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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

One- and two-photon ionization of hydrogen atom embedded in Debye plasmas

We present a detailed analysis of the plasma-induced resonance-like atomic structures near the ionization threshold in one- and two-photon ionization of hydrogen atom. Such resonance-like structures result from the migration of the upper bound excited states of bound-bound atomic transitions into the continuum due to the less attractive screened Coulomb potential which simulates the external environmental effect for an atom embedded in Debye plasma. The change from the resonance-like narrow structures into broad continuous spectra as the plasma effect increases could be accounted for by the overlap between the respective wavefunctions of the atomic electron in the initial state and its corresponding outgoing ionized state in the continuum.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Excited states of lutetium oxide and its singly charged cation

Vibronic spectra of lutetium oxide (LuO) seeded in supersonic molecule beams are investigated with mass-analyzed threshold ionization (MATI) spectroscopy and second-order multiconfigurational quasi-degenerate perturbation (MCQDPT2) theory. Six states of LuO and four states of LuO + are located by the MCQDPT2 calculations, and an a 3 Π(LuO + ) ← C 2 Σ + (LuΟ) transition is observed by the MATI measurement. Finally, the vibronic spectra show abnormal vibrational intervals for both the neural and cation excited states, and the abnormality is attributed to vibrational perturbations induced by interactions with neighboring states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Spin–orbit coupling of electrons on separate lanthanide atoms of Pr 2 O 2 and its singly charged cation

Although it plays a critical role in the photophysics and catalysis of lanthanides, spin–orbit coupling of electrons on individual lanthanide atoms in small clusters is not well understood. The major objective of this work is to probe such coupling of the praseodymium (Pr) 4f and 6s electrons in Pr 2 O 2 and Pr 2 O 2 +. The approach combines mass-analyzed threshold ionization spectroscopy and spin–orbit multiconfiguration second-order quasi-degenerate perturbation theory. The energies of six ionization transitions are precisely measured; the adiabatic ionization energy of the neutral cluster is 38 045 (5) cm –1 . Most of the electronic states involved in these transitions are identified as spin–orbit coupled states consisting of two or more electron spins. The electron configurations of these states are 4f 4 6s 2 for the neutral cluster and 4 f 46 s for the singly charged cation, both in planar rhombus-type structures. Finally, the spin–orbit splitting due to the coupling of the electrons on the separate Pr atoms is on the order of hundreds of wavenumbers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Nanocluster ionization energies and work function of aluminum, and their temperature dependence

Ionization threshold energies of Al{sub n} (n = 32-95) nanoclusters are determined by laser ionization of free neutral metal clusters thermalized to several temperatures in the range from 65 K to 230 K. The photoion yield curves of cold clusters follow a quadratic energy dependence above threshold, in agreement with the Fowler law of surface photoemission. Accurate data collection and analysis procedures make it possible to resolve very small (few parts in a thousand) temperature-induced shifts in the ionization energies. Extrapolation of the data to the bulk limit enables a determination of the thermal shift of the polycrystalline metal work function, found to be in excellent agreement with theoretical prediction based on the influence of thermal expansion. Small clusters display somewhat larger thermal shifts, reflecting their greater susceptibility to thermal expansion. Ionization studies of free size-resolved nanoclusters facilitate understanding of the interplay of surface, electronic, and lattice properties under contamination-free conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Alignment Thresholds of Molecules

