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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 649 records · Page 36
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Study of perovskite CsPbBr 3 detector polarization and its mitigation with ultrahigh x-ray flux

High-flux capable semiconductor x-ray detectors are essential in various applications, but the detrimental effects of detector polarization limit their use in many cases. Here, for this work, we studied the polarization of perovskite CsPbBr 3 semiconductor detectors using ultrahigh flux synchrotron x rays (10 6 –10 12 photons s –1 mm –2 at 58.61 keV). The CsPbBr 3 detectors did not show immediate polarization prominently until a flux higher than 10 10 photons s –1 mm –2 . Using the pump-and-probe technique, we visualized the spatial and temporal effects of polarization. The polarized region, represented by reduced photocurrent, extended beyond the area under direct irradiation, and the reduced photocurrent persisted after potential de-polarization treatments. We found that stronger applied electric fields and fewer carrier traps can mitigate polarization, represented by less photocurrent deficit. By examining the detectors’ current response under controlled ambient light, low, and high-flux x rays, we studied the trap filling and release behavior of CsPbBr 3 . We discovered that the polarization is caused by partial detector damage due to deep defects generated by ultrahigh flux x-ray irradiation. Our work provides insight into CsPbBr 3 polarization under extremely intense x-ray radiation and shows that reducing crystal defects and increasing detector bias voltage are effective solutions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1973

Parametric instability of a relativistically strong electromagnetic wave.

The stability of a circularly polarized electromagnetic wave that is strong enough to make plasma electrons, but not ions, relativistic is studied. Small perturbations are considered which propagate parallel to the large-amplitude driver. A relativistically strong wave can be unstable on time scales as short as twice its own oscillation period, and decays into a forward-going plasma oscillation and either one or two electromagnetic waves. Ion motion introduces an additional instability which can be important at short perturbation wavelengths, where the driver would otherwise be stable. The unstable ion and electron modes both have potential for producing anomalously large acceleration of relativistic particles, as well as significant amounts of backscattered light. These effects may be important in two applications: (1) the use of intense lasers to heat or compress plasma, and (2) the plasma surrounding a pulsar, if the pulsar is losing energy by radiation of electromagnetic waves at its rotation frequency. Instability persists in the nonrelativistic regime, reducing to stimulated Raman scattering as a special case.

Max, C. E.↗
DOE OSTI2023

Overview and first measurements of the MAST Upgrade bolometer diagnostic

Here, a suite of multi-channel resistive bolometers has been implemented to measure the total radiation from Mega Amp Spherical Tokamak Upgrade plasmas, with cameras covering the core plasma and lower divertor chamber. Data are digitized and processed using novel field-programmable gate array-based electronics, offering improved compactness and new operational capabilities. A synthetic diagnostic has been developed to explore the quality of 2D reconstructions available from the system and to quantify the uncertainty on quantities such as the total radiated power. Measurements in the first campaign have demonstrated correct functioning of the diagnostic while also highlighting issues with electrical noise and some failure mechanisms of the detectors, as well as significant neutral beam fast-particle losses.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Microwave Heating of Nanocrystals for Rapid, Low-Aggregation Intermetallic Phase Transformations

The use of intermetallic Pt–Co nanocrystals (NCs) for the electrocatalytic oxygen reduction reaction is quickly gaining interest thanks to the higher electrochemical stability of the intermetallic L1 o phase compared to a random alloy A1 phase. However, the thermal treatment that enables the intermetallic phase transformation also causes considerable NC aggregation, resulting in a significant loss of electrochemically active surface area. Herein, we report the use of microwave radiation to induce the intermetallic phase transformation in Cu-doped Pt–Co NCs. We demonstrate that microwave radiation reduces NC aggregation while allowing for a complete phase transformation in only 30 s. Furthermore, these microwave-treated NCs demonstrate higher mass activity for the oxygen reduction reaction while maintaining electrochemical stability similar to the thermally annealed samples.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Improvements to the characterization of Agfa x-ray film for use on opacity spectroscopy diagnostics

