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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Binary Blend All‐Polymer Solar Cells with a Record Efficiency of 17.41% Enabled by Programmed Fluorination Both on Donor and Acceptor Blocks

Abstract Despite remarkable breakthrough made by virtue of “polymerized small‐molecule acceptor (PSMA)” strategy recently, the limited selection pool of high‐performance polymer acceptors and long‐standing challenge in morphology control impede their further developments. Herein, three PSMAs of PYDT‐2F, PYDT‐3F, and PYDT‐4F are developed by introducing different fluorine atoms on the end groups and/or bithiophene spacers to fine‐tune their optoelectronic properties for high‐performance PSMAs. The PSMAs exhibit narrow bandgap and energy levels that match well with PM6 donor. The fluorination promotes the crystallization of the polymer chain for enhanced electron mobility, which is further improved by following n ‐doping with benzyl viologen additive. Moreover, the miscibility is also improved by introducing more fluorine atoms, which promotes the intermixing with PM6 donor. Among them, PYDT‐3F exhibits well‐balanced high crystallinity and miscibility with PM6 donor; thus, the layer‐by‐layer processed PM6/PYDT‐3F film obtains an optimal nanofibril morphology with submicron length and ≈23 nm width of fibrils, facilitating the charge separation and transport. The resulting PM6/PYDT‐3F devices realizes a record high power conversion efficiency (PCE) of 17.41% and fill factor of 77.01%, higher than the PM6/PYDT‐2F (PCE = 16.25%) and PM6/PYDT‐4F (PCE = 16.77%) devices.

Zhou, Dehong↗
DOE OSTI2020

Engineering Atomically Dispersed FeN 4 Active Sites for CO 2 Electroreduction

Atomically dispersed FeN 4 active sites have exhibited exceptional catalytic activity and selectivity for the electrochemical CO 2 reduction reaction (CO2RR) to CO. However, the understanding behind the intrinsic and morphological factors contributing to the catalytic properties of FeN 4 sites is still lacking. By using a Fe-N-C model catalyst derived from the ZIF-8, we deconvoluted three key morphological and structural elements of FeN 4 sites, including particle sizes of catalysts, Fe content, and Fe-N bond structures. Furthermore, their respective impacts on the CO2RR were comprehensively elucidated. Engineering the particle size and Fe doping is critical to control extrinsic morphological factors of FeN 4 sites for optimal porosity, electrochemically active surface areas, and the graphitization of the carbon support. In contrast, the intrinsic activity of FeN 4 sites was only tunable by varying thermal activation temperatures during the formation of FeN 4 sites, which impacted the length of the Fe-N bonds and the local strains. The structural evolution of Fe-N bonds was examined at the atomic level. First-principles calculations further elucidated the origin of intrinsic activity improvement associated with the optimal local strain of the Fe-N bond.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

In situ X-ray Scattering and Dynamical Modeling of Pd Catalyst Nanoparticles Formed in Flames

It has previously been demonstrated that organopalladium precursors can break down under combustion conditions, forming nanoparticles that catalyze ignition. Here, we use in situ small-angle X-ray scattering (SAXS) to probe the formation and growth of palladium nanoparticles in an ethylene fl ame doped with 28 ppm (mol) of Pd(acetate) 2 . The particles appear to nucleate in the fl ame front and are observed by SAXS to grow in size and mass in the high-temperature region of the fl ame ( ~ 2200 K) with median diameters that evolve from 1.5 to 3.0 nm. Transmission electron microscopy of particles collected on a grid located outside the fl ame shows that the particles are metallic palladium with sizes comparable to those determined by SAXS. Molecular dynamics simulation of particles of selected sizes indicates that at the fl ame temperature the particles are molten and the average mass density of the particle material is notably smaller than that of bulk, liquid Pd at the melting point. Both experimental and computational results point to homogeneous nucleation and particle - particle coalescence as mechanisms for particle formation and growth. Aerosol dynamics simulation reproduces the time evolution of the particle size distribution and suggests that a substantial fraction of the particles must be electrically charged during their growth process.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Field-induced quantum critical point in the itinerant antiferromagnet Ti 3 Cu 4

