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NASA NTRS1988

Transmission electron microscopy study of the formation of epitaxial CoSi2/Si (111) by a room-temperature codeposition technique

Co and Si have been codeposited on Si (111) substrates near room temperature in a stoichiometric 1:2 ratio in a molecular beam epitaxy system. Annealing of these deposits yields high-quality single-crystal CoSi2 layers. Transmission electron microscopy has been used to examine as-deposited layers and layers annealed at 300, 500, and 600 C. Single-crystal epitaxial grains of CoSi2 embedded in a matrix of amorphous Co/Si are observed in as-deposited samples, while the layer is predominantly single-crystal, inhomogeneously strained CoSi2 at 300 C. At 600 C, a homogeneously strained single-crystal layer with a high density of pinholes is observed. In contrast to other solid phase epitaxy techniques used to grow CoSi2 on Si (111), no intermediate silicide phases are observed prior to the formation of CoSi2.

D'Anterroches, Cecile↗

NASA NTRS1994

Three-dimensional numerical simulation of current collection by a probe in a magnetized plasma

A three-dimensional numerical model for current collection in a magnetized plasma is reported. The model is based on an electrostatic particle-in-cell code. The model yields self-consistent sheath structure including distributions of plasma and the electric potential around the body and the collection of electrons. The analytical theory of current collection by a body in a magnetized plasma yields an upper bound for the collected current determined by the conservation of energy and canonical angular momentum. The theory shows that the collected charged particles come from a cylindrical volume aligned with the magnetic shadow of the body; the maximum radius r(sub o) of this volume is determined by the body size, body potential, and the ambient magnetic field. This theory does not deal with the sheath structure around the body. The condition for the actual current to approach the upper-bound value has been a matter of debate. Our simulations reveal when and why the collected current becomes equal to its upper-bound value. Sheath size in the radial direction perpendicular to the axial ambient magnetic field is determined by the current-limiting radius r(sub o). Our simulation yields time-average current in good agreement with its upper bound. This feature of the current collection is explained as follows: Once electrons enter the sheath, some of them are freely accelerated perpendicular to the magnetic field because they are demagnetized by the large gradients in the perpendicular electric fields. Simulations show a large perpendicular acceleration, producing perpendicular energy as large as that determined by the potential on the body, especially in the region where perpendicular electric fields (E perpendicular) are the strongest. An analysis shows that the demagnetization of electrons occurs above a threshold potential on the body. This threshold condition follows from the breakdown of the adiabaticity of the electron dynamics inside the sheath.

Singh, Nagendra↗

NASA NTRS1983

Luminescence induced by dehydration of kaolin - Association with electron-spin-active centers and with surface activity for dehydration-polymerization of glycine

Experimental data concerning emission of light upon dehydration as a function of preheating and pre-gamma-irradiation are correlated with reported studies of electron-spin resonance (ESR) activity after similar pretreatments. The effect of these pretreatments on the kaolin-promoted incorporation of glycine into peptide oligomers in a wet/cold, hot/dry fluctuating environment is compared to their effect on the ESR and luminescent signals. The existence of spectroscopically active centers appears to be loosely anticorrelated with reaction yield; these yields are increased by increasing the overall energy content of the material. It is concluded that some part of the chemical yield is produced by a mechanism involving intrinsic, excited electronic states of the clay crystal lattice. These states may be derived from thermally, interfacially, and/or mechanically induced charge reorganization within interspersed energy levels in the band structure of the material.

Coyne, L.↗

DOE OSTI2023

Effects of a nuclear-disturbed environment on electromagnetic wave propagation through the atmosphere

This paper investigates the effects of a nuclear-disturbed environment on the transmission of electromagnetic (EM) waves through the atmosphere. An atmospheric nuclear detonation can produce heightened free electron densities in the surrounding atmosphere that can disrupt EM waves that propagate through the disturbed region. Radiation transport models simulated the ionization and free electron densities created in the atmosphere from a 1 MT detonation at heights of burst of 5 km, 25 km, and 75 km. Recombination rates for the free electrons in the atmosphere were applied, from previous work in the literature, to determine the nuclear-induced electron densities as a function of time and space after the detonation. A ray-tracing algorithm was applied to determine the refraction and reflection of waves propagating in the different nuclear-disturbed environments. The simulation results show that the free electron plasma created from an atmospheric nuclear detonation depend on the height of burst of the weapon, the weapon yield, and the time after detonation. Detonations at higher altitudes produce higher free electron densities for greater durations and over larger ranges. The larger the free electron densities, the greater the impact on EM wavelengths in regards to refraction, reflection, and absorption in the atmosphere. An analysis of modern infrastructure and the effects of nuclear-disturbed atmospheres on different signal wavelengths and systems is discussed.

