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At least 487 records · Page 27

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DOE OSTI2026

Analysis of an irradiated uranium sample for source attribution without chemical separation using microplasma ionization and ultrahigh resolution mass spectrometry

The use of element isotope ratios has great potential in not only determining the reactor type used to produce plutonium (Pu) but also in determining the burnup and the time since irradiation. While a powerful nuclear forensic technique, determining element isotope ratios is complicated by severe isobaric interferences when performed on typical inductively coupled plasma mass spectrometers. Such analyses require extensive chemical separations prior to analysis to alleviate the inter-elemental isobars. Ultrahigh mass resolution spectrometry provides a potential alternative, greatly reducing the complexity of sample preparation and turnaround times for these critical measurements. To demonstrate the power of the approach, a sample of irradiated, depleted uranium was analyzed with the liquid sampling—atmospheric pressure glow discharge ion source coupled to an Orbitrap mass spectrometer. The Orbitrap is augmented with an external data acquisition system, Spectroswiss’s FTMS-Booster X2T, allowing collection of extended ion transients, providing higher mass resolution. In using this approach, the 150 Sm/ 149 Sm and 152 Sm/ 149 Sm isotope ratios were found to be within 20% of predicted values without any chemical separations and without mass bias corrections. In addition, the 240 Pu/ 239 Pu isotope ratio was determined, free from the 238 UH + interferences common to the ICP-MS platforms, while at the same time allowing for the determination of U isotopic signatures. While these demonstrative results are from a single sample, the advantages of the microplasma/ultrahigh mass resolution approach to intra-element isotope ratio determinations are clear.

Fuel burnup↗

NASA NTRS1978

Quantum mechanical theory of collisional ionization in the presence of intense laser radiation

The paper presents a quantum mechanical formalism for treating ionizing collisions occurring in the presence of an intense laser field. Both the intense laser radiation and the internal electronic continuum states associated with the emitted electrons are rigorously taken into account by combining discretization techniques with expansions in terms of electronic-field representations for the quasi-molecule-plus-photon system. The procedure leads to a coupled-channel description of the heavy-particle dynamics which involves effective electronic-field potential surfaces and continua. It is suggested that laser-influenced ionizing collisions can be studied to verify the effects of intense laser radiation on inelastic collisional processes. Calculation procedures for electronic transition dipole matrix elements between discrete and continuum electronic states are outlined.

Bellum, J. C.↗

DOE OSTI2025

Versatile system for ion energy measurements generated by pulsed laser ionization: Insights into electron-ion dynamics

Ion energy distributions generated by pulsed laser interactions with materials are essential for applications ranging from materials science to oncology. Ion energy characterization is particularly important for an emerging mass spectrometry technique called virtual-slit cycloidal mass spectrometry (VS-CMS). The ion energy distribution influences the design and performance of VS-CMS instruments, as well as the efficacy of laser-driven ionization methods in various fields. Several established techniques, including the retarding potential method, time-of-flight (TOF) analysis, and electrostatic energy analyzers, have been employed to measure ion energy distributions. The wide range of ion energies reported highlights the strong dependence of ion energy on laser parameters, target materials, and experimental conditions, as well as the necessity of making independent measurements of the ion energy distribution for specific laser systems and materials. This paper presents the design and characterization of a simple TOF-based apparatus for measuring ion energy distributions from pulsed laser ionization without external fields. This approach minimizes perturbation of electron-ion dynamics and enables simultaneous energy measurements at multiple spatial positions. Here, the apparatus was tested using a nanosecond pulsed Nd:YAG laser operating at 1064 nm, 532 nm, and 266 nm on solid copper sheets at various laser fluences. Simultaneous measurements at different distances provide new insights into ion-electron interactions post-ionization and demonstrate the influence of laser wavelength and fluence on ion energy distributions.

