics of the ionization parameter of our model slabs.

Kallman, T. R.↗

Photoionization in Ultraviolet Processing of Astrophysical Ice Analogs at Cryogenic Temperatures

Two recent experimental studies have demonstrated that amino acids or amino acid precursors are generated when astrophysical ice analogs are subjected to ultraviolet (UV) irradiation at cryogenic temperatures. Understanding the complete phenomenology of photoprocessing is critical to elucidating chemical reaction mechanisms that can function within an ice matrix under very cold conditions. Pushing beyond the much better characterized study of photolytic dissociation of chemical bonds through electronic excitation, this work explored the ability of UV radiation present in the interstellar medium to ionize small molecules embedded in ices. Quantum chemical calculations, including bulk solvation effects, were used to study the ionization of hydrogen (H2), water, and methanol (CH3OH) bound in small clusters of water. Ionization potentials were found to be much smaller in the condensed phase than in the gas phase; even a small cluster can account for large changes in the ionization potentials in ice, as well as the known formation of an OH--H3O+ pair in the case of H2O photoionization. To gauge the impact of photoionization on subsequent grain chemistry, the reaction between OH and CO in the presence of H3O+ was studied and compared with the potential energy surface without hydronium present, which is relevant to chemistry following photolysis. The differences indicate that the reaction is somewhat more likely to proceed to products (H + CO2) in the case of photoionization.

Woon, David E.↗

K-Shell Photoionization of Nickel Ions Using R-Matrix

We present R-matrix calculations of photoabsorption and photoionization cross sections across the K edge of the Li-like to Ca-like ions stages of Ni. Level-resolved, Breit-Pauli calculations were performed for the Li-like to Na-like stages. Term-resolved calculations, which include the mass-velocity and Darwin relativistic corrections, were performed for the Mg-like to Ca-like ion stages. This data set is extended up to Fe-like Ni using the distorted wave approximation as implemented by AUTOSTRUCTURE. The R-matrix calculations include the effects of radiative and Auger dampings by means of an optical potential. The damping processes affect the absorption resonances converging to the K thresholds causing them to display symmetric profiles of constant width that smear the otherwise sharp edge at the K-shell photoionization threshold. These data are important for the modeling of features found in photoionized plasmas.

Witthoeft, M. C.↗

K-shell Photoionization of Na-like to Cl-like Ions of Mg, Si, S, Ar, and Ca

We present R-matrix calculations of photoabsorption and photoionization cross sections across the K edge of Mg, Si, S, Ar, and Ca ions with more than 10 electrons. The calculations include the effects of radiative and Auger damping by means of an optical potential. The wave functions are constructed from single-electron. orbital bases obtained using a Thomas-Fermi-Dirac statistical model potential. Configuration interaction is considered among all states up to n = 3. The damping processes affect the resonances converging to the K-thresholds causing them to display symmetric profiles of constant width that smear the otherwise sharp edge at the photoionization threshold. These data are important for the modeling of features found in photoionized plasmas.

Witthoeft, M. C.↗

X-ray heating and electron temperature of laboratory photoionized plasmas

We discuss experimental and modeling results for the x-ray heating and temperature of laboratory photoionized plasmas. A method is used to extract electron temperature based on the analysis of transmission spectroscopy data that is independent of atomic kinetics modeling. Boltzmann kinetic and radiation-hydrodynamics simulations emphasized the critical interplay between atomic physics and heating in photoionized plasmas. They also demonstrated the dramatic impact of photoexcitation on excited state populations, line emissivity, and radiation cooling. Temperature calculations performed with astrophysical codes significantly overestimated the measurement.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