Molecules have long been known to align in moderately intense, far off-resonance laser fields with a large variety of applications in physics and optics. Here, we illustrate and describe the physical origin of a previously unexplored phenomenon in the adiabatic alignment dynamics of molecules, which is fundamentally interesting and also has an important practical implication. Specifically, the intensity dependence of the degree of adiabatic alignment exhibits a threshold behavior, below which molecules are isotropically distributed rotationally and above which the alignment rapidly reaches a plateau. Furthermore, we show that both the intensity and the temperature dependencies of the alignment of all linear molecules exhibit universal curves and derive analytical forms to describe these dependencies. Finally, we illustrate that the alignment threshold occurs very generally at a lower intensity than the off-resonance ionization threshold, a numerical observation that is readily illustrated analytically. The threshold behavior is attributed to a tunneling mechanism that rapidly switches off at the threshold intensity, where tunneling between the potential wells corresponding to the two orientations of the aligned molecules becomes impossible. The universal threshold behavior of molecular alignment is a simple phenomenon, but one that was not realized before and can be readily tested experimentally.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Influences of the propyl group on the van der Waals structures of 4-propylaniline complexes with one and two argon atoms studied by electronic and cationic spectroscopy

4-propylaniline complexes with one and two argon atoms formed in the molecular beam were studied in the first excited electronic state, S{sub 1}, using resonance enhanced two-photon ionization spectroscopy and in the cation ground state, D{sub 0}, using mass analyzed threshold ionization spectroscopy. The combination of electronic and cationic spectra of the clusters allows two conformations to be identified in both aniline-Ar{sub 1} and aniline-Ar{sub 2}, which are assigned to either the gauche configuration or anti-configuration of 4-propylaniline. The gauche isomer exhibits complex bands shifted 29 cm{sup −1} and 89 cm{sup −1} from the S{sub 1} origin bands and 83 cm{sup −1} and 148 cm{sup −1} from the ionization potential assigned to the Ar{sub 1} and Ar{sub 2} complexes, respectively. For the anti-rotamer, the corresponding shifts actually become nearly additive, 53 cm{sup −1} and 109 cm{sup −1} for the S{sub 1} origin bands, and 61 cm{sup −1} and 125 cm{sup −1} for the ionization potentials. Ab initio calculations provide insights into the influences of the propyl and amino groups on the positions of the argon atoms within the clusters. In addition, the binding energy of one argon with the gauche isomer of 4-propylaniline has been measured to be 550 ± 5 cm{sup −1} in the D{sub 0} state, 496 ± 5 cm{sup −1} in the S{sub 1} state, and 467 ± 5 cm{sup −1} in the neutral ground state, S{sub 0}.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Search for lightly ionizing particles in superCDMS and simulation of neutron backgrounds

The Super Cryogenic Dark Matter Search (SuperCDMS) is a direct-detection dark matter search experiment that primarily aims to search for Weakly Interacting Massive Particles (WIMPs) using state-of-the-art solid-state detection technology. During its operation at the Soudan underground laboratory, germanium detectors were operated with high bias voltage mode known as the CDMS low ionization threshold experiment (CDMSlite) to achieve below-keV thresholds. CDMSlite, for being able to measure small energy depositions in detectors, also provides sensitivity to Lightly Ionizing Particles (LIPs) with very small fractional charges. This thesis will discuss an analysis to search LIPs with the data acquired in CDMSlite mode. An important component for LIPs search is the expected energy-deposition distributions for LIPs falling on the CDMSlite detector. In this thesis, a simulation framework to calculate the energy-deposition distributions is developed. This thesis presents first direct-detection limits on the intensity of cosmogenic LIPs with electric charges smaller than e/(3 × 105) as well as the strongest limits for charges ≤ e/160, with a minimum intensity of 1.36 × 10-7 cm-2s-1sr-1 at charge e/160.In any rare-event search experiment, understanding background is crucial. Neutrons capable of mimicking dark matter signals are a major background for any dark matter search experiment. A simulationmore » study to estimate the neutron background for an India based dark matter search experiment at Jaduguda Underground Science Laboratory (JUSL) is performed. The experiment at JUSL will be the first phase of a proposed Dark matter search at India-based Neutrino Observatory (DINO). It will be a direct detection experiment with primary aims to search for WIMPs as dark matter candidates. In this thesis, we discuss the methodology of estimating neutron flux at JUSL and report the results. The total neutron flux reaching the laboratory above 1 MeV energy threshold is found to be 5.76(±0.69) × 10-6 cm-2s-1. The impact of neutron background on the sensitivity of the experiment to detect dark matter at JUSL is also discussed. The thesis is organized as follows. Chapter 1 provides a brief introduction to the Lightly Ionizing Particle (LIPs). The analysis to search LIPs in SuperCDMS is briefly outlined in the chapter. This chapter also discusses the importance of neutron background estimates in a dark matter search experiment, more specifically, in the context of a proposed India-based dark matter search experiment at Jaduguda Underground Science Laboratory. In Chapter 2, the SuperCDMS experiment is introduced. In Chapter 3, the framework developed to perform simulations for Lightly Ionizing Particles is presented. In Chapter 4, the LIPs search analysis with the CDMSlite data and the results are discussed. In Chapter 5, the simulation of neutron background and the feasibility of dark-matter search at JUSL is discussed. Finally, conclusions from all the results discussed in this thesis are presented in Chapter 6.« less