New phases of matter emerge at the edge of magnetic instabilities, which can occur in materials with moments that are localized, itinerant or intermediate between these extremes. In local moment systems, such as heavy fermions, the magnetism can be tuned towards a zero-temperature transition at a quantum critical point (QCP) via pressure, chemical doping, and, rarely, magnetic field. By contrast, in itinerant moment systems, QCPs are more rare, and they are induced by pressure or doping; there are no known examples of field induced transitions. This means that no universal behaviour has been established across the whole itinerant-to-local moment range—a substantial gap in our knowledge of quantum criticality. Here we report an itinerant antiferromagnet, Ti 3 Cu 4 , that can be tuned to a QCP by a small magnetic field. We see signatures of quantum criticality and the associated non-Fermi liquid behaviour in thermodynamic and transport measurements, while band structure calculations point to an orbital-selective, spin density wave ground state, a consequence of the square net structural motif in Ti 3 Cu 4 . Ti 3 Cu 4 thus provides a platform for the comparison and generalisation of quantum critical behaviour across the whole spectrum of magnetism.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Emergent magnetism at the 3d-5d interface: SrMnO3/SrIrO3

Recent experiments have found new magnetic behaviors, which are different from the parent bulk materials, at the interfaces between 3 d and 5 d oxides such as SrMnO 3 (SMO) and SrIrO 3 (SIO). The system is of considerable interest due to the strong spin-orbit coupling in the 5 d materials on one hand and the double exchange physics in SMO on the other, which belongs to the class of the colossal magnetoresistive (CMR) manganites. In order to gain insight into the physics of the system, we have performed density-functional studies on a selected interface structure, viz., the (SMO) 1 (SIO) 1 superlattice, which has been experimentally grown and studied. Our density-functional results show that the interfacial magnetism is controlled by a net charge transfer at the interface from the SIO to the SMO side, turning both of them into ferromagnetic metal from the original antiferromagnetic insulating state in the bulk. The transferred electrons to the SMO side make it ferromagnetic through the Anderson-Hasegawa double exchange interaction, while the SIO part becomes ferromagnetic due to the doping of the half-filled Mott-Hubbard insulator as suggested by the Nagaoka Theorem. Our results are discussed in the context of the experiments for the same structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Probing the electronic properties of gap states near the surface of n -SrTiO 3-δ / i -Si (001) heterojunctions with high sensitivity

We have measured soft x-ray resonant photoemission for the n–SrTiO 3–δ /i–Si⁡(001) (δ=~0.0003) hybrid semiconductor heterojunction with the goal of probing occupied electronic states in the band gap near the surface. By utilizing both swept energy, angle-integrated and fixed-energy, and angle-resolved spectroscopies, we identify the atomic and orbital character of the in-gap state as well as the different electronic phases that contribute to it. Specifically, we isolate the state associated with trapped charge on the n–SrTiO 3–δ surface that causes surface depletion from the localized gap state resulting from electron correlation effects in the complex oxide. Using an x-ray energy close to select dipole allowed TiL 3 → 3⁢d x-ray absorption resonances results in a 40-fold increase in sensitivity. Furthermore, this feature makes photoemission possible when probing electrons from dopants at concentrations as low as a few hundredths of a percent.

36 MATERIALS SCIENCE↗
NASA NTRS1985

New high-efficiency silicon solar cells

A design for silicon solar cells was investigated as an approach to increasing the cell open-circuit voltage and efficiency for flat-plate terrestrial photovoltaic applications. This deviates from past designs, where either the entire front surface of the cell is covered by a planar junction or the surface is textured before junction formation, which results in an even greater (up to 70%) junction area. The heavily doped front region and the junction space charge region are potential areas of high recombination for generated and injected minority carriers. The design presented reduces junction area by spreading equidiameter dot junctions across the surface of the cell, spaced about a diffusion length or less from each other. Various dot diameters and spacings allowed variations in total junction area. A simplified analysis was done to obtain a first-order design optimization. Efficiencies of up to 19% can be obtained. Cell fabrication involved extra masking steps for selective junction diffusion, and made surface passivation a key element in obtaining good collection. It also involved photolithography, with line widths down to microns. A method is demonstrated for achieving potentially high open-circuit voltages and solar-cell efficiencies.