42 ENGINEERING↗

NASA NTRS2008

The (55)Fe X-ray Energy Response of Mercury Cadmium Telluride Near-Infrared Detector Arrays

The accurate determination of a detector's fundamental parameters, including read noise, dark current, and QE, relies on a proper measurement of a detector's conversion gain (e- ADU(exp -1)). Charge coupling effects, such as interpixel capacitance, attenuate photon shot noise and result in an overestimation of conversion gain when implementing the photon transfer technique. An approach involving (55)Fe X-rays provides a potentially straightforward measurement of conversion gain by comparing the observed instrumental counts (ADU) to the known charge (e-) liberated by the X-ray. This technique is already preferred within the CCD community, as the pair production energy for silicon is well established. In contrast, to date the pair production energy is unknown for HgCdTe, a material commonly used for near-infrared detectors. In this paper, we derive a preliminary calibration of the (55)Fe X-ray energy response of HgCdTe using 8 HST WFC3 1.7 micrometers flight grade detectors. Our conversion of the X-ray intensities from counts into electrons implements a technique that restores the 'true' gain via classical propagation of errors. For these detectors, our analysis yields preliminary results of good statistical precision: each Ka event generates 1849 +/- 46 electrons, which corresponds to a pair production energy of 3.21+/-f 0.08 eV. We are continuing to assess potential systematic effects to further refine the accuracy of this result.

Fox, Ori↗

NASA NTRS1992

Accuracies Of Optical Processors For Adaptive Optics

Paper presents analysis of accuracies and requirements concerning accuracies of optical linear-algebra processors (OLAP's) in adaptive-optics imaging systems. Much faster than digital electronic processor and eliminate some residual distortion. Question whether errors introduced by analog processing of OLAP overcome advantage of greater speed. Paper addresses issue by presenting estimate of accuracy required in general OLAP that yields smaller average residual aberration of wave front than digital electronic processor computing at given speed.

Downie, John D.↗

NASA NTRS2013

New Evidence for Efficient Collisionless Heating of Electrons at the Reverse Shock of a Young Supernova Remnant

Although collisionless shocks are ubiquitous in astrophysics, certain key aspects of them are not well understood. In particular, the process known as collisionless electron heating, whereby electrons are rapidly energized at the shock front, is one of the main open issues in shock physics. Here, we present the first clear evidence for efficient collisionless electron heating at the reverse shock of Tycho's supernova remnant (SNR), revealed by Fe K diagnostics using high-quality X-ray data obtained by the Suzaku satellite. We detect K beta (3p yields 1s) fluorescence emission from low-ionization Fe ejecta excited by energetic thermal electrons at the reverse shock front, which peaks at a smaller radius than Fe K alpha (2p yields 1s) emission dominated by a relatively highly ionized component. Comparisons with our hydrodynamical simulations imply instantaneous electron heating to a temperature 1000 times higher than expected from Coulomb collisions alone. The unique environment of the reverse shock, which is propagating with a high Mach number into rarefied ejecta with a low magnetic field strength, puts strong constraints on the physical mechanism responsible for this heating and favors a cross-shock potential created by charge deflection at the shock front. Our sensitive observation also reveals that the reverse shock radius of this SNR is about 10% smaller than the previous measurement using the Fe K alpha morphology from the Chandra observations. Since strong Fe K beta fluorescence is expected only from low-ionization plasma where Fe ions still have many 3p electrons, this feature is key to diagnosing the plasma state and distribution of the immediate postshock ejecta in a young SNR.

Fe K diagnostics↗

DOE OSTI2025

Optical interference effect in strong-field electronic coherence spectroscopy

Here, we investigate strong-field-induced electronic coherences in argon and molecular nitrogen ions created by high-intensity, few-cycle infrared laser pulses. This is a step toward the long-sought goal of strong-field coherent control in molecular chemistry. We employ high-intensity, few-cycle infrared laser pulses in a pump-probe setup to investigate a recent prediction that electronic coherences in nitrogen molecules change the ion yields versus pump-probe delay. [Yuen et al., Phys. Rev. A 109, L011101 (2024)]. The predicted coherence signals in molecular nitrogen could not be resolved above the optical interference of the pump and probe pulses; a simultaneous measurement clearly resolved the induced cation fine-structure coherence in strong-field-ionized argon. The results of our comparison with simulations suggest that optical interference effects manifest differently in each ionic species and must be carefully accounted for when interpreting experimental data. We find that nonsequential double ionization in the low-intensity region of the focal volume can reduce the visibility of coherence generated by two-pulse sequential ionization, and we quantify the importance of pulse shape and spectral characteristics for isolating the desired coherence signals.

