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At least 757 records · Page 42

All sources NASA NTRS DOE OSTI

DOE OSTI2021

Single-Step Direct Laser Writing of Multimetal Oxygen Evolution Catalysts from Liquid Precursors

We investigate a laser direct-write method to synthesize and deposit metastable, mixed transition metal oxides and evaluate their performance as oxygen evolution reaction catalysts. This laser processing method enabled the rapid synthesis of diverse heterogeneous alloy and oxide catalysts directly from cost-effective solution precursors, including catalysts with a high density of nanocrystalline metal alloy inclusions within an amorphous oxide matrix. The nanoscale heterogenous structures of the synthesized catalysts were consistent with reactive force-field Monte Carlo calculations. By evaluating the impact of varying transition metal oxide composition ratios, we created a stable Fe 0.63 Co 0.19 Ni 0.18 O x /C catalyst with a Tafel slope of 38.23 mV dec -1 and overpotential of 247 mV, a performance similar to that of IrO 2 . Synthesized Fe 0.63 Co 0.19 Ni 0.18 O x /C and Fe 0.14 Co 0.46 Ni 0.40 O x /C catalysts were experimentally compared in terms of catalytic performance and structural characteristics to determine that higher iron content and a less crystalline structure in the secondary matrix decreases the charge transfer resistance and thus is beneficial for electrocatalytic activity. Furthermore, this conclusion is supported by density-functional theory calculations showing distorted active sites in ternary metal catalysts are key for lowering overpotentials for the oxygen evolution reaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Spatial separation of triplet excitons drives endothermic singlet fission

Molecules that undergo singlet fission, converting singlet excitons into pairs of triplet excitons, have potential as photovoltaic materials. The possible advantages of endothermic singlet fission (enhanced use of photon energy and larger triplet energies for coupling with common absorbers) motivated us to assess the role of exciton delocalization in the activation of this process. Here we report the synthesis of a series of linear perylene oligomers that undergo endothermic singlet fission and have endothermicities in the range 5-10 kBT at room temperature in solution. We study these compounds using transient spectroscopy and modelling to unravel the singlet and triplet dynamics. We show that the minimal number of coupled chromophores needed to undergo endothermic singlet fission is three, which provides sufficient statistical space for triplet excitons to separate and avoid annihilation - and a subsequent fast return to the singlet state. Our data additionally suggest that torsional motion of chromophores about the molecular axis following triplet-pair separation contributes to the increase in entropy, thus lengthening the triplet lifetime in longer oligomers.

14 SOLAR ENERGY↗

DOE OSTI2020

Colloidal quantum wells for optoelectronic devices

Colloidal quantum wells, also called nanoplatelets, are nanoscopic materials displaying quantum confinement in two dimensions. Unlike colloidal quantum dots, colloidal quantum well ensembles have no inhomogeneous broadening due to an atomically-precise definition of the short axis, a fact which results in much narrower ensemble absorption and emission. Thus, colloidal quantum wells can translate many advantages of colloidal nanocrsytals or other solution-processable materials, such as scalable synthesis and substrate-agnostic deposition (particularly compared to epitaxial quantum wells), without sacrificing material uniformity. Furthermore, due to very narrow photoluminescnece peaks, these materials have found a home in applications involving light emission, such as downconversion enhancement films, light-emitting diodes, and lasers, in which they represent some of the best performers among solution-cast materials. As argued in this review, the full spectrum of epitaxial quantum well devices offers a roadmap to other potential applications, such as detection, electronics, electro-optics, non-linear optics, or intersubband devices, in which only nascent efforts have been made.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Rigid cationic ligands enable high-efficiency NIR-II photoluminescence in copper( i ) iodide hybrid semiconductors

Near-infrared (NIR) luminescent materials are pivotal for advanced optoelectronic and biomedical applications, yet attaining efficient emission in the NIR-II region (950-1400 nm) remains challenging. Here, we introduce a ligand cationization strategy for designing copper(i) iodide-organic hybrid materials that emit in the NIR-II region (920-1120 nm) with PLQYs up to 8.58%. By incorporating rigid cationic ligands with CuI modules, we synergistically achieve bandgap narrowing (to 1.51 eV) and structural rigidification via ionic-dative bonding, effectively suppressing non-radiative decay while extending emission beyond 1100 nm. Coupled with solution processability-enabled by the successful synthesis of nanometer-sized nanoparticles in various shapes-and excellent thermal stability (≥210 °C), this work establishes ligand cationization as a universal approach for designing efficient NIR-II emitters.

