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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 703 records · Page 39
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Kinetic isotope effects for dissociative recombination of tritiated ketenyl ion ( 3 HCCO + ): A surface-hopping ab initio molecular dynamics study

Dissociative recombination (DR) reactions are important when modeling charged species in the presence of free electrons. While experimental measurements of DR reaction rates are challenging, surface hopping ab initio molecular dynamics (SH-AIMD) simulations provide an attractive alternative. SH-AIMD is especially well-suited for estimating branching ratios, i.e., the relative rates of competing production channels, for DR reactions. Although the radiolysis of diatomic tritium has been studied experimentally, previous attempts to model these systems have failed to account for isotope effects in DR reactions. Previous SH-AIMD studies have also not investigated tritium isotope effects for the branching ratios of DR reactions. In this study, we compute the DR branching ratios of the protiated and tritiated ketenyl ion. Comparison with literature values for the protiated branching ratios provides confidence in the reliability of our SH-AIMD results. Our simulations predict a significant increase of the HC + CO branching ratio for the tritiated system.

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

Controlled Single-Electron Transfer via Metal–Ligand Cooperativity Drives Divergent Nickel-Electrocatalyzed Radical Pathways

Electrocatalysis enables the construction of C-C bonds under mild conditions via controlled formation of carbon-centered radicals. For sequences initiated by alkyl halide reduction, coordinatively unsaturated Ni complexes commonly serve as single-electron transfer agents, giving rise to the foundational question of whether outer- or inner-sphere electron transfer oxidative addition prevails in redox mediation. Indeed, rational design of electrochemical processes requires the discrimination of these two electron transfer pathways, as they can have outsized effects on the rate of substrate bond activation and thus impact radical generation rates and downstream product selectivities. We present results from combined synthetic, electroanalytical, and computational studies that examine the mechanistic differences of single electron transfer to alkyl halides imparted by Ni metal-ligand cooperativity. Electrogenerated reduced Ni species, stabilized by delocalized spin density onto a redox-active tpyPY2Me polypyridyl ligand, activates alkyl iodides via outer-sphere electron transfer, allowing for the selective activation of alkyl iodide substrates over halogen atom donors and the controlled generation and sequestration of electrogenerated radicals. In contrast, the Ni complex possessing a redox-innocent pentapyridine congener activates the substrates in an inner-sphere fashion owning to a purely metal-localized spin, thereby activating both substrates and halogen atom donors in an indiscriminate fashion, generating a high concentration of radicals and leading to unproductive dimerization. Overall, our data establish that controlled electron transfer via Ni-ligand cooperativity can be used to limit undesired radical recombination products and promote selective radical processes in electrochemical environments, providing a generalizable framework for designing redox mediators with distinct rate and potential requirements.

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

Electrically driven amplified spontaneous emission from colloidal quantum dots

Colloidal quantum dots (QDs) are attractive materials for realizing solution-processable laser diodes that could benefit from size-controlled emission wavelengths, low optical-gain thresholds and ease of integration with photonic and electronic circuits. However, the implementation of such devices has been hampered by fast Auger recombination of gain-active multicarrier states, poor stability of QD films at high current densities and the difficulty to obtain net optical gain in a complex device stack wherein a thin electroluminescent QD layer is combined with optically lossy charge-conducting layers. Here we resolve these challenges and achieve amplified spontaneous emission (ASE) from electrically pumped colloidal QDs. The developed devices use compact, continuously graded QDs with suppressed Auger recombination incorporated into a pulsed, high-current-density charge-injection structure supplemented by a low-loss photonic waveguide. These colloidal QD ASE diodes exhibit strong, broadband optical gain and demonstrate bright edge emission with instantaneous power of up to 170 μW.

36 MATERIALS SCIENCE↗
NASA NTRS1983

Photoelectrochemical electrodes

The surface of a moderate band gap semiconductor such as p-type molybdenum sulfide is modified to contain an adherent film of charge mediating ionene polymer containing an electroactive unit such as bipyridimium. Electron transport between the electrode and the mediator film is favorable and photocorrosion and recombination processes are suppressed. Incorporation of particles of catalyst such as platinum within the film provides a reduction in overvoltage. The polymer film is readily deposited on the electrode surface and can be rendered stable by ionic or addition crosslinking. Catalyst can be predispersed in the polymer film or a salt can be impregnated into the film and reduced therein.

