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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Excitation-Dependent High-Lying Excitonic Exchange via Interlayer Energy Transfer from Lower - to - Higher Bandgap 2D Material

High light absorption (~15%) and strong photoluminescence (PL) emission in monolayer (1L) transition metal dichalcogenides (TMDs) make them ideal candidates for optoelectronic device applications. Competing interlayer charge transfer (CT) and energy transfer (ET) processes control the photocarrier relaxation pathways in TMD heterostructures (HSs). In TMDs, long-distance ET can survive up to several tens of nm, unlike the CT process. Our experiment shows that an efficient ET occurs from the 1Ls WSe 2 -to-MoS 2 with an interlayer hexagonal boron nitride (hBN), due to the resonant overlapping of the high-lying excitonic states between the two TMDs, resulting in enhanced HS MoS 2 PL emission. This type of unconventional ET from the lower-to-higher optical bandgap material is not typical in the TMD HSs. With increasing temperature, the ET process becomes weaker due to the increased electron–phonon scattering, destroying the enhanced MoS 2 emission. Our work provides new insight into the long-distance ET process and its effect on the photocarrier relaxation pathways.

2D material↗
DOE OSTI2026

Final Technical Report for DE-SC0021049: Manipulating interfacial reactivity with atomically layered heterostructures

This final technical report summarizes the work accomplished in this DOE Early Career Research Program project that has established moiré superlattice materials and two-dimensional (2D) heterostructures as a highly tunable platform for controlling heterogeneous charge transfer (ET) kinetics at solid-liquid interfaces. By precisely engineering van der Waals heterostructures of atomically thin 2D materials, particularly bilayer and trilayer graphene with controlled twist angles, this project demonstrated systematic control of interfacial charge transfer rates spanning three orders of magnitude. This research addresses fundamental questions about how electronic structure, charge localization, and atomic layer-dependent properties govern charge transfer at electrochemical interfaces, with broad implications for energy conversion, electrocatalysis, and next-generation electrochemical devices.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Resolution of Virtual Depth Sectioning from Four-Dimensional Scanning Transmission Electron Microscopy

Abstract One approach to three-dimensional structure determination using the wealth of scattering data in four-dimensional (4D) scanning transmission electron microscopy (STEM) is the parallax method proposed by Ophus et al. (2019. Advanced phase reconstruction methods enabled by 4D scanning transmission electron microscopy, Microsc Microanal25, 10–11), which determines the scattering matrix and uses it to synthesize a virtual depth-sectioning reconstruction of the sample structure. Drawing on an equivalence with a hypothetical confocal imaging mode, we derive contrast transfer and point spread functions for this parallax method applied to weakly scattering objects, showing them identical to earlier depth-sectioning STEM modes when only bright field signal is used, but that improved depth resolution is possible if dark field signal can be used. Through a simulation-based study of doped Si, we show that this depth resolution is preserved for thicker samples, explore the impact of shot noise on the parallax reconstructions, discuss challenges to making use of dark field signal, and identify cases where the interpretation of the parallax reconstruction breaks down.

3D imaging↗
DOE OSTI2021

Forward and backward stimulated Raman scattering in multi-speckled beams: Density dependence and effects on cross-beam energy transfer

Particle-in-cell simulations of cross-beam energy transfer (CBET) between multi-speckled beams reveal a potentially prominent energy loss from forward stimulated Raman scattering (FSRS) in the amplified seed beam [Yin et al., Phys. Plasmas 26, 082708 (2019)]. In this work, an intensity scan is used to examine this energy loss in the CBET-amplified seed beam at intensities of a few times 1014 W/cm2. Electron tracers demonstrate both the trapping in the electron plasma waves that is sustained over multiple speckles and the subsequent acceleration to velocities well beyond the phase velocity. Motivated by expanding our understanding of this energy loss mechanism, we isolate the FSRS density dependence by using a 2×1014 W/cm2 pulse to scan densities between 0.06 ncr and 0.12 ncr; a spectral analysis characterizes the energy losses from scattering with the changing densities. At saturation, both greater beam attenuation is measured at the laser frequency and larger scattering FSRS angles are observed as density increases, along with a rapid transition to primarily backscatter SRS between 0.10 ncr and 0.12 ncr, earlier than predicted by linear theory. Density gradients are shown to effectively mitigate oblique FSRS and beam energy losses in the two lower density cases, whereas 0° forward scattering is primarily suppressed in the higher density cases. Finally returning to the two-beam CBET system of interest, the interplay and mitigation of the secondary instabilities at larger domain and beam spatial scales are discussed, here also examining backward stimulated Brillouin scattering.

