Experiments for Photoionized Plasma Emission from Accretion-Powered X-Ray Sources.
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Loisel, Guillaume Pascal↗
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Inner-shell photoionization and core-hole decay of Xe and XeF{sub 2}
Photoionization cross sections and partial ion yields of Xe and XeF{sub 2} from Xe 3d{sub 5/2}, Xe 3d{sub 3/2}, and F 1s subshells in the 660–740 eV range are compared to explore effects of the F ligands. The Xe 3d-ϵf continuum shape resonances dominate the photoionization cross sections of both the atom and molecule, but prominent resonances appear in the XeF{sub 2} cross section due to nominal excitation of Xe 3d and F 1s electrons to the lowest unoccupied molecular orbital (LUMO), a delocalized anti-bonding MO. Comparisons of the ion products from the atom and molecule following Xe 3d photoionization show that the charge-state distribution of Xe ions is shifted to lower charge states in the molecule along with production of energetic F{sup +} and F{sup 2+} ions. This suggests that, in decay of a Xe 3d core hole, charge is redistributed to the F ligands and the system dissociates due to Coulomb repulsion. The ion products from excitation of the F 1s-LUMO resonance are different and show strong increases in the yields of Xe{sup +} and F{sup +} ions. The subshell ionization thresholds, the LUMO resonance energies, and their oscillator strengths are calculated by relativistic coupled-cluster methods and agree well with measurements.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Correlation between photoeletron and photoion in ultrafast multichannel photoionization of Ar
We theoretically investigate coherent dynamics of ions created through ultrafast multichannel photoionization from a viewpoint of photoelectron-photoion correlation. The model calculation on single-photon ionization of Ar reveals that the coherent hole dynamics in Ar{sup +} associated with a superposition of the spin-orbit states {sup 2}PJ (J = 3/2 and 1/2) can be identified by monitoring only the photoion created by a Fourier-transform limited extreme ultraviolet (EUV) pulse with the fs pulse duration, while the coherence is lost by a chirped EUV pulse. It is demonstrated that by coincidence detection of the photoelectron and photoion the coherent hole dynamics can be extracted even in the case of ionization by a chirped EUV pulse with the sufficiently wide bandwidth.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Fine- and hyperfine-structure effects in molecular photoionization. I. General theory and direct photoionization
We develop a model for predicting fine- and hyperfine intensities in the direct photoionization of molecules based on the separability of electron and nuclear spin states from vibrational-electronic states. Using spherical tensor algebra, we derive highly symmetrized forms of the squared photoionization dipole matrix elements from which we derive the salient selection and propensity rules for fine- and hyperfine resolved photoionizing transitions. Our theoretical results are validated by the analysis of the fine-structure resolved photoelectron spectrum of O{sub 2} reported by Palm and Merkt [Phys. Rev. Lett. 81, 1385 (1998)] and are used for predicting hyperfine populations of molecular ions produced by photoionization.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DESIGN OF LABORATORY EXPERIMENTS TO STUDY PHOTOIONIZATION FRONTS DRIVEN BY THERMAL SOURCES
This paper analyzes the requirements of a photoionization-front experiment that could be driven in the laboratory, using thermal sources to produce the necessary flux of ionizing photons. It reports several associated conclusions. Such experiments will need to employ the largest available facilities, capable of delivering many kJ to MJ of energy to an X-ray source. They will use this source to irradiate a volume of neutral gas, likely of N, on a scale of a few mm to a few cm, increasing with source energy. For a gas pressure of several to ten atmospheres at room temperature, and a source temperature near 100 eV, one will be able to drive a photoionization front through a system of tens to hundreds of photon mean free paths. The front should make the familiar transition from the so-called R-Type to D-Type as the radiation flux diminishes with distance. The N is likely to reach the He-like state. Preheating from the energetic photons appears unlikely to become large enough to alter the essential dynamics of the front beyond some layer near the surface. For well-chosen experimental conditions, competing energy transport mechanisms are small.
