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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 973 records · Page 54
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Novel Electroforming-Free Nanoscaffold Memristor with Very High Uniformity, Tunability, and Density

Dynamical tuning of the concentration of defects in oxides provides a route to controlling new functionalities. [ 1 ] The chemical potential to capture the functionalities driven by mobile ions and defects can be one of the key control parameters (as well as electric field, magnetic field, and stress) for tuning the functionality of complex oxides. [ 1 ] Interesting signatures related to oxygen vacancies have been explicitly observed in widespread physical applications, including solid oxide fuel cells, [ 2 ] catalysts, [ 3 ] optoelectronics, [ 4 ] and electronics. [ 5–14 ]

36 MATERIALS SCIENCE↗
DOE OSTI2019

Functional Materials Under Stress: In Situ TEM Observations of Structural Evolution

The operating conditions of functional materials usually involve varying stress fields, resulting in structural changes, whether intentional or undesirable. Complex multiscale microstructures including defects, domains, and new phases, can be induced by mechanical loading in functional materials, providing fundamental insight into the deformation process of the involved materials. On the other hand, these microstructures, if induced in a controllable fashion, can be used to tune the functional properties or to enhance certain performance. In situ nanomechanical tests conducted in scanning/transmission electron microscopes (STEM/TEM) provide a critical tool for understanding the microstructural evolution in functional materials. In our study, select results on a variety of functional material systems in the field are presented, with a brief introduction into some newly developed multichannel experimental capabilities to demonstrate the impact of these techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Reduced Stochastic Resistive Switching in Organic-Inorganic Hybrid Memristors by Vapor-Phase Infiltration

We report resistive random-access memory (RRAM) is promising for next-generation data storage and non-von Neumann computing hardware. However, tuning device switching characteristics and particularly, controlling their stochastic variation remain as critical challenges. Here, new organic-inorganic hybrid RRAM media are reported whose bipolar switching characteristics and stochasticity can be controlled by vapor-phase infiltration (VPI), an ex situ hybridization technique derived from atomic layer deposition. Hybrid RRAMs based on AlO x -infiltrated SU-8 feature facile tunability of device switching voltages, off-state current, and on-off ratio by adjusting the amount of infiltrated AlO x in the hybrid. Furthermore, a significant reduction in the stochastic, cycle-to-cycle variations of switching parameters is enabled by AlO x infiltration, driven by the infiltration-induced changes in mechanical, dielectric, and chemical properties of organic medium and their influence on the dimension and formation characteristics of conductive filaments. Finally, multi-level analog switching potentially useful for neuromorphic applications are demonstrated, along with direct, one-step device patterning exploiting the negative-tone resist feature of SU-8. With the demonstrated control over switching characteristics and stochastic variation, combined with analog switching and one-step patterning capabilities, the results not only present a novel hybrid medium for RRAM applications but also showcase the utility of VPI for developing new, high-performance hybrid RRAM devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Size‐Controlled Cobalt Nanoplates and Their Impact on Oxygen Evolution Catalysis

Controlling the size of nanoparticles is important in catalytic reactions, not only for tuning the surface area but also for modifying the electronic structure. However, achieving precise size control in 2D structures remains challenging. In this work, we demonstrate precise size control of cobalt nanoplates, ranging from 19 nm to 80 nm, which is achieved by tuning the ratio of two surfactants used in the synthesis. The 19 nm of Co nanoplates exhibit higher oxygen evolution reaction activity due to a higher proportion of {10$\overline{1}$1} to {0001} facets. In conclusion, this size control allows systematic investigation into how nanoplate dimensions influence catalytic performance in the oxygen evolution reaction, offering new insights into structure-activity relationships of cobalt nanocatalysts.

defect↗
DOE OSTI2017

Ferromagnetic–Antiferromagnetic Coupling by Distortion of Fe/Mn Oxygen Octahedrons in (BiFeO 3 ) m (La 0.7 Sr 0.3 MnO 3 ) n Superlattices

Interface enhanced magnetism attracts much attention due to its potential use in exploring novel structure devices. Nevertheless, the magnetic behavior at interfaces has not been quantitatively determined. In this study, abnormal magnetic moment reduction is observed in La 0.7 Sr 0.3 MnO 3 (LSMO)/BiFeO 3 (BFO) superlattices, which is induced by ferromagnetic (FM)/antiferromagnetic (AFM) coupling in the interface. With reduced repetition of the superlattice's unit cell [(LSMO) n /(BFO) n ] 60/ n ( n = 1, 2, 5, 10) on a SrTiO 3 substrate, magnetic moment reduction from 25.5 emu cc −1 ([(LSMO) 10 /(BFO) 10 ] 6 ) to 1.5 emu cc −1 ([(LSMO) 1 /(BFO) 1 ] 60 ) is obtained. Ab initio simulations show that due to the different magnetic domain formation energies, the magnetic moment orientation tends to be paramagnetic in the FM/AFM interface. The work focuses on the magnetic domain formation energy and provides a pathway to construct artificial heterostructures that can be an effective way to tune the magnetic moment orientation and control the magnetization of ultrathin films.

