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NASA NTRS2006

Qualification of Technologies and Lessons Learned from Satellite LIDAR and Altimeter Missions

Flight qualified laser transmitters for remote sensing applications from space have progressed significantly over the past decade. More laser-based missions are underway and several are recently launched and on route, under flight build, or being proposed. However, most of the progress made in the solid state laser field has not been solely in the technology front, but more in the design and implementation of existing technologies. Recent events in flight laser performance and delivery have resulted in a more conservative process in the selection of laser-based instruments for space. The result of these efforts will hopefully be an improved rate of success and more flight laser mission awards. An overview of these efforts and some results will be presented as well as current and future work at NASA.

Coyle, Donald B.↗

DOE OSTI2013

Single Molecule Junctions: Probing Contact Chemistry and Fundamental Circuit Laws

By exploiting selective link chemistry, formation of single molecule junctions with reproducible conductance has become established. Systematic studies reveal the structure-conductance relationships for diverse molecules. I will draw on experiments from my collaborators at Columbia University, atomic-scale calculations and theory to describe progress in two areas. First, I will describe a novel route to form single molecule junctions, based on SnMe3 terminated molecules, in which gold directly bonds to carbon in the molecule backbone resulting in near ideal contact resistance [1]. Second, comparison of the conductance of junctions formed with molecular species containing either one backbone or two backbones in parallel allows demonstration of the role of quantum interference in the conductance superposition law at the molecular scale [2].

36 MATERIALS SCIENCE↗

DOE OSTI2017

Inducing superconductivity in Weyl semimetal microstructures by selective ion sputtering

By introducing a superconducting gap in Weyl or Dirac semimetals, the superconducting state inherits the nontrivial topology of their electronic structure. As a result, Weyl superconductors are expected to host exotic phenomena, such as nonzero-momentum pairing due to their chiral node structure, or zero-energy Majorana modes at the surface. These are of fundamental interest to improve our understanding of correlated topological systems, and, moreover, practical applications in phase-coherent devices and quantum applications have been proposed. Proximity-induced superconductivity promises to allow these experiments on nonsuperconducting Weyl semimetals. Here, we show a new route to reliably fabricate superconducting microstructures from the nonsuperconducting Weyl semimetal NbAs under ion irradiation. Furthermore, the significant difference in the surface binding energy of Nb and As leads to a natural enrichment of Nb at the surface during ion milling, forming a superconducting surface layer (Tc ~ 3.5 K). Being formed from the target crystal itself, the ideal contact between the superconductor and the bulk may enable an effective gapping of the Weyl nodes in the bulk because of the proximity effect. Simple ion irradiation may thus serve as a powerful tool for the fabrication of topological quantum devices from monoarsenides, even on an industrial scale.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Characterization of mechano-thermally synthesized Curie temperature-adjusted La{sub 0.8}Sr{sub 0.2}MnO{sub 3} nanoparticles coated with (3-aminopropyl) triethoxysilane

This research aimed to synthesize nanostructured strontium-doped lanthanum manganite, La{sub 0.8}Sr{sub 0.2}MnO{sub 3} (LSMO), with its Curie temperature (T{sub c}) adjusted to the therapeutic range, through a mechanothermal route. In order to investigate the effect of heat treatment temperature and duration on the resulting crystallite size, morphology, magnetic behavior and Curie temperature, the starting powder mixture was milled in a planetary ball mill before being subsequently heat treated at distinct temperatures for different time lengths. The composition, morphology, and magnetic behavior were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED) and vibrating sample magnetometer (VSM). In addition, magnetic properties were further investigated using an alternating current (AC) susceptometer and thermo-magnetic analyzer. 20 h of milling produced a crystallite size reduction leading to a decrease in the heat treatment temperature of LSMO synthesis to 800 °C. Moreover, SEM analysis has shown the morphology of a strong agglomeration of fine nanoparticles. HRTEM showed clear lattice fringes of high crystallinity. The mean crystallite and particle size of 20-hour milled sample heat treated at 1100 °C for 10 h are relatively 69 and 100 nm, respectively. The VSM data at room temperature, indicated a paramagnetic behavior for samples heat treated at 800 °C. However, by increasing heat treatment temperature to 1100 °C, LSMO indicates a ferromagnetic behavior with well-adjusted Curie temperature of 320 K, suitable for hyperthermia applications. Also, reentrant spin glass (RSG) behavior has been found in heat treated samples. The particles are coated with (3-aminopropyl) triethoxysilane (APTES) for biocompatibility purposes; Fourier transform infrared spectroscopy (FTIR) and thermo-gravimetric analysis (TGA) are used for further confirmation of APTES coating. - Highlights: • La{sub 0.8}Sr{sub 0.2}MnO{sub 3} nanoparticles were synthesized via a mechanothermal route. • We report a significant reduction in the heat treatment temperature. • The Curie temperature was tuned within the therapeutic range. • The particles were coated with (3-aminopropyl) triethoxysilane for biocompatibility purposes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2020