Daud, T.↗
DOE OSTI2018

Methylxanthine Drug Monitoring with Wearable Sweat Sensors

Drug monitoring plays crucial roles in doping control and precision medicine. It helps physicians tailor drug dosage for optimal benefits, track patients' compliance to prescriptions, and understand the complex pharmacokinetics of drugs. Conventional drug tests rely on invasive blood draws. While urine and sweat are attractive alternative biofluids, the state-of-the-art methods require separate sample collection and processing steps and fail to provide real-time information. In this paper, a wearable platform equipped with an electrochemical differential pulse voltammetry sensing module for drug monitoring is presented. A methylxanthine drug, caffeine, is selected to demonstrate the platform's functionalities. Sweat caffeine levels are monitored under various conditions, such as drug doses and measurement time after drug intake. Elevated sweat caffeine levels upon increasing dosage and confirmable caffeine physiological trends are observed. This work leverages a wearable sweat sensing platform toward noninvasive and continuous point-of-care drug monitoring and management.

47 OTHER INSTRUMENTATION↗
NASA NTRS1990

Resonant tunneling IR detectors

Researchers propose a novel semiconductor heterojunction photodetector which would have a very low dark current and would be voltage tunable. A schematic diagram of the device and its band structure are shown. The two crucial components of the device are a cathode (InGaAs) whose condition band edge is below the conduction band edge of the quantum wells and a resonant tunneling filter (GaAs-AlGaAs). In a standard resonant tunneling device the electrodes are made of the same material as the quantum wells, and this device becomes highly conducting when the quantum levels in the wells are aligned with the Fermi level in the negatively biased electrode. In contrast, the researchers device is essentially non-conducting under the same bias conditions. This is because the Fermi Level of the cathode (InGaAs) is still well below the quantum levels so that no resonant transport occurs and the barriers (AlGaAs) effectively block current flow through the device. However, if light with the same photon energy as the conduction-band discontinuity between the cathode and the quantum wells, E sub c3-E sub c1, is shone on the sample, free carriers will be excited to an energy corresponding to the lowest quantum level in the well closest to the cathode (hv plue E sub c1 = E sub o). These electrons will resonantly tunnel through the quantum wells and be collected as a photocurrent in the anode (GaAs). To improve the quantum efficiency, the cathode (InGaAs) should be very heavily doped and capped with a highly reflective metal ohmic contact. The thickness of the device should be tailored to optimize thin film interference effects and afford the maximum absorption of light. Because the device relies on resonant tunneling, its response should be very fast, and the small voltages needed to change the responsivity should allow for very high frequency modulation of the photocurrent. In addition, the device is tuned to a specific photon energy so that it can be designed to detect a fairly narrow range of wavelengths. This selectivity is important for reducing the photocurrent due to spurious light sources.

Woodall, Jerry M.↗
DOE OSTI2025

Spatially Aligned Binary Single-Site Catalyst on Defective SiO 2 for Cascading Reactions

Capitalizing on the success of single-atom catalysts (SACs), dual-atom catalysts (DACs) have emerged as a new frontier in heterogeneous catalysis. However, most SACs and DACs studies seek to uniformly distribute the catalytic sites on the support material, which can hinder their effectiveness in intricate multistep cascading reactions. Particularly, it is a grand challenge to precisely control the spatial distribution of two different single sites forming binary sites so that reactants and intermediates contact the catalytic sites in the exact sequence required by the reaction steps. Here, in this work, we report a new type of binary single-site catalyst, Cu 1 –Zr 1 @SiO 2 , with Cu 1 and Zr 1 sites spatially aligned with the reaction sequence of the cascade reactions. The catalyst is synthesized by a modified reverse microemulsion approach, with single Cu sites anchored by nonbridging oxygen hole centers, which were induced by doping single Zr sites into SiO 2 . Low-energy ion scattering spectroscopy (LEIS) reveals that the outermost surface of the catalyst contains only Cu single sites, while the Zr sites are dispersed in the bulk. The catalytic performance is demonstrated in ethanol conversion to butenes, a model cascade reaction which includes ethanol dehydrogenation and aldol condensation steps. The precisely spatially controlled binary sites enable ethanol to first undergo dehydrogenation to acetaldehyde on Cu sites, followed by aldol condensation of acetaldehyde on Zr sites. As a result, C 3+ olefins selectivity as high as 77.0% (56.0% selectivity of butenes) is achieved by suppressing ethylene formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2010