Xiong, Jie↗
DOE OSTI2026

Backbone Stiffness‐Dependent Photoluminescence of Pendant Fluorophores in Organic Nanoparticles

Fluorescent organic nanoparticles (FoNPs) with backbone stiffness‐dependent photoluminescence were synthesized via microemulsion atom transfer radical polymerization (ATRP) of 2‐(2‐bromoisobutyryloxy)ethyl methacrylate (BiBEM), ethylene glycol dimethacrylate (EGDMA), and methacrylate monomers bearing pendant fluorophores, 1‐pyrenemethyl methacrylate (PyMMA), or 4‐(1,2,2‐triphenylethenyl)benzenemethyl methacrylate (TPEMMA). The crosslinking density precisely tuned the intraparticle rigidity, enabling systematic control over emission mechanisms. Pyrene‐containing FoNPs exhibited a rigidity‐dependent transition from excimer‐dominated to monomer‐dominated fluorescence, whereas TPE‐based FoNPs displayed aggregation‐induced emission (AIE) enhancement as intramolecular motion was restricted. Solvent‐dependent studies revealed that increased polarity and viscosity, particularly in benzyl alcohol and DMSO, promoted cooperative rigidification and enhanced emission intensity through specific polymer–solvent interactions. Furthermore, the retained alkyl bromide chain ends on FoNPs enabled dual roles as initiators and crosslinkers in UV‐induced polymerization of poly(ethylene glycol) acrylates, forming luminescent FoNP–OEG hybrid gels with improved mechanical robustness. This work establishes a versatile platform for integrating tunable optical and mechanical properties into a single polymeric nanoparticle framework, offering new design principles for multifunctional soft materials and providing a platform for future sensing, imaging, and photonic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Enhanced Exciplex Emission of Pyrene Thin Films Doped by Perylene: Structural, Photophysical and Morphological Investigation

The present work reports on the preparation of thin films of pyrene luminophors doped by varying amounts of perylene by spin coating technique. The structural, morphological, and photophysical properties of pyrene thin films have been investigated as a function of perylene contents. X-ray diffraction studies of doped thin films show well-defined peaks, and estimated crystallite size decreases with increasing perylene content, due to the formation of closed packed crystal structure. SEM images of pure pyrene revealed smooth, and compact and separated crystals with amounts of perylene. The result of absorption spectra showed decrease in intensity with perylene content. However, the fluorescence spectra of pyrene containing higher amounts of perylene showed broad and structureless exciplex emission at 510 nm. The emission colour of pyrene luminophors tuned from blue to green by controlling the concentration of perylene. The phenomenon of change in colour was seen due to efficient excitation energy transfer from pyrene to perylene in thin films. It also found that the intensity of exciplex emission increases with increasing concentration of perylene is of high demand in fluorescent lamp as well as green organic light emitting diodes.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Equivariant graph convolutional neural networks for the representation of homogenized anisotropic microstructural mechanical response

Composite materials with different microstructural material symmetries are common in engineering applications where grain structure, alloying and particle/fiber packing are optimized via controlled manufacturing. In fact these microstructural tunings can be done throughout a part to achieve functional gradation and optimization at a structural level. To predict the performance of particular microstructural configuration and thereby overall performance, constitutive models of materials with microstructure are needed. In this work we provide neural network architectures that provide effective homogenization models of materials with anisotropic components. These models satisfy equivariance and material symmetry principles inherently through a combination of equivariant and tensor basis operations. We demonstrate them on datasets of stochastic volume elements with different textures and phases where the material undergoes elastic and plastic deformation, and show that the these network architectures provide significant performance improvements.

anisotropy↗
DOE OSTI2021

Topology and ground state control in open-shell donor-acceptor conjugated polymers

