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At least 1,171 records · Page 65
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

The Driving Force Controls Charge Separation Distance in Solid-State Organic Donor/Acceptors

In this work, charge pairs of varying separation distance are interpreted from photoinduced absorption detected magnetic resonance (PADMR) spectroscopy of organic, small molecule dilute donor/acceptor thin films. We report that a donor/acceptor film that generates few free charges at room temperature yet has a relatively large, calculated driving force for electron transfer generates a large concentration of tightly bound CT states when measured with PADMR. These states are markedly absent in films with smaller driving forces yet higher free charge yields which instead only show charge-separated state signals with weaker spin coupling. We interpret this result to be in support of a hypothesis where a larger reorganization energy associated with charge transfer to tightly bound CT states means that they are primarily generated in systems far from the Marcus optimum for free charge yield. And the highest free charge yielding systems instead predominantly undergo long-range charge separation into the acceptor host.

charge separation↗
DOE OSTI2024

Integrated design of aluminum-enriched high-entropy refractory B2 alloys with synergy of high strength and ductility

Refractory high-entropy alloys (RHEAs) are promising high-temperature structural materials. Their large compositional space poses great design challenges for phase control and high strength-ductility synergy. The present research pioneers using integrated high-throughput machine learning with Monte Carlo simulations supplemented by ab initio calculations to effectively navigate phase selection and mechanical property predictions, developing single-phase ordered B2 aluminum-enriched RHEAs (Al-RHEAs) demonstrating high strength and ductility. These Al-RHEAs achieve remarkable mechanical properties, including compressive yield strengths up to 1.7 gigapascals, fracture strains exceeding 50%, and notable high-temperature strength retention. They also demonstrate a tensile yield strength of 1.0 gigapascals with a ductility of 9%, albeit with B2 ordering. Furthermore, we identify valence electron count domains for alloy ductility and brittleness with the explanation from density functional theory and provide crucial insights into elemental influence on atomic ordering and mechanical performance. The work sets forth a strategic blueprint for high-throughput alloy design and reveals fundamental principles governing the mechanical properties of advanced structural alloys.

Science & Technology - Other Topics↗
DOE OSTI2022

Resolution requirements for energy conservation in kinetic plasma simulations

The kinetic codes used to model the coupled dynamics of electromagnetic fields and charged particle transport have requirements for spatial, temporal, and charge resolution. These requirements may vary by the solution technique and scope of the problem. In this report, we investigate the resolution limits in the energy-conserving implicit particle-in-cell code CHICAGO. This report has the narrow aim of determining the maximum acceptable grid spacing for the dense plasmas generated in models of z-pinch target gases and power-flow electrode plasmas. In the 2D sample problem, the plasma drifts without external forces with velocity of 10 cm/µs. Simulations are scaled by plasma density to maintain uniform strides across the plasma and from the plasma to the boundaries. Additionally, the cloud-in-cell technique is used with 400 particles per cell and Δ t = 0.85× the Courant limit. For the linear cloud distribution, the criterion for conserving energy is Δ E/E tot < 0.01 for 50,000 time steps. The grid resolution is determined to crudely be Δx ≲ 3 l s , where l s is the electron collisionless skin depth. For the second-order cloud distribution the criterion is Δ E/E tot < 0.005 yielding Δx ≤ 15 l s . These scalings are functions of the chosen v d , Δ t , particles-per-cell, and number of steps.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1972

The IR emission spectrum of N2 excited under auroral conditions.

Recently determined experimental and theoretical cross sections for electron impact excitation of six triplet states of N2 (A, B, W, C, E, D) have been utilized to predict the absolute IR volume emission rates from N2 under nighttime auroral conditions. Secondary electron fluxes appropriate to an IBC II normal aurora were used in the calculations. The cascade contributions coupling the various electronic states were included as well as the most important quenching processes. The results indicate that the B yields reversibly A and W yields reversibly B cascade processes, which are important in the population of the A, B, and W states, produce appreciable radiation in the 1- to 5-micron wavelength region.