Williams, R. M.↗
NASA NTRS1987

Molecular processes in a high temperature shock layer

Research was completed on several aspects of dissociative recombination (DR) for the molecules NO(+), N2(+), and O2(+). For O2(+), DR with an electron is described by, O2(+) + e(-) yields O + O. Model studies were completed of the windows arising in DR cross section from excited ion vibrational levels and of the variation of the DR cross section with the intersection point of the ion and neutral dissociative state potential curves.

Guberman, Steven L.↗
NASA NTRS2016

Enhanced O2 Loss at Mars Due to an Ambipolar Electric Field from Electron Heating

Recent results from the MAVEN Langmuir Probe and Waves (LPW) instrument suggest higher than predicted electron temperatures (T sub e) in Mars dayside ionosphere above approx. 180 km in altitude. Correspondingly, measurements from Neutral Gas and Ion Mass Spectrometer (NGIMS) indicate significant abundances of O2+ up to approx. 500 km in altitude, suggesting that O2+ may be a principal ion loss mechanism of oxygen. In this article, we investigate the effects of the higher T(sub e) (which results from electron heating) and ion heating on ion outflow and loss. Numerical solutions show that plasma processes including ion heating and higher T(sub e) may greatly increase O2+ loss at Mars. In particular, enhanced T(sub e) in Mars ionosphere just above the exobase creates a substantial ambipolar electric field with a potential (e) of several k(sub b)T(sub e), which draws ions out of the region allowing for enhanced escape. With active solar wind, electron and ion heating, direct O2+ loss could match or exceed loss via dissociative recombination of O2+. These results suggest that direct loss of O2+ may have played a significant role in the loss of oxygen at Mars over time.

Mars↗
NASA NTRSDate not supplied

Dissociative Recombination (DR) and Associative Ionization (AI) Cross Section Calculations for the NO+ + e yields N + O (2D+3P, 2P+3P, and 2D+1D) Reaction for Atmospheric Entry Modeling

During entry of a space craft into Earth atmosphere, the flow surrounding the vehicle becomes partially ionized leading to significant cation and free-electron production. Subsequently, electron impact excitation and dissociation form radiating excited state species that contribute to the heat load on the vehicle. While experimental data on selected total cross sections are available, few experiments address the need for accurate AI cross sections for metastable atomic states at the high temperatures realized in atmospheric re-entry. In order to maintain desired safety margins during atmospheric entry of a space vehicle, chemical reaction models need to accurately account for this process. For the present study, we have computed vibrationally resolved cross sections for the DR of NO+ for electron energies between 0.01 to 10 eV and apply microscopic reversibility to obtain the AI cross sections and rate coefficients. For the DR cross section calculations, we use state-of-the-art MRCI potential energy curves. The resulting adiabatic potential curves are transformed to a diabatic representation, which is used in time-dependent wave packet calculations to describe the nuclear motion of the dissociating cation upon collision with an electron. Based on the wave function evolution in time, these calculations provide T-matrix and cross sections for the DR including recombination into the low energy metastable atomic states. The DR and AI rate coefficients are compared with the available experimental data.

Ewa Papajak↗
DOE OSTI2020

Fermi Level Engineering of Passivation and Electron Transport Materials for p-Type CuBi 2 O 4 Employing a High-Throughput Methodology

Metal oxide semiconductors are promising for solar photochemistry if the issues of excessive charge carrier recombination and material degradation can be resolved, which are both influenced by surface quality and interface chemistry. Coating the semiconductor with an overlayer to passivate surface states is a common remedial strategy but is less desirable than application of a functional coating that can improve carrier extraction and reduce recombination while mitigating corrosion. Here, a data-driven materials science approach utilizing high-throughput methodologies, including inkjet printing and scanning droplet electrochemical cell measurements, is used to create and evaluate multi-element coating libraries to discover new classes of candidate passivation and electron-selective contact materials for p-type CuBi 2 O 4 . The optimized overlayer (Cu 1.5 TiO z ) improves the onset potential by 110 mV, the photocurrent by 2.8×, and the absorbed photon-to-current efficiency by 15.5% compared to non-coated photoelectrodes. It is shown that these enhancements are related to reduced surface recombination through passivation of surface defect states as well as improved carrier extraction efficiency through Fermi level engineering. This work presents a generalizable, high-throughput method to design and optimize passivation materials for a variety of semiconductors, providing a powerful platform for development of high-performance photoelectrodes for incorporation into solar-fuel generation systems.

