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Results for “below- threshold ionization”

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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Control of electron recollision and molecular nonsequential double ionization

Abstract Intense laser pulses lasting a few optical cycles, are able to ionize molecules via different mechanisms. One such mechanism involves a process whereby within one optical period an electron tunnels away from the molecule, and is then accelerated and driven back as the laser field reverses its direction, colliding with the parent molecule and causing correlated non-sequential double ionization (NSDI). Here we report control over NSDI via spectral-phase pulse shaping of femtosecond laser pulses. The measurements are carried out on ethane molecules using shaped pulses. We find that the shaped pulses can enhance or suppress the yield of dications resulting from electron recollision by factors of 3 to 6. This type of shaped pulses is likely to impact all phenomena stemming from electron recollision processes induced by strong laser fields such as above threshold ionization, high harmonic generation, attosecond pulse generation, and laser-induced electron diffraction.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

High-resolution photoabsorption spectrum of jet-cooled propyne

The absolute photoabsorption cross section of propyne was recorded between 62 000 and 88 000 cm{sup −1} by using the vacuum-ultraviolet, Fourier-transform spectrometer at the Synchrotron Soleil. This cross section spans the region including the lowest Rydberg bands and extends above the Franck-Condon envelope for ionization to the ground electronic state of the propyne cation, X{sup ~+}. Room-temperature spectra were recorded in a flowing cell at 0.9 cm{sup −1} resolution, and jet-cooled spectra were recorded at 1.8 cm{sup −1} resolution and a rotational temperature of ∼100 K. The reduced widths of the rotational band envelopes in the latter spectra reveal new structure and simplify a number of assignments. Although nf Rydberg series have not been assigned previously in the photoabsorption spectrum of propyne, arguments are presented for their potential importance, and the assignment of one nf series is proposed. As expected from previous photoelectron spectra, Rydberg series are also observed above the adiabatic ionization threshold that converge to the v{sub 3}{sup +} = 1 and 2 levels of the C≡C stretching vibration.

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

Quantum-mechanical predictions of electron-induced ionization cross sections of DNA components

Ionization of biomolecules remains still today rarely investigated on both the experimental and the theoretical sides. In this context, the present work appears as one of the first quantum mechanical approaches providing a multi-differential description of the electron-induced ionization process of the main DNA components for impact energies ranging from the target ionization threshold up to about 10 keV. The cross section calculations are here performed within the 1st Born approximation framework in which the ejected electron is described by a Coulomb wave whereas the incident and the scattered electrons are both described by a plane wave. The biological targets of interest, namely, the DNA nucleobases and the sugar-phosphate backbone, are here described by means of the GAUSSIAN 09 system using the restricted Hartree-Fock method with geometry optimization. The theoretical predictions also obtained have shown a reasonable agreement with the experimental total ionization cross sections while huge discrepancies have been pointed out with existing theoretical models, mainly developed within a semi-classical framework.

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

Gas-to-cluster effects in S 2p-excited SF{sub 6}

High resolution X-ray spectroscopic studies on free SF{sub 6} molecules and SF{sub 6} clusters near the S 2p ionization thresholds are reported. Spectral changes occurring in clusters for the intense molecular-like S 2p{sub 1/2,3/2}{yields} 6a{sub 1g}-, 2t{sub 2g}-, and 4e{sub g}-resonances are examined in detail. Neither gas-to-cluster spectral shifts nor changes in peak shape are observed for the pre-edge 6a{sub 1g}-band. Significant changes in band shape and distinct gas-to-cluster shifts occur in the S 2p{sub 1/2,3/2}{yields} 2t{sub 2g}- and 4e{sub g}-transitions. These are found in the S 2p-ionization continua. The quasiatomic approach is used to assign the experimental results. It is shown that a convolution of asymmetric and symmetric contributions from Lorentzian and Gaussian line shapes allows us to model the spectral distribution of oscillator strength for the S 2p{sub 1/2,3/2}{yields} 2t{sub 2g}-, and 4e{sub g}-transitions. The asymmetry is due to trapping of the photoelectron within the finite size potential barrier. The Lorentzian contribution is found to be dominating in the line shape of the S 2p{yields} 2t{sub 2g}- and 4e{sub g}-bands. The spectroscopic parameters of the spin-orbit components of both the 2t{sub 2g}- and 4e{sub g}-bands are extracted and their gas-to-cluster changes are analyzed. The photoelectron trapping times in free and clustered SF{sub 6} molecules are determined. Specifically, it is shown that spectral changes in clusters reflected in core-to-valence-transitions are due to a superposition of the singly scattered photoelectron waves at the neighboring molecules with the primary and multiply scattered waves within the molecular cage.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