79 ASTRONOMY AND ASTROPHYSICS↗
Photoionization of Ne Atoms and Ne{sup +} Ions Near the K Edge: PrecisionSpectroscopy and Absolute Cross-sections
Single, double, and triple photoionization of Ne{sup +} ions by single photons have been investigated at the synchrotron radiation source PETRA III in Hamburg, Germany. Absolute cross-sections were measured by employing the photon–ion merged-beams technique. Photon energies were between about 840 and 930 eV, covering the range from the lowest-energy resonances associated with the excitation of one single K-shell electron up to double excitations involving one K- and one L-shell electron, well beyond the K-shell ionization threshold. Also, photoionization of neutral Ne was investigated just below the K edge. The chosen photon energy bandwidths were between 32 and 500 meV, facilitating the determination of natural line widths. The uncertainty of the energy scale is estimated to be 0.2 eV. For comparison with existing theoretical calculations, astrophysically relevant photoabsorption cross-sections were inferred by summing the measured partial ionization channels. Discussion of the observed resonances in the different final ionization channels reveals the presence of complex Auger-decay mechanisms. The ejection of three electrons from the lowest K-shell-excited Ne{sup +}(1s2s{sup 2}2p{sup 62}S{sub 1/2}) level, for example, requires cooperative interaction of at least four electrons.
79 ASTRONOMY AND ASTROPHYSICS↗
Determination of photoionization branching ratios and total photoionization cross sections at 304 A from experimental ionospheric photoelectron fluxes
High-resolution measurements of the ionospheric photoelectron spectrum are used to derive photoionization cross sections and branching ratios for N2 and O at 304 A, the wavelength of the intense He II solar radiation. Based on a theory in which the measured fluxes at energies 22.5, 24.5, 25.5 and 27.5 eV are determined by the ratio of the production rate and the loss rate coefficient, values are obtained for the ratio of molecular nitrogen density to atomic oxygen density as a function of altitude, the sum of the total photoionization cross sections, the 2P/4S and 2D/4S branching ratios for O and the B/X and A/X branching ratios for N2 photoionization and the ratios and the interspecies cross section ratios 2D/A, 4S/X and 2P/B. The values obtained are in accord with the photoionization cross sections of Kirby et al. (1979).
Richards, P. G.↗
Vacuum ultraviolet laser photoion and pulsed field ionization–Photoion study of Rydberg SERIES of chlorine atoms prepared in the {sup 2}P{sub J} (J = 3/2 and 1/2) fine-structure states
We have measured the high-resolution vacuum ultraviolet (VUV) photoion (VUV-PI) and VUV pulsed-field ionization–photoion (VUV-PFI-PI) spectra of chlorine atoms (Cl) in the VUV energy range 103,580–105,600 cm{sup −1} (12.842–13.093 eV) using a tunable VUV laser as the photoexcitation and photoionization source. Here, Cl atoms are prepared in the Cl({sup 2}P{sub 3/2}) and Cl({sup 2}P{sub 1/2}) fine-structure states by 193.3 nm laser photodissociation of chlorobenzene. The employment of VUV-PFI-PI detection has allowed the identification of Rydberg transitions that are not observed in VUV-PI measurements. More than 180 new Rydberg transition lines with principal quantum number up to n = 61 have been identified and assigned to members of nine Rydberg series originating from the neutral Cl({sup 2}P{sub 3/2}) and Cl({sup 2}P{sub 1/2}) fine-structure states. Two of these Rydberg series are found to converge to the Cl{sup +}({sup 3}P{sub 2}), four to the Cl{sup +}({sup 3}P{sub 1}), and three to the Cl{sup +}({sup 3}P{sub 0}) ionization limits. Based on the convergence limits determined by least-squares fits of the observed Rydberg transitions to the modified Ritz formula, we have obtained a more precise ionization energy (IE) for the formation of the ionic Cl{sup +}({sup 3}P{sub 2}) from the ground Cl({sup 2}P{sub 3/2}) state to be 104,591.01 ± 0.13 cm{sup −1}. This is consistent with previous IE measurements, but has a smaller uncertainty. The analysis of the quantum defects obtained for the Rydberg transitions reveals that many high-n Rydberg transitions are perturbed.