A de novo sacrificial-MOF strategy to construct enhanced-flux nanofiltration membranes for efficient dye removal

Nanofiltration membanes play a critical role in alleviating global water scarcity, affecting more than 4 billion people. Here, a new metal organic framework (MOF) sacrificicial strategy is designed to synthesize flux-enhancing nanofiltration membrane for efficient dye removal. With the aid of polyphenol chemistry, ZIF-67 MOF was first coated onto a porous support and in situ transformed into a selective layer by virtue of pyrrole polymerization. Trigerred by ammonium persulfate, polypyrrole selective layer functioalized nanofiltration membrane was fabricated when accompanying pore regulation by MOF self-sacrifice. The membrane demonstrated a flux enhancement of 745% than pristine polypyrrole (PPy) one with maintained rejection. Furthermore, the synergistic interactions among polypyrrole, polyphenol, and porous support endowed membrane with excellent stability during long term test. The designed MOF sacrificed route may open a new avenue for fabricating advanced energetic-efficient membranes with the reconstructed architecture towards diverse separation applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Pulsed Electrolysis Promotes Catalyst Activity in Dilute CO 2 Streams

Industrial CO 2 streams vary widely in composition, from pure to as low as 3%, posing challenges for purification or direct conversion. Electrochemical reduction offers a route for converting dilute CO 2 streams but faces severe mass transport limitations. This study demonstrates that pulsed electrolysis effectively overcomes these limitations, enhancing CO 2 electroreduction across variable feed compositions and current densities, particularly at low CO 2 concentrations and high current densities. At 25% CO 2 and 400 mA cm −2 , pulsing improved selectivity from 25.6 to 78.6%, production rate from 13.7 to 21.0 mol m −2 h −1 , and energy productivity from 0.77 to 2.59 mol kWh −1 . A dynamic, multiphysics continuum model confirms a 64% increase in CO 2 concentration within the catalyst layer during pulsing, resolving the transient chemical microenvironment. These findings establish pulsed electrolysis as a viable strategy for converting dilute industrial CO 2 streams into valuable feedstocks, bypassing costly pre-separation.

Orfali, Dania Muhieddine [New York University (NYU↗

DOE OSTI2011

Rank restriction for the variational calculation of two-electron reduced density matrices of many-electron atoms and molecules

Variational minimization of the ground-state energy as a function of the two-electron reduced density matrix (2-RDM), constrained by necessary N-representability conditions, provides a polynomial-scaling approach to studying strongly correlated molecules without computing the many-electron wave function. Here we introduce a route to enhancing necessary conditions for N representability through rank restriction of the 2-RDM. Rather than adding computationally more expensive N-representability conditions, we directly enhance the accuracy of two-particle (2-positivity) conditions through rank restriction, which removes degrees of freedom in the 2-RDM that are not sufficiently constrained. We select the rank of the particle-hole 2-RDM by deriving the ranks associated with model wave functions, including both mean-field and antisymmetrized geminal power (AGP) wave functions. Because the 2-positivity conditions are exact for quantum systems with AGP ground states, the rank of the particle-hole 2-RDM from the AGP ansatz provides a minimum for its value in variational 2-RDM calculations of general quantum systems. To implement the rank-restricted conditions, we extend a first-order algorithm for large-scale semidefinite programming. The rank-restricted conditions significantly improve the accuracy of the energies; for example, the percentages of correlation energies recovered for HF, CO, and N{sub 2} improve from 115.2%, 121.7%, and 121.5% without rank restriction to 97.8%, 101.1%, and 100.0% with rank restriction. Similar results are found at both equilibrium and nonequilibrium geometries. While more accurate, the rank-restricted N-representability conditions are less expensive computationally than the full-rank conditions.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