36 MATERIALS SCIENCE↗
DOE OSTI2023

The role of native defects and their diffusivity in CdTe

CdTe is a leading thin-film technology for solar-cell applications. Basic features such as the optimum band gap of 1.5 eV and simple manufacturing process have been driving the research on improving the current record efficiency of 22% for CdTe solar cells toward the theoretical limit of 32%. Low p-type doping and short carrier lifetimes in the CdTe absorber have been suggested as the main limiting factors and attributed to defect compensation and carrier recombination. Understanding the role of point defects and impurities in CdTe is crucial to solving these problems. Despite many years of research, the sources of compensation and the microscopic recombination mechanisms are still unclear. By using hybrid density functional calculations with spin-orbit coupling and large supercells, we investigate the electronic properties, the formation energies, and the diffusivities of the native defects in CdTe. As possible sources of compensation for p-type conductivity, we discuss the structural and electronic properties of Cd interstitial, Te vacancies, and TeCd antisites. The stability of each defect is discussed in terms of both the defect formation energy and the migration barrier. We also address possible mechanisms that lead to non-radiative recombination.

14 SOLAR ENERGY↗
DOE OSTI2023

Design of InGaN-ZnSnGa 2 N 4 quantum wells for high-efficiency amber light emitting diodes

A novel type-II InGaN-ZnSnGa 2 N 4 quantum well (QW) structure is proposed based on recent experimental achievements for the successful epitaxy of ZnSnN 2 -GaN alloys and the determination of their band offsets with GaN. The simulation results indicate that this structure is promising as the active region for high-efficiency InGaN-based amber (λ ~ 590 nm) light-emitting diodes (LEDs). The hole wavefunction in the valence band is better confined with the insertion of a monolayer scale of ZnSnGa 2 N 4 into the InGaN QW while the electron wavefunction in the conduction band is better confined with the incorporation of an AlGaN layer in the GaN quantum barrier. The band structure of the InGaN-ZnSnGa 2 N 4 QW is numerically simulated based on the experimentally measured band offsets between ZnSnGa 2 N 4 and GaN. With the InGaN-ZnSnGa 2 N 4 QW design, a low In content (20%) is required in the InGaN layer to reach a peak emission wavelength of ~590 nm, yet an In composition of 25% is needed to reach the same emission wavelength for a conventional InGaN QW with the same layer thicknesses. Moreover, the electron-hole wavefunction overlap (Гe1-hh1) for the InGaN-ZnSnGa 2 N 4 QW design reaches 18% for an emission wavelength at ~590 nm. This result is much improved over the conventional InGaN QW overlap of 5% emitting at the same wavelength. The increase in electron-hole wavefunction overlap results in an approximately 14 times enhancement in the predicted spontaneous emission radiative recombination rate of the InGaN-ZnSnGa 2 N 4 QW as compared to that of the conventional InGaN QW. This InGaN-ZnSnGa 2 N 4 QW structure design can be promising to pave a new way to achieve high efficiency amber LEDs.

