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At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
NASA NTRS1961

Concerning Certain Collisionless Plasma-Shock Wave Models

A shock-wave model proposed by both Kahn and Parker for the collision of two interstellar gas clouds or of the solar wind with the ionized gas around the earth is re-evaluated in the light of recent developments in plasma stability theory. It is shown that the instability which was supposed to arrest the counter-streaming of the ions and to transfer much of their kinetic energy to the electrons does not occur in many important examples. Specifically, it is absent if the initial ion thermal energy exceeds 4.2 x 10 (sup -4) times their translational energy. While other plausible shock structures are known which yield supra-thermal electrons, they depend on magnetic fields, leaving no satisfactory theory in the limit of zero magnetic field.

Noerdlinger, Peter D.↗
NASA NTRS1993

Excitation cross sections for the ns 2S yields np 2P resonance transitions in Mg(+) (n = 3) and Zn(+) (n = 4) using electron-energy-loss and merged-beams methods

Electron-excitation cross sections are reported for the 3s 2S yields 3p 2P(h, k) resonance transition in Mg(+) at energies from threshold (4.43 eV) to approximately 9 times threshold (40.0 eV). The electron-energy-loss merged-beams technique used in these measurements is described in detail. In addition, the method of separating contributions of the elastically scattered (Coulomb) and the inelastically scattered electrons in the present Mg(+) case and previously reported Zn(+) results is described. Comparisons in the experimental energy range are made for Mg(+) with the two five-state close-coupling theoretical calculations carried out herein, and with other published close-coupling, distorted-wave, and semiempirical calculations. The present Mg(+) cross sections and Zn(+) cross sections from earlier measurements are tabulated.

Smith, Steven J.↗
NASA NTRS2004

Analysis of the Variation of Energetic Electron Flux with Respect to Longitude and Distance Normal to the Magnetic Equatorial Plane for Galileo Energetic Particle Detector Data

In this study we examine ten-minute omni-directional averages of energetic electron data measured by the Galileo spacecraft Energetic Particle Detector (EPD). Count rates from electron channels B1, DC2, and DC3 are evaluated using a power law model to yield estimates of the differential electron fluxes from 1 MeV to 11 MeV at distances between 8 and 51 Jupiter radii. Whereas the orbit of the Galileo spacecraft remained close to the rotational equatorial plane of Jupiter, the approximately 11 degree tilt of the magnetic axis of Jupiter relative to its rotational axis allowed the EPD instrument to sample high energy electrons at limited distances normal to the magnetic equatorial plane. We present a Fourier analysis of the semi-diurnal variation of electron fluxes with longitude.

synchrotron radiation↗
NASA NTRS1994

Comptonization of diffuse ambient radiation by a relativistic jet: The source of gamma rays from blazars?

Recent Energy Gamma Ray Experiment Telescope (EGRET) observations of blazars have revealed strong, variable gamma-ray fluxes with no signatures of gamma-ray absorption by pair production. This radiation probably originates from the inner parts of relativistic jets which are aimed nearly toward us. On sub-parsec scales, the jet will be pervaded by radiation from the broad-line region, as well as by photons from the central continuum source (some of which will be scattered by thermal plasma). In a frame moving with the relativistic outflow, the energy of this ambient radiation would be enhanced. This radiation would be Comptonized by both cold and relativistic electrons in the jet, yielding (in the observer's frame) a collimated beam of X-rays and gamma rays. On the assumption that this process dominates self-Comptonization of synchrotron radiation, we develop a self-consistent model for variable gamma-ray emission, involving a single population of relativistic electrons accelerated by a disturbance in the jet. The spectral break between the X-ray and gamma-ray band, observed in 3C 279 and deduced for other blazars, results from inefficient radiative cooling of lower energy electrons. The existence of such a break strongly favors a model involving Comptonization of an external radiation field over a synchrotron self-Compton model. We derive constraints on such model parameters as the location and speed of the source, its dimensions and internal physical parameters, the maximum photon energies produced in the source, and the density and distribution of ambient radiation. Finally, we discuss how observations might discriminate between our model and alternative ones invoking Comptonization of ambient radiation.

