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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Chlorine Gas as a Lewis Acid–Base Probe for Molten Salts of Divalent Metal Ions

In the context of energy applications for salts and, more specifically, in the case of molten salt reactors, the solvation of corrosion species, the nature and behavior of radiation-produced excess electrons, transient radicals, and molecular gas species all depend on the Lewis acid–base behavior of the constituent salt melt. Speciation of dissolved species and their transport properties are also influenced by the ability of the melt to form networks. This article focuses on the structural properties of melts composed of alkaline earth metal ions coupled with the Cl – anion, and the quantum mechanical behavior of Cl 2 , a typical product of the reaction of radiation-produced chlorine radicals in Cl – -based molten salts. We explore the effect of M 2+ Lewis acidity on chlorobasicity, seen in this work as the availability of Cl – ions to chemically react with Cl 2 to produce Cl 3 – .

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

Poly(lactic acid)-Based Ink for Biodegradable Printed Electronics With Conductivity Enhanced through Solvent Aging

Biodegradable electronics is a rapidly growing field, and the development of controllably biodegradable, high-conductivity materials suitable for additive manufacturing under ambient conditions remains a challenge. Here, printable conductive pastes that employ poly(lactic acid) (PLA) as a binder and tungsten as a conductor are demonstrated. These composite conductors can provide enhanced stability in applications where moisture may be present, such as environmental monitoring or agriculture. Post-processing the printed traces using a solvent-aging technique increases their conductivity by up to 2 orders of magnitude, with final conductivities approaching 5000 S/m. Such techniques could prove useful when thermal processes including heating or laser sintering are limited by the temperature constraints of typical biodegradable substrates. Finally, both accelerated oxidative and hydrolytic degradation of the printed composite conductors are examined, and a fully biodegradable capacitive soil moisture sensor is fabricated and tested.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Switching of electrochemical selectivity due to plasmonic field-induced dissociation

Electrochemical reactivity is known to be dictated by the structure and composition of the electrocatalyst–electrolyte interface. Here, we show that optically generated electric fields at this interface can influence electrochemical reactivity insofar as to completely switch reaction selectivity. We study an electrocatalyst composed of gold–copper alloy nanoparticles known to be active toward the reduction of CO 2 to CO. However, under the action of highly localized electric fields generated by plasmonic excitation of the gold–copper alloy nanoparticles, water splitting becomes favored at the expense of CO 2 reduction. Real-time time-dependent density functional tight binding calculations indicate that optically generated electric fields promote transient-hole-transfer-driven dissociation of the O─H bond of water preferentially over transient-electron-driven dissociation of the C─O bond of CO 2 . These results highlight the potential of optically generated electric fields for modulating pathways, switching reactivity on/off, and even directing outcomes.

Alcorn, Francis M.↗
DOE OSTI2025

Radio Frequency Transients Correlated with Electron Flux Measured On-Board the STP-Sat6

We analyzed transient electromagnetic signatures, referred to as spacecraft environment discharges (SEDs) or on-board discharges (OBDs), and the in-situ particle environment simultaneously measured by the Radio Frequency Sensor (RFS) and the Space and Atmospheric Burst Reporting System Z-plasma spectrometer (SABRS-ZPS), respectively. These sensors are on-board the U.S. Department of Defense Space Test Program Satellite 6 (STP-Sat6) in geostationary orbit. Radio frequency signatures of SEDs on STP-Sat6 have relatively high peak amplitudes; they often caused amplitude-saturation in the so-called high band (120–140 MHz frequency range) of the RFS likely due to the proximity of their source to the RFS’s dipole antennas. We examined the occurrence rate of SEDs reported by the RFS and its temporal relationship to electron flux in the 7.9–12.2 keV range. Peaks in SED count rates were time-correlated with peaks in electron flux. The electron-flux peaks appeared to lead the SED count rate peaks by 24–45 min for the 7.9–12.2 keV energies. This indicates that incidence of electrons at this relatively low-energy range likely resulted in ramping up of the charging of the spacecraft leading to periods of high occurrence rates of discharges in and around the spacecraft.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Interdiffusion and Formation of Intermetallic Compounds in High-Temperature Power Electronics Substrate Joints Fabricated by Transient Liquid Phase Bonding