Fabrication and Modification of Nanoporous Silicon Particles

Silicon-based nanoporous particles as biodegradable drug carriers are advantageous in permeation, controlled release, and targeting. The use of biodegradable nanoporous silicon and silicon dioxide, with proper surface treatments, allows sustained drug release within the target site over a period of days, or even weeks, due to selective surface coating. A variety of surface treatment protocols are available for silicon-based particles to be stabilized, functionalized, or modified as required. Coated polyethylene glycol (PEG) chains showed the effective depression of both plasma protein adsorption and cell attachment to the modified surfaces, as well as the advantage of long circulating. Porous silicon particles are micromachined by lithography. Compared to the synthesis route of the nanomaterials, the advantages include: (1) the capability to make different shapes, not only spherical particles but also square, rectangular, or ellipse cross sections, etc.; (2) the capability for very precise dimension control; (3) the capacity for porosity and pore profile control; and (4) allowance of complex surface modification. The particle patterns as small as 60 nm can be fabricated using the state-of-the-art photolithography. The pores in silicon can be fabricated by exposing the silicon in an HF/ethanol solution and then subjecting the pores to an electrical current. The size and shape of the pores inside silicon can be adjusted by the doping of the silicon, electrical current application, the composition of the electrolyte solution, and etching time. The surface of the silicon particles can be modified by many means to provide targeted delivery and on-site permanence for extended release. Multiple active agents can be co-loaded into the particles. Because the surface modification of particles can be done on wafers before the mechanical release, asymmetrical surface modification is feasible. Starting from silicon wafers, a treatment, such as KOH dipping or reactive ion etching (RIE), may be applied to make the surface rough. This helps remove the nucleation layer. A protective layer is then deposited on the wafer. The protective layer, such as silicon nitride film or photoresist film, protects the wafer from electrochemical etching in an HF-based solution. A lithography technique is applied to pattern the particles onto the protective film. The undesired area of the protective film is removed, and the protective film on the back side of the wafer is also removed. Then the pattern is exposed to HF/surfactant solution, and a larger DC electrical current is applied to the wafers for a selected time. This step removes the nucleation layer. Then a DC current is applied to generate the nanopores. Next, a large electrical current is applied to generate a release layer. The particles are mechanically suspended in the solvent and collected by filtration or centrifuge.

Ferrari, Mauro↗
DOE OSTI2015

Up-conversion routines of Er{sup 3+}–Yb{sup 3+} doped Y{sub 6}O{sub 5}F{sub 8} and YOF phosphors