74 ATOMIC AND MOLECULAR PHYSICS↗
Absolute single-photoionization cross sections of Se 2 + : Experiment and theory
Absolute single-photoionization cross-section measurements for Se 2+ ions were performed at the Advanced Light Source at Lawrence Berkeley National Laboratory using the merged-beams photo-ion technique. Measurements were made at a photon energy resolution of 24 ± 3 meV in the photon energy range 23.5-42.5 eV, spanning the ground state and low-lying metastable state ionization thresholds. Here, to clearly resolve the resonant structure near the ground-state threshold, high-resolution measurements were made from 30.0 to 31.9 eV at a photon energy resolution of 6.7 ± 0.7 meV. Numerous resonance features observed in the experimental spectra are assigned and their energies and quantum defects tabulated. The high-resolution cross-section measurements are compared with large-scale, state-of-the-art theoretical cross-section calculations obtained from the Dirac Coulomb R -matrix method. Suitable agreement is obtained over the entire photon energy range investigated. In conclusion, these results are an experimental determination of the absolute photoionization cross section of doubly ionized selenium and include a detailed analysis of the photoionization resonance spectrum of this ion.
74 ATOMIC AND MOLECULAR PHYSICS↗
A discharge flow-photoionization mass spectrometric study of the FO(X 2 Pi i) radical. Photoionization efficiency spectrum and ionization energy
Photoionization efficiency spectra of FO were measured over the wavelength range 80.0-100.0 nm and in the ionization threshold region, 94.0-100.0 nm, using a discharge flow-photoionization mass spectrometer apparatus coupled to a synchrotron radiation source. FO was generated by the reaction of F2P atoms with NO3 and via a F2O2 discharge. A value of 12.78 +/- 0.03 eV was obtained for the adiabatic ionization energy of FO from photoion thresholds which corresponds to FO(+)(X 3 Sigma -) from FO(X 2 Pi i). These results, which are the first to be obtained by direct Photo-ionization mass spectrometry (PIMS) measurements, corroborate those of a photoelectron spectroscopy (PES) study; however, the ionization energy determined here is free from interferences due to other species which complicated the PES measurement. A value of 109.5 +/- 8.0 kJ/mol for Delta f H 0 298(FO) is computed from the present value of IE(FO) and a previous appearance energy measurement, and a value for the proton affinity of FO is calculated to be 511.5 +/- 10.0 kJ/mol.
Zhang, Zhengyu↗
New Insights into Low-Temperature Oxidation of Propane from Synchrotron Photoionization Mass Spectrometry and Multiscale Informatics Modeling
We investigated the low-temperature oxidation of propane at 4 Torr and temperatures of 530, 600, and 670 K. The oxidation is initiated by pulsed laser photolysis of oxalyl chloride, (COCl)2, at 248 nm, which rapidly generates a ~1:1 mixture of 1-propyl (n-propyl) and 2-propyl (i-propyl) radicals via the fast Cl + propane reaction. Reactants, intermediates and products are probed with isomeric selectivity by time-resolved multiplexed photoionization mass spectrometry (MPIMS) with tunable synchrotron vacuum UV radiation as the ionization source. At all three temperatures, the major stable product species is propene, formed in the C3H7 + O2 reactions by direct HO2-elimination from both n- and i-propyl peroxy radicals. The experimentally derived propene yields relative to the initial concentration of Cl atoms are (20 ± 4)% at 530 K, (55 ± 11)% at 600 K, and (86 ± 17)% at 670 K at a reaction time of 20 ms. The lower yield of propene at low temperature reflects substantial formation of propyl peroxy radicals, which do not completely decompose on the experimental time scale. In addition, we detect the C3H6O isomers methyloxirane, oxetane, acetone and propanal as minor products. Our measured yields of oxetane and methyloxirane, which are co-products of OH radicals, suggest a revision of the OH formation pathways in models of low-temperature propane oxidation. The experimental results are modeled and interpreted using a multi-scale informatics approach that is presented in detail in a separate publication (Burke, M. P.; Goldsmith, C. F.; Klippenstein, S. J.; Welz, O.; Huang H.; Antonov I. O.; Savee J. D.; Osborn D. L.; Zádor, J.; Taatjes, C. A.; Sheps, L., Multi-Scale Informatics for Low-Temperature Propane Oxidation: Further Complexities in Studies of Complex Rections, submitted, 2015). The model predicts the time profiles and yields of the experimentally observed primary products well, and shows satisfactory agreement for products formed mostly via secondary radical-radical reactions.
