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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 OSTI2022

Direct Monitoring of Conical Intersection Passage via Electronic Coherences in Twisted X-Ray Diffraction

Quantum coherences in electronic motions play a critical role in determining the pathways and outcomes of virtually all photophysical and photochemical molecular processes. However, the direct observation of electronic coherences in the vicinity of conical intersections remains a formidable challenge. Here we propose a novel time-resolved twisted x-ray diffraction technique that can directly monitor the electronic coherences created as the molecule passes through a conical intersection. We show that the contribution of electronic populations to this signal is canceled out when using twisted x-ray beams that carry a light orbital angular momentum, providing a direct measurement of transient electronic coherences in gas-phase molecules.

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

Mechanism of Tyrosine-Driven Deprotonation in Photosystem II Revealed by Multiscale Simulations

Photosystem II (PSII) drives light-induced water oxidation via stepwise redox transitions of its oxygen-evolving complex (OEC), a Mn 4 Ca cluster advancing through five intermediate S-states (S 0 –S 4 ). The S 2 → S 3 transition involves a redox event in which a Mn ion donates an electron to the redox-active tyrosine YZ, coupled to deprotonation of an OEC-bound water ligand─yet the underlying coupling mechanism remains unresolved. Time-resolved serial femtosecond crystallography (TR-SFX) has revealed transient electron density shifts near the redox-active tyrosine Y Z , interpreted as sequential oxidation and reduction, with reduction initiating ∼1 μs after excitation and substantially progressed by 30 μs. However, this interpretation conflicts with kinetics from photothermal beam deflection (PBD), time-resolved X-ray absorption spectroscopy (TR-XAS), and electron paramagnetic resonance (EPR), which place electron transfer at 190–400 μs and proton transfer around 30 μs. Here, we reconcile these discrepancies using quantum mechanics/molecular mechanics (QM/MM) and molecular dynamics (MD) simulations. We show that oxidation of P680 and Y Z breaks the symmetry of the nearby hydrogen bonds involving water molecule W4, displacing Y Z and replicating the TR-SFX features of Y Z and Q165 observed at 1 μs. This local perturbation propagates through a hydrogen-bond network, transmitting the electrostatic signal from Y Z to the E65-E312 dyad and triggering redox-coupled deprotonation via the Cl1 channel. By 30 μs, the hydrogen-bond symmetry is restored through deprotonation of W2 (or alternatively W1), reproducing the disappearance of TR-SFX density differences around Y Z and Q165 without requiring Y Z reduction. Our proposed mechanism also gives molecular insights into the O6* density, assigning it to water reorganization rather than a discrete Ca-bound hydroxide species. Here, our results reveal a detailed atomistic mechanism linking Y Z oxidation to long-range proton release and suggest a functional role for the nearby Cl – ion in proton transfer. More broadly, this study underscores the importance of hydrogen-bond dynamics in mediating redox-driven proton transport and demonstrates how integrative simulations can resolve mechanistic ambiguities.

Deprotonation↗
DOE OSTI2022

Observation of site-selective chemical bond changes via ultrafast chemical shifts

The concomitant motion of electrons and nuclei on the femtosecond time scale marks the fate of chemical and biological processes. Here we demonstrate the ability to initiate and track the ultrafast electron rearrangement and chemical bond breaking site-specifically in real time for the carbon monoxide diatomic molecule. We employ a local resonant x-ray pump at the oxygen atom and probe the chemical shifts of the carbon core-electron binding energy. We observe charge redistribution accompanying core-excitation followed by Auger decay, eventually leading to dissociation and hole trapping at one site of the molecule. The presented technique is general in nature with sensitivity to chemical environment changes including transient electronic excited state dynamics. This work provides a route to investigate energy and charge transport processes in more complex systems by tracking selective chemical bond changes on their natural timescale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Research on Orbital Plasma-Electrodynamics (ROPE)

Since the development of probe theory by Langmuir and Blodgett, the problem of current collection by a charged spherically or cylindrically symmetric body has been investigated by a number of authors. This paper overviews the development of a fully three-dimensional particle simulation code which can be used to understand the physics of current collection in three dimensions and can be used to analyze data resulting from the future tethered satellite system (TSS). According to the TSS configurations, two types of particle simulation models were constructed: a simple particle simulation (SIPS) and a super particle simulation (SUPS). The models study the electron transient response and its asymptotic behavior around a three dimensional, highly biased satellite. The potential distribution surrounding the satellite is determined by solving Laplace's equation in the SIPS model and by solving Poisson's equation in the SUPS model. Thus, the potential distribution in space is independent of the density distribution of the particles in the SUPS model but it does depend on the density distribution of the particles in the SUPS model. The evolution of the potential distribution in the SUPS model is described. When the spherical satellite is charged to a highly positive potential and immersed in a plasma with a uniform magnetic field, the formation of an electron torus in the equatorial plane (the plane in perpendicular to the magnetic field) and elongation of the torus along the magnetic field are found in both the SIPS and the SUPS models but the shape of the torus is different. The areas of high potential that exist in the polar regions in the SUPS model exaggerate the elongation of the electron torus along the magnetic field. The current collected by the satellite for different magentic field strengths is investigated in both models. Due to the nonlinear effects present in SUPS, the oscillating phenomenon of the current collection curve during the first 10 plasma periods can be seen (this does not appear in SIPS). From the parametric studies, it appears that the oscillating phenomenon of the current collection curve occurs only when the magnetic field strength is less than 0.2 gauss for the present model.