42 ENGINEERING↗
NASA NTRS2004

The Gas Chromatograph Mass Spectrometer for the Huygens Probe

Titan is unique in the solar system, the only moon that has a dense atmosphere. The major constituents of the atmosphere, nitrogen and methane, are continuously broken apart by a combination of solar UV, impinging electrons from Saturn s magnetosphere, and a steady flux of cosmic rays. The resulting molecular fragments recombine and form a variety of new species, many of which were detected for the first time by Voyager1 . The ubiquitous, surface- hiding aerosol blanket manifests the existence of still more complex compounds. In addition to hydrocarbons and nitriles, the atmosphere is known to contain CO, CO2 and externally delivered H2O. The Gas Chromatograph Mass Spectrometer (GCMS) on the Huygens Probe will measure the chemical composition of the atmosphere of Titan from 170 Km altitude (approximately 1hPa) to the surface (approximately 1500hPa) and determine the isotope ratios of the major constituents. The GCMS will also analyze gas samples from the Aerosol Collector Pyrolyser (ACP) and may be able to obtain compositional information of several surface materials. The GCMS consists of a quadrupole mass spectrometer (QP) with a secondary electron multiplier ion detector, a three-column gas chromatograph (GC) and an elaborate gas sampling system. The gas sampling system will provide atmospheric samples to the QP for nearly continuous analysis during the Probe descent and batch samples at several altitudes for GC analysis. It also contains a chemical scrubber for noble gas analysis and an enrichment cell for trace constituent enhancement. In addition to the sampling of the atmosphere periodic gas samples, derived from the pyrolysis of aerosols, will be transferred from the ACP to the GCMS for direct QP and full GCMS analysis. The QP can analyze molecular masses from 2 to 141Dalton. The nominal detection threshold is at a mixing ratio of 10E-8. Data rate is 885 bits/sec. The mass of the instrument is 17.3 kg and the energy required for operation during the descent is 110 Watt-hours.

Niemann, H. B.↗
NASA NTRS1980

Recombination lasing in a magnetoplasmadynamic arcjet

The plasmadynamic recombination laser concept is verified experimentally in a high-power quasisteady MPD arcjet operating at 4 kA and 12 g/sec of argon. Measurements of the spatial variation of electron temperature, electron density, and population densities in the arc exhaust flow confirm that inverted populations of the 4p to 4s Ar II transitions are established by collisional-radiative recombination of the Ar III ion. Using an optical cavity aligned transversely to the flow, recombination lasing of seven such transitions, 5145, 4880, 4764, 4727, 4658, 4579, and 4545 A, is observed spectrophotographically and photoelectrically over the entire 1-msec discharge.

Campbell, E. M.↗
NASA NTRS2004

The Gas Chromatograph Mass Spectrometer for the Huygens Probe

Titan is unique in the solar system, the only moon that has a dense atmosphere. The major constituents of the atmosphere, nitrogen and methane, are continuously broken apart by a combination of solar UV, impinging electrons from Saturn's magnetosphere, and a steady flow of cosmic rays. The resulting molecular fragments recombine and form a variety of new species, many of which were detected for the first time by Voyager 1. The ubiquitous, surface-hiding aerosol blanket manifests the existence of still more complex compounds. In addition to hydrocarbons and nitriles, the atmosphere is known to contain CO, CO2 and externally delivered H2O. The Gas Chromatograph Mass Spectrometer (GCMS) on the Huygens Probe will measure the chemical composition of the atmosphere of Titan from 170 km altitude (approximately lhPa) to the surface (approximately 1500hPa) and determine the isotope ratios of the major constituents. The GCMS will also analyze gas samples from the Aerosol Collector Pyrolyser (ACP) and may be able to obtain compositional information of several surface materials. The GCMS consists of a quadrupole mass spectrometer (QP) with a secondary electron multiplier ion detector, a three-column gas chromatograph (GC) and an elaborate gas sampling system. The gas sampling system will provide atmospheric samples to the QP for nearly continuous analysis during the Probe descent and batch samples at several altitudes for GC analysis. It also contains a chemical scrubber for noble gas analysis and an enrichment cell for trace constituent enhancement. In addition to the sampling of the atmosphere periodic gas samples, derived from the pyrolysis of aerosols, will be transferred from the ACP to the GCMS for direct QP and full GCMS analysis. The QP can analyze molecular masses from 2 to 14lDalton. The nominal detection threshold is at a mixing ratio of 10E-8. Data rate is 885 bits/sec. The mass of the instrument is 17.3 kg and the energy required for operation during the descent is 110 Watt-hours.

Niemann, H. B.↗
NASA NTRS1977

Recombination lasing in a magnetoplasmadynamic arcjet

The plasmadynamic recombination laser concept is verified experimentally in a high power quasi-steady MPD arcjet operating at 4 kA and 12 g/sec of argon. Measurements of the spatial variation of electron temperature, electron density, and population densities in the arc exhaust flow confirm that inverted populations of the 4p to 4s Ar II transitions are established by collisional-radiative recombination of the Ar III ion. Using an optical cavity aligned transversely to the flow, recombination lasing of four such transitions, 5145, 4880, 4764 and 4727 A, is observed spectro-photographically and photoelectrically over the entire 1-msec discharge.