Ion energy↗

NASA NTRS1995

High-resolution measurements of the K-alpha spectra of low-ionizationm species of iron: A new spectral signature of nonequilibrium ionization conditions in young supernova remnants

We present the first systematic laboratory measurements of high-resolution K-alpha spectra of intermediate ions of iron, Fe X-XVII. These lines are not produced in collisional equilibrium plasmas because of the relevant charge states cannot exist at the high electron temperatures required for appreciable excitation of the K-alpha transitions. However, they can provide excellent spectral diagnostics for nonequilibrium ionization conditions, such the ionizing plasmas of young supernova remnants. To facilitate the line identifications, we compare our spectra with theoretical atomic calculations performed using multiconfiguration parametric potential and Dirac-Fock atomic codes. Our measurements also allow direct comparison with time-dependent ionization balance calculations for ionizing plasmas, and good agreement is found.

Decaux, V.↗

DOE OSTI2021

Stability and pulsation of the first dark stars

ABSTRACT The first bright objects to form in the Universe might not have been ‘ordinary’ fusion-powered stars, but ‘dark stars’ (DSs) powered by the annihilation of dark matter (DM) in the form of weakly interacting massive particles (WIMPs). If discovered, DSs can provide a unique laboratory to test DM models. DSs are born with a mass of the order of M⊙ and may grow to a few million solar masses; in this work we investigate the properties of early DSs with masses up to $\sim \! 1000 \, \mathrm{ M}_\odot$, fueled by WIMPS weighing 100 GeV. We improve the previous implementation of the DM energy source into the stellar evolution code mesa. We show that the growth of DSs is not limited by astrophysical effects: DSs up to $\sim \!1000 \, \mathrm{ M}_{\odot }$ exhibit no dynamical instabilities; DSs are not subject to mass-loss driven by super-Eddington winds. We test the assumption of previous work that the injected energy per WIMP annihilation is constant throughout the star; relaxing this assumption does not change the properties of the DSs. Furthermore, we study DS pulsations, for the first time investigating non-adiabatic pulsation modes, using the linear pulsation code gyre. We find that acoustic modes in DSs of masses smaller than $\sim \! 200 \, \mathrm{ M}_\odot$ are excited by the κ − γ and γ mechanism in layers where hydrogen or helium is (partially) ionized. Moreover, we show that the mass-loss rates potentially induced by pulsations are negligible compared to the accretion rates.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Inactivation of Fluorescent Lipid Bilayers by Irradiation With 300 keV Electrons Using Liquid Cell Transmission Electron Microscopy

Liquid cell transmission electron microscopy allows for imaging of samples in a fully hydrated state at high resolution and has the potential for visualizing static or dynamic biological structures. However, the ionizing nature of the electron beam makes it difficult to discern real physiological dynamics from radiation induced artifacts within liquid cell samples. Electron flux thresholds for achieving high resolution structures from biological samples frozen in ice have been described extensively by the cryo-electron microscopy field, while electron flux thresholds which do not result in a functional change for biological samples within the hydrated environment of a transmission electron microscope liquid cell is less clear. Establishing these functional thresholds for biologically relevant samples is important for accurate interpretation of results from liquid cell experiments. Here we demonstrate the electron damage threshold of fluorescently tagged lipid bilayers by quantifying the change in fluorescence before and after electron exposure. We observe the reduction of fluorescent signal in bilayers by 25% after only 0.0005 e − /Å 2 and a reduction of over 90% after 0.01 e − /Å 2 . These results indicate that the loss of function occurs at irradiation thresholds far below a typical single high resolution (scanning) transmission electron microscopy image and orders of magnitude below fluxes used for preserving structural features with cryo-electron microscopy.

Moser, Trevor↗

NASA NTRS1977

Thermodynamics of Thomas-Fermi screened Coulomb systems

We obtain in closed analytic form, estimates for the thermodynamic properties of classical fluids with pair potentials of Yukawa type, with special reference to dense fully ionized plasmas with Thomas-Fermi or Debye-Hueckel screening. We further generalize the hard-sphere perturbative approach used for similarly screened two-component mixtures, and demonstrate phase separation in this simple model of a liquid mixture of metallic helium and hydrogen.