Banik, Samir↗
DOE OSTI2021

Search for Lightly Ionizing Particles in SuperCDMS and simulation of neutron backgrounds

The Super Cryogenic Dark Matter Search (SuperCDMS) is a direct-detection dark matter search experiment that primarily aims to search for Weakly Interacting Massive Particles (WIMPs) using state-of-the-art solid-state detection technology. During its operation at the Soudan underground laboratory, germanium detectors were operated with high bias voltage mode known as the CDMS low ionization threshold experiment (CDMSlite) to achieve below-keV thresholds. CDMSlite, for being able to measure small energy depositions in detectors, also provides sensitivity to Lightly Ionizing Particles (LIPs) with very small fractional charges. This thesis will discuss an analysis to search LIPs with the data acquired in CDMSlite mode. An important component for LIPs search is the expected energy-deposition distributions for LIPs falling on the CDMSlite detector. In this thesis, a simulation framework to calculate the energy-deposition distributions is developed. This thesis presents first direct-detection limits on the intensity of cosmogenic LIPs with electric charges smaller than e /(3 × 10 5 ) as well as the strongest limits for charges ≤ e /160, with a minimum intensity of 1.36 × 10 -7 cm -2 s -1 sr -1 at charge e /160.In any rare-event search experiment, understanding background is crucial. Neutrons capable of mimicking dark matter signals are a major background for any dark matter search experiment. A simulation study to estimate the neutron background for an India based dark matter search experiment at Jaduguda Underground Science Laboratory (JUSL) is performed. The experiment at JUSL will be the first phase of a proposed Dark matter search at India-based Neutrino Observatory (DINO). It will be a direct detection experiment with primary aims to search for WIMPs as dark matter candidates. In this thesis, we discuss the methodology of estimating neutron flux at JUSL and report the results. The total neutron flux reaching the laboratory above 1 MeV energy threshold is found to be 5.76(±0.69) × 10 -6 cm -2 s -1 . The impact of neutron background on the sensitivity of the experiment to detect dark matter at JUSL is also discussed. The thesis is organized as follows. Chapter 1 provides a brief introduction to the Lightly Ionizing Particle (LIPs). The analysis to search LIPs in SuperCDMS is briefly outlined in the chapter. This chapter also discusses the importance of neutron background estimates in a dark matter search experiment, more specifically, in the context of a proposed India-based dark matter search experiment at Jaduguda Underground Science Laboratory. In Chapter 2, the SuperCDMS experiment is introduced. In Chapter 3, the framework developed to perform simulations for Lightly Ionizing Particles is presented. In Chapter 4, the LIPs search analysis with the CDMSlite data and the results are discussed. In Chapter 5, the simulation of neutron background and the feasibility of dark-matter search at JUSL is discussed. Finally, conclusions from all the results discussed in this thesis are presented in Chapter 6.