Chen, Jingwen↗

DOE OSTI2025

Structure and ultrafast dynamics of tri-nuclear Ag-/Tl–Pt 2 POP 4 complexes in solution

The energetics and dynamics of ion assembly in solution has broad influence in nanomaterials and inorganic synthesis. To investigate the fundamental processes involved, we present a time-resolved x-ray solution scattering (TR-XSS) study of the trinuclear silver and thallium complexes of the diplatinum ion PtPOP [Pt 2 (H 2 P 2 O 5 )$_4^{4−}$] in aqueous solution. These complexes, their structural properties, and their electronic structure are not well understood and afford a unique opportunity to study the metal–metal bond formation that influences molecular and material assembly in solution. We present model-independent analysis of the observed dynamics as well as an analysis incorporating time-resolved structural refinements of key bond lengths with $<$100 fs time resolution. We find that upon photoexcitation, the Pt atoms contract ∼0.25 Å toward the center of both the Ag- and the Tl-PtPOP complexes, as previously observed for the PtPOP anion. For the AgPtPOP system, an ultrafast Ag-Pt bond expansion of ∼0.2 Å is observed, whereas in contrast, the TlPtPOP system exhibits a Tl-Pt bond contraction of ∼0.3 Å upon photoexcitation. For both complexes, the change in electronic state leads to coherent (“wave-packet”) oscillations along the metal–Pt coordinates. Based on these structural dynamics, we propose an electronic structure model that describes the metal–metal bonding behavior in both the ground and excited state for both complexes.

Lenzen, Philipp [Technical Univ. of Denmark, Lyngb↗

DOE OSTI2023

Sustainable chemistry with plasmonic photocatalysts

There is a pressing global need to increase the use of renewable energy sources and limit greenhouse gas emissions. Towards this goal, highly efficient and molecularly selective chemical processes that operate under mild conditions are critical. Plasmonic photocatalysis uses optically resonant metallic nanoparticles and their resulting plasmonic, electronic, and phononic light-matter interactions to drive chemical reactions. The promise of simultaneous high-efficiency and product-selective reactions with plasmon photocatalysis provides a compelling opportunity to rethink how chemistry is achieved. Plasmonic nanoparticles serve as nanoscale ‘antennas’ that enable strong light–matter interactions, surpassing the light-harvesting capabilities one would expect purely from their size. Complex composite structures, combining engineered light harvesters with more chemically active components, are a focal point of current research endeavors. In this review, we provide an overview of recent advances in plasmonic catalysis. We start with a discussion of the relevant mechanisms in photochemical transformations and explain hot-carrier generation and distributions from several ubiquitous plasmonic antennae. Then we highlight three important types of catalytic processes for sustainable chemistry: ammonia synthesis, hydrogen production and CO 2 reduction. To help elucidate the reaction mechanism, both state-of-art electromagnetic calculations and quantum mechanistic calculations are discussed. This review provides insights to better understand the mechanism of plasmonic photocatalysis with a variety of metallic and composite nanostructures toward designing and controlling improved platforms for green chemistry in the future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1973

M-ary Laguerre detection.

In a communication system using optical devices, the receiver is modeled as a counter of electrons which are emitted from a photodetector when a modulated optical wave is incident on it. The synthesis of the optimal receiver processing and its resulting performance depend upon the statistics associated with this counting. In an M-ary system, the transmitter selects one of a set of M intensities for the optical process. Questions of error probability are investigated.