Highlights: • Single-phase optical materials of Y{sub 6}O{sub 5}F{sub 8}:Er and YOF:Er were prepared. • Effective spectral converting properties were observed in Y{sub 6}O{sub 5}F{sub 8}:Er,Yb. • 980 nm diode laser was irradiated for up-converting analysis. • A multi-photon process in the phosphors was investigated. - Abstract: Optical materials composed of a Y{sub 6(1−p−q)}Er{sub 6p}Yb{sub 6q}O{sub 5}F{sub 8} (p = 0.001–0.1, q = 0.005–0.1) solid solution with Y{sub 0.99}Er{sub 0.01}OF were prepared via a solid-state reaction using excess NH{sub 4}F flux at 950 °C for 30 min. X-ray diffraction patterns of Y{sub 6(1−p−q)}Er{sub 6p}Yb{sub 6q}O{sub 5}F{sub 8} and Y{sub 0.99}Er{sub 0.01}OF were compared upon altering the synthesis temperature and the molar ratio of the NH{sub 4}F flux to the Y{sup 3+} (Er{sup 3+}, Yb{sup 3+}) ions. The effective spectral-conversion properties of Er{sup 3+} and Er{sup 3+}–Yb{sup 3+} ions in Y{sub 6}O{sub 5}F{sub 8} phosphors were monitored during excitation with a 980 nm wavelength diode-laser. Selection of appropriate Er{sup 3+} and/or Yb{sup 3+} concentrations in the Y{sub 6}O{sub 5}F{sub 8} structure led to achievement of the desired up-conversion emission, from the green to the red regions of the spectra. Furthermore, the mechanism of up-conversion in the phosphors was described by an energy-level schematic. Up-conversion emission spectra and the dependence of the emission intensity on pump power (between 193 and 310 mW) in the Y{sub 6(0.995−q)}Er{sub 0.03}Yb{sub 6q}O{sub 5}F{sub 8} phosphors were also investigated.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Data-enabled structure–property mappings for lanthanide-activated inorganic scintillators

The use of machine learning (ML) models toward development of validated structure–property relationships for two fundamental properties of activated inorganic scintillators for high energy radiation detection, namely the light yield (LY) and the decay time constant, is explored. The ML models are built on easily accessible proxies of materials—interchangeably referred to as features, descriptors or fingerprints—that are carefully selected on the basis of a physical understanding of the scintillation mechanism. Our study indicates that the developed physics-based ML models employing kernel ridge regression (KRR) and AdaBoost algorithm applied on top of a decision tree-based regression are able to “learn” the underlying design rules in a multi-dimensional feature space and thereby enable reasonably accurate predictions of the two target properties on unseen compounds (i.e., on a held-out test set). For instance, within a set of twenty-five cerium- or europium-doped scintillator materials, our analysis reveals a strong correlation between the average ionic part of the dielectric constant and the LY, irrespective of the specific chemistry of the compounds, indicating that the average ionic part of the dielectric constant is a particularly relevant descriptor toward prediction of the LY. Our results also demonstrate that, despite the use of small training datasets, the developed models are able to quickly distinguish high performing chemistries from those with relatively poor performance and therefore can play a crucial role in screening of new compounds with an attractive combination of targeted properties. Finally, the present study provides necessary motivation for future efforts involving ML models with relatively large training datasets, vast feature space explorations, and experimental design in search of promising novel scintillator chemistries.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Continuous-wave GaAs/AlGaAs quantum cascade laser at 5.7 THz

Design strategies for improving terahertz (THz) quantum cascade lasers (QCLs) in the 5–6 THz range are investigated numerically and experimentally, with the goal of overcoming the degradation in performance that occurs as the laser frequency approaches the Reststrahlen band. Two designs aimed at 5.4 THz were selected: one optimized for lower power dissipation and one optimized for better temperature performance. The active regions exhibited broadband gain, with the strongest modes lasing in the 5.3–5.6 THz range, but with other various modes observed ranging from 4.76 to 6.03 THz. Pulsed and continuous-wave (cw) operation is observed up to temperatures of 117 K and 68 K, respectively. In cw mode, the ridge laser has modes up to 5.71 THz – the highest reported frequency for a THz QCL in cw mode. The waveguide loss associated with the doped contact layers and metallization is identified as a critical limitation to performance above 5 THz.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Measuring Charged Current Muon Neutrino Cross Sections on Oxygen with the Accelerator Neutrino Neutron Interaction Experiment

The Accelerator Neutrino Neutron Interaction Experiment (ANNIE) is a $26$-ton gadolinium-doped water Cherenkov detector on-axis of the Booster Neutrino Beam (BNB) at Fermilab. With ANNIE, this dissertation provides the first results of a high statistics muon neutrino charged current cross section on oxygen at a short baseline on axis. This thesis explains the necessity of the measurements and details how the measurements are performed. Focus is given on the physics behind the models used to predict neutrino cross sections. The measurements include the CC inclusive and CC$0\pi$ cross section channels. This thesis details the processes of event selection, reconstruction, handling systematics, and unfolding as part of cross section measurements. A data unblinding procedure is documented and acts as the first implementation of data unblinding in ANNIE. These results provide additional constraints on existing neutrino interaction models and are the necessary steps for a joint analysis with liquid Argon experiments also on the BNB line.