Banik, Samir↗
DOE OSTI2024

Ultrafast dynamics of fluorene initiated by highly intense laser fields

Here, we present an investigation of the ultrafast dynamics of the polycyclic aromatic hydrocarbon fluorene initiated by an intense femtosecond near-infrared laser pulse (810 nm) and probed by a weak visible pulse (405 nm). Using a multichannel detection scheme (mass spectra, electron and ion velocity-map imaging), we provide a full disentanglement of the complex dynamics of the vibronically excited parent molecule, its excited ionic states, and fragments. We observed various channels resulting from the strong-field ionization regime. In particular, we observed the formation of the unstable tetracation of fluorene, above-threshold ionization features in the photoelectron spectra, and evidence of ubiquitous secondary fragmentation. We produced a global fit of all observed time-dependent photoelectron and photoion channels. This global fit includes four parent ions extracted from the mass spectra, 15 kinetic-energy-resolved ionic fragments extracted from ion velocity map imaging, and five photoelectron channels obtained from electron velocity map imaging. The fit allowed for the extraction of 60 lifetimes of various metastable photoinduced intermediates.

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

Low-Mass Dark Matter Search Results and Radiogenic Backgrounds for the Cryogenic Dark Matter Search

An ever-increasing amount of evidence suggests that approximately one quarter of the energy in the universe is composed of some non-luminous, and hitherto unknown, “dark matter”. Physicists from numerous sub-fields have been working on and trying to solve the dark matter problem for decades. The common solution is the existence of some new type of elementary particle with particular focus on weakly interacting massive particles (WIMPs). One avenue of dark matter research is to create an extremely sensitive particle detector with the goal of directly observing the interaction of WIMPs with standard matter. The Cryogenic Dark Matter Search (CDMS) project operated at the Soudan Underground Laboratory from 2003–2015, under the CDMS II and SuperCDMS Soudan experiments, with this goal of directly detecting dark matter. The next installation, SuperCDMS SNOLAB, is planned for near-future operation. The reason the dark-matter particle has not yet been observed in traditional particle physics experiments is that it must have very small cross sections, thus making such interactions extremely rare. In order to identify these rare events in the presence of a background of known particles and interactions, direct detection experiments employ various types and amounts of shielding to prevent known backgrounds from reaching the instrumented detector(s). CDMS utilized various gamma and neutron shielding to such an effect that the shielding, and other experimental components, themselves were sources of background. These radiogenic backgrounds must be understood to have confidence in any WIMP-search result. For this dissertation, radiogenic background studies and estimates were performed for various analyses covering CDMS II, SuperCDMS Soudan, and SuperCDMS SNOLAB. Lower-mass dark matter t c2 inent in the past few years. The CDMS detectors can be operated in an alternative, higher-biased, mode v to decrease their energy thresholds and correspondingly increase their sensitivity to low-mass WIMPs. This is the CDMS low ionization threshold experiment (CDMSlite), which has pushed the frontier at lower WIMP masses. This dissertation describes the second run of CDMSlite at Soudan: its hardware, operations, analysis, and results. The results include new WIMP mass-cross section upper limits on the spin-independent and spin-dependent WIMP-nucleon interactions. Thanks to the lower background and threshold in this run compared to the first CDMSlite run, these limits are the most sensitive in the world below WIMP masses of ⇠4 GeV/c2. This demonstrates also the great promise and utility of the high-voltage operating mode in the SuperCDMS SNOLAB experiment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Discrepancies between Theory and Experiment in Determining the Ionization Energy of NF 3

High-accuracy ab initio thermochemical predictions for the ionization energy of NF 3 , the barrier height (to inversion) of NF 3 + , and the dissociative ionization threshold of NF 3 to NF 2 + + F are presented and incorporated into Active Thermochemical Tables. The adiabatic ionization energy of the first ionization band of NF 3 , calculated at 12.647 ± 0.010 eV, is at odds with previous experimental interpretations by nearly 0.36 eV due to unfavorable Franck-Condon factors associated with this transition. The barrier (to inversion) height is calculated to be about 0.6 eV lower in energy than the prior interpretation, which instigates a discussion of the supposed vibrational structure of the first ionization band of NF 3 . Updated assignments of the photoelectron spectrum are proposed, and the loss in vibrational spacing on the high-energy side of the experimental ionization band is discussed. Rudimentary anharmonic Franck-Condon simulations qualitatively reproduce the broad spectral features observed in experiment.