Power electronics packages typically comprise a dielectric substrate bonded to a metal layer and attached to heat sinks using a low-thermal-conductivity solder. These multiple layers increase the effective thermal resistance of the package and are responsible for package failures under cyclic thermal loads. Bonding the aluminum nitride dielectric layer (AlN) directly to a low coefficient of thermal expansion (CTE) aluminum silicon carbide (AlSiC) cold plate using copper-aluminum (Cu-Al) transient liquid phase (TLP) bonding has been shown to improve the mechanical reliability of the power electronic packages while making the package more compact by bringing the cooling solutions closer to the devices. This study aims to characterize the Cu-Al bonds formed during the TLP bonding of AlSiC with three different power electronics substrates: pure aluminum nitride (AlN), aluminum (DBA), and copper (DBC). The material compositions and microstructures of the bonds were analyzed using scanning electron microscopy (SEM), x-ray spectroscopy (EDS), confocal scanning acoustic microscopy (C-SAM), and x-ray diffraction (XRD). ..alpha..-Al solid compound was identified as the dominant phase in AlN-AlSiC and Al-AlSiC, with a notable presence of SiC particles. In contrast, three intermetallic phases - ..theta..-CuAl2, ..eta..-CuAl, and ..gamma..'- Cu9Al4 - were observed in the Cu-AlSiC bond. A computational solid-state diffusion model was developed to predict the intermetallic compounds (IMCs) formed during Cu-Al TLP bonding in each system, which supported the observation that an initial Cu volume fraction of 20 % in the material layers produced a final bond composition of >95 % Al with minimal IMC growth. However, increased Cu concentrations produced higher concentration gradients, leading to increased growth of IMCs, Kirkendall voids, and interstitial cracks.

DIRECT ENERGY CONVERSION↗
DOE OSTI2024

Time-resolved cryogenic electron tomography for the study of transient cellular processes

Cryogenic electron tomography (cryo-ET) is the highest resolution imaging technique applicable to the life sciences, enabling sub-nanometer visualization of specimens preserved in their near native states. The rapid plunge freezing process used to prepare samples lends itself to time-resolved studies, which researchers have pursued for in vitro samples for decades. Here, we focus on developing a freezing apparatus for time-resolved studies in situ. The device mixes cellular samples with solution-phase stimulants before spraying them directly onto an electron microscopy grid that is transiting into cryogenic liquid ethane. By varying the flow rates of cell and stimulant solutions within the device, we can control the reaction time from tens of milliseconds to over a second prior to freezing. In a proof-of-principle demonstration, the freezing method is applied to a model bacterium, Caulobacter crescentus, mixed with an acidic buffer. Through cryo-ET we resolved structural changes throughout the cell, including surface-layer protein dissolution, outer membrane deformation, and cytosolic rearrangement, all within 1.5 seconds of reaction time. This new approach, Time-Resolved cryo-ET (TR-cryo-ET), enhances the capabilities of cryo-ET by incorporating a sub-second temporal axis and enables the visualization of induced structural changes at the molecular, organelle, or cellular level.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Protocols for x-ray transient grating pump/optical probe experiments at x-ray free electron lasers

Abstract Transient grating spectroscopy is a specialized application of the four-wave-mixing methodology and constitutes a versatile technique for investigating the dynamics of vibrational, magnetic and electronic degrees of freedom of matter in a background-free fashion. Recent developments in free-electron laser sources have enabled the extension of this technique into the extreme ultraviolet range. Ongoing efforts to expand transient grating spectroscopy into the x-ray regime promise numerous advantages: (1) substantial penetration depths that allow for probing bulk material properties, (2) element specificity via specific core-excited states, and (3) short wavelengths that allow for excitation gratings with higher momentum transfer and improved spatial resolution. In this study, we comprehensively outline the procedures for conducting x-ray transient grating pump/optical probe experiment. The process encompasses the design and alignment of the experimental setup, as well as the subsequent steps involved in data acquisition and analysis. This paper is intended as a comprehensive guide for researchers interested in implementing x-ray transient grating spectroscopy, providing valuable insights into the intricacies of the experimental workflow required for this novel technique. Furthermore, we discuss the potential for extending this methodology to an x-ray pump/x-ray probe scheme, envisioning a future direction that holds promise for enhancing the capabilities and scope of x-ray transient grating spectroscopy, opening new opportunities for studying ultrafast processes with unprecedented temporal and spatial resolutions.