Donor-acceptor (DA) conjugated polymers (CPs) with narrow bandgaps and open-shell (diradical) character represent an emerging class of materials whose rich behavior emanates from their collective electronic properties and diminished electron pairing. However, the structural and electronic heterogeneities that define these materials complicate bandgap control at low energies and connections linking topology, exchange interactions, and (opto)electronic functionality remain nascent. To address these challenges, we demonstrate structurally rigid and strongly π-conjugated copolymers comprised of a solubilizing thiadiazoloquinoxaline acceptor and cyclopenta[2,1-b:3,4-b']dithiophene or dithieno[3,2-b:2',3'-d]thiophene donors. Atom-specific substitution modulates local aromatic character within the donor resulting in dramatic differences in structural, physicochemical, electronic, and magnetic properties of the polymers. These long-range π-mediated interactions facilitate control between low-spin aromatic and high-spin quinoidal forms. This work provides a strategy to understand the evolution of the electronic structure within DA CPs, control the ground state spin multiplicity, tune spin-spin interactions, and articulate the emergence of their novel properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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 OSTI2020

Assembly of Building Blocks by Double-End-Anchored Polymers in the Dilute Regime Mediated by Hydrophobic Interactions at Controlled Distances

Hierarchical assembly of building blocks via competing, orthogonal interactions is a hallmark of many of nature’s composite materials that do not require highly specific ligand-receptor interactions. To mimic this assembly mechanism requires the development of building blocks capable of tunable interactions. In the present work, we explored the interplay between repulsive (steric and electrostatic) and attractive hydrophobic forces. The designed building blocks allow hydrophobic forces to effectively act at controlled, large distances, to create and tune the assembly of membrane-based building blocks under dilute conditions and affect their interactions with cellular membranes via physical cross-bridges. Specifically, we employed double-end-anchored poly(ethylene glycol)s (DEA-PEGs)—hydrophilic PEG tethers with hydrophobic tails on both ends. Using differential-interference-contrast optical microscopy, synchrotron small angle X-ray scattering (SAXS), and cryogenic electron microscopy, we investigated the ability of DEA-PEGs to mediate assembly in the dilute regime on multiple length scales and on practical time scales. The PEG length, anchor hydrophobicity, and molar fraction of DEA-PEG molecules within a membrane strongly affect the assembly properties. Additional tuning of the intermembrane interactions can be achieved by adding repulsive interactions via PEG-lipids (steric) or cationic lipids to the DEA-PEG-mediated attractions. Further, while the optical and electron microscope imaging methods provided qualitative evidence of the ability of DEA-PEGs to assemble liposomes, the SAXS measurements and quantitative line-shape analysis in dilute preparations demonstrated that the ensemble average of loosely organized liposomal assemblies maintains DEA-PEG concentration-dependent tethering on defined nanometer length scales. For cationic liposome–DNA nanoparticles (CL–DNA NPs), aggregation induced by DEA-PEGs decreased internalization of NPs by cells, but tuning the DEA-PEG-induced attractions by adding repulsive steric interactions via PEG-lipids limited aggregation and increased NP uptake. However, confocal microscopy imaging together with colocalization studies with Rab11 and LysoTracker as markers of intracellular pathways showed that modifying CL–DNA NPs with DEA-PEGs alters their interactions with the plasma and endosomal membranes.

- x-ray scattering↗
DOE OSTI2021

Ion Pairing Mediates Molecular Organization Across Liquid/Liquid Interfaces

Liquid/liquid interfaces play a central role in scientific fields ranging from nanomaterial synthesis and soft matter electronics to nuclear waste remediation and chemical separations. This diversity of functions arises from an interface’s ability to respond to changing conditions in its neighboring bulk phases. Understanding what drives this interfacial flexibility can provide novel avenues for designing new functional interfaces. However, limiting this progress is an inadequate understanding of the subtle intermolecular and interphase interactions taking place at the molecular level. Here, we use surface-specific vibrational sum frequency generation spectroscopy combined with atomistic molecular dynamics simulations to investigate the self-assembly and structure of model ionic oligomers consisting of an oligodimethylsiloxane (ODMS) tail covalently attached to a positively charged methyl imidazolium (MIM + ) head group at buried oil/aqueous interfaces. We show how the presence of seemingly innocuous salts can impart dramatic changes to the ODMS tail conformations in the oil phase via specific ion effects and ion-pairing interactions taking place in the aqueous phase. These specific ion interactions are shown to drive enhanced amphiphile adsorption, induce morphological changes, and disrupt emergent hydrogen-bonding structures at the interface. Tuning these interactions allows for independent control over the oligomer structure in the oil phase versus interfacial population changes and represents key mechanistic insight that is needed to control chemical reactions at liquid/liquid interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Electronic and Morphological Studies of Conjugated Polymers Incorporating a Disk-Shaped Polycyclic Aromatic Hydrocarbon Unit