Mohanty, N. C.↗

NASA NTRS1986

A new readily processable polyimide

As part of an effort to develop tough solvent resistance thermoplastics for potential use as structural resins on aerospace vehicles, a new processable polyimide was evaluated. The synthesis involved the reaction of a new diamine, 1,3-bis 2-(3-aminophenoxy)ethyl ether, with 3,3',4,4'-benzophenonetetracarboxylic dianhydride to form the polyamic acid and subsequent conversion of it to the polyimide. Various physical properties such as thermal stability, solvent resistance, glass transition temperature, crystalline melt temperature, melt viscosity and mechanical properties such as fracture toughness, adhesive, film and composite properties are reported. Of particular interest is the extremely high titanium to titanium tensile shear strength obtained for this polyimide.

Harris, F. W.↗

NASA NTRS1987

A new readily processable polyimide

Harris, F. W.↗

NASA NTRS1987

Detection of interstellar PN - The first phosphorus-bearing species observed in molecular clouds

Phosphorus nitride (PN) has been detected in the interstellar medium. The J = 2-1, 3-2, 5-4, and 6-5 rotational lines of this species have been observed toward Orion-KL, and the J = 2-1 transition in Sgr B2 and W51. The PN line profiles in Orion indicate that the molecule's emission arises from the 'plateau' or 'doughnut' region associated with the outflow from IRc2. The species is thus primarily present in hot, dense gas. Column densities derived for PN toward Orion-KL are (3-4) x 10 to the 13th/sq cm, but may be as high as 10 to the 14th/sq cm, if the species is located in a 10-arcsec region. These column densities imply a fractional abundance for PN in the Orion 'plateau' of (1-4) x 10 to the -10th. Such a large abundance for PN is not predicted by quiescent cloud ion-molecule chemistry and suggests that high-temperature processes are responsible for the synthesis of PN in the KL outflow.

Ziurys, L. M.↗

NASA NTRS1990

Developing a taxonomy for mission architecture definition

The Lunar and Mars Exploration Program Office (LMEPO) was tasked to define candidate architectures for the Space Exploration Initiative to submit to NASA senior management and an externally constituted Outreach Synthesis Group. A systematic, structured process for developing, characterizing, and describing the alternate mission architectures, and applying this process to future studies was developed. The work was done in two phases: (1) national needs were identified and categorized into objectives achievable by the Space Exploration Initiative; and (2) a program development process was created which both hierarchically and iteratively describes the program planning process.

Neubek, Deborah J.↗

NASA NTRS1992

Self-replication of chemical systems based on recognition within a double or a triple helix - A realistic hypothesis

A scenario is proposed for the non-enzymatic self-replication of short RNA molecules. The self-replication of an oligopyrimidine strand is considered and the process of template-directed synthesis based on recognition within a double helix is discussed. Replication mechanisms are suggested for selected oligonucleotides. The mechanisms are based on Watson-Crick base pairing between complementary nucleotides as well as Hoogsteen base pairing between a duplex and the complementary third strand. It is suggested that self-replication based on these mechanisms may be accomplished but may result in a substantial amount of misinformation transfer when mixed oligonucleotides are used.

Kanavarioti, Anastassia↗

NASA NTRS1991

A new variable testability measure

In this paper, we propose a new Variable Testability Measure (VTM) for implementing testability at the high-level synthesis stage of the design process of integrated circuits. This new approach, based on binary decision diagrams, representing fully functional blocks of a circuit, and on their cyclomatic testability measures. It manipulates dataflow blocks to predict whether the circuit is testable and the vector set required to test it.

Jamoussi, M.↗

NASA NTRS1995

How far away is plug 'n' play? Assessing the near-term potential of sonification and auditory display