Firey, B.↗

NASA NTRS1992

Nitrogen escape from Mars

The mass spectrometer on the Viking spacecraft measured anomalous N-15:N-14 ratio of about 1.62 times the terrestrial value. This enhancement presumably results from differential escape of N-15. The escape of N is non-thermal and potential escape mechanisms include photodissociation, photoionization, and electron impact dissociative ionization of N2, and ion-molecule reactions and dissociative recombination of N2(+). The authors propose some calculations to explain the N ratio, but even with all escape mechanisms considered, the ratios don't balance. This leads to the assumption that some other escape mechanisms must exist that are unexplained.

Fox, J. L.↗

NASA NTRS2004

Evolutionary Models of Cold, Magnetized, Interstellar Clouds

We modeled the long-term and small-scale evolution of molecular clouds using direct 2D and 3D magnetohydrodynamic (MHD) simulations. This work followed up on previous research by our group under auspices of the ATP in which we studied the energetics of turbulent, magnetized clouds and their internal structure on intermediate scales. Our new work focused on both global and smallscale aspects of the evolution of turbulent, magnetized clouds, and in particular studied the response of turbulent proto-cloud material to passage through the Galactic spiral potential, and the dynamical collapse of turbulent, magnetized (supercritical) clouds into fragments to initiate the formation of a stellar cluster. Technical advances under this program include developing an adaptive-mesh MHD code as a successor to ZEUS (ATHENA) in order to follow cloud fragmentation, developing a shearing-sheet MHD code which includes self-gravity and externally-imposed gravity to follow the evolution of clouds in the Galactic potential, and developing radiative transfer models to evaluate the internal ionization of clumpy clouds exposed to external photoionizing UV and CR radiation. Gammie's work at UIUC focused on the radiative transfer aspects of this program.

Gammie, Charles F.↗

NASA NTRS2004

Immunofluorescent Detection of DNA Double Strand Breaks induced by High-LET Radiation

Within cell nuclei, traversing charged heavy ion particles lead to the accumulation of proteins related to DNA lesions and repair along the ion trajectories. Irradiation using a standard geometric setup with the beam path perpendicular to the cell monolayer generates discrete foci of several proteins known to localize at sites of DNA double strand breaks (DSBs). One such molecule is the histone protein H2AX (gamma-H2AX), which gets rapidly phosphorylated in response to ionizing radiation. Here we present data obtained with a modified irradiation geometry characterized by a beam path parallel to a monolayer of human fibroblast cells. This new irradiation geometry leads to the formation of gamma-H2AX aggregates in the shape of streaks stretching over several micrometers in the x/y plane, thus enabling the analysis of the fluorescence distributions along the particle trajectories. Qualitative analysis of these distributions presented insights into the DNA repair kinetics along the primary track structure and visualization of possible chromatin movement. We also present evidence of colocalization of gamma-H2AX with several other proteins in responses to ionizing radiation exposure. Analysis of gamma-H2AX has the potential to provide useful information on human cell responses to high LET radiation after exposure to space-like radiation.

Cucinotta, Francis A.↗

DOE OSTI2024

Rapid 235 U/ 238 U determination by matrix assisted ionization–time-of-flight mass spectrometry

Matrix-assisted ionization (MAI) of inorganic analytes is a nascent research domain that holds promise for rapid, potentially facility-deployable analytical applications. Here, we present results of MAI uranium isotopic analysis ( 235 U/ 238 U) obtained on the timescale of minutes utilizing simple sample preparation and an ambient ionization time-of-flight mass spectrometer (ToF MS). Experimental MAI-ToF MS characterization of uranium Certified Reference Materials (CRMs) was used to establish method calibration and validate quantitative 235 U/ 238 U determination spanning depleted, natural, and low-enriched uranium isotopic compositions. Secondary standard analyses with total uranium mass loadings of 5–500 ng per analysis yield accurate calibrated 235 U/ 238 U results and relative uncertainties of 4.7–17.2% (approx. ±95% confidence level), with weighted-mean uncertainties approaching 1.5%. This method permits accurate determination of uranium isotopic composition in a sample with uranium content as low as 200 pg for equal atom 235 U: 238 U. Instrument detection limits constrain the minimum uranium mass required to identify the presence of highly enriched uranium (HEU ≥20% 235 U) as only 500 pg using the method presented here. MAI-ToF MS quantitation of relatively extreme isotope ratios ( 235 U/ 238 U ≤ 0.01) is limited by detection of minor 235 U (LoD 100 pg 235 U/analysis ≈ 10 ng total U/analysis), and subsequent method optimization is anticipated to further reduce these limits. These findings underscore the potential of MAI-ToF MS for isotopic characterization of uranium and other inorganic species for both basic and applied science.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH 3 I probed by coincident ion momentum imaging