Cartwright, D. C.↗
NASA NTRS1974

Hot ion plasma heating experiments in SUMMA

Initial results are presented for the hot-ion plasma heating experiments conducted in the new SUMMA (superconducting magnetic mirror apparatus) at NASA Lewis Research Center. A discharge is formed by applying a radially inward dc electric field between cylindrical anodes and hallow cathodes located at the peak of the mirrors. Data were obtained at midplane magnetic field strengths from 1.0 to 3.5 tesla. Charge-exchange neutral particle energy analyzer data were reduced to ion temperatures using a plasma model that included a Maxwellian energy distribution superimposed on an azimuthal drift, finite ion orbits, and radial variations in density and electric field. The best ion temperatures in a helium plasma were 5 keV and in hydrogen the H2(+) and H(+) ions were 1.2 keV and 1 keV respectively. Optical spectroscopy line broadening measurements yielded ion temperatures about 50 percent higher than the charge-exchange neutral particle analyzer results. Spectroscopically obtained electron temperature ranged from 3 to 30 eV. Ion temperature was found to scale roughly linearly with the ratio of power input-to-magnetic field strength, P/B.

Reinmann, J. J.↗
NASA NTRS1975

The Pioneer 10 radio occultation measurements of the ionosphere of Jupiter

Data from the Pioneer 10 radio occultation measurements are utilized to study the vertical electron number density distribution in the Jovian ionosphere. The immersion measurements were made at 26 North latitude in the late afternoon local time. The solar zenith angle in this region was 81 deg. Emersion measurements were made at 58 North latitude near the morning terminator where the solar zenith angle was 95 deg. The detectable portion of the Jovian ionosphere consists of a number of layers distributed over an altitude range of more than 3000 km. The maximum density appears to be on the order of 30,000 electrons per cu cm. Assuming that H(+) is the principal ion in the upper portion of the ionosphere yields a topside plasma temperature of 900 plus or minus 400 K.

Fjeldbo, G.↗
NASA NTRS1978

C III density diagnostics in nonequilibrium plasmas

Mass flow through a temperature gradient can produce substantial departures of the ionization states from their equilibrium values and can change the character of line emission. The effect of such flows on extreme ultraviolet intensities in the solar atmosphere is evaluated for the beryllium-sequence ion C III, which is an easily observed and powerful diagnostic of electron density in a collisionally dominated plasma. A downflow of material in a transition region can lead to an underestimate of the electron density; outflow of material, as in a stellar or solar wind passing from chromospheric to coronal temperatures, yields a reliable density diagnostic. Ambiguities in the analysis of ultraviolet emission lines can be circumvented by measurement of several transitions.

Raymond, J. C.↗
NASA NTRS1979

The determination of atmospheric trace gases using the correlation interferometer technique

The theoretical feasibility inherent in the correlation interferometry technique is demonstrated. High signal to noise and increased information content in a given partial interferogram are attractive features of the technique. The separation of interfering gas species is overcome by a precise measurement program for spectral line parameters of methane and other species. There are optical, mechanical, and electronic difficulties with the interferometry hardware design. Flight data from Cessna 402 over southeastern Virginia during April 1978 yielded amplitude fluctuations that are explainable only as internal nonlinearities. Misalignment of the AGC/interferometer optical axis also contributed to a large error source in the flight data. It is concluded that no useful data on gas burdens was obtained from these flights.

Kindle, E. C.↗
NASA NTRS1991

A new self-calibration method applied to TOMS and SBUV backscattered ultraviolet data to determine long-term global ozone change

The currently archived (1989) total ozone mapping spectrometer (TOMS) and solar backscattered ultraviolet (SBUV) total ozone data (version 5) show a global average decrease of about 9.0 percent from November 1978 to November 1988. This large decrease disagrees with an approximate 3.5-percent decrease estimated from the ground-based Dobson network. The primary source of disagreement was found to arise from an overestimate of reflectivity change and its incorrect wavelengths dependence for the diffuse plate used when measuring solar irradiance. Both of these factors have led to an overestimate of the rate of atmospheric ozone depletion by SBUV and TOMS. For total ozone measured by TOMS, a means has been found to use the measured radiance-irradiance ratio from several wavelengths pairs to construct an internally self-consistent calibration. The method uses the wavelength dependence of the sensitivity to calibration errors and the requirement that albedo ratios for each wavelength pair yield the same total ozone amounts. Smaller errors in determining spacecraft attitude, synchronization problems with the photon counting electronics, and sea-glint contamination of boundary reflectivity data have been corrected or minimized. New climatological low-ozone profiles have been incorporated into the TOMS algorithm that are appropriate for Antarctic ozone hole conditions and other low ozone cases. The combined corrections have led to a new determination of the global average total ozone trend (version 6) as a 2.9 + or - 1.3 percent decrease over 11 years (October 1978 to November 1989).