Wu, S. T.↗
DOE OSTI2024

Ultrafast Formation of Charge Transfer Trions at Molecular‐Functionalized 2D MoS 2 Interfaces

Abstract In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr‐ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge‐transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr‐ESFG especially sensitive to the trion formation dynamics. The presence of charge‐transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers a potential for transferring unique electronic attributes of TMD to the molecular layers.

Jing, Yuancheng↗
DOE OSTI2024

Ultrafast Formation of Charge Transfer Trions at Molecular‐Functionalized 2D MoS 2 Interfaces

In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr-ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge-transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr-ESFG especially sensitive to the trion formation dynamics. The presence of charge-transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers a potential for transferring unique electronic attributes of TMD to the molecular layers.

Time-resolved↗
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.↗
NASA NTRS1992

A theory for narrow-banded radio bursts at Uranus - MHD surface waves as an energy driver

A possible scenario for the generation of the narrow-banded radio bursts detected at Uranus by the Voyager 2 planetary radio astronomy experiment is described. In order to account for the emission burstiness which occurs on time scales of hundreds of milliseconds, it is proposed that ULF magnetic surface turbulence generated at the frontside magnetopause propagates down the open/closed field line boundary and mode-converts to kinetic Alfven waves (KAW) deep within the polar cusp. The oscillating KAW potentials then drive a transient electron stream that creates the bursty radio emission. To substantiate these ideas, Voyager 2 magnetometer measurements of enhanced ULF magnetic activity at the frontside magnetopause are shown. It is demonstrated analytically that such magnetic turbulence should mode-convert deep in the cusp at a radial distance of 3 RU.

Farrell, W. 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↗
NASA NTRS2016

Analysis and Simulations of Space Radiation Induced Single Event Effects and Transients

Spacecraft electronic are affected by the space radiation environment. Among the different types of radiation effects that can affect spacecraft electronics is the single event transient (SET). The space environment is responsible for many of the single event transients which can upset the performance of the spacecraft avionics hardware. In this chapter we first explore the origins of single event transients, then explore the modeling of a single event transient in digital and analog circuit. The chapter also addresses the concept of crosstalk that could develop among digital circuits in the present of a SET event. The chapter also provides a discussion of SET hardening. We then provide a discussion concerning propagation of a single event transient event at the local, subsystem, and system level in a spacecraft using two different models, one of the models developed by the author, known as the state transition model. The final goal of the chapter is to provide a qualitatively methodology for assessing single event transients and its effects so that spacecraft avionics engineers can develop either hardware or software countermeasures in their designs. SET is not a form of electromagnetic interference (EMI) in its origin, but semantically SET is very similar to EMI because they are both caused a current source not previously accounted for. SET has the same effects as EMI and it can cause interference problems in electronic circuits via multiple coupling mechanisms similar to EMI, and therefore makes such circuits incompatible.

Perez, Reinaldo J.↗
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↗
NASA NTRS1984

Ultraviolet converter transients induced by electrons

The output of ultraviolet converters typically used in satellite astronomy was monitored during irradiation with electrons from a sealed SR-90 source which approximated the peak flux in earth's outer electron belt. The signal induced by irradiation was attributed to two mechanisms: (1) photoelectrons resulting from photons created in the MgF2 window and (2) the direct impact of electrons on the phosphor. For irradiation at about 1 x 10 to the 7th e/sq cm sec, these two effects produced signals which were, in order of magnitude, the same as those produced by an incident UV flux (254 nm) of 10 to the 8th and 10 to the 7th photons/sq cm sec, respectively. In addition, the induced signal was investigated as a function of electron energy by irradiating another converter with 0.4-1.8-MeV electrons from a Van de Graaff. These results suggest that the dominant contribution to the electron-induced signal is Cerenkov photon production in the MgF2 window.

Kernell, R. L.↗
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↗
NASA NTRS1995

Electronically controlled mechanical seal for aerospace applications--Part 2: Transient tests

An electronically controlled mechanical seal for use as the purge gas seal in a liquid oxygen turbopump has been fabricated and tested under transient operating conditions. The thickness of the lubricating film is controlled by adjusting the coning of the carbon face. This is accomplished by applying a voltage to a piezoelectric actuator to which the carbon face is bonded. The seal has been operated with a closed-loop control system that utilizes either the leakage rate or seal face temperature as the feedback. Both speed and pressure transients have been imposed on the seal. The transient tests have demonstrated that the seal is capable of maintaing low leakage rates while limiting face temperatures.

Wolff, Paul J.↗