Sikora, Marek↗
DOE OSTI2021

Photosynthetic reaction center variants made via genetic code expansion show Tyr at M210 tunes the initial electron transfer mechanism

Significance Reaction centers (RCs) are critical to photosynthetic energy conversion. RCs in all characterized photosynthetic organisms contain two symmetrically arranged branches of chromophores and enable light-induced electron transfer with high yield. We fine-tune the properties of a key bacterial RC symmetry-breaking tyrosine via its replacement with noncanonical tyrosine analogs and determine kinetic outcomes. Results are interpreted through energetic characterization made possible by resonance Stark spectroscopy. Analysis indicates this tyrosine modulates the mechanism of the initial light-induced electron transfer, affording an alternative functional pathway that maintains the RC’s robust electron transfer. Modern molecular biology, ultrafast spectroscopy, crystallography, and energetic characterization enable the mechanistic model we describe. Our results deepen understanding of RC function and may have implications for other photocatalysts and enzymes.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Atomic-Layer-Deposited Aluminum Oxide Thin Films Probed with X-ray Scattering and Compared to Molecular Dynamics and Density Functional Theory Models

A better understanding of amorphous aluminum oxide’s structure and electronic properties is obtained through combined experimental and computational approaches. Grazing incidence X-ray scattering measurements were carried out on aluminum oxide thin films grown using thermal atomic layer deposition. The corresponding pair distribution functions (PDFs) showed structures similar to previously reported PDFs of solid-state amorphous alumina and molten alumina. Structural models based on crystalline alumina polymorphs (PDFgui) and amorphous alumina (molecular dynamics, MD) were examined for structural comparisons to the experimental PDF data. Smaller MD models were optimized and verified against larger models to allow for quantum chemical electronic structure calculations. The electronic structure of the amorphous alumina models yields additional insight into the band structure and electronic defects present in amorphous alumina that are not present in crystalline samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Ultrafast photochemistry of gas-phase transition metal carbonyls

Organometallic photochemistry lies at the heart of photochemical energy conversions in applications such as photocatalysis, photovoltaic cells, and luminescent materials. Thus, understanding how metal and ligand interactions in organometallic complexes modify electronic excited-state properties and reactivity has been the subject of intense studies for decades. Transition metal carbonyls [M n (CO) m ] have long served as prototypical organometallic complexes for understanding metal–ligand bonding and photochemistry and have been studied extensively in solution, matrices, and the gas phase on time scales ranging from femtoseconds to microseconds and longer. This review chronicles the past two and a half decades of efforts in understanding the ultrafast (sub-nanosecond) dynamics of transition metal carbonyls in the gas phase, where complicating solvent influences are absent and multiple experimental probes and high-level electronic structure theory can come together to yield rich information on the intricate interplay of electronic and structural dynamics. This review first lays the groundwork by briefly describing the electronic structure of transition metal carbonyls and introducing the various ultrafast techniques that have been applied to study their unimolecular dynamics. We then provide a detailed historical account on the ultrafast photochemistry of iron pentacarbonyl, nickel tetracarbonyl, and transition metal hexacarbonyls and decacarbonyls, putting the more recent ultrafast studies in the context of prior investigations. In conclusion, we end this review with an outlook on open questions and future possibilities.