Active Thermochemical Tables↗
DOE OSTI2019

Isomer-Selective Detection of Keto-Hydroperoxides in the Low-Temperature Oxidation of Tetrahydrofuran

Keto-hydroperoxides (KHPs) are reactive, partially oxidized intermediates that play a central role in chain-branching reactions during the gas-phase low-temperature oxidation of hydrocarbons and oxygenated species. Although multiple isomeric forms of the KHP intermediate are possible in complex oxidation environments when multiple reactant radicals exist that contain nonequivalent O 2 addition sites, isomer-resolved data of KHPs have not been reported. In this work, we provide partially isomer-resolved detection and quantification of the KHPs that form during the low-temperature oxidation of tetrahydrofuran (THF, cycl. -O–CH 2 CH 2 CH 2 CH 2 –). We describe how these short-lived KHPs were detected, identified, and quantified using integrated experimental and theoretical approaches. The experimental approaches were based on direct molecular-beam sampling from a jet-stirred reactor operated at near-atmospheric pressure and at temperatures between 500 and 700 K, followed by mass spectrometry with single-photon ionization via tunable synchrotron-generated vacuum-ultraviolet radiation, and the identification of fragmentation patterns. The interpretation of the experiments was guided by theoretical calculations of ionization thresholds, fragment appearance energies, and photoionization cross sections. On the basis of the experimentally observed and theoretically calculated ionization and fragment appearance energies, KHP isomers could be distinguished as originating from H-abstraction reactions from either the α-C adjacent to the O atom or the β-C atoms. Temperature-dependent concentration profiles of the partially resolved isomeric KHP intermediates were determined in the range of 500–700 K, and the results indicate that the observed KHP isomers are formed overwhelmingly (~99%) from the α-C THF radical. Furthermore, the comparisons of the partially isomer-resolved quantification of the KHPs to up-to-date kinetic modeling results reveal new opportunities for the development of a next-generation THF oxidation mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Probing multirescattering dynamics and electron quantum paths for below- and near-threshold harmonic generation of H 2 in an intense laser field

Most previous studies of high-order-harmonic generation have focused on the regime beyond the ionization threshold; the dynamical origin of below- and near-threshold harmonics, particularly for the molecular systems, is less understood and largely unexplored. Here, we report a self-interaction free time-dependent density-functional-theory study along with an extended semiclassical study for the nonperturbative probing of the dynamical origin of below- and near-threshold harmonic generation of the H 2 molecule in an intense near-infrared laser field. Our approach allows an accurate study of the electron trajectories as a function of energy, time, and position for below-, near-, and above-threshold harmonics for electrons departing initially from each of the individual hydrogen cores of the H 2 molecule. We discover that short trajectories are multiphoton dominated and can have multiple returns for below-threshold harmonics, and excited-state resonances can have significant effects on the generation of neighboring below-threshold harmonics. Furthermore, we find that the electron dynamics for below-threshold long, short, and resonant trajectories differ greatly depending upon which hydrogen core (left or right) the electron was released from initially. An intuitive and appealing picture of near- and below-threshold harmonic generation discovered in our study can give guidance to future experiments in this forefront area of ultrafast atomic, molecular, and optical physics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Interference patterns from post-collision interaction in below-threshold photoexcitation Auger processes

In this work, we focus on the post-collision interaction in Auger processes where the photoelectron energy is near or below the ionization threshold. Time-dependent quantum and classical calculations are performed. When the photoelectron is more deeply bound, interference patterns can be seen in the angular and photoelectron energy distributions. These interference patterns are visible in quantum calculations, but not in purely classical calculations. A semiclassical analysis using actions from two-path trajectories gives the relative locations of the interference maxima very close to those from the full quantum calculations.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2013