The National Ignition Facility uses a soft x-ray opacity spectrometer for x-ray spectral imaging in high-energy-density experiments. The increased demand for a better spectral resolution prompted the investigation into the Agfa D4 film. Characterization is already under way for the film. A Manson x-ray source using six different anodes was used to expose film to the linear optical density (OD) region. This is a continuation of the previous work, and the updated analysis process is communicated here. The identified uncertainties have been reduced with the updated steps that improve the results of the characterization process. In conclusion, when the Stanford Synchrotron Radiation Lightsource Beamline 16-2 was operational, the film was characterized at that source. Its beam offered a higher fluency with a lower exposure time needed to reach saturation. Results for both sources are compared in this paper.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

A perspective on the device physics of lead halide perovskite semiconducting detector for gamma and x-ray sensing

Metal-halide perovskites are emerging materials for radiation sensing featuring high absorption cross section, high charge mobility, and long carrier lifetime enabling superior detection efficiencies even at room temperature. Perovskite detector technologies are more complex involving different detecting modes and device architectures. Here, to elucidate the working principles, we provide a Perspective on the device structures and the operational principles of halide perovskite direct conversion detectors for radiation sensing. We will first discuss different detection modes and introduce the commonly used device architectures and their working principles. Based on our work and pioneer developments in the field, we will next compare the performances of the reported detectors. Additionally, we will summarize the single crystal detectors and polycrystalline thin film devices and discuss their advantages and disadvantages for different applications. Finally, we provide a future Perspective on the critical problems that must be addressed to commercialize this technology.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Direct Measurement of the Selective Microwave-Induced Heating of Agglomerates of Dipolar Molecules: The Origin of and Parameters Controlling a Microwave Specific Superheating Effect

Agglomerates of polar molecules in nonpolar solvents are selectively heated by microwave radiation. The magnitude of the selective heating was directly measured by using the temperature dependence of the intensities of the Stokes and anti-Stokes bands in the Raman spectra of p-nitroanisole (pNA) and mesitylene. Under dynamic heating conditions, a large apparent temperature difference (ΔT) of over 100 °C was observed between the polar pNA solute and the nonpolar mesitylene solvent. This represents the first direct measurement of the selective microwave heating process. The magnitude of the selective microwave heating was affected by the properties of the agglomerated pNA. As the concentration of the pNA increases, the magnitude of the selective heating of the pNA was observed to decrease. This is explained by the tendency of the pNA dipoles to orient in an antiparallel fashion in the aggregates as measured by the Kirkwood g value, which decreased with increasing concentration. This effect reduces the net dipole moment of the agglomerates, which decreases the microwave absorption. After the radiation was terminated, the effective temperature of the dipolar molecules returned slowly to that of the medium. The slow heat transfer was modeled successfully by treating the solutions as a biphasic solvent/solute system. Based on modeling and the fact that the agglomerate can be heated above the boiling temperature of the solvent, an insulating layer of solvent vapor is suggested to form around the heated agglomerate, slowing convective heat transfer out of the agglomerate. Furthermore, this is an effect unique to microwave heating.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1987

A new formulation of electromagnetic wave scattering using an on-surface radiation boundary condition approach

A new formulation of electromagnetic wave scattering by convex, two-dimensional conducting bodies is reported. This formulation, called the on-surface radiation condition (OSRC) approach, is based upon an expansion of the radiation condition applied directly on the surface of a scatterer. It is now shown that application of a suitable radiation condition directly on the surface of a convex conducting scatterer can lead to substantial simplification of the frequency-domain integral equation for the scattered field, which is reduced to just a line integral. For the transverse magnetic case, the integrand is known explicitly. For the transverse electric case, the integrand can be easily constructed by solving an ordinary differential equation around the scatterer surface contour. Examples are provided which show that OSRC yields computed near and far fields which approach the exact results for canonical shapes such as the circular cylinder, square cylinder, and strip. Electrical sizes for the examples are ka = 5 and ka = 10. The new OSRC formulation of scattering may present a useful alternative to present integral equation and uniform high-frequency approaches for convex cylinders larger than ka = 1. Structures with edges or corners can also be analyzed, although more work is needed to incorporate the physics of singular currents at these discontinuities. Convex dielectric structures can also be treated using OSRC.