Core level spectroscopy↗
DOE OSTI2021

Theoretical kinetics predictions for NH 2 + HO 2

Recent modeling studies of NH 3 oxidation, which are motivated by the prospective role of ammonia as a zero-carbon fuel, have indicated significant discrepancies between existing literature mechanisms. In this study high level theoretical kinetics predictions have been obtained for the reaction of NH 2 with HO 2 , which has previously been highlighted as an important reaction with high sensitivity and high uncertainty. The potential energy surface is explored with coupled cluster calculations including large basis sets and high-level corrections to yield high accuracy (~0.2 kcal/mol) estimates of the stationary point energies. Variational transition state theory is used to predict the microcanonical rate constants, which are then incorporated in master equation treatments of the temperature and pressure dependent kinetics. For the radical-radical channels, the microcanonical rates are obtained from variable reaction coordinate transition state theory implementing directly evaluated multireference electronic energies. The analysis yields predictions for the total rate constant as well as the branching to the NH 3 + O 2 , H 2 NO + OH, and HNO + H 2 O channels. Rate constants are also reported for the H 2 NO + OH reaction as they arise naturally from the analysis. The rate constant and branching fraction determined in this work for the NH 2 + HO 2 reaction deviate significantly from values used in most previous modeling studies. The fact that the main product channel is chain terminating, rather than propagating, has strong implications for modeling NH 3 ignition and oxidation, in particular at intermediate temperatures and elevated pressure.

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

Localized high concentration electrolytes decomposition under electron-rich environments

Localized high concentration electrolytes have been proposed as an effective route to construct stable solid–electrolyte interphase (SEI) layers near Li-metal anodes. However, there is still a limited understanding of decomposition mechanisms of electrolyte components during SEI formation. In this work, we investigate reactivities of lithium bis(fluorosulfonyl)imide (LiFSI, salt), 1,2-dimethoxyethane (DME, solvent) and tris(2,2,2-trifluoroethyl)orthoformate (TFEO, diluent) species in DME+TFEO mixed solvents and 1M LiFSI/DME/TFEO solutions. By supplying excess of electrons into the simulation cell, LiFSI is initially reduced via a 4-electron charge transferring reaction yielding F - and N(SO 2 ) 2 3- . The local solvation environment has little effect on the subsequent TFEO reaction, which typically requires 6 |e| to decompose into F - , HCOO - , CH2CF and - OCH 2 CF 3 . Besides, TFEO dehydrogenation reaction mechanism under the attack of anions is also identified. Unlike salt and diluent, DME shows good stability with any excess of electrons. Here, the energetics of most relevant reactions are characterized. Most reactions are thermodynamically favorable with low activation barriers.

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

Anion Resonances and Photoelectron Spectroscopy of the Tetracenyl Anion

The photoelectron spectroscopy of the tetracenyl anion using slow electron velocity-map imaging (SEVI) of cryogenically cooled ions is presented here. The total photodetachment yield as a function of photon energy is used to reveal a rich manifold of anion excited states above the detachment threshold. The lowest energy anionic resonance has a sufficiently long lifetime to yield a vibrationally resolved absorption spectrum that can be directly compared with theoretical predictions. Excitation of this state mostly results in electron detachment via thermionic emission. The total photodetachment yield spectrum is used to select photon wavelengths that minimize the indirect detachment signal to allow acquisition of vibrationally-resolved photoelectron spectra that can inform on the neutral tetracenyl radical. Assignment of spectral features corresponding to the ground and first excited state of the neutral 12-tetracenyl isomer is made with the aid of Franck-Condon simulations. This yields adiabatic electron affinity and term energies that differ significantly from the previously reported values. Weak features corresponding to the ground state of the minor 2-teracenyl and 1-tetracenyl isomers are also identified, which allows for the experimental determination of their electron affinities for the first time.

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

Theoretical Kinetics Predictions for Reactions on the NH 2 O Potential Energy Surface

Recent modeling studies of ammonia oxidation, which are motivated by the prospective role of ammonia as a zero-carbon fuel, have indicated significant discrepancies among the existing literature mechanisms. In this study, high-level theoretical kinetics predictions have been obtained for reactions on the NH 2 O potential energy surface, including the NH 2 + O, HNO + H, and NH + OH reactions. These reactions have previously been highlighted as important reactions in NH 3 oxidation with high sensitivity and high uncertainty. The potential energy surface is explored with coupled cluster calculations, including large basis sets and high-level corrections to yield high-accuracy (~0.2 kcal/mol 2σ uncertainty) estimates of the stationary point energies. Variational transition state theory is used to predict the microcanonical rate constants, which are then incorporated in master equation treatments of the temperature- and pressure-dependent kinetics. For radical–radical channels, the microcanonical rates are obtained from variable reaction coordinate transition state theory implementing directly evaluated multireference electronic energies. The analysis yields predictions for the total rate constants as well as the branching ratios. We find that the NO + H 2 channel contributes 10% of the total NH 2 + O flux at combustion temperatures, although this channel is not included in modern NH 3 oxidation mechanisms. Modeling is used to illustrate the ramifications of these rate predictions on the kinetics of NH 3 oxidation and NO x formation. Finally, the present results for NH 2 + O are important for predicting the chain branching and formation of NO in the oxidation of NH 3 and thermal DeNO x .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1982