Electronic Absorption Spectroscopy and Photochemistry of Criegee Intermediates

Interest in Criegee intermediates (CIs), often termed carbonyl oxides, and their role in tropospheric chemistry has grown massively since the demonstration of laboratory-based routes to their formation and characterization in the gas phase. This article reviews current knowledge regarding the electronic spectroscopy of atmospherically relevant CIs like CH 2 OO, CH 3 CHOO, (CH 3 ) 2 COO and larger CIs like methyl vinyl ketone oxide and methacrolein oxide that are formed in the ozonolysis of isoprene, and of selected conjugated carbene-derived CIs of interest in the synthetic chemistry community. Of the aforementioned atmospherically relevant CIs, all except CH 2 OO and (CH 3 ) 2 COO exist in different conformers which, under tropospheric conditions, can display strikingly different thermal loss rates via unimolecular and bimolecular processes. Calculated photolysis rates based on their absorption properties suggest that solar photolysis will rarely be a significant contributor to the total loss rate for any CI under tropospheric conditions. Nonetheless, there is ever-growing interest in the absorption cross sections and primary photochemistry of CIs following excitation to the strongly absorbing 1 ππ* state, and how this varies with CI, with conformer and with excitation wavelength. Furthermore, the later part of this review surveys the photochemical data reported to date, including a range of studies that demonstrate prompt photo-induced fission of the terminal O–O bond, and speculates about possible alternate decay processes that could occur following non-adiabatic coupling to, and dissociation from, highly internally excited levels of the electronic ground state of a CI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2016

Landsat 9: Status and Plans

The Landsat 9 mission, currently under development and proceeding towards a targeted launch in late 2020, will be very similar to the Landsat 8 mission, launched in 2013. Like Landsat 8, Landsat 9 is a joint effort between NASA and USGS with two sensors, the Operational Land Imager 2 (OLI-2), essentially a copy of the OLI on Landsat 8 and the Thermal Infrared Sensor 2 (TIRS-2), very similar to the TIRS on Landsat 8. The OLI-2, like OLI, provides 14-bit image data, though for Landsat 9, all 14 bits will be retained and transmitted to the ground. The focal plane modules to be used for OLI-2 were flight spares for OLI and are currently being retested by Ball Aerospace. Results indicate radiometric performance comparable to OLI. The TIRS was a class C instrument, with a 3-year design lifetime, and therefore had limited redundancy. TIRS-2 will be a class B instrument, with a 5-year design lifetime, like OLI (and OLI-2), necessitating design changes to increase redundancy. The stray light and Scene Select Mechanism (SSM) encoder problems observed on orbit with TIRS have also instigated a few design changes to TIRS-2. Stray light analysis and testing have indicated that additional baffles in the TIRS-2 optical system will suppress the out-of-field response. The SSM encoder problems have not been definitively traced to a route cause, though conductive anodic filament growth in the circuit boards is suspected. Improved designs for the encoder are being considered for TIRS-2. The spare Focal Plane Array (FPA) from TIRS is planned for use in TIRS-2; FPA spectral and radiometric performance testing is scheduled for September of this year at NASA's Goddard Space Flight Center.

Landsat↗

DOE OSTI2019

Design and Synthesis of Highly-Dispersed WO 3 Catalyst with Highly Effective NH 3 –SCR Activity for NO x Abatement

The development of high-efficiency catalysts, especially for selective catalytic reduction of NO x with NH 3 (NH 3 –SCR) catalysts, with outstanding low-temperature catalytic reactivity and impressive lifetime remains a great challenge in the field of eliminating vehicle engine exhausts. In this work, we present a novel gas-bubbling-assisted dispersed hybrid nanocrystal-assisted hydrothermal deposition (GBD-HNHD) strategy to fabricate a W@CeZrAlO x catalyst with highly dispersed WO 3 nanocrystals (10 wt %) (W@CZA-HNHD). Compared with the W/CeZrAlO x catalyst prepared with the impregnation method (W@CZA-IM), W@CZA-HNHD not only exhibits highly effective low-temperature deNO x activity (the light-off temperature being lowered 45 °C) but also shows an exceptional stability (100 h time-on-stream testing with seven measurement cycles) and long lifetime (compares well with 135,000 miles). This work not only provides a new route to prepare an advanced catalyst with high loading isolated active sites but also lays a foundation for optimizing the utilization efficiency of the catalytically active species in the practical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Tunable catalytic activity of cobalt-intercalated layered MnO2 for water oxidation through confinement and local ordering