Kriegsmann, Gregory A.↗
DOE OSTI2025

Coherent frequency combs from electrons colliding with a laser pulse

Highly coherent and powerful light sources capable of generating soft x-ray frequency combs are essential for high precision measurements and rigorous tests of fundamental physics. In this work, we derive the analytical conditions required for the emission of coherent radiation from an electron beam colliding with a laser pulse, modeled as a plane wave. These conditions are applied in a series of numerical simulations, where we show that a soft x-ray frequency comb can be produced if the electrons are regularly-spaced and sufficiently monoenergetic. High quality beams of this kind may be produced in the near future from laser-plasma interactions or linear accelerators. Furthermore, we highlight the advantageous role of employing few-cycle laser pulses in relaxing the stringent monoenergeticity requirements for coherent emission. The conditions derived here can also be used to optimize coherent emission in other frequency ranges, such as the terahertz domain.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Multiterminal Inverse AC Josephson Effect

When a Josephson junction is exposed to microwave radiation, it undergoes the inverse AC Josephson effect–the phase of the junction locks to the drive frequency. As a result, the I–V curves of the junction acquire “Shapiro steps” of quantized voltage. If the junction has three or more superconducting contacts, coupling between different pairs of terminals must be taken into account and the state of the junction evolves in a phase space of higher dimensionality. Here, we study the multiterminal inverse AC Josephson effect in a graphene sample with three superconducting terminals. We observe robust fractional Shapiro steps and correlated switching events, which can only be explained by considering the device as a completely connected Josephson network. We successfully simulate the observed behaviors using a modified two-dimensional RCSJ model. Our results suggest that multiterminal Josephson junctions are a playground to study highly connected nonlinear networks with novel topologies.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Toward an integrated multi-gigahertz ionizing particle diagnostic

Needs arising at both current and future accelerator facilities call for the development of radiation-hardened position-sensing diagnostics that can operate with multi-GHz repetition rates. Such instruments are likely to also have applications in the diagnosis of rapid plasma behavior. Here, building on the recent work of our Advanced Accelerator Diagnostics Collaboration, we are exploring the development of integrated multi-GHz ionizing particle detection systems based on chemical-vapor deposition diamond sensors, with the initial goal of producing a quadrant detector that can determine the intensity and centroid position of a particle beam at a repetition rate between 5 and 10 GHz. Results from our initial high-speed characterization work are presented, including those from a single-channel sensor with a GHz response. Approaches to achieving multi-GHz (5–10 GHz) rate capability, including the design of a dedicated Application Specific Integrated Circuit and the use of 3D RF-solver computer aided design software, are presented and discussed in more detail. 3D RF simulations suggest clean pulses of duration less than 250 ps (FWHM less than 125 ps) can be achieved with the approaches developed by this work.

43 PARTICLE ACCELERATORS↗
DOE OSTI2024

Demonstration of low-mode shape control in indirect-drive double shell implosions at the NIF

Double shell inertial confinement fusion is a concept for achieving robust thermonuclear burn that uses dense metal shells to compress deuterium-tritium (DT) fuel to fusion conditions. Double shell implosions are typically indirectly driven and involve a target that consists of a low-Z ablator, a foam layer, and a high-Z pusher surrounding the DT fuel. The goal of the campaign is to achieve a volumetric burn as radiation losses from the DT fuel are trapped by the opaque high-Z shell. The overall performance of double shell implosions relies on the efficient collisional transfer of kinetic energy between layers. The efficiency of this transfer (and therefore the overall performance of a given implosion) is degraded by the presence of low-mode asymmetries. P2 asymmetries are often observed in spatially resolved 2D radiographs of nominal double shell implosions. This work discusses three such experiments: one with an oblate P2 asymmetry, one with a prolate P2 asymmetry, and one with an approximate spherical symmetry. After performing a shape analysis of the oblate and prolate implosions to quantify asymmetries, these experimental results were compared with the results of hydrodynamic simulations for the two experiments. Differences between the experiment and simulation were then used to design an approximately spherical implosion by altering the incident laser cone fraction. Radiographs from the experiment that implemented the modified cone fraction show evidence of an implosion that is approximately spherical until bang time. This design is intended to serve as a point design for future studies that will seek to optimize various aspects of the double shell target.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

0D, 1D, 2D, and 3D simulations of an idealized coaxial impedance-matched Marx generator