Measurement of total electron content of midlatitude ionosphere and protonosphere via Faraday rotation and group relay techniques using transmission from geostationary satellites ATS-3 and ATS-6

Measurement of integrated columnar electron content and total electron content for the local ionosphere and the overlying protonosphere via Faraday rotation and group delay techniques has proven very useful. A field station was established having the geographic location of 31.5 deg N latitude and 91.06 deg W longitude to accomplish these objectives. A polarimeter receiving system was set up in the beginning to measure the Faraday rotation of 137.35 MHz radio signal from geostationary satellite ATS 3 to yield the integrated columnar electron content of the local ionosphere. The measurement was continued regularly, and the analysis of the data thus collected provided a synopsis of the statistical variation of the ionosphere along with the transient variations that occurred during the periods of geomagnetic and other disturbances.

Paul, M. P.↗
NASA NTRS1990

Photon sputtering of H2O ices: A preliminary report

A preliminary measurement of the total yields of ejected ions and electrons from H2O ices has been carried out using the He I 584 A resonance line as the incident photon beam. The H2O ices were prepared at 77 K in an ultrahigh vacuum system. The total yield of the ejected ion species and electrons was determined to be 8.8x10(exp -5) and 4.2x10(exp -4), respectively.

Wu, C. Y. Robert↗
DOE OSTI2020

Real-Time Time-Dependent Electronic Structure Theory

Real-time electronic structure methods provide an unprecedented view of electron dynamics and ultrafast spectroscopy on the atto- and femtosecond time scale with vast potential to yield new insights into the electronic behavior of molecules and materials. Here, we discuss the fundamental theory underlying various real-time electronic structure methods as well as advantages and disadvantages of each. We give an overview of the numerical techniques that are widely used for real-time propagation of the quantum electron dynamics with an emphasis on Gaussian basis set methods. We also showcase many of the chemical applications and scientific advances made by using real-time electronic structure calculations and provide an outlook of possible new directions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1991

Procedures for Including Secondary Electron Emission in Numerical Simulations of Plasma-Insulator Interactions

Previous Monte Carlo simulations provide a data base for properties of secondary electron emission (SEE) from insulators and metals. Incident primary electrons are considered at energies up to 1200 eV. The behavior of secondary electrons is characterized by (1) yield vs. primary energy E(sub p), (2) distribution vs. secondary energy E(sub s), and (3) distribution vs. angle of emission theta. Special attention is paid to the low energy range E(sub p) up to 50 eV, where the number and energy of secondary electrons is limited by the finite band gap of the insulator. For primary energies above 50 eV the SEE yield curve can be conveniently parameterized by a Haffner formula. The energy distribution of secondary electrons is described by an empirical formula with average energy about 8.0 eV. The angular distribution of secondaries is slightly more peaked in the forward direction than the customary cos theta distribution. Empirical formulas and parameters are given for all yield and distribution curves. Procedures and algorithms are described for using these results to find the SEE yield, and then to choose the energy and angle of emergence of each secondary electron. These procedures can readily be incorporated into numerical simulations of plasma-solid surface interactions in low earth orbit.

Beyst, Brian↗
DOE OSTI2024

Exploiting a derivative discontinuity estimate for accurate G0W0 ionization potentials and electron affinities

Abstract The GW approximation has become an important tool for predicting charged excitations of isolated molecules and condensed systems. Its popularity can be attributed to many factors, including a favorable scaling and relatively good accuracy. In practical applications, the GW is often performed as a one-shot perturbation known as G 0 W 0 . Unfortunately, G 0 W 0 suffers from a strong starting point dependence and is often not as accurate as one would need. Self-consistent GW methodologies alleviate these problems but come with a marked increase in computational cost. In this manuscript, we propose the use of an estimate of the exchange-correlation derivative discontinuity to provide a remarkably good starting point for G 0 W 0 calculations, yielding ionization potentials and electron affinities with eigenvalue self-consistent GW quality at no additional cost. We assess the quality of the resulting methodology with the GW 100 benchmark set and compare its advantages over other similar methods.

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

Characterization of Self-Magnetic Pinch (SMP) Radiographic Diode Performance on RITS-6 at Sandia National Laboratories

The goals of an electron beam-driven radiographic source are the focusing of high current at high voltage to a minimal spot size with excellent shot-to-shot reproducibility. The Self-Magnetic Pinch (SMP) diode makes use of such an intense electron beam impinging on a high-atomic weight (tantalum) converter, a counter-streaming ion beam to help minimize the spot size, and operation in a magnetic field-free diode region which further encourages small spot size. Through a series of diode development experiments, output voltages up to 12.5 MV and output currents up to 225 kA have been characterized, with resulting spot sizes below ~ few mm. Scaling studies with parameter variation, such as diode aspect ratio and anode-cathode (A-K) gap variation, give systematic validation to what has heretofore been noted anecdotally by other research groups. While the lack of an imbedded magnetic field helps minimize the SMP spot size, a secondary result may be the generation of beam instabilities which can terminate the radiation pulse. There is anecdotal evidence that in-situ DC heating of the diode region can help stabilize the beam pinch. Clear experimental evidence exists that DC heating/RF cleaning results in better control over the counter-streaming ion population. Expanded use of spatial dose-rate detection is shown to yield new insights into electron beam dynamics in the SMP diode. An attendant study of the SMP diode as a load for an Inductive Voltage Adder (IVA) driver leads to insights into the behavior of the IVA-SMP diode configuration, viewed as a total system, and yields constraints on the overall impedance behavior of the SMP diode load.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Direct Evidence of Visible Light-Induced Homolysis in Chlorobis(2,9-dimethyl-1,10-phenanthroline)copper(II)

Developments in the field of photoredox catalysis that leveraged the long-lived excited states of Ir(III) and Ru(II) photosensitizers to enable radical coupling processes paved the way for explorations of synthetic transformations that would otherwise remain unrealized. While first row transition metal photocatalysts have not been as extensively investigated, valuable synthetic transformations covering broad scopes of olefin functionalization have been recently reported featuring photoactivated chlorobis(phenanthroline) Cu(II) complexes. In this study, the photochemical processes underpinning the catalytic activity of [Cu(dmp) 2 Cl]Cl (dmp = 2,9-dimethyl-1,10-phenanthroline) were studied. The combined results from static spectroscopic measurements and conventional photochemistry, ultrafast transient absorption, and electron paramagnetic resonance spin trapping experiments strongly support blue light (λ ex = 427 or 470 nm)-induced Cu–Cl homolytic bond cleavage in [Cu(dmp) 2 Cl] + occurring in <100 fs. On the basis of electronic structure calculations, this bond-breaking photochemistry corresponds to the Cl → Cu(II) ligand-to-metal charge transfer transition, unmasking a Cu(I) species [Cu(dmp) 2 ] + and a Cl atom, thereby serving as a departure point for both Cu(I)- or Cu(II)-based photoredox transformations. No net photochemistry was observed through direct excitation of the ligand-field transitions in the red (λ ex = 785 or 800 nm), and all combined experiments indicated no evidence of Cu–Cl bond cleavage under these conditions. As a result, the underlying visible light-induced homolysis of a metal–ligand bond yielding a one-electron-reduced photosensitizer and a radical species may form the basis for novel transformations initiated by photoinduced homolysis featuring in situ-formed metal–substrate adducts utilizing first row transition metal complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