The UV-induced photodissociation dynamics of iodomethane (CH 3 I) in its A-band are investigated by time-resolved coincident ion momentum imaging using strong-field ionization as a probe. The delay-dependent kinetic energy distribution of the photofragments resulting from double ionization of the molecule maps the cleavage of the carbon–iodine bond and shows how the existence of a potential well in the di-cationic potential energy surfaces shapes the observed distribution at small pump–probe delays. Furthermore, the competition between single- and multi-photon excitation and ionization of the molecule is studied as a function of the intensity of the UV-pump laser pulse. Two-photon excitation to Rydberg states is identified by tracking the transformation of the delay-dependent singly-charged iodomethane yield from a pure Gaussian distribution at low intensity to a Gaussian with an exponentially decaying tail at higher intensities. In conclusion, dissociative ionization induced by absorption of three UV photons is resolved as an additional delay-dependent feature in the kinetic energy of the fragment ions detected in coincidence.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2004

High Power Light Gas Helicon Plasma Source For VASMIR

The VASIMR space propulsion development effort relies on a high power (greater than 10kW) helicon source to produce a dense flowing plasma (H, D and He) target for ion cyclotron resonance (ICR) acceleration of the ions. Subsequent expansion in an expanding magnetic field (magnetic nozzle) converts ion lunetic energy to directed momentum. This plasma source must have critical features to enable an effective propulsion device. First, it must ionize most of the input neutral flux of gas, thus producing a plasma stream with a high degree of ionization for application of ICR power. This avoids propellant waste and potential power losses due to charge exchange. Next, the plasma stream must flow into a region of high magnetic field (approximately 0.5 T) for efficient ICR acceleration. Third, the ratio of input power to plasma flux must be low, providing an energy per ion-electron pair approaching 100 eV. Lastly, the source must be robust and capable of very long life-times (years). In our helicon experiment (VX-10) we have measured a ratio of input gas to plasma flux near 100%. The plasma flows from the helicon region (B approximately 0.1 T) into a region with a peak magnetic field of 0.8 T. The energy input per ion-electron pair has been measured at 300 plus or minus 100 eV. Recent results at Oak Ridge National Laboratory (ORNL) show an enhanced efficiency mode of operation with a high power density, over 5 kW in a 5 cm diameter tube. Our helicon is presently 9 cm in diameter and operates up to 3.5 kW of input power. An upgrade to a power level of 10 kW is underway. Much of our recent work has been with a Boswell double-saddle antenna design. We are also converting the antenna design to a helical type. With these modifications, we anticipate an improvement in the ionization efficiency. This paper presents the results from scaling the helicon in the VX-10 device from 3.5 to 10 kW. We also compare the operation with a double-saddle to a helical antenna design. Finally, we discuss modeling of these configurations using ORNL's EMIR code.