Optics↗
DOE OSTI2022

Microwave-Free Dynamic Nuclear Polarization via Sudden Thermal Jumps

Dynamic nuclear polarization (DNP) presently stands as the preferred strategy to enhance the sensitivity of nuclear magnetic resonance measurements, but its application relies on the use of high-frequency microwave to manipulate electron spins, an increasingly demanding task as the applied magnetic field grows. Here we investigate the dynamics of a system hosting a polarizing agent formed by two distinct paramagnetic centers near a level anticrossing. We theoretically show that nuclear spins polarize efficiently under a cyclic protocol that combines alternating thermal jumps and radio-frequency pulses connecting hybrid states with opposite nuclear and electronic spin alignment. Central to this process is the difference between the spin-lattice relaxation times of either electron spin species, transiently driving the electronic spin bath out of equilibrium after each thermal jump. Without the need for microwave excitation, this route to enhanced nuclear polarization may prove convenient, particularly if the polarizing agent is designed to feature electronic level anticrossings at high magnetic fields.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Radicals as Exceptional Electron-Withdrawing Groups: Nucleophilic Aromatic Substitution of Halophenols Via Homolysis-Enabled Electronic Activation

While heteroatom-centered radicals are understood to be highly electrophilic, their ability to serve as transient electron-withdrawing groups and facilitate polar reactions at distal sites has not been extensively developed. Here, we report a new strategy for the electronic activation of halophenols, wherein generation of a phenoxyl radical via formal homolysis of the aryl O-H bond enables direct nucleophilic aromatic substitution of the halide with carboxylate nucleophiles under mild conditions. Pulse radiolysis and transient absorption studies reveal that the neutral oxygen radical (O • ) is indeed an extraor-dinarily strong electron-withdrawing group [σ p - (O • ) = 2.79 vs. σ p - (NO 2 ) = 1.27]. Additional mechanistic and computational studies indicate that the key phenoxyl intermediate serves as an open-shell electron-withdrawing group in these reactions, lowering the barrier for nucleophilic substitution by more than 20 kcal/mol relative to the closed-shell phenol form of the substrate. Finally, by using radicals as transient activating groups, this homolysis-enabled electronic activation strategy provides a powerful platform to expand the scope of nucleophile-electrophile couplings and enable previously challenging transformations.

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

Photocatalyzed electron exchange between organic chromophores and hematite nanoparticles and the role of solid-state charge transport

Understanding photocatalyzed redox interactions between Fe(III)–(oxyhydr)oxide mineral nanoparticles and adsorbed chromophoric organic matter is critical for accurately predicting bioavailable iron fluxes in the euphotic zone of natural aquatic systems, and for improving the effectiveness of nano-iron-based water purification systems. However, the electron transfer processes that underpin photoreductive dissolution at particle/organic/solution interfaces occur on ultrafast timescales and thus remain difficult to probe. In this work, we report an ultrafast transient absorption spectroscopy (TAS) study of suspensions of hematite nanoplatelets (HNPs) sensitized by adsorbed rhodamine B (RhB) dye as a function of solution media and pH. The TAS results indicate a substantially longer fluorescence lifetime of RhB adsorbed on HNPs across a wide range of pH conditions, consistent with transient photoinduced electron transfer to the oxide with recombination kinetics controlled by electron migration back to the interface via small polaron hopping. Normalization of the observed kinetics to the measured surface loading of RhB at different pH values shows that the recombination rates are insensitive to environmental variables, likely controlled instead by particle properties that determine small polaron diffusion behavior.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

LICS Modeling [Slides]