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↗
DOE OSTI2015

Bound and resonance states of the dipolar anion of hydrogen cyanide: Competition between threshold effects and rotation in an open quantum system

In this paper, bound and resonance states of the dipole-bound anion of hydrogen cyanide HCN – are studied using a nonadiabatic pseudopotential method and the Berggren expansion technique involving bound states, decaying resonant states, and nonresonant scattering continuum. We devise an algorithm to identify the resonant states in the complex energy plane. To characterize spatial distributions of electronic wave functions, we introduce the body-fixed density and use it to assign families of resonant states into collective rotational bands. We find that the nonadiabatic coupling of electronic motion to molecular rotation results in a transition from the strong-coupling to weak-coupling regime. In the strong-coupling limit, the electron moving in a subthreshold, spatially extended halo state follows the rotational motion of the molecule. Above the ionization threshold, the electron's motion in a resonance state becomes largely decoupled from molecular rotation. Finally, the widths of resonance-band members depend primarily on the electron orbital angular momentum.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Electron-impact ionization of P-like ions forming Si-like ions

We have calculated electron-impact ionization (EII) for P-like systems from P to Zn{sup 15+} forming Si-like ions. The work was performed using the flexible atomic code (FAC) which is based on a distorted-wave approximation. All 3ℓ → nℓ' (n = 3-35) excitation-autoionization (EA) channels near the 3p direct ionization threshold and 2ℓ → nℓ' (n = 3-10) EA channels at the higher energies are included. Close attention has been paid to the detailed branching ratios. Our calculated total EII cross sections are compared both with previous FAC calculations, which omitted many of these EA channels, and with the available experimental results. Moreover, for Fe{sup 11+}, we find that part of the remaining discrepancies between our calculations and recent measurements can be accounted for by the inclusion of the resonant excitation double autoionization process. Lastly, at the temperatures where each ion is predicted to peak in abundances in collisional ionization equilibrium, the Maxwellian rate coefficients derived from our calculations differ by 50%-7% from the previous FAC rate coefficients, with the difference decreasing with increasing charge.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2016

Observation of extreme ultraviolet transitions in highly charged Ba{sup 16+} to Ba{sup 23+} ions with electron beam ion trap

We have investigated extreme ultraviolet emission from highly charged barium using a compact electron beam ion trap at the Tokyo EBIT laboratory. The spectra were recorded for several beam energies ranging from 440 to 740 eV, while keeping the electron beam current constant at 10 mA. Radiation from charge states Zr-like Ba{sup 16+} to As-like Ba{sup 23+} were recorded and identified by varying the electron beam energy across the ionization thresholds and comparing with calculated results. The calculations were performed with a detailed relativistic configuration interaction approach using the Flexible Atomic Code. Several new lines belonging to electric dipole transitions were observed and identified.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Isomerization and Fragmentation of Cyclohexanone in a Heated Micro-Reactor

Here, the thermal decomposition of cyclohexanone (C 6 H 10 =O) has been studied in a set of flash-pyrolysis microreactors. Decomposition of the ketone was observed when dilute samples of C 6 H 10 =O were heated to 1200 K in a continuous flow microreactor. Pyrolysis products were detected and identified by tunable VUV photoionization mass spectroscopy and by photoionization appearance thresholds. Complementary product identification was provided by matrix infrared absorption spectroscopy. Pyrolysis pressures were roughly 100 Torr, and contact times with the microreactors were roughly 100 μs. Thermal cracking of cyclohexanone appeared to result from a variety of competing pathways, all of which open roughly simultaneously. Isomerization of cyclohexanone to the enol, cyclohexen-1-ol (C 6 H 9 OH), is followed by retro-Diels–Alder cleavage to CH 2 =CH 2 and CH 2 =C(OH)–CH=CH 2 . Further isomerization of CH 2 =C(OH)–CH=CH 2 to methyl vinyl ketone (CH 3 CO–CH=CH 2 , MVK) was also observed. Photoionization spectra identified both enols, C 6 H 9 OH and CH 2 =C(OH)–CH=CH 2 , and the ionization threshold of C 6 H 9 OH was measured to be 8.2 ± 0.1 eV. Coupled cluster electronic structure calculations were used to establish the energetics of MVK. The heats of formation of MVK and its enol were calculated to be Δ f H 298 (cis-CH 3 CO–CH=CH 2 ) = -26.1 ± 0.5 kcal mol –1 and Δ f H 298 (s-cis-1-CH 2 =C(OH)–CH=CH 2 ) = -13.7 ± 0.5 kcal mol –1 . The reaction enthalpy Δ rxn H 298 (C 6 H 10 =O → CH 2 =CH 2 + s-cis-1-CH 2 =C(OH)–CH=CH 2 ) is 53 ± 1 kcal mol –1 and Δ rxn H 298 (C 6 H 10 =O → CH 2 =CH 2 + cis-CH 3 CO–CH=CH 2 ) is 41 ± 1 kcal mol –1 . At 1200 K, the products of cyclohexanone pyrolysis were found to be C 6 H 9 OH, CH 2 =C(OH)–CH=CH 2 , MVK, CH 2 CHCH 2 , CO, CH 2 =C=O, CH 3 , CH 2 =C=CH 2 , CH 2 =CH–CH=CH 2 , CH 2 =CHCH 2 CH 3 , CH 2 =CH 2 , and HC≡CH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Photoionization of the I 4d and valence orbitals of methyl iodide