Squire, J. P.↗

DOE OSTI2023

Ab initio calculation of carrier mobility in semiconductors including ionized-impurity scattering

The past decade has seen the emergence of ab initio computational methods for calculating phonon-limited carrier mobilities in semiconductors with predictive accuracy. More realistic calculations ought to take into account additional scattering mechanisms such as, for example, impurity and grain-boundary scattering. Here, in this paper, we investigate the effect of ionized-impurity scattering on the carrier mobility. We model the analytical impurity potential parameterized from first principles by a collection of randomly distributed Coulomb scattering centers, and we include this relaxation channel into the ab initio Boltzmann transport equation, as implemented in the EPW code. We demonstrate this methodology by considering silicon, silicon carbide, and gallium phosphide, for which detailed experimental data are available. Our calculations agree well with experiments over a broad range of temperatures and impurity concentrations. For each compound investigated here, we compare the relative importance of electron-phonon scattering and ionized-impurity scattering, and we critically assess the reliability of Matthiessen's rule. We also show that an accurate description of dielectric screening and carrier effective masses can improve quantitative agreement with experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Thermodynamic behavior of correlated electron-hole fluids in van der Waals heterostructures

Abstract Coupled two-dimensional electron-hole bilayers provide a unique platform to study strongly correlated Bose-Fermi mixtures in condensed matter. Electrons and holes in spatially separated layers can bind to form interlayer excitons, composite Bosons expected to support high-temperature exciton condensates. The interlayer excitons can also interact strongly with excess charge carriers when electron and hole densities are unequal. Here, we use optical spectroscopy to quantitatively probe the local thermodynamic properties of strongly correlated electron-hole fluids in MoSe 2 /hBN/WSe 2 heterostructures. We observe a discontinuity in the electron and hole chemical potentials at matched electron and hole densities, a definitive signature of an excitonic insulator ground state. The excitonic insulator is stable up to a Mott density of ~0.8 × 10 12 cm −2 and has a thermal ionization temperature of ~70 K. The density dependence of the electron, hole, and exciton chemical potentials reveals strong correlation effects across the phase diagram. Compared with a non-interacting uniform charge distribution, the correlation effects lead to significant attractive exciton-exciton and exciton-charge interactions in the electron-hole fluid. Our work highlights the unique quantum behavior that can emerge in strongly correlated electron-hole systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Dissociative electron attachment to 5-bromo-uracil: non-adiabatic dynamics on complex-valued potential energy surfaces

Electron induced dissociation reactions are relevant to many fields, ranging from prebiotic chemistry to cancer treatments. However, the simulation of dissociation electron attachment (DEA) dynamics is very challenging because the auto-ionization widths of the transient negative ions must be accounted for. We propose an adaptation of the ab initio multiple spawning (AIMS) method for complex-valued potential energy surfaces, along the lines of recent developments based on surface hopping dynamics. Our approach combines models for the energy dependence of the auto-ionization widths, obtained from scattering calculations, with survival probabilities computed for the trajectory basis functions employed in the AIMS dynamics. The method is applied to simulate the DEA dynamics of 5-bromouracil in full dimensionality, i.e., taking all the vibrational modes into consideration. The propagation starts on the $π_{2}^{*}$ resonance state and describes the formation of Br - anions mediated by non-adiabatic couplings. The potential energies, gradients and non-adiabatic couplings were computed with the fractional-occupancy molecular orbital complete-active-space configuration-interaction method, and the calculated DEA cross section are consistent with the observed DEA intensities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1980

Another look at aircraft-triggered lightning

There is positive evidence that a rapidly moving aircraft charged to high potentials by triboelectric processes can trigger lightning discharges by passage through freezing precipitation. The freezing zone in a nonstormy rain cloud is shown to be an electrically volatile region because of the potent charge exchange mechanisms which are active in agitated mixtures of supercooled water droplet and ice. Several intensifying effects are suggested which can be produced by the passage of an aircraft through this precipitation, resulting in a highly-ionized wake which acts like a trailing conductor. If weak charge centers are present in the cloud, the ionized wake acts to short out the gradient field resulting in very high potentials at the aircraft. The high potentials explain the electrical activity at the aircraft described by pilots, including intense corona, sparks and radio interference terminating in a loud discharge. Lightning strikes to naval aircraft towing gunnery targets at the end of long steel cables are described, showing that the same triggering mechanism may be involved in those cases. Recommendations are made to include triggering experiments in government flight programs now in progress.

Clifford, D. W.↗

DOE OSTI2020

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↗