The commercial music industry offers a broad range of plug 'n' play hardware and software scaled to music professionals and scaled to a broad consumer market. The principles of sound synthesis utilized in these products are relevant to application in virtual environments (VE). However, the closed architectures used in commercial music synthesizers are prohibitive to low-level control during real-time rendering, and the algorithms and sounds themselves are not standardized from product to product. To bring sound into VE requires a new generation of open architectures designed for human-controlled performance from interfaces embedded in immersive environments. This presentation addresses the state of the sonic arts in scientific computing and VE, analyzes research challenges facing sound computation, and offers suggestions regarding tools we might expect to become available during the next few years. A list of classes of audio functionality in VE includes sonification -- the use of sound to represent data from numerical models; 3D auditory display (spatialization and localization, also called externalization); navigation cues for positional orientation and for finding items or regions inside large spaces; voice recognition for controlling the computer; external communications between users in different spaces; and feedback to the user concerning his own actions or the state of the application interface. To effectively convey this considerable variety of signals, we apply principles of acoustic design to ensure the messages are neither confusing nor competing. We approach the design of auditory experience through a comprehensive structure for messages, and message interplay we refer to as an Automated Sound Environment. Our research addresses real-time sound synthesis, real-time signal processing and localization, interactive control of high-dimensional systems, and synchronization of sound and graphics.

Bargar, Robin↗

NASA NTRS1996

Potential Commercial Applications from Combustion and Fire Research in Space

The near-zero (microgravity) environment of orbiting spacecraft minimizes buoyant flows, greatly simplifying combustion processes and isolating important phenomena ordinarily concealed by the overwhelming gravity-driven forces and flows. Fundamental combustion understanding - the focus to date of the NASA microgravity-combustion program - has greatly benefited from analyses and experiments conducted in the microgravity environment. Because of the economic and commercial importance of combustion in practice, there is strong motivation to seek wider applications for the microgravity-combustion findings. This paper reviews selected technology developments to illustrate some emerging applications. Topics cover improved fire-safety technology in spacecraft and terrestrial systems, innovative combustor designs for aerospace and ground propulsion, applied sensors and controls for combustion processes, and self-sustaining synthesis techniques for advanced materials.

Friedman, Robert↗

NASA NTRS1996

Overview of Microgravity Combustion Research at NASA Lewis Research Center and its Potential Commercial Impact

The near-zero (microgravity) environment of orbiting spacecraft minimizes buoyant flows, greatly simplifying combustion processes and isolating important phenomena ordinarily concealed by the overwhelming gravity-driven forces and flows. Fundamental combustion understanding has greatly benefited from analyses and experiments conducted in the microgravity environment. Because of the economic and commercial importance of combustion in practice, there is strong motivation to seek wider applications for the microgravity-combustion findings. This paper reviews selected technology developments to illustrate some emerging applications. Topics cover improved fire-safety technology in spacecraft and terrestrial systems, innovative combustor designs for aerospace and ground propulsion, applied sensors and controls for combustion processes, and self-sustaining synthesis techniques for advanced materials.

Lyons, Valerie↗

NASA NTRS1994

The r-, s-, and p-Processes in Nucleosynthesis

A goal of this paper is to review the recent progress astrophysicists, astronomers, and physicists have made in the r-, s-, and p-processes in nucleosynthesis and to point out the problems that remain in our understanding of the formation of the heavy nuclei. Another, perhaps deeper, goal is to to seek some understanding of why there are three major processes available to nature for synthesis of heavy elements.

Meyer, Bradley S.↗

NASA NTRS1998

A Novel Approach for Adaptive Signal Processing

Adaptive linear predictors have been used extensively in practice in a wide variety of forms. In the main, their theoretical development is based upon the assumption of stationarity of the signals involved, particularly with respect to the second order statistics. On this basis, the well-known normal equations can be formulated. If high- order statistical stationarity is assumed, then the equivalent normal equations involve high-order signal moments. In either case, the cross moments (second or higher) are needed. This renders the adaptive prediction procedure non-blind. A novel procedure for blind adaptive prediction has been proposed and considerable implementation has been made in our contributions in the past year. The approach is based upon a suitable interpretation of blind equalization methods that satisfy the constant modulus property and offers significant deviations from the standard prediction methods. These blind adaptive algorithms are derived by formulating Lagrange equivalents from mechanisms of constrained optimization. In this report, other new update algorithms are derived from the fundamental concepts of advanced system identification to carry out the proposed blind adaptive prediction. The results of the work can be extended to a number of control-related problems, such as disturbance identification. The basic principles are outlined in this report and differences from other existing methods are discussed. The applications implemented are speech processing, such as coding and synthesis. Simulations are included to verify the novel modelling method.

Chen, Ya-Chin↗