Herman, J. R.↗
NASA NTRS1993

Vibrational predissociation of methylnitrite using phase-locked ultrashort laser pulses

We solve numerically the time-dependent Schroedinger equation to study the behavior of a molecule interacting with two phase-locked ultrashort laser pulses. The 2D model used in the calculations mimics the properties of the CH3ONO molecule. The two pulses are identical except for their relative phase and are tuned to excite an upper electronic state of the molecule. After excitation the molecule predissociates, and we calculate the dependence of the NO yield and of the NO vibrational population on the delay time between the pulses.

Dateo, Christopher E.↗
NASA NTRS1997

Design of Inorganic Water Repellent Coatings for Thermal Protection Insulation on an Aerospace Vehicle

In this report, thin film deposition of one of the model candidate materials for use as water repellent coating on the thermal protection systems (TPS) of an aerospace vehicle was investigated. The material tested was boron nitride (BN), the water-repellent properties of which was detailed in our other investigation. Two different methods, chemical vapor deposition (CVD) and pulsed laser deposition (PLD), were used to prepare the BN films on a fused quartz substrate (one of the components of thermal protection systems on aerospace vehicles). The deposited films were characterized by a variety of techniques including X-ray diffraction, X-ray photoelectron spectroscopy, and scanning electron microscopy. The BN films were observed to be amorphous in nature, and a CVD-deposited film yielded a contact angle of 60 degrees with water, similar to the pellet BN samples investigated previously. This demonstrates that it is possible to use the bulk sample wetting properties as a guideline to determine the candidate waterproofing material for the TPS.

Fuerstenau, D. W.↗
NASA NTRS1997

New Potential Sources for Black Onaping Carbon

One intriguing and important issue of the Sudbury Structure concerns the source of the relatively large amount of C in the Onaping Formation Black member. This dilemma was recently addressed, and the conclusion was reached that an impactor could not have delivered all of the requisite C. Becker et al. have suggested that much of the C came from the impactor and reported the presence of interstellar He "caged" inside some fullerenes that may have survived the impact. So, conceivably, the C inventory in the Sudbury Structure comes from both target and impactor materials, although the known target rocks have little C. We discuss here the possibility of two terrestrial sources for at least some of the C: (1) impact evaporation/dissociation of C from carbonate target rocks and (2) the presence of heretofore-unrecognized C-rich (up to 26 wt%) siliceous "shale," fragments, which are found in the upper, reworked Black member. Experimental: Hypervelocity impact of a 0.635-diameter Al projectile into dolomite at 5.03 km/s (performed at the Ames Research Center vertical gun range) produced a thin, black layer (= 0.05 mm thick) that partially lined the crater and coated impactor remnants. Scanning electronic microscope (SEM) imagery shows this layer to be spongelike on a submicron scale and Auger spectroscopic analyses yield: 33% C, 22% Mg, 19% 0, and 9% Al (from the projectile). Elemental mapping shows that all of the available 0 is combined with Ca and Mg, Al is not oxidized, and C is in elemental form. Dissociation efficiency of C from CO2 is estimated to be <10% of crater volume. Raman spectroscopy indicates that the C is highly disorganized graphite. Another impact experiment [4] also produced highly disordered graphite from a limestone target (reducing collector), in addition to small amounts of diamond/lonsdaleite/chaoite (oxidizing collector). These experiments confirm the reduction of C from carbonates in impact vapor plumes. Observational: SEM observations and microprobe analyses of small, black shalelike inclusions in the upper Black Onaping indicate high C contents (7-26 wt% avg. = 16%). They contain mostly quartz and carbonaceous matter with small amounts of altered K-feldspar, clays, Fe oxide, and a sulfide. No evidence of shock is seen in quartz, and overall characteristics indicate a natural, lightly metamorphosed carbonaceous shale or mudstone that probably existed as a preimpact rock in the target region and distal fragments washed in during early crater filling. Fragments range in size from tens of microns to cm and increase in abundance in the upper Black toward the Onwatin contact, although their distribution is highly irregular. This increase corresponds to an increase in "organic" C with increasingly negative delta-13 C values and S, together with a decrease in fullerene abundance. In addition, we have found soot in acid-demineralized residues of the Onwatin but not in the Onaping samples. These data could be consistent with impact plume and atmospheric chemical processes, with possible diageneric ovedays. We are analyzing carbonaceous fractions of the Onaping and Onwatin to determine diagnostic C isotopic signatures Analyses by Whitehead et al. on bulk samples revealed no definitive source or processes, although delta-13 C values for "organic" C overlapped those for some meteorites. Discussion: If impact evaporation of Sudbury target carbonates did occur, then where are the carbonates? Distal carbonate (limestone/dolostone) exposures of the Espanola Formation (Huronian Supergroup) are generally thin-bedded, although remnants that partially encompass the Sudbury Crater are variable in thickness and may locally reach 250 m . If a carbonate thickness of 100-200 in existed at the target site, then copious amounts of C could have been reduced by impact processing of carbonates and also C-shale, depending on the efficiency of the processing and the amount of postimpact oxidation. Conclusion: The Sudbury crater offers a unique opportunity to study preserved characteristics of immediate carbonaceous fallback matter and particles of short-term residency in the impact plume as well as dust/aerosols from postimpact atmospheric processing.