We propose to design a new diagnostic based on laser inverse Compton scattering (LICS) to study the dynamics of runaway electron formation during killer-pellet triggered disruptions in DIII-D, and their subsequent loss. Obtaining a better understanding of transient runaway electrons (and how to suppress them) is one of the highest priorities of the US fusion program. To enable this, we need better measurements of the runaway electron population during and after disruptions. We intend to measure point-wise time-resolved spatial profile and energy distributions of the runaway electrons while they are in the core of the tokamak plasma. While LICS measurements of relativistic e-beams have been successfully made on accelerators, they have never been done in a tokamak. We bring two innovations to this diagnostic concept which should enable 10 times better signal-to-noise ratios than previously envisioned. In particular, we will marry bright short pulse (10’s of picosecond) laser technologies with the availability of short-pulse gated x-ray imagers developed at Los Alamos for the National Ignition Facility (NIF), to reject noise generated by the tokamak and plasma environment. We will generate a Conceptual Physics Basis, a Preliminary Design, and a Final Design package, with associated DIII-D reviews, along with prototype component testing for the diagnostic over the course of the two year duration of this proposal.

42 ENGINEERING↗
DOE OSTI2025

Electrons and Their Multiple Kinetic Fates in an Ionic Liquid

Ionic liquids (ILs) for electrochemical, nuclear, and solar energy applications operate under harsh conditions, where electrons and transient radical species can form. This communication discusses why anions such as bis(trifluoromethylsulfonyl)imide (Tf 2 N − ) are reduced at the electron-rich electrode whereas in laser photoionization or pulse radiolysis studies, where electrons are ejected from species in the bulk, we often detect long-lived electrons in cavities that interact with IL cations instead. This work argues that bulk excess electrons generated photolytically or radiolytically follow kinetically favored pathways. As such, cavity electrons may not be the most energetically favorable states, but when they form, and they do form, they are kinetically stable. Reduction reactions of anions or electron localization in cavities and subsequent reactions are all expected outcomes. Here we focus on a pyrrolidinium-based IL of the dicyanamide (N(CN) 2 − ) anion because of its large electrochemical window and very low viscosity, which are ideal for energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Signatures of nonthermal carriers in nonlinear photoluminescence

Ultrafast light emission from plasmonic nanostructures provides a sensitive probe of the energetic electrons generated by intense optical excitation. The way this emission scales with excitation intensity has long been read through the lens of heated electron populations at an elevated temperature, yet this picture cannot reconcile the variety of behaviors seen across different materials and experiments. We argue that transient nonthermal electrons play a far larger role than has been appreciated. We present a unified description that reproduces emission behavior across diverse systems and outline experiments needed to resolve their signatures.

nanoscale materials↗
DOE OSTI2020

Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using ultrafast transient polarization spectroscopy, extending the well-known technique of optical Kerr effect spectroscopy to excited electronic states. The third-order nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S 1 excited state. By measuring this response, which is highly sensitive to details of the excited state character and structure, as a function of time delays between the three pulses involved, we extract the dephasing time of the wave packet on the excited state. The dephasing time, measured as a function of time delay after pump excitation, shows oscillations indicating oscillatory wave packet dynamics on the excited state. Finally, from the experimental measurements and supporting theoretical calculations, we deduce that the wave packet completely leaves the S 1 state potential energy surface after three traversals of the intersystem crossing between the singlet S 1 and triplet T 2 states.

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

Bioresorbable Primary Battery Anodes Built on Core–Double-Shell Zinc Microparticle Networks

Bioresorbable implantable electronics require power sources that are also bioresorbable with controllable electrical output and lifetime. In this paper, we report a bioresorbable zinc primary battery anode filament based on a zinc microparticle (MP) network coated with chitosan and Al 2 O 3 double shells. When discharged in 0.9% NaCl saline, a Zn MP filament with a 0.17 × 2 mm 2 cross-sectional area exhibited a stable voltage output of 0.55 V at a current of 0.01 mA. Covered by chitosan and Al 2 O 3 double shells, the zinc MP filament exhibited a directional dissolution behavior with a tunable lifetime approximately linear to its length. A stable 200 h discharging time was achieved with a 15 mm Zn MP filament. The maximum output power was found to be 12 μW at 0.03 mA for one filament. The linearity relationship between the current output and the filament cross-sectional area suggested a facile strategy to raise the power output at constant discharging voltage. The filaments could also be connected in series and in parallel to boost its overall voltage and current output, demonstrating their excellent integration capability. Furthermore, this work presents a promising pathway toward bioresorbable transient batteries with controllable lifetime and power output, demonstrating a great potential for powering transient implantable biomedical devices.

25 ENERGY STORAGE↗