We have conducted 0D, 1D, 2D, and 3D simulations of an idealized coaxial impedance-matched Marx generator (IMG) []. The 0D calculations were conducted with a four-element circuit model; the 1D, 2D, and 3D calculations were conducted with highly resolved, fully electromagnetic representations. The IMG consists of 30 stages distributed axially and connected electrically in series. Each stage is powered by two bricks separated by 180° and connected electrically in parallel. Each brick comprises two opposite-polarity capacitors in series with a single switch. The bricks drive an internal impedance-matched coaxial transmission line terminated by a resistive load. The simulations neglect effects due to the switch-triggering circuit, the capacitor-charging circuit, external conducting boundaries, and reactive components of the load. We find dimensionality does not significantly affect the electrical power delivered by the IMG to its load: peak load powers estimated by the 0D, 1D, 2D, and 3D simulations agree to within 1%. The 3D calculations demonstrate that electromagnetic power radiated by the bricks, and axial gaps between stages, reduces the peak load power by less than ∼ 1 % . Each simulation assumes the load impedance is 34% above that at which the load power is maximized. Operating an IMG with such an overmatched load offers several advantages while decreasing the peak load power by only 2%. The 0D, 1D, 2D, and 3D models outlined herein could be adapted to assess computationally competing IMG designs, and conduct a variety of numerical IMG experiments, an IMG is constructed. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗
DOE OSTI2022

Photobiocatalysis for Abiological Transformations

Harnessing biocatalysts for novel abiological transformations is a longstanding goal of synthetic chemistry. Combining the merits of biocatalysis and photocatalysis allows for selective transformations fueled by visible light and offers many advantages including new reactivity, high enantioselectivity, greener syntheses, and high yields. Photoinduced electron or energy transfer enables synthetic methodologies that complement conventional two electron processes or offer orthogonal pathways for developing new reactions. Enzymes are well suited and can be tuned by directed evolution to exert control over radical intermediates thereby suppressing undesirable reactions and delivering high chemo- and stereoselectivities. Within the past decade, the combination of biocatalysis and photocatalysis was mainly focused on exploiting light-regenerated cofactors to increase native enzymatic activity. However, recent developments have demonstrated that the combination can unlock new-to-nature chemistry. Particularly, the discovery and application of new strategies are well poised to expand the applications of photobiocatalysis. In the past three years, our lab has been studying the combinations of photocatalysis and biocatalysis which can be applied to create new synthetic methodologies and solve challenges in synthetic organic chemistry. Our efforts have expanded the strategies for combining external photocatalysts with enzymes through the construction of a synergistic cooperative stereoconvergent reduction system consisting of photosensitized energy transfer and ene-reductase catalyzed alkene reduction. Additionally, our efforts have also extended the capability of cofactor-dependent photoenzymatic systems to include enantioselective bimolecular radical hydroalkylations of alkenes by irradiating electron donor-acceptor complexes comprised of enzymatic redox active cofactors and unnatural substrates. In this Account, we highlight strategies developed by our group and others for combining biocatalysis and photocatalysis with the aim of introducing nonnatural reactivity to enzymes. Presently, strategies applied to achieve this goal include the repurposing of newly discovered photoactive enzymes, the elucidation of new photoreactivity within cofactor-dependent enzymes, the combination of external photocatalysts with enzymes, and the construction of artificial photoenzymes. By demonstrating the successful application of these strategies for achieving selective new-to-nature transformations, we hope to spur interest in the expanding the scope of photobiocatalytic systems through the use and extension of these strategies and creation of new strategies. In addition, we hope to elucidate the intuition in synergizing the unique capabilities of biocatalysis and photocatalysis so that photobiocatalysis can be recognized as a potential solution to difficult challenges in synthetic organic chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Robust and Highly Conductive Water-Stable Copper Iodide-Based Hybrid Single Crystals

High conductivity, carrier mobility as well as long diffusion length are critical for highly efficient solar cells. Here, we report new types of crystalline inorganic-organic hybrid semiconductors, 2D-Cu 2 I 2 (L) [L = benzo[c][1,2,5]thiadiazole (bs) and benzo[c][1,2,5] selenadiazole (bse)], composed of one-dimensional (1D) copper iodide staircase-like chain and benzodiazole-based ligands. These compounds possess narrow and tunable band gaps and high conductivity. High-quality large single crystals of 2D-Cu 2 I 2 (bse) were grown and used to evaluate the charge transport properties of the material. State-of-the-art time-resolved microwave conductivity (TRMC) techniques were used to investigate the charge carrier dynamics, from which a high conductivity of 2 × 10 -4 S/cm, a carrier mobility of ~1 cm 2 V -1 s -1 , a maximum doping/carrier density of 2 +/- 1 × 10 15 cm -3 , and a diffusion length of ~0.17 um were obtained. We report the excellent water/chemical stability combined with high conductivity makes this I-VII-based hybrid material family promising candidates for potential optoelectronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