Minock, James [Rutgers U., Piscataway (main)]↗
DOE OSTI2024

Atomically Dispersed Ru-doped Ti 4 O 7 Electrocatalysts for Chlorine Evolution Reaction with a Universal Activity

Chlorine has been supplied by the chlor-alkali process that deploys dimensionally stable anodes (DSAs) for the electrochemical chlorine evolution reaction (ClER). The paramount bottlenecks have been ascribed to an intensive usage of precious elements and inevitable competition with the oxygen evolution reaction. Herein, a unique case of Ru 2+ -O 4 active motifs anchored on Magnéli Ti 4 O 7 (Ru-Ti 4 O 7 ) via a straightforward wet impregnation and mild annealing is reported. The Ru-Ti 4 O 7 performs radically active ClER with minimal deployment of Ru (0.13 wt%), both in 5 m NaCl (pH 2.3) and 0.1 $\tiny{M}$ NaCl (pH 6.5) electrolytes. Scanning electrochemical microscopy demonstrates superior ClER selectivity on Ru-Ti 4 O 7 compared to the DSA. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a universally active ClER (over a wide range of pH and [Cl - ]), through a direct adsorption of Cl - on Ru 2+ -O 4 sites as the most plausible pathway, together with stabilized ClO* at low [Cl - ] and high pH.

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

Single‐Atomic Site Catalyst with Heme Enzymes‐Like Active Sites for Electrochemical Sensing of Hydrogen Peroxide

Abstract Heme enzymes, with the pentacoordinate heme iron active sites, possess high catalytic activity and selectivity in biosensing applications. However, they are still subject to limited catalytic stability in the complex environment and high cost for broad applications in electrochemical sensing. It is meaningful to develop a novel substitute that has a similar structure to some heme enzymes and mimics their enzyme activities. One emerging strategy is to design the Fe‐N‐C based single‐atomic site catalysts (SASCs). The obtained atomically dispersed Fe‐N x active sites can mimic the active sites of heme enzymes effectively. In this work, a SASC (Fe‐SASC/NW) is synthesized by doping single iron atoms in polypyrrole (PPy) derived carbon nanowire via a zinc‐atom‐assisted method. The proposed Fe‐SASC/NW shows high heme enzyme‐like catalytic performance for hydrogen peroxide (H 2 O 2 ) with a specific activity of 42.8 U mg −1 . An electrochemical sensor based on Fe‐SASC/NW is developed for the detection of H 2 O 2 . This sensor exhibits a wide detection concentration range from 5.0 × 10 −10 m to 0.5 m and an excellent limit of detection (LOD) of 46.35 × 10 −9 m . Such excellent catalytic activity and electrochemical sensing sensitivity are attributed to the isolated Fe‐N x active sites and their structural similarity with natural metalloproteases.

Ding, Shichao↗
DOE OSTI2018

Experimental Insights into the Growth of Single Truncated Anatase Bipyramids

Fluorine has been recognized to selectively stabilize anatase titani-um dioxide (TiO2) crystal facets, however, resolving its physical location at the nanometer scale remains empirically elusive. Here, we provide direct experimental evidence to reveal the spatial distri-bution of fluorine on single truncated anatase bipyramids (TABs) using nanoscale secondary ion mass spectrometry (NanoSIMS). Fluorine was found to preferentially adsorb on the (001) facet over the (101) facet of TABs. Moreover, NanoSIMS depth profiling exhibited a significantly different fluorine distribution between these two facets in the near-surface region, illustrating the essential role of lattice-doped fluorine in the anisotropic crystal growth of TABs.

Mulcahy, Justin R.↗