Multicomponent dynamics of coupled quantum subspaces and field-induced molecular ionizations

To describe successive ionization steps of a many-electron atom or molecule driven by an ultrashort, intense laser pulse, we introduce a hierarchy of successive two-subspace Feshbach partitions of the N-electron Hilbert space, and solve the partitioned time-dependent Schrödinger equation by a short-time unitary algorithm. The partitioning scheme allows one to use different level of theory to treat the many-electron dynamics in different subspaces. We illustrate the procedure on a simple two-active-electron model molecular system subjected to a few-cycle extreme Ultra-Violet (XUV) pulse to study channel-resolved photoelectron spectra as a function of the pulse's central frequency and duration. We observe how the momentum and kinetic-energy distributions of photoelectrons accompanying the formation of the molecular cation in a given electronic state (channel) change as the XUV few-cycle pulse's width is varied, from a form characteristic of an impulsive ionization regime, corresponding to the limit of a delta-function pulse, to a form characteristic of multiphoton above-threshold ionization, often associated with continuous-wave infinitely long pulse.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Electron impact ionization of cycloalkanes, aldehydes, and ketones

The theoretical calculations of electron impact total ionization cross section for cycloalkane, aldehyde, and ketone group molecules are undertaken from ionization threshold to 2 keV. The present calculations are based on the spherical complex optical potential formalism and complex scattering potential ionization contribution method. The results of most of the targets studied compare fairly well with the recent measurements, wherever available and the cross sections for many targets are predicted for the first time. The correlation between the peak of ionization cross sections with number of target electrons and target parameters is also reported. It was found that the cross sections at their maximum depend linearly with the number of target electrons and with other target parameters, confirming the consistency of the values reported here.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Constraints on Lightly Ionizing Particles from CDMSlite

The Cryogenic Dark Matter Search low ionization threshold experiment (CDMSlite) achieved effcient detection of very small recoil energies in its germanium target, resulting in sensitivity to Lightly Ionizing Particles (LIPs) in a previously unexplored region of charge, mass, and velocity parameter space. We report first direct-detection limits on the vertical intensity of cosmogenically-produced LIPs with an electric charge smaller than e/(3x10^5), as well as the strongest limits for charge <= e/160, with a minimum vertical intensity of 1.36 x 10^-7 cm^-2s^-1sr^-1 at charge e/160. These results apply over a wide range of LIP masses (5 MeV/c^2 to 100 TeV/c^2) and cover a wide range of beta-gamma values (0.1--10^6), thus excluding non-relativistic LIPs with beta-gamma as small as 0.1 for the first time.

Alkhatib, I↗
DOE OSTI2019

Tracing intermolecular Coulombic decay of carbon-dioxide dimers and oxygen dimers after valence photoionization

In this study, we have conducted an experimental study on the photo double ionization (PDI) of carbon-dioxide dimers at photon energies of 37 and 55 eV and oxygen dimers at photon energies of 38, 41.5, and 46 eV, while focusing on the dissociation dynamics upon single-photon absorption. The investigation was performed by applying the cold-target recoil-ion momentum spectroscopy method in order to collect and record the three-dimensional momenta of the ionic fragments and emitted electrons from the dissociating dimer in coincidence. The kinetic-energy release upon fragmentation and the electron angular distributions in the laboratory and body-fixed frames, as well as the relative electron-electron emission angle, show unambiguous experimental evidence of intermolecular Coulombic decay (ICD) in carbon-dioxide dimers upon photoionization below and above the double-ionization threshold of CO 2 monomers. The PDI of oxygen dimers is less conclusive and shows contributions from ICD and knock-off ionization mechanisms. As for atomic dimers, the present results reveal that ICD in CO 2 dimers after valence PDI can also serve as a source for low-energy electrons, known to be very relevant in biological systems, cells, and tissues.

74 ATOMIC AND MOLECULAR PHYSICS↗