Campbell, E. M.↗
NASA NTRS1992

Spectroscopy of a Balmer-dominated filament in the Cygnus Loop with the Hopkins Ultraviolet Telescope

A fair UV spectrum of a nonradiative filament in the Cygnus Loop covering the wavelength range 830-1860 A at 3.5-A resolution was obtained using the Hopkins Ultraviolet Telescope (HUT) on the Astro-1 space shuttle mission. Nonradiative shock models which include a more sophisticated treatment of Lyman line transfer are calculated. It is found that the HUT spectrum can be explained in terms of a shock with velocity 175-185 km/s propagating into a low-density medium. This shock velocity can be reconciled with the 135-km/s width of the broad component of H-alpha in this filament if equilibration of the postshock electron and ion temperatures proceeds much more rapidly than Coulomb equilibration time scales. The time required for a 180-km/s shock to develop a partial recombination zone is short, about 200 yr if n is approximately equal to 2/cu cm. This suggests that the shock is decelerating as it encounters denser material. The current analysis patently favors rapid equilibration of electrons and ions behind the shock.

Long, Knox S.↗
NASA NTRS2006

Electronics Shielding and Reliability Design Tools

It is well known that electronics placement in large-scale human-rated systems provides opportunity to optimize electronics shielding through materials choice and geometric arrangement. For example, several hundred single event upsets (SEUs) occur within the Shuttle avionic computers during a typical mission. An order of magnitude larger SEU rate would occur without careful placement in the Shuttle design. These results used basic physics models (linear energy transfer (LET), track structure, Auger recombination) combined with limited SEU cross section measurements allowing accurate evaluation of target fragment contributions to Shuttle avionics memory upsets. Electronics shielding design on human-rated systems provides opportunity to minimize radiation impact on critical and non-critical electronic systems. Implementation of shielding design tools requires adequate methods for evaluation of design layouts, guiding qualification testing, and an adequate follow-up on final design evaluation including results from a systems/device testing program tailored to meet design requirements.

Wilson, John W.↗
DOE OSTI2021

Efficient interlayer electron transfer in a MoTe 2 /WS 2 /MoS 2 trilayer heterostructure

Electron transfer and carrier dynamics in MoTe 2 /WS 2 /MoS 2 trilayer heterostructures are investigated by transient absorption and photoluminescence measurements. Monolayer flakes of MoTe 2 , WS 2 , and MoS 2 are obtained by mechanical exfoliation from their bulk crystals and are used to fabricate the heterostructures by a dry-transfer technique. Here, photoluminescence spectroscopic measurements indicate that the recombination of the MoS 2 and WS 2 intralayer excitons is significantly suppressed in the heterostructure, illustrating the efficient interlayer charge transfer processes. Layer-selective time-resolved differential reflectance measurements show that the electrons excited in MoTe 2 can transfer to MoS 2 within 0.3 ps. The transferred electrons show a long lifetime of several hundred picoseconds due to their slow recombination with the spatially separated holes that reside in MoTe 2 . Furthermore, the charge transfer and recombination processes are weakly dependent on the injected carrier density. These results demonstrate the feasibility of constructing van der Waals multilayer heterostructures involving the infrared-sensitive MoTe 2 with emergent properties and provide important information to quantify the performance of MoTe 2 - based devices.

2D materials↗
DOE OSTI2024

Photo‐Induced Charge State Dynamics of the Neutral and Negatively Charged Silicon Vacancy Centers in Room‐Temperature Diamond

Abstract The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi‐color confocal microscopy and density functional theory are used to examine photo‐induced SiV recombination — from neutral, to single‐, to double‐negatively charged — over a broad spectral window in chemical‐vapor‐deposition (CVD) diamond under ambient conditions. For the SiV 0 to SiV ‐ transition, a linear growth of the photo‐recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV ‒ , on the other hand, yields only fractional recombination into SiV 2‒ , a finding that is interpreted in terms of a photo‐activated electron tunneling process from proximal nitrogen atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