Bunch, T. E.↗
NASA NTRS2003

"DUST BUSTER" - A Single Photon Ionization TOF MS for Cometary Dusts

It is hard to predict the properties and composition of dust that will be returned by STARDUST from WED- 2. The most interesting but challenging case would be grains, pg to fg in weight, each carrying its own isotopic signature characteristic of its source zones in a variety of stars. How do we extract the maximum amount of science from such grains? Clearly, the best that can be accomplished is to measure every atom in each grain.Academia Sinica and Argonne National Laboratory (ANL) have entered into a collaboration to develop a SPI TOF MS instrument for analysis of stardust grains. A new instrument will be built at Academia Sinica based on the new TOF mass spectrometer design developed, built and operating at ANL. The instrument is intended for SPI TOF MS analysis of elements from Ca to Cu plus Li after first using SIMS to measure H, C, N, 0, Si, and S. There are still technical challenges facing the technique. We will need to improve submicrometer sample handling, avoid the effects of space charge, and increase the Mamie range of the detector. The most difficult obstacle to overcome may be the fact that the flux density of present high repetition rate, WV lasers is below the level needed to ensure full ionization (saturation) in the source region, which must be several mm in size to achieve the high useful yield needed for analysis of small stardust grains. A potential breakthrough effort is to exploit the novel free electron laser being pioneered at ANL. In principle, this FEL can reach ionization saturation and is tunable up to photon energies of 25 eV, which is higher than the ionization potential of any element.

Chen, C.-Y.↗
NASA NTRS1999

A Mossbauer investigation of iron-rich terrestrial hydrothermal vent systems: lessons for Mars exploration

Hydrothermal spring systems may well have been present on early Mars and could have served as a habitat for primitive life. The integrated instrument suite of the Athena Rover has, as a component on the robotic arm, a Mossbauer spectrometer. In the context of future Mars exploration we present results of Mossbauer analysis of a suite of samples from an iron-rich thermal spring in the Chocolate Pots area of Yellowstone National Park (YNP) and from Obsidian Pool (YNP) and Manitou Springs, Colorado. We have found that Mossbauer spectroscopy can discriminate among the iron-bearing minerals in our samples. Those near the vent and on the surface are identified as ferrihydrite, an amorphous ferric mineraloid. Subsurface samples, collected from cores, which are likely to have undergone inorganic and/or biologically mediated alteration (diagenesis), exhibit spectral signatures that include nontronite (a smectite clay), hematite (alpha-Fe2O3), small-particle/nanophase goethite (alpha-FeOOH), and siderite (FeCO3). We find for iron minerals that Mossbauer spectroscopy is at least as efficient in identification as X-ray diffraction. This observation is important from an exploration standpoint. As a planetary surface instrument, Mossbauer spectroscopy can yield high-quality spectral data without sample preparation (backscatter mode). We have also used field emission scanning electron microscopy (FESEM), in conjunction with energy-dispersive X ray (EDX) fluorescence spectroscopy, to characterize the microbiological component of surface sinters and the relation between the microbiological and the mineralogical framework. Evidence is presented that the minerals found in these deposits can have multi-billion-year residence times and thus may have survived their possible production in a putative early Martian hot spring up to the present day. Examples include the nanophase property and the Mossbauer signature for siderite, which has been identified in a 2.09-billion-year old hematite-rich chert stromatolite. Our research demonstrates that in situ Mossbauer spectroscopy can help determine whether hydrothermal mineral deposits exist on Mars, which is significant for exobiology because of the issue of whether that world ever had conditions conductive to the origin of life. As a useful tool for selection of samples suitable for transport to Earth, Mossbauer spectroscopy will not only serve geological interests but will also have potential for exopaleontology.