(NH 3 (CH 2 ) 7 NH 3 ) 2 Sn 3 I 10 , a Vacancy-Ordered Three-Dimensional Tin(II) Perovskite-Derived Semiconductor

Ordering vacancies in hybrid Sn(II) halide semiconductors provides a strategy for preventing uncontrolled oxidation and formation of mobile holes. In this study, we report the structure and optical and electronic properties of (NH 3 (CH 2 ) 7 NH 3 ) 2 Sn 3 I 10 , a vacancy-ordered perovskite derivative with three-dimensional inorganic connectivity. The crystal structure resembles that of a Dion–Jacobson layered perovskite derivative, but with [SnI 5 ] square pyramids bridging the layers. UV–vis diffuse reflectance spectroscopy reveals a sharp onset of light absorption at 1.86(1) eV with the photoluminescence emission maximum at 1.90(1) eV. However, the maximum excitation occurs from 3.42 to 3.81 eV (325 to 370 nm), revealing a significant Stokes shift of 1.3 eV. The electronic properties determined from dark and time-resolved microwave conductivity measurements reveal a minimum carrier mobility of 4.3 × 10 –2 cm 2 V –1 s –1 and a maximum carrier density of 5.96 × 10 16 cm –3 , a uniquely low value for a hybrid Sn(II) halide semiconductor. The transport behavior in combination with first-principles calculations of the electronic band structure and dielectric permittivity suggest polaron-mediated electronic transport, yet the photogenerated carriers have a fast and fluence-dependent nonradiative recombination rate, suggestive of localized “defect-like” states at the band edge. The observed photoluminescence is most consistent with single-ion-like behavior of an asymmetric Sn(II) environment. Together, these results suggest that defect ordering presents a strategy for the reduction of mobile charge carriers at equilibrium.

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

Microwave-Assisted Reactive CO 2 Capture with the SrCO 3 -Graphite System

This study details the initial development of a microwave heat-driven reactive CO 2 capture (RCC) process using the SrO/SrCO 3 cycle and graphitic carbon to absorb ppm-levels of CO 2 from humidified room temperature air and selectively convert it into CO. By combining first-principles density functional theory (DFT) simulations with thermogravimetric analysis (TGA) and X-ray diffraction (XRD) verification, it is demonstrated that SrO spontaneously absorbs moisture to generate Sr(OH) 2 followed by Sr(OH) 2 *1H 2 O, which then can spontaneously react with atmospheric levels of CO 2 to form SrCO 3 . The resulting SrCO 3 can then react with solid carbon at elevated temperatures to selectively produce CO and regenerate SrO. Graphitic carbon is an excellent microwave absorber that can quickly generate temperatures approaching 1000 °C and then cool to room temperature within minutes, potentially allowing for integration with intermittent electricity. It is shown that using microwaves to selectively heat a mixture of graphitic carbon and SrCO 3 produced CO with 85 ± 3% selectivity and stable performance over ten cycles. The rapid heating for release and room temperature CO 2 uptake processes appeared to prevent performance loss from particle sintering typically observed with traditional thermal systems. In conclusion, these results demonstrate a new RCC approach that adds to the growing number of potential technologies available for converting CO 2 to useful chemicals.

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

Temperature Homogeneity under Selective and Localized Microwave Heating in Structured Flow Reactors

Selective heating of different phases of multiphase systems via microwaves can result in energy savings and suppression of side reactions. However, materials properties and operating conditions that maximize temperature gradients are poorly understood. Here we utilize computational fluid dynamics (CFD) computations and temperature measurements in structured flow reactors (monoliths) in a monomodal microwave cavity to assess the temperature difference between the walls and the fluid and develop a simple lumped model to estimate when temperature gradients exist. We also explore the material’s thermal and electrical properties of structured reactors for isothermal catalyst conditions. We propose that CFD simulations can be used as a nonintrusive, predictive tool of temperature homogeneity. Importantly, we demonstrate that localized heating in the bed under several conditions rather than selective heating is responsible for the selectivity enhancement. Furthermore, our results indicate that structured beds made of high thermal conductivity materials avoid arcing and enable temperature homogeneity and low electrical conductivity materials allow microwaves to penetrate the domain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