Combustion↗
Experimental assignment of many-electron excitations in the photoionization of NiO
The absorption of a photon and the emission of an electron is not a simple, two-particle process. The complicated many-electron features observed during core photoionization can therefore reveal many of the hidden secrets about the ground and excited-state electronic structures of a material. Careful analysis of the photon-energy dependence of the Ni KLL Auger deexcitation spectra at and above the Ni 1s photoionization threshold has identified the satellite structure that appears in both the photoelectron emission and the x-ray absorption spectra of NiO as Ni metal 3d e g → Ni metal 3d e g and O ligand 2p e g → Ni metal 3d e g charge-transfer excitations, respectively. These assignments clarify the conflicting theoretical predictions of the last five decades in addition to other anomalous effects in the spectroscopy of this unique material.
36 MATERIALS SCIENCE↗
Experimental longitudinal emittance manipulation using laser-based photoionization in the Fermilab Linac
A series of simulations and beam studies were conducted at Fermilab’s linear accelerator to evaluate the effectiveness of longitudinal emittance control via laser-induced photoionization. While similar laser techniques have been employed at Fermilab to enhance injection and extraction efficiency into the Booster, the work presented here focuses on extending these methods to bunch-by-bunch manipulation. This approach utilizes fine-scale correction of the H- bunches’ longitudinal spatial distribution. In theory, loosely confined particles in longitudinal phase space contribute to emittance growth during acceleration. By selectively removing these outlying particles through laser scraping (H- + γ → H + e-), this growth can be reduced. This report presents experimental results from both symmetric and asymmetric longitudinal scraping of H⁻ bunches in the Fermilab linac, which were subsequently injected into Booster, and evaluates the broader applicability of this method for future high-intensity accelerator operations.
Landon, Parker [Boston U.; Fermilab]↗
Photoionization research on atomic beams. 2: The photoionization cross section of atomic oxygen
An experiment to determine the absolute value of the photo-ionization cross section of atomic oxygen is described. The atoms are produced in an electrical discharge in oxygen gas with 1% hydrogen added. In order to prevent recombination a crossed beam technique is employed. The ions formed are detected by a time-of-flight mass spectrometer. The concentration of oxygen atoms in the beam is 57%. The measured photoionization cross section of atomic oxygen is compared with theoretical data. The results show the participation of autoionization processes in ionization. The cross section at the autoionizing levels detected is considerably higher than the absorption due to the unperturbed continuum. Except for wavelengths where autoionization occurs, the measured ionization cross section is in fair agreement with theory. This holds up to 550 A whereas for shorter wavelengths the theoretical values are much higher.
Comes, F. J.↗
Electron ionization, photoionization and photoelectron/photoion coincidence spectroscopy in mass-spectrometric investigations of a low-pressure ethylene/oxygen flame
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Felsmann, Daniel↗
Probing sulphur clusters in a microfluidic electrochemical cell with synchrotron-based photoionization mass spectrometry
We present synchrotron-based mass spectrometry to probe products formed in the lithium sulphide electrolyte. In operando analysis was obtained at two different potentials in a vacuum compatible microfluidic electrochemical cell. Mass spectral observations show that the charged electrolyte formed sulfur clusters under dynamic conditions, demonstrating electrolyte electron shuttling.
sulphur cluster, lithium – sulphur battery electro↗