We report that the lowering of reaction overpotentials is a persistent and universal goal in the development of catalysts for (photo)electrochemistry, which can usually be facilitated by selectively stabilizing one reaction inter-mediate over another. In this mechanistic study of the oxygen evolution reaction (OER) catalyzed by cobalt-intercalated layered MnO 2 , we show that confinement effects and local cobalt atomic ordering in the interlayer space can be synergistically used to tune the adsorption energies of O, OH, and OOH reaction intermediates and the scaling relationship between them. In general, the interlayer confinement destabilizes the adsorption of intermediates for the OER, but clustering Co atoms can selectively stabilize the adsorption of OOH in particular. After considering both effects, our model predicts an overpotential of 0.30 V for the Co-intercalated MnO 2 catalyzed OER, in excellent agreement with the experimental result of 0.36 V. These new insights explain the enhanced catalytic performance of MnO 2 by intercalating atoms and illuminate a route for engineering non-toxic precious-metal-free catalysts through designed layered materials.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Amorphous TiO 2 Compact Layers via ALD for Planar Halide Perovskite Photovoltaics

A low temperature (< 120 °C) route to pinhole-free amorphous TiO 2 compact layers may pave the way to more efficient, flexible, and stable inverted perovskite halide device designs. Toward this end, we utilize low-temperature thermal atomic layer deposition (ALD) to synthesize ultra-thin (12 nm) compact TiO 2 underlayers for planar halide perovskite PV. While device performance with as-deposited TiO 2 films is poor, we identify room temperature UV-O 3 treatment as a route to device efficiency comparable to crystalline TiO 2 thin films synthesized by higher temperature methods. Here, we further explore the chemical, physical, and interfacial properties 2 that might explain the improved performance through x-ray diffraction, spectroscopic ellipsometry, Raman spectroscopy, and x-ray photoelectron spectroscopy. These findings challenge our intuition about effective electron selective layers as well as point the way to a greater selection of flexible substrates and more stable inverted device designs.

14 SOLAR ENERGY↗

DOE OSTI2022

Fabrication of Biofunctionalized PVA/PEI Nanofibers for Rare Earth Element Extraction from Coal Mine Tailings

The need for rare earth elements (REEs) for new technology is becoming increasingly stiff with demand at a record high. Biological ligands like lanmodulin and lanthanide binding tags (LBT) have gained noticeable attention for their selective extraction of valuable lanthanide metals in aqueous solution. Building on previous work using microbeads as the extraction media, we propose that nanofibers can improve extraction capabilities. Nanofibers could provide more efficient flow and higher extraction yields due to their high surface area to volume ratio. Relying on thiolmaleimide click chemistry as the biological ligand immobilization route, electrospinning as the nanofiber manufacturing method, and numerous characterization techniques, we produced electrospinning polymer solutions and nanofibers with a maximum neodymium adsorbent capacity of 12.1 μmol/g of extraction media immobilized with LBT. Although the prior work produced an extraction media with an equivalent capacity of ~40 μmol/g, the electrospinning process is much more economical and scalable. This work paves the way for an industrially relevant, environmentally-friendly REE extraction material. Further work is required to produce higher quality nanofibers, to investigate common ion interference with REE adsorbance, and to scale production up to a relevant scale.

01 COAL, LIGNITE, AND PEAT↗

NASA NTRS2010

Methods and circuitry for reconfigurable SEU/SET tolerance

A device is disclosed in one embodiment that has multiple identical sets of programmable functional elements, programmable routing resources, and majority voters that correct errors. The voters accept a mode input for a redundancy mode and a split mode. In the redundancy mode, the programmable functional elements are identical and are programmed identically so the voters produce an output corresponding to the majority of inputs that agree. In a split mode, each voter selects a particular programmable functional element output as the output of the voter. Therefore, in the split mode, the programmable functional elements can perform different functions, operate independently, and/or be connected together to process different parts of the same problem.

Shuler, Jr., Robert L.↗

NASA NTRS2011

Shape Memory Alloy Actuator Design: CASMART Collaborative Best Practices

Upon examination of shape memory alloy (SMA) actuation designs, there are many considerations and methodologies that are common to them all. A goal of CASMART's design working group is to compile the collective experiences of CASMART's member organizations into a single medium that engineers can then use to make the best decisions regarding SMA system design. In this paper, a review of recent work toward this goal is presented, spanning a wide range of design aspects including evaluation, properties, testing, modeling, alloy selection, fabrication, actuator processing, design optimization, controls, and system integration. We have documented each aspect, based on our collective experiences, so that the design engineer may access the tools and information needed to successfully design and develop SMA systems. Through comparison of several case studies, it is shown that there is not an obvious single, linear route a designer can adopt to navigate the path of concept to product. SMA engineering aspects will have different priorities and emphasis for different applications.