Here, the photoabsorption and photoionization dynamics of the I 4d and valence orbitals in methyl iodide have been studied both experimentally and theoretically. Synchrotron radiation has been employed to measure the total ion yield in the vicinity of the I 4d ionization thresholds. The observed structure, due to excitations into Rydberg or valence states, has been assigned using transition energies and relative intensities computed with time-dependent density functional theory within the Tamm–Dancoff approximation. Photoelectron spectra, recorded with plane polarized radiation in two polarization geometries, have allowed the effect of autoionization on the valence electron angular distributions to be investigated. The spectra obtained at photon energies of 50.62 and 52.34 eV, coinciding respectively with the I 4d 5/2 → σ* and 4d 3/2 → σ* transitions, reveal, in addition to valence shell photoelectron bands, features not associated with simple photoionization of the parent molecule. High resolution photoelectron spectra of the I 4d main-lines display structure resulting from spin–orbit coupling and molecular field splitting. The binding energies of the five states contributing to the (I 4d) -1 ionization have been determined. The iodine (in CH 3 I) N 45 VV Auger spectrum has been measured and the observed structure has been assigned using the core hole binding energies derived in the present work together with established ionization energies of the doubly charged ion. The experimentally determined Auger electron angular distributions have been discussed in relation to the theoretical angular distribution parameter characterizing the spatial alignment of molecular axes in the (I 4d) -1 state.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Single-photon photoionization of oxygen-like Ne III

Here, we offer a theoretical and experimental study of the single-photon photoionization of Ne III. The high photon flux and the high-resolution capabilities of the Advanced Light Source at the LBNL were employed to measure absolute photoionization cross sections. The resulting spectrum has been benchmarked against high accuracy relativistic Breit-Pauli R-matrix calculations. Additionally, a large close-coupling wave function expansion which comprises up to 58 fine-structure levels of the residual ion Ne IV of configurations 2 s 2 2 p 3 , 2 s 2 p 4 , 2 p 5 , 2 s 2 2 p 2 3 s , 2 s 2 2 p 2 3 p and 2 s 2 2 p 2 3 d was included. A complete identification of the measured features was achieved by considering seven low-lying levels of Ne III. We found that the photoionization cross-section ( σ PI ) exhibits the presence of prominent resonances in the lowenergy region near the ionization thresholds that correspond to low-lying levels. These include highpeak narrow resonances with almost zero background introduced by relativistic effects. However, there does not exist a significant contribution to σ PI from relativistic effects at the high-energy interval of the present study.

32.30.Rj↗
DOE OSTI2011

Enhanced Nonlinear Double Excitation of He in Intense Extreme Ultraviolet Laser Fields

Nonlinear, three-photon double excitation of He in intense extreme ultraviolet free-electron laser fields ({approx}24.1 eV, {approx}5 TW/cm{sup 2}) is presented. Resonances to the doubly excited states converging to the He{sup +} N=3 level are revealed by the shot-by-shot photoelectron spectroscopy and identified by theoretical calculations based on the time-dependent Schroedinger equation for the two-electron atom under a laser field. It is shown that the three-photon double excitation is enhanced by intermediate Rydberg states below the first ionization threshold, giving a greater contribution to the photoionization yields than the two-photon process by more than 1 order of magnitude.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2011

Long-lived states of antiprotonic lithium pLi {sup +} produced in p+ Li collisions

Antiproton capture by lithium atoms (p+Li{yields}pLi{sup +}+e) is investigated at collision energies from 0.01 to 10 eV by using a semiclassical (also know as quantum-classical hybrid) method, in which the radial distance between the antiproton and the Li{sup +} ion is treated as a classical variable, and the other degrees of freedom are described by quantum mechanics. Analyzing the wave packet of the emitted electrons and making use of the energy conservation rule enable us to calculate the state distribution of the produced antiprotonic lithium pLi{sup +} atoms and also to distinguish between the capture and ionization ({yields}p+Li{sup +}+e) channels at collisional energies above the ionization threshold. This method is tested for the capture of negative muons by hydrogen atoms, which was rigorously investigated in previous quantum mechanical studies. Most of the pLi{sup +} atoms produced in p+Li are found to be sufficiently stable against Auger decays and are experimentally observable as long-lived states. The present system bears close similarities to the system of p+He(2S). It is therefore expected that long-lived antiprotonic helium pHe{sup +} atoms can be efficiently produced in the p capture by metastable He(2 {sup 3}S) atoms.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2011

Electron-impact rotationally elastic total cross sections for H{sub 2}CO and HCOOH over a wide range of incident energy (0.01-2000 eV)

This paper reports computational results of the total cross sections for electron impact on H{sub 2}CO and HCOOH over a wide range of electron impact energies from 0.01 eV to 2 keV. The total cross section is presented as sum of the elastic and electronic excitation cross sections for incident energies. The calculation uses two different methodologies, below the ionization threshold of the target the cross section is calculated using the UK molecular R-matrix code through the Quantemol-N software package while cross sections at higher energies are evaluated using the spherical complex optical potential formalism. The two methods are found to be consistent at the transition energy ({approx}15 eV). The present results are, in general, found to be in good agreement with previous experimental and theoretical results (wherever available) and, thus, the present results can serve as a benchmark for the cross section over a wide range of energy.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2012

Near-field focused photoemission from polystyrene microspheres studied with photoemission electron microscopy

We use photoemission electron microscopy(PEEM) to image 3 μm diameter polystyrene spheres supported on a metalthin film illuminated by 400 nm (~3.1 eV) and 800 nm (~1.5 eV) femtosecond (fs) laser pulses. Intense photoemission is generated by microspheres even though polystyrene is an insulator and its ionization threshold is well above the photon energies employed. We observe intense photoemission from the far side (the side opposite the incident light) of the illuminated microsphere that is attributed to light focusing within the microsphere. For the case of p-polarized, 800 nm fs laser pulses, we observe photoemission exclusively from the far side of the microsphere and additionally resolve sub-50 nm hot spots in the supporting Pt/Pd thin film that are located only within the focal region of the microsphere. We compare the PEEM images with finite difference time domain(FDTD) electrodynamic simulations to model our experimental results. Finally, the FDTD simulations predict light focusing in the microsphere and subsequent interaction with the supporting metal surface that is consistent with the experimental observations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2018

Near- K -edge single, double, and triple photoionization of C + ions

Single, double, and triple ionization of the C + ion by a single photon have been investigated in the energy range 286 to 326 eV around the K-shell single-ionization threshold at an unprecedented level of detail. At energy resolutions as low as 12 meV, corresponding to a resolving power of 24 000, natural linewidths of the most prominent resonances could be determined. From the measurement of absolute cross sections, oscillator strengths, Einstein coefficients, multielectron Auger decay rates, and other transition parameters of the main K-shell excitation and decay processes are derived. The cross sections are compared to results of previous theoretical calculations. Mixed levels of agreement are found despite the relatively simple atomic structure of the C + ion with only five electrons. Finally, this paper is a followup to a previous Letter [A. Müller, Phys. Rev. Lett. 114, 013002 (2015)PRLTAO0031-900710.1103/PhysRevLett.114.013002].

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2016

SU-F-T-125: Radial Dose Distributions From Carbon Ions of Therapeutic Energies Calculated with Geant4-DNA

Purpose: Radial dose distribution D(r) is the dose as a function of lateral distance from the path of a heavy charged particle. Its main application is in modelling of biological effects of heavy ions, including applications to hadron therapy. It is the main physical parameter of a broad group of radiobiological models known as the amorphous track models. Our purpose was to calculate D(r) with Monte Carlo for carbon ions of therapeutic energies, find a simple formula for D(r) and fit it to the Monte Carlo data. Methods: All calculations were performed with Geant4-DNA code, for carbon ion energies from 10 to 400 MeV/u (ranges in water: ∼ 0.4 mm to 27 cm). The spatial resolution of dose distribution in the lateral direction was 1 nm. Electron tracking cut off energy was 11 eV (ionization threshold). The maximum lateral distance considered was 10 µm. Over this distance, D(r) decreases with distance by eight orders of magnitude. Results: All calculated radial dose distributions had a similar shape dominated by the well-known inverse square dependence on the distance. Deviations from the inverse square law were observed close to the beam path (r<10 nm) and at large distances (r >1 µm). At small and large distances D(r) decreased, respectively, slower and faster than the inverse square of distance. A formula for D(r) consistent with this behavior was found and fitted to the Monte Carlo data. The accuracy of the fit was better than 10% for all distances considered. Conclusion: We have generated a set of radial dose distributions for carbon ions that covers the entire range of therapeutic energies, for distances from the ion path of up to 10 µm. The latter distance is sufficient for most applications because dose beyond 10 µm is extremely low.

60 APPLIED LIFE SCIENCES↗