As more research findings have shown the correlation between ordering in organic semiconductor thin films and device performance, it is becoming more essential to exercise control of the ordering through structural tuning. Many recent studies have focused on the influence of side chain engineering on polymer packing orientation in thin films. However, the impact of the size and conformation of aromatic surfaces on thin film ordering has not been investigated in great detail. Here we introduce a disk-shaped polycyclic aromatic hydrocarbon building block with a large π surface, namely, thienoazacoronenes (TACs), as a donor monomer for conjugated polymers. Here, a series of medium bandgap conjugated polymers have been synthesized by copolymerizing TAC with electron donating monomers of varying size. The incorporation of the TAC unit in such semiconducting polymers allows a systematic investigation, both experimentally and theoretically, of the relationships between polymer conformation, electronic structure, thin film morphology, and charge transport properties. Field effect transistors based on these polymers have shown good hole mobilities and photoresponses, proving that TAC is a promising building block for high performance optoelectronic materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ionic-liquid-Assisted Fabrication of Lignocellulosic Thin Films with Tunable Hydrophobicity

Thin films with enhanced water repellency and mechanical strength can be fabricated from renewable lignocellulosic feedstock as a replacement for petrochemical-derived synthetic polymers, such that it minimizes life cycle impact on the environment and human health. In this work, hybrid poplar wood, either untreated (control) or pretreated with hot water at 160 °C for 20 min (HWE-20), 60 min (HWE-60), and 90 min (HWE-90), was dissolved in 1-ethyl-3-methylimidazolium acetate and regenerated to fabricate thin films. The HWE-90 films were enriched in lignin by 74%, specifically on the surface, which along with hemicellulose depletion imparted hydrophobicity (108° water contact angle) when compared to the control (56°), HWE-20 (77°), and HWE-60 (84°) films. They also exhibited 86% reduced water vapor sorption hysteresis and 75% improved storage modulus compared to the control. Thus, we demonstrate how to tune the lignocellulosic film properties via a combination of hot water pretreatment and ionic liquid dissolution.

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

Strong correlations elucidate the electronic structure and phase diagram of LaAlO3/SrTiO3 interface

The interface between the two band insulators SrTiO3 and LaAlO3 has the unexpected properties of a two-dimensional electron gas. It is even superconducting with a transition temperature, Tc, that can be tuned using gate bias Vg, which controls the number of electrons added or removed from the interface. The gate bias–temperature (Vg, T) phase diagram is characterized by a dome-shaped region where superconductivity occurs, that is, Tc has a non-monotonic dependence on Vg, similar to many unconventional superconductors. Here, we report, the frequency of the quantum resistance-oscillations versus inverse magnetic field for various Vg. This frequency follows the same non-monotonic behaviour as Tc; a similar trend is seen in the low field limit of the Hall coefficient. We theoretically show that electronic correlations result in a non-monotonic population of the mobile band, which can account for the experimental behaviour of the normal transport properties and the superconducting dome.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Coherent terahertz radiation with 2.8-octave tunability through chip-scale photomixed microresonator optical parametric oscillation

High-spectral-purity frequency-agile room-temperature sources in the terahertz spectrum are foundational elements for imaging, sensing, metrology, and communications. Here we present a chip-scale optical parametric oscillator based on an integrated nonlinear microresonator that provides broadly tunable single-frequency and multi-frequency oscillators in the terahertz regime. Through optical-to-terahertz down-conversion using a plasmonic nanoantenna array, coherent terahertz radiation spanning 2.8-octaves is achieved from 330 GHz to 2.3 THz, with ≈20 GHz cavity-mode-limited frequency tuning step and ≈10 MHz intracavity-mode continuous frequency tuning range at each step. By controlling the microresonator intracavity power and pump-resonance detuning, tunable multi-frequency terahertz oscillators are also realized. Furthermore, by stabilizing the microresonator pump power and wavelength, sub-100 Hz linewidth of the terahertz radiation with 10 –15 residual frequency instability is demonstrated. The room-temperature generation of both single-frequency, frequency-agile terahertz radiation and multi-frequency terahertz oscillators in the chip-scale platform offers unique capabilities in metrology, sensing, imaging and communications.

42 ENGINEERING↗