NASA Discipline Exobiology↗
DOE OSTI2022

Precision Tomography of a Three-Qubit Donor Quantum Processor in Silicon

Nuclear spins were among the first physical platforms to be considered for quantum information processing, because of their exceptional quantum coherence and atomic-scale footprint. However, their full potential for quantum computing has not yet been realized, owing to the lack of methods with which to link nuclear qubits within a scalable device combined with multi-qubit operations with sufficient fidelity to sustain fault-tolerant quantum computation. Here we demonstrate universal quantum logic operations using a pair of ion-implanted 31 P donor nuclei in a silicon nanoelectronic device. A nuclear two-qubit controlled-Z gate is obtained by imparting a geometric phase to a shared electron spin, and used to prepare entangled Bell states with fidelities up to 94.2(2.7)%. The quantum operations are precisely characterized using gate set tomography (GST), yielding one-qubit average gate fidelities up to 99.95(2)%, two-qubit average gate fidelity of 99.37(11)% and two-qubit preparation/measurement fidelities of 98.95(4)%. These three metrics indicate that nuclear spins in silicon are approaching the performance demanded in fault-tolerant quantum processors. We then demonstrate entanglement between the two nuclei and the shared electron by producing a Greenberger-Horne-Zeilinger three-qubit state with 92.5(1.0)% fidelity. Because electron spin qubits in semiconductors can be further coupled to other electrons or physically shuttled across different locations, these results establish a viable route for scalable quantum information processing using donor nuclear and electron spins.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2026

Revealing ultrafast proton-transfer-mediated autoionization as a source of low-energy electrons in hydrogen-bonded systems

Ionizing radiation can trigger ultrafast proton transfer, a central mechanism in many chemical and biological functions, that in turn can enable or suppress electron relaxation processes and consequently cause abrupt changes in the reaction pathway. This study combines theory and experiment to probe ultrafast relaxation and dissociation in water dimers following inner- and outer-valence photoionization. By tracking electron and nuclear motion simultaneously, we reveal competing fragmentation pathways that produce low-energy electrons, which are key agents in radiation-induced chemistry, including DNA damage. While low-energy electrons are known to arise via intermolecular Coulombic decay, here we identify a faster relaxation mechanism gated by proton transfer following inner-valence ionization, which we call proton-transfer-mediated autoionization. Occurring within 10 femtoseconds, this process alters fragmentation outcomes, yielding either D 3 O + + OD + or D 2 O + + D 2 O + , depending on the interplay of proton migration and hydrogen back-transfer. Our findings underscore the intricate coupling between electronic and nuclear dynamics in hydrogen-bonded systems and establish proton-transfer-mediated autoionization as a significant pathway for low-energy electron generation.

Atomic and molecular interactions with photons↗
NASA NTRS1992

The contribution of electron collisions to rotational excitations of cometary water

The e-H2O collisional rate for exciting rotational transitions in cometary water is evaluated for conditions found in comet Halley during the Giotto spacecraft encounter. In the case of the O(sub 00) yields 1(sub 11) rotational transition, the e-H2O collisional rate exceeds that for excitation by neutral-neutral collisions at distances exceeding 3000 km from the cometary nucleus. Thus, the rotational temperature of the water molecule in the intermediate coma may be controlled by collisions with electrons rather than with neutral collisions, and the rotational temperature retrieved from high resolution infrared spectra of water in comet Halley may reflect electron temperatures rather than neutral gas temperature in the intermediate coma.

Xie, Xingfa↗
NASA NTRS1980

The heating of gas in clusters of galaxies by relativistic electrons - Collective effects

We show that the rate at which gas is heated in X-ray clusters of galaxies by streaming relativistic electrons can be much greater than the Coulomb heating rate because of the stimulated growth of a high level of electrostatic turbulence and its subsequent collapse to shorter wavelengths. This enhanced heating (and, hence, energy loss) rate allows the X-ray emitting gas to be heated by those particles which are observable through their synchrotron emission at low radio frequencies and yields a radio source size consistent with the observed radio halo sizes in the Coma cluster. The heating of gas in clusters of galaxies by relativistic electrons will significantly affect the cluster gas dynamics.

Scott, J. S.↗