charge migration↗

NASA NTRS1973

Low-frequency instabilities and plasma turbulence

A theoretical and experimental study is reported of steady-state and time-dependent characteristics of the positive column and the hollow cathode discharge (HCD). The steady state of a non-isothermal, cylindrical positive column in an axial magnetic field is described by three moment equations in the plasma approximation. Volume generation of electron-ion pairs by single-stage ionization, the presence of axial current, and collisions with neutrals are considered. The theory covers the range from the low pressure, collisionless regime to the intermediate pressure, collisional regime. It yields radial profiles of the charged particle velocities, density, potential, electron and ion temperatures, and demonstrates similarity laws for the positive column. The results are compared with two moment theories and with experimental data on He, Ar and Hg found in the literature for a wide range of pressures. A simple generalization of the isothermal theory for an infinitely long cylinder in an axial magnetic field to the case of a finite column with axial current flow is also demonstrated.

Ilic, D. B.↗

NASA NTRS1989

Photodissociation of pernitric acid (HO2NO2) at 248 nm

The photodissociation of pernitric acid (PNA) was studied at 248 nm. The quantum yield for production of OH radicals is 34 + or - 16 percent. The yield of OH from PNA was measured relative to that of H2O2. The translational and rotational energy content of the OH photofragment from PNA was characterized. A fluorescent emission was also observed and characterized. It is attributed to electronically excited NO2 produced in the PNA photodissociation. A maximum yield of 30 percent for NO2 production was determined. The intensity of this emission, and a mass spectrometric peak at m/e = 33, were found to be useful means of characterizing the purity of the PNA sample.

Macleod, Helene↗

DOE OSTI2023

Temperature separation under compression of moderately coupled plasma

In moderately coupled plasmas, a significant fraction of the internal energy resides in electric fields. As these plasmas are heated or compressed, the shifting partition of energy between particles and fields leads to surprising effects, particularly when ions and electrons have different temperatures. In this work, quasi-equations of state (quasi-EOS) are derived for two-temperature moderately coupled plasma in a thermodynamic framework and expressed in a simple form. These quasi-EOS readily yield expressions for correlation heating, in which heating of the electrons causes a rapid increase in ion temperature even in the absence of collisional energy exchange between species. It is also shown that, remarkably, compression of moderately coupled plasma drives a temperature difference between electrons and ions, even when the species start at equal temperatures. These additional channels for ion heating may be relevant in designing ignition schemes for inertial confinement fusion.

Fetsch, H. (ORCID:0000000256133975)↗

DOE OSTI2022

Electrochemical Structure of the Plasma–Liquid Interface

Nonthermal atmospheric pressure plasma in contact with a liquid yields a variety of energetic photons, ions, and electrons, which can be transported into the plasma–liquid interface (PLI). Similar to the electrochemical interface formed between a solid electrode and electrolyte in conventional electrochemical systems, the charge-transfer process across the PLI is able to promote reduction–oxidation (redox) reactions. However, in the case of free plasma jets in contact with liquids, the absence of solid electrodes obscures the spatial locations of the electrochemical half-reactions. Herein, we present a spatial electrochemical measurement technique used to characterize an aqueous solution in contact with an atmospheric pressure plasma jet. The technique is based on measuring the potential difference between two identical Ag/AgCl electrochemical electrodes positioned at different locations within the solution. More specifically, electrochemical maps were made by measuring the potential of one electrochemical electrode positioned at different locations near the PLI with respect to the other electrochemical electrode positioned far away from the PLI in the bulk solution. Regions in the map with negative and positive potential differences between these electrochemical electrodes were used to identify the electrodeless cathode and anode, respectively. Here, visualization of the spatial distribution of molecular colorimetric redox indicators by multispectral imaging revealed that reduction was occurring near the plasma jet centerline while oxidation was occurring further away in solution, which constitutes an independent confirmation of the electrochemical maps.