Stark, D. J. (ORCID:0000000203642733)↗
NASA NTRS1994

Collisional-Radiative Nonequilibrium and Precursor Effects in a Nitrogen Shock Wave

Improvements to a plasma code with a Collisional-Radiative (CR) non-equilibrium model are made, allowing for a more accurate description of the physical processes. The code allows for non-Boltzmann distributions of the electronic excited states by convecting separately each excited state, as a pseudo-specie. Each molecular state has also its own vibrational temperature, while a global rotational temperature is assumed. The free electron temperature is different from those of the excited states, and the electron heat conduction is also included. The CR model also uses a unique coupling between chemistry and vibrational energy (C-V coupling), which is fully coherent, and has the property of establishing thermal equilibrium as well as chemical equilibrium, on its own. We have also included a coupling between electronic excitations and vibrational energy (X-V coupling), which can have a strong influence on the vibrational temperature of some states. The recent improvements include the multi- temperature dependence of the chemical rates for associative ionization, as well as the estimation of the internal energies transferred during this process. Additionally, the distribution of energy into different translational modes (electron and heavy particles) is now correctly modeled. This provides a very rapid heating mechanism for the free electrons, since it is found that the electrons are generated with an average thermal energy of the same order as the heavy particle translational energy. This effect was observed by Gorelov et al in a recent paper, and lead to pronounced peaks in electron temperature immediately behind the shock. We will attempt ro reproduce this phenomenon. The last modification concerns the inclusion of the radiative terms into the calculations, thus enabling us to observe the effect of radiative losses and radiation transport. Preliminary tests have shown that the radiative losses are not negligible, i.e. the shock velocity drops when the radiative emission is included. In addition, we have observed some precursor excitation and ionization phenomena. These may be important at high shock velocities, and this will be investigated in detail. Precursor phenomena were also observed (in air) by Gorelov et al, and our results (for pure nitrogen) will be qualitatively compared with theirs.

Cambier, Jean-Luc↗
DOE OSTI2020

Improving collaborations between empiricists and modelers to advance grassland community dynamics in ecosystem models

Climate change, increasing atmospheric CO 2 , and land use change have altered biogeochemical and hydrologic cycles world-wide, with grassland systems being particularly vulnerable to resulting vegetation shifts (Komatsu et al., 2019). Therefore, incorporating plant community dynamics into ecosystem models is critical for accurate forecasting of ecosystem responses to global change (Levine, 2016). Process-based ecosystem models, which simulate the biogeochemical transfers of mass and energy among biota, the subsurface, and atmosphere, require representation of dynamic composition of organisms within ecosystems. For example, these models simulate leaf and plant-level characteristics, such as electron transport rate and allometry of carbon (C) allocation, to predict how net primary productivity and other ecosystem processes respond to abiotic drivers. These models are particularly useful in scaling from organismal to ecosystem levels but are still underdeveloped in their ability to capture community change, especially in grassland ecosystems. To represent compositional changes, these models must simulate competition, mortality, establishment, and reproduction of plant populations within communities. Yet, current ecosystem modeling approaches to forecast plant community change have derived from studies of forested systems and are either too coarse to capture fine-scale community dynamics (e.g. dynamic global vegetation models (DGVMs)) or too complex to be used at large spatial scales (e.g. forest gap models).

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1983

Electrode kinetics of oxygen reduction - A theoretical and experimental analysis of the rotating ring-disc electrode method

In order to calculate most of the rate constants for the intermediate formation of H2O2 in the electroreduction of O2 to H2O, the theoretical treatments of the rotating ring-disc electrode method by Damjanovic et al. (1966, 1967), Bagotskii et al. (1968, 1969), and Wroblowa et al. (1976) are modified. Rotating ring-disc electrode experimental data obtained for O2 reduction in Pt in 0.55 M H2SO4 are used to illustrate the calculations of rate constants according to the above theoretical treatments. A simple reaction model as proposed by the first author is consistent with the experimental data. The results indicate that O2 (97 percent) reduces to H2O in a direct four-electron transfer reaction. The adsorption of O2 is probably the rate-determining step in the potential region more negative than 0.5 V vs. reversible hydrogen electrode.

