Mapping Resonance Structures in Transient Core-Ionized Atoms
Not Available
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
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Results for “ionization and excitation processes”
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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Feasibility study to use neutron capture for an ultralow energy nuclear-recoil calibration in liquid xenon
The feasibility of an ultra-low energy nuclear-recoil measurement in liquid xenon using neutron capture is investigated for a small (sub-kilogram) liquid xenon detector that is optimized for a high scintillation gain, and a pulsed neutron source. Further, the measurement uses the recoil energies imparted to xenon nuclei during the de-excitation process following neutron capture, where promptly emitted γ cascades can provide the nuclei with up to 0.3 keV nr of recoil energy due to conservation of momentum. A successful calibration of scintillation photon and ionization electron yields below this energy will contribute to a greater sensitivity for liquid xenon experiments in searches for light WIMPs.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Strong-field nonsequential double photoionization using virtual-detector theory with path summation
We present an ab initio study of the nonsequential strong-field ionization dynamics of a model two-electron atom with helium character. Single- and double-ionization events are characterized and displayed using detector signals extracted at different points in the two-electron two-dimensional space. The double photoelectron momentum distribution is calculated via coherent path-summation over virtual-particle trajectories. A comparison is made between the momentum distributions obtained with the virtual-detector method, the Schrödinger wave function, and the time-dependent surface flux method developed by Tao and Scrinzi [New J. Phys. 14, 013021 (2012)]. Insights into different ionization and electron recollision pathways are gained from detailed virtual-particle tracking and energy-time readouts. Furthermore, this study demonstrates the extension of virtual-detector theory to strong-field multielectron quantum dynamics and highlights the importance of the evolving quantum phase in quasiclassical electron propagation.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Establishing criteria for the transition from kinetic to fluid modeling in hollow cathode analysis
Hollow cathodes for plasma switch applications are investigated via 2D3V particle-in-cell simulations of the channel and plume region. The kinetic nature of the plasma within the channel is dependent on the thermalization rate of electrons, emitted from the insert. When Coulomb collisions occur at a much greater rate than ionization or excitation collisions, the electron energy distribution function rapidly relaxes to a Maxwellian and the plasma within the channel can be described accurately via a fluid model. In contrast, if inelastic processes are much faster than Coulomb collisions, then the electron energy distribution function in the channel exhibits a notable high-energy tail, and a kinetic treatment is required. This criterion is applied to hollow cathodes from the literature, revealing that a fluid approach is suitable for most electric propulsion applications, whereas a kinetic treatment can be more critical to accurate modeling of plasma switches.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Nonlinear ionization dynamics of hot dense plasma observed in a laser-plasma amplifier
Understanding the behaviour of matter under conditions of extreme temperature, pressure, density and electromagnetic fields has profound effects on our understanding of cosmologic objects and the formation of the universe. Lacking direct access to such objects, our interpretation of observed data mainly relies on theoretical models. However, such models, which need to encompass nuclear physics, atomic physics and plasma physics over a huge dynamic range in the dimensions of energy and time, can only provide reliable information if we can benchmark them to experiments under well-defined laboratory conditions. Due to the plethora of effects occurring in this kind of highly excited matter, characterizing isolated dynamics or obtaining direct insight remains challenging. High-density plasmas are turbulent and opaque for radiation below the plasma frequency and allow only near-surface insight into ionization processes with visible wavelengths. Here, the output of a high-harmonic seeded laser-plasma amplifier using eight-fold ionized krypton as the gain medium operating at a 32.8 nm wavelength is ptychographically imaged. A complex-valued wavefront is observed in the extreme ultraviolet (XUV) beam with high resolution. Ab initio spatio-temporal Maxwell–Bloch simulations show excellent agreement with the experimental observations, revealing overionization of krypton in the plasma channel due to nonlinear laser-plasma interactions, successfully validating this four-dimensional multiscale model. This constitutes the first experimental observation of the laser ion abundance reshaping a laser-plasma amplifier. The presented approach shows the possibility of directly modelling light-plasma interactions in extreme conditions, such as those present during the early times of the universe, with direct experimental verification.
36 MATERIALS SCIENCE↗
Electron scattering with ethane adsorbed on rare gas multilayers: Hole transfer, coulomb decay, and ion dissociation
Positive ion desorption following electron impact dissociative ionization of ethane adsorbed on Ar, Kr, and Xe multilayers has been studied as a function of incident electron energy from threshold to 100 eV. Based on the dependence of ion yields on the identity of the rare gas, it is likely that the majority of ethane molecules undergo indirect ionization following hole transfer from the ionized underlying rare gas. Further, this has also been corroborated by density of states calculations showing the energetic alignment of the outer valence states of ethane and the condensed rare gas ionization energies. Due to the near-resonant nature of charge transfer for single-hole states, the ethane molecular ion is excited to different final ionic states on different rare gases, which leads to differences in ion desorption yields and branching ratios. The quantitative yields increase with increasing ionization energy gap between the rare gas and ethane, in the order Ar > Kr >Xe. The large increase in yields from 25 eV onwards for all rare gases is likely due to the formation and decay of two-hole states on neighboring rare gas and ethane molecules due to interatomic and intermolecular Coulomb decay (ICD) and not electron transfer mediated decay (ETMD). The ICD and ETMD pathways become accessible when the incoming electron has sufficient energy to excite the inner valence ns level of the rare gas to a Rydberg state or ionize it. The experimental findings are supported by calculations of thresholds, density of states for the final configurations of these processes, and coupling strengths for hole transfer between ethane and rare gases. The fragment ion branching ratios vary with energy from threshold to about 35 eV, showing the fragmentation pattern changes with the mode of hole transfer and availability of excess energy. Sigma C–C bonds are more likely to break than C–H bonds in the mid-20 eV range, and this effect is most pronounced for Xe, followed by Kr, and then Ar.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Nonadiabatic Strong-Field Photoionization Revisited
We measure strong field ionization of cesium atoms, observing a robust feature near 2𝑈p in the photoelectron spectrum, which we call the intermediate energy structure (IES). Using a Coulomb-corrected strong-field approximation, we show it arises from electrons born with large inward velocities that rapidly undergo forward scattering off the Coulomb potential. The IES is similar to the previously identified low energy structure in that they are both due to forward scattering. However, it is different in that IES requires both nonadiabatic ionization conditions (as defined by the Keldysh parameter) and a more weakly bound initial state. Furthermore, our joint experimental and theoretical study supports the need for an additional parameter in characterization of strong field ionization, which depends both on nonadiabaticity of the process and the principal quantum number of the target. Together with Reiss and Keldysh parameters, this dimensionless parameter expands the description of strong field ionization across a broad range of atomic targets and incorporates ionization from excited states.
74 ATOMIC AND MOLECULAR PHYSICS↗
Angle-resolved nonresonant two-photon single ionization of argon using 9.3-eV photons produced via high-order harmonic generation
Here we present an experimental study on the photoionization dynamics of nonresonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3-eV photons produced via high harmonic generation and a three-dimensional momentum imaging spectrometer, we detect the photoelectrons and ions produced from nonresonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$- and $f$-partial-wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the vacuum ultraviolet polarization. The comparison between the present results and the two previous sets of theoretical calculations [Phys. Rev. A 44, 324 (1991), and J. Phys. B: At. Mol. Phys. 16, 2737 (1983)] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.
74 ATOMIC AND MOLECULAR PHYSICS↗
Ultrabroadband microwave radiation from near- and mid-infrared laser-produced plasmas in air
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70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
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↗
Uncovering extreme nonlinear dynamics in solids through time-domain field analysis
Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Furthermore, time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters.
74 ATOMIC AND MOLECULAR PHYSICS↗
Atomic autoionization in the photo-dissociation of super-excited deuterated water molecules fragmenting into D + + O + + D
We present the relaxation dynamics of deuterated water molecules via autoionization, initiated by the absorption of a 61 eV photon, producing the very rare D + + O + + D breakup channel. We employ the COLd target recoil ion momentum spectroscopy method to measure the 3D momenta of the ionic fragments and emitted electrons from the dissociating molecule in coincidence. We interpret the results using the potential energy surfaces extracted from multi-reference configuration interaction calculations. The measured particle energy distributions can be related to a super-excited monocationic state located above the double ionization threshold of D 2 O. The autoionized electron energy shows a sharp distribution centered around 0.5 eV, which is a signature of the atomic oxygen autoionization occurring in the direct and sequential dissociation processes of D 2 O + * at a large internuclear distance. In this way, an O + radical fragment and a low-energy electron are created, both of which can trigger secondary reactions in their environment.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Wave packet dynamics and control in excited states of molecular nitrogen
Wave packet interferometry with vacuum ultraviolet light has been used to probe a complex region of the electronic spectrum of molecular nitrogen, N 2 . Wave packets of Rydberg and valence states were excited by using double pulses of vacuum ultraviolet (VUV), free-electron-laser (FEL) light. These wave packets were composed of contributions from multiple electronic states with a moderate principal quantum number (n ~ 4-9) and a range of vibrational and rotational quantum numbers. The phase relationship of the two FEL pulses varied in time, but as demonstrated previously, a shot-by-shot analysis allows the spectra to be sorted according to the phase between the two pulses. The wave packets were probed by angle-resolved photoionization using an infrared pulse with a variable delay after the pair of excitation pulses. The photoelectron branching fractions and angular distributions display oscillations that depend on both the time delays and the relative phases of the VUV pulses. The combination of frequency, time delay, and phase selection provides significant control over the ionization process and ultimately improves the ability to analyze and assign complex molecular spectra.
74 ATOMIC AND MOLECULAR PHYSICS↗
Fragmentation Dynamics of Fluorene Explored Using Ultrafast XUV-Vis Pump-Probe Spectroscopy
We report on the use of extreme ultraviolet (XUV, 30.3 nm) radiation from the Free-electron LASer in Hamburg (FLASH) and visible (Vis, 405 nm) photons from an optical laser to investigate the relaxation and fragmentation dynamics of fluorene ions. The ultrashort laser pulses allow to resolve the molecular processes occurring on the femtosecond timescales. Fluorene is a prototypical small polycyclic aromatic hydrocarbon (PAH). Through their infrared emission signature, PAHs have been shown to be ubiquitous in the universe, and they are assumed to play an important role in the chemistry of the interstellar medium. Our experiments track the ionization and dissociative ionization products of fluorene through time-of-flight mass spectrometry and velocity-map imaging. Multiple processes involved in the formation of each of the fragment ions are disentangled through analysis of the ion images. The relaxation lifetimes of the excited fluorene monocation and dication obtained through the fragment formation channels are reported to be in the range of a few tens of femtoseconds to a few picoseconds.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
CF + excitation in the interstellar medium
The detection of CF + in interstellar clouds potentially allows astronomers to infer the elemental fluorine abundance and the ionization fraction in ultraviolet-illuminated molecular gas. Because local thermodynamic equilibrium (LTE) conditions are hardly fulfilled in the interstellar medium (ISM), the accurate determination of the CF + abundance requires one to model its non-LTE excitation via both radiative and collisional processes. Here, we report quantum calculations of rate coefficients for the rotational excitation of CF + in collisions with para- and ortho-H 2 (for temperatures up to 150 K). As an application, we present non-LTE excitation models that reveal population inversion in physical conditions typical of ISM photodissociation regions (PDRs). We successfully applied these models to fit the CF + emission lines previously observed toward the Orion Bar and Horsehead PDRs. The radiative transfer models achieved with these new rate coefficients allow the use of CF + as a powerful probe to study molecular clouds exposed to strong stellar radiation fields.
79 ASTRONOMY AND ASTROPHYSICS↗
Multichannel photoelectron phase lag across atomic barium autoionizing resonances
Phase lag associated with coherent control where an excited system decays into more than one product channel has been subjected to numerous investigations. Although previous theoretical studies have treated the phase lag across resonances in model calculations, quantitative agreement has never been achieved between the theoretical model and an experimental measurement of the phase lag from the ω-2ω ionization of atomic barium. Yamazaki and Elliot, Phys. Rev. Lett. 98, 053001 (2007); Phys. Rev. A 76, 053401 (2007), suggesting that a toy model with phenomenological parameters is inadequate to describe the observed phase lag behavior. Here the phase lag is treated quantitatively in a multichannel coupling formulation, and our calculation based on a multichannel quantum defect and R-matrix treatment achieves good agreement with the experimental observations. Our treatment also develops formulas to describe the effects of hyperfine depolarization on multiphoton ionization processes. Moreover, we identify resonances between Ba + 5d 3/2 and 5d 5/2 thresholds that have apparently never been experimentally observed and classified.
74 ATOMIC AND MOLECULAR PHYSICS↗
Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
Not Available
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
One-dimensional air temperature measurements by air resonance enhanced multiphoton Ionization thermometry (ART)
In this work, a detailed calibration study is performed to establish non-intrusive one-dimensional (1D) rovibrational temperature measurements in unseeded air, based on air resonance enhanced multiphoton ionization thermometry (ART). ART is generated by REMPI (resonance enhanced multi-photon ionization) of molecular oxygen and subsequent avalanche ionization of molecular nitrogen in a single laser pulse. ART signal, the fluorescence from the first negative band of molecular nitrogen, is directly proportional to the 2-photon transition of molecular oxygen C 3 Π (v = 2) ← X 3 Σ (v’=0), which is used to determine temperature. Experimentally, hyperfine structures of the O 2 rotational branches with high temperature sensitivity are selectively excited through a frequency-doubled dye laser. Electron-avalanche ionization of N 2 results in the fluorescence emissions from the first negative bands of N 2 + near 390, 425, and 430nm, which are captured as a 1D line by a gated intensified camera. Post processing of the N 2 + fluorescence yields a 1D thermometry line that is representative of the air temperature. It is demonstrated that the technique provides ART fluorescence of ∼5cm in length in the unseeded air, presenting an attractive thermometry solution for high-speed wind tunnels and other ground test facilities.
42 ENGINEERING↗