Benafan, Othmane↗

NASA NTRS2016

Essential SpaceWire Hardware Capabilities for a Robust Network

The Geostationary Operational Environmental Satellite R-Series Program (GOES-R) mission is a joint program between National Oceanic & Atmospheric Administration (NOAA) and National Aeronautics & Space Administration (NASA) Goddard Space Flight Center (GSFC). GOES-R project selected SpaceWire as the best solution to satisfy the desire for simple and flexible instrument to spacecraft command and telemetry communications. GOES-R development and integration is complete and the observatory is scheduled for launch October 2016. The spacecraft design was required to support redundant SpaceWire links for each instrument side, as well as to route the fewest number of connections through a Slip Ring Assembly necessary to support Solar pointing instruments. The final design utilized two different router designs. The SpaceWire standard alone does not ensure the most practical or reliable network. On GOES-R a few key hardware capabilities were identified that merit serious consideration for future designs. Primarily these capabilities address persistent port stalls and the prevention of receive buffer overflows. Workarounds were necessary to overcome shortcomings that could be avoided in future designs if they utilize the capabilities, discussed in this paper, above and beyond the requirements of the SpaceWire standard.

SpaceWire↗

DOE OSTI2018

Management of Metals from Decommissioning of Nuclear Facilities - 18411

The EDF group companies within the Cyclife platform have for decades performed treatment and recycling of metals. With different approaches but all considered international Good Practice, as valuable materials are recovered for safe recycling and volumes in the repositories for radioactive waste are saved. For an efficient decommissioning project, a well-defined waste management process is one of the critical paths, not least when it comes to routes for clearance and recycling of materials. It is easy to underestimate the complexity and bottlenecks caused by shortage of logistic space. In order to mitigate these risks, activities such as strengthening categorization, quantification and adopting different routes based on the material properties should be implemented. By categorization of the of waste and materials considered/classified as contaminated or potentially contaminated it is obvious that the management of the metals is a key parameter in nuclear decommissioning. Analyses performed by the EDF companies shows that a majority of the materials, classified as contaminated, from a BWR/PWR plant are metals. Experience gives that a high percentage of these metals from decommissioning can be subject to recycling either directly upon completion of the clearance process or after certain treatment. Non-technical key parameters like the regulatory requirements on applying the waste hierarchy, the impact on repository programs as well as, not at least, the regulatory and public acceptance of recycling of materials from the nuclear industry are, together with costs essential factors when forming the routing of metals and other waste materials from a decommissioning project. Today the EDF group companies are positioned to provide a wide range of services for management of the contaminated metals from decommissioning projects, spanning from industrial management of metals which directly will be subject general clearance after verification measurements up to decontamination and melting of selected reactor internals for recycling to public domain or within the nuclear industry. In this paper the typical waste material composition for BWR and PWR plants, the different ways to treat/manage the radioactive and potentially radioactive metals including a comparison of the different approach commonly used in a technical, logistical and economical perspectives. A few success stories will be resented as well as lessons learned. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Radiochemical Characterization of PWR Control Rods - 19030

NRG has, in cooperation with the German partner Hoefer and Bechtel, performed a radiochemical characterization of the control rods from a German Pressurized Water Reactor. To perform the cutting and sampling of the spent control rods at the reactor site NRG has developed a dedicated, remotely operated tool. This tool enabled the sampling of both the stainless steel tube and the absorber material from the upper, middle and lower parts of selected rods. The samples were transported from the reactor site to NRG's laboratories at Petten, the Netherlands, were they were analysed chemically and radiologically. Due to the different chemical constitution of the control rod tubes and the absorber, the procedures for the chemical separation of the different compounds, prior to the radiological characterization, varied. The route for the stainless steel tube samples turned out more complex than that for the absorber samples: there are more nuclides to be determined, and therefore more treatment steps and component separations were necessary. Subsequently to the component separations, the radiochemical characterization was performed using alpha and gamma spectrometry and the Liquid Scintillation Counting (LSC) technique. The results of the measurements in combination with simulations performed with a reactor physics code provided for a better understanding about the distribution of radionuclides in absorber rods, both in the rod tubes and the absorber core. In addition, the results of the measurements can be used to validate reactor physics codes. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