Hsueh, K.-L.↗
DOE OSTI2026

Restoring Symmetry and Enhancing Exchange via Chiral Molecular-Magnetic Hexagons

Modified behaviors of molecules, designed for device or energy applications, can occur due to lattice-molecule incompatibilities in point-group symmetries (PGS), long-range interactions between neighboring molecules, or latticemolecule charge transfer. Such sensitivities are prerequisite for the use of quantum molecules as devices, but removing certain broken symmetries is desirable from the standpoint of simplifying their behaviors. Here, we demonstrate symmetry restoration to molecular-magnetic lattices and show that it leads to strengthened exchange-coupling due to dipolar electrostatic interactions between neighboring molecules and due to manifestations of an earlier identification of a spin-sensitive slightly mobile electron by Hooshmand et al. Starting with a broken symmetry molecular magnet of current interest, we demonstrate a more robust structure composed of six molecular magnets on a h-BN-like surface. The broken point-group symmetry is healed by constructing interpenetrating equilateral triangular structures that are appropriately ratcheted to preserve three-fold rotational symmetry and inversion symmetry.

Pederson, Mark R.↗
NASA NTRS2000

A semiempirical study for the ground and excited states of free-base and zinc porphyrin-fullerene dyads

The ground and excited states of a covalently linked porphyrin-fullerene dyad in both its free-base and zinc forms (D. Kuciauskas et al., J. Phys. Chem. 100 (1996) 15926) have been investigated by semiempirical methods. The excited-state properties are discussed by investigation of the character of the molecular orbitals. All frontier MOs are mainly localized on either the donor or the acceptor subunit. Thus, the absorption spectra of both systems are best described as the sum of the spectra of the single components. The experimentally observed spectra are well reproduced by the theoretical computations. Both molecules undergo efficient electron transfer in polar but not in apolar solvents. This experimental finding is explained theoretically by explicitly considering solvent effects. The tenth excited state in the gas phase is of charge-separated character where an electron is transferred from the porphyrin donor to the fullerene acceptor subunit. This state is stabilized in energy in polar solvents due to its large formal dipole moment. The stabilization energy for an apolar environment such as benzene is not sufficient to lower this state to become the first excited singlet state. Thus, no electron transfer is observed, in agreement with experiment. In a polar environment such as acetonitrile, the charge-separated state becomes the S, state and electron transfer takes place, as observed experimentally. The flexible single bond connecting both the donor and acceptor subunits allows free rotation by ca. +/- 30 degrees about the optimized ground-state conformation. For the charge-separated state this optimized geometry has a maximum dipole moment. The geometry of the charge-separated state thus does not change relatively to the ground-state conformation. The electron-donating properties of porphyrin are enhanced in the zinc derivative due to a reduced porphyrin HOMO-LUMO energy gap. This yields a lower energy for the charge-separated state compared to the free-base dyad.

Bridged Compounds/chemistry↗
NASA NTRS2006

Self-Consistent Model of Magnetospheric Ring Current and Propagating Electromagnetic Ion Cyclotron Waves: Waves in Multi Ion Magnetosphere - 1

The further development of a self-consistent theoretical model of interacting ring current ions and electromagnetic ion cyclotron waves [Khazanov et al., 2003] is presented. In order to adequately take into account the wave propagation and refraction in a multi-ion plasmasphere, we explicitly include the ray tracing equations in our previous self-consistent model and use the general form of the wave kinetic equation. This is a major new feature of the present model and, to the best of our knowledge, the ray tracing equations for the first time are explicitly employed on a global magnetospheric scale in order to self-consistently simulate spatial, temporal, and spectral evolutions of the ring current and electromagnetic ion cyclotron waves. To demonstrate the effects of EMIC wave propagation and refraction on the EMIC wave energy distributions and evolution we simulate the May 1998 storm. The main findings of our simulation can be summarized as follows. First, due to the density gradient at the plasmapause, the net wave refraction is suppressed, and He(+)-mode grows preferably at plasmapause. This result is in a total agreement with the previous ray tracing studies, and very clear observed in presented B-field spectrograms. Second, comparison the global wave distributions with the results from other ring current model [Kozyra et al., 1997] reveals that our model provides more intense and higher plasmapause organized distributions during the May, 1998 storm period. Finally, the found He(+)-mode energy distributions are not Gaussian distributions, and most important that wave energy can occupy not only the region of generation, i. e. the region of small wave normal angles, but the entire wave normal angle region and even only the region near 90 degrees. The latter is extremely crucial for energy transfer to thermal plasmaspheric electrons by resonant Landau damping, and subsequent downward heat transport and excitation of stable auroral red arcs.