Absorption↗

DOE OSTI2020

Visible-Light-Driven Triplet Sensitization of Polycyclic Aromatic Hydrocarbons Using Thionated Perinones

Metal-free chromophores that efficiently generate triplet excited states represent enticing alternatives with respect to transition metal-containing photosensitizers, such as those featuring metal-to-ligand charge transfer excited states. Yet, such molecular constructs have remained underexplored due to the unclear relationship(s) between molecular structure and efficient/rapid intersystem crossing. In this regard, we present a series of three thionated perinone chromophores serving as a newly conceived class of heavy metal-free triplet photosensitizers. We demonstrate that thionation of the lone C=O substituent in each highly fluorescent perinone imparts red-shifted absorbance bands that maintain intense extinction coefficients across the visible spectrum, as well as unusually efficient triplet excited state formation as inferred from the measured singlet O 2 quantum yields at 1270 nm (Φ Δ = 0.78–1.0). Electronic structure calculations revealed the emergence of a low energy S 1 (n → π*) excited state in the proximity of a slightly higher energy S 2 (π → π*) excited state. The distinct character in each of the two lowest-lying singlet state manifolds resulted in the energetic inversion of the corresponding triplet excited states due to differences in electron exchange interactions. Rapid S 1 → T 1 intersystem crossing was thereby facilitated in this manner through spin–orbit coupling as predicted by the El Sayed rules. The lifetimes of the resultant triplet excited states persisted into the microsecond time regime, as measured by transient absorbance spectroscopy, enabling effective bimolecular triplet sensitization of some common polycyclic aromatic hydrocarbons. The synthetically facile interchange of a single O atom to an S atom in the investigated perinones resulted in marked changes to their photophysical properties, namely, conversion of dominant singlet state fluorescence in the former to long-lived triplet excited states in the latter. The combined results suggest a general strategy for accessing long-lived triplet excited states in organic chromophores featuring a lone C=O moiety residing within its structure, valuable for the design of metal-free triplet photosensitizers.

14 SOLAR ENERGY↗

DOE OSTI2022

Hierarchical, Self-Assembled Metasurfaces via Exposure-Controlled Reflow of Block Copolymer-Derived Nanopatterns

Here, nanopatterning for the fabrication of optical metasurfaces entails a need for high-resolution approaches like electron beam lithography that cannot be readily scaled beyond prototyping demonstrations. Block copolymer thin film self-assembly offers an attractive alternative for producing periodic nanopatterns across large areas, yet the pattern feature sizes are fixed by the polymer molecular weight and composition. Here, a general strategy is reported that overcomes the limitation of fixed feature size by treating the copolymer thin film as a hierarchical resist, in which the nanoscale pattern motif is defined by self-assembly. Feature sizes can then be tuned by thermal reflow controlled locally by irradiative crosslinking or chemical alteration using lithographic ultraviolet light or electron beam exposure. Using blends of polystyrene-block-poly(methylmethacrylate) (PS-b-PMMA) with PS and PMMA homopolymer, we demonstrate both self-assembled PS grating and hexagonal hole patterns; exposure-controlled reflow is then used to reduce hole diameter by as much as 50% or increase PS grating linewidth by more than 180%. Transferring these nanopatterns, or their inverse obtained by a lift-off approach, into silicon yields structural colors that may be prescriptively controlled based on nanoscale feature size. Furthermore, patterned exposure enables area-selective feature size control, yielding uniform structural color patterns across centimeter square areas. Electron beam lithography is also used to show that the lithographic resolution of this selective-area control can be extended to the nanoscale dimensions of the self-assembled features. The exposure-controlled reflow approach demonstrated here takes a pivotal step towards fabricating complex, hierarchical optical metasurfaces using scalable self-assembly methods.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2022

Internal conversion and intersystem crossing dynamics based on coupled potential energy surfaces with full geometry-dependent spin–orbit and derivative couplings. Nonadiabatic photodissociation dynamics of NH 3 (A) leading to the NH(X 3 Σ – , a 1 Δ) + H 2 channel

Here we simulate the photodissociation of NH 3 originating from its first excited singlet state S 1 into the NH 2 + H (radical) and NH + H 2 (molecular) channels. The states considered are the ground singlet state S 0 , the first excited singlet state S 1 and the lowest-lying triplet state T 1 , which permit for the first time a uniform treatment of the internal conversion and intersystem crossing. The simulations are based on a diabatic potential energy matrix (DPEM) of S 0 , S 1 coupled by a conical intersection seam, as well as a potential energy surface (PES) for T 1 coupled by spin-orbit coupling (SOC) to the two singlet states. The DPEM and PES are fitted to ab initio electronic structure data (ESD) including energies, energy gradients, and derivative couplings. The DPEM also defines an adiabatic to diabatic state (AtD) transformation, which is used to transform the singular adiabatic SOC into a smooth function of the nuclear coordinates in the diabatic representation, allowing the diabatic SOC to be fit to an analytical functional form. ESD and SOC data obtained from these surfaces can serve as input for either quantum or semi-classical characterization of the nonadiabatic dynamics. Using the SHARC suite of programs, nonadiabatic simulations based on over 40 000 semi-classical trajectories assess the convergence of our results. The production of NH + H 2 is not direct, but is only achieved through a quasi-statistical dissociation mechanism after internal conversion to the ground electronic state. This leads to a much lower yield comparing with the main NH 2 + H channel. The NH(X 3 Σ_) radical produced through the intersystem crossing from S 0 to T 1 is rare (~0.2%) compared to NH(a 1 Δ) due to the process being spin forbidden.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Scintillation characteristics of the EJ-299-02H scintillator

Here a study of the dead layer thickness and quenching factor of a plastic scintillator for use in ultracold neutron (UCN) experiments is described. Alpha spectroscopy was used to determine the thickness of a thin surface dead layer to be 630 ± 110 nm. The relative light outputs from the decay of 241 Am and Compton scattering of electrons were used to extract Birks’ law coefficient, yielding a kB value of 0.087 ± 0.003 mm/MeV, consistent with some previous reports for other polystyrene-based scintillators. The results from these measurements are incorporated into the simulation to show that an energy threshold of (∼9 keV) can be achieved for the UCNProBe experiment. This low threshold enables high beta particle detection efficiency and the indirect measurement of UCN. The ability to make the scintillator deuterated, accompanied by its relatively thin dead layer, gives rise to unique applications in a wide range of UCN experiments, where it can be used to trap UCN and detect charged particles in situ.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

High repetition-rate 0.5 Hz broadband neutron source driven by the Advanced Laser Light Source

Neutron beams are an essential tool to investigate material structure and perform nondestructive analysis, as they give unique access to element composition, thus ideally complementing density analysis allowed by standard x-rays investigation. Laser-driven neutron sources, though compact and cost-effective, currently have lower average flux than conventional neutron sources, due to the limited repetition rate of the lasers used so far. However, advancements in laser technology allow nowadays to address this challenge. Here, we report results obtained at the Advanced Laser Light Source characterizing stable production of broadband (0.1–2 MeV) neutrons produced at a high repetition rate (0.5 Hz). The interaction of laser pulses of 22 fs duration and 3.2 J on-target energy with 2-μm-thick tantalum targets produced protons in the Target Normal Sheath Acceleration (TNSA) regime up to 7.3 MeV. These protons were subsequently converted into neutrons by (p,n) reactions in lithium fluoride (LiF). Activation measurements and bubble detectors were used to characterize neutron emissions, with a neutron fluence of up to ∼1.4×105 neutrons/shot/sr and energies mainly between a few hundred of kilo-electron volt and 2 MeV. The total neutron yield was ∼5×105 neutrons/shot. This paves the way for numerous applications, e.g., in homeland security, materials science, or cultural heritage.

Physics↗

DOE OSTI2022

Characterization of beam ion loss in high poloidal beta regime on EAST

A critical issue for achieving the integrated operation of steady-state long-pulse high-confinement (H-mode) plasmas on experimental advanced superconducting tokamak (EAST) is to improve beam ion population confinement during neutral beam injection (NBI). To study the characterization of beam ion loss and improve beam ion confinement, the steady-state long pulse scenario discharges were conducted on EAST (β p $\geqslant$ 2.0, β N $\geqslant$ 1.7, q 95 $\geqslant$ 6.7 and H 98y2 $\geqslant$ 1.1) with NBI heating. Based on neutron yield, the beam voltage and line-averaged electron density were adjusted from 50 kV to 60 kV and 4.4 × 10 19 m –3 to 5.0 × 10 19 m –3 , respectively. The results show that the dominant mechanisms of beam ion loss are shine-through loss, prompt loss, and stochastic ripple loss. The shine-through loss fraction is determined by initial velocity, flight time and entire beam path. The change in prompt loss fraction is caused by the change in the deposition of beam ions. The change in stochastic ripple loss fraction is caused by the change in the initial fraction of trapped-confined ions. Detailed physics shows that the prompt loss fraction during counter-Ip injections (~45%) is far larger than during co-Ip injections (~5%) due to the finite orbit width. The lost ions are mainly deposited on the lower divertor or below the midplane since the direction of magnetic drift is vertical down. The orbit types of prompt loss during counter-Ip injections are mainly trapped-lost and ctr-passing lost. To minimize the prompt loss fraction during counter-Ip injections, a reversed Ip configuration (rev-Ip) discharge #94758 was conducted. The result suggests that the beam ion wall load fraction during counter-Ip tangential injection (~3%) is far lower than that in normal Ip configuration (nor-Ip) discharge #94820. It is also found that the confinement of beam ion population in the counter-Ip injection #94758 was greatly improved when compared to #94820. Finally, this study can provide unique support for the improvement of beam ion population confinement and for the performance evaluation of the NBI system on EAST and future tokamaks.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