Khazanov, G. V.↗
NASA NTRS2006

Self-Consistent Model of Magnetospheric Ring Current and Propagating Electromagnetic Ion Cyclotron Waves: Waves in Multi-Ion Magnetosphere

The further development of a self-consistent theoretical model of interacting ring current ions and electromagnetic ion cyclotron waves (Khazanov et al., 2003) is presented In order to adequately take into account wave propagation and refraction in a multi-ion magnetosphere, we explicitly include the ray tracing equations in our previous self-consistent model and use the general form of the wave kinetic equation. This is a major new feature of the present model and, to the best of our knowledge, the ray tracing equations for the first time are explicitly employed on a global magnetospheric scale in order to self-consistently simulate the spatial, temporal, and spectral evolution of the ring current and of electromagnetic ion cyclotron waves To demonstrate the effects of EMIC wave propagation and refraction on the wave energy distribution and evolution, we simulate the May 1998 storm. The main findings of our simulation can be summarized as follows. First, owing to the density gradient at the plasmapause, the net wave refraction is suppressed, and He+-mode grows preferably at the plasmapause. This result is in total agreement with previous ray tracing studies and is very clearly found in presented B field spectrograms. Second, comparison of global wave distributions with the results from another ring current model (Kozyra et al., 1997) reveals that this new model provides more intense and more highly plasmapause-organized wave distributions during the May 1998 storm period Finally, it is found that He(+)-mode energy distributions are not Gaussian distributions and most important that wave energy can occupy not only the region of generation, i.e., the region of small wave normal angles, but all wave normal angles, including those to near 90 . The latter is extremely crucial for energy transfer to thermal plasmaspheric electrons by resonant Landau damping and subsequent downward heat transport and excitation of stable auroral red arcs.

Khazanov, G. V.↗
DOE OSTI2021

Emerged Metallicity in Molecular Ferromagnetic Wires

Supramolecular engineering bridges molecular assembly with macromolecular charge-transfer salts, promising the design to construct supramolecular architectures that integrate cooperative properties difficult or impossible to find in conventional lattices. Here, we report the crystal engineering design and kinetic growth of one-dimensional supramolecular wires composed of bis(ethylenedithio)tetrathiafulvalene (ET + ) cation and polymeric Cu[N(CN) 2 ] 2 – anion. A bulk ferromagnetic order is discovered for filling up the gap where strong ferromagnetism is missing in such ET molecule-based charge-transfer salts. Metallicity is induced by electric current from the semiconducting wire, which is attributed to strain effect by tuning its close molecular contact. This structural feature is evidenced through the combination of various mechanistic spectroscopic studies. Further, electric dipole is established from the close molecular contacts and is suggestive to stabilize ferromagnetic spin interaction through anions bridging spin sites. The breakthrough shown here provides a pathway to explore low-dimensional supramolecular materials exhibiting strong electron correlation, metallicity, and ferromagnetism.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRS1993

Measurement of the transition probability of the C III 190.9 nanometer intersystem line

A radio-frequency ion trap has been used to store C(2+) ions created by electron bombardment of CO. The transition probability for the 2s2p 3Po1-2s2 1S0 intersystem line of C m has been measured by recording the radiative decay at 190.9 nm. The measured A-value is 121 +/- 7/s and agrees, within mutual uncertainty limits, with that of Laughlin et al. (1978), but is 20 percent larger than that of Nussbaumer and Storey (1978). The effective collision mixing rate coefficient among the fine structure levels of 3Po and the combined quenching and charge transfer rate coefficients out of the 3Po1 level with the CO source gas have also been measured.

Kwong, Victor H. S.↗
DOE OSTI2023

Effects of ion trapping and fluctuations of electron temperature and plasma flow on cross-beam energy transfer

The influences of ion trapping and fluctuations of electron temperature and plasma flow on cross-beam energy transfer (CBET) are examined using two- and three-dimensional particle-in-cell simulations in parameter regimes relevant to recent CBET experiments at the OMEGA laser facility. In mid-Z plasma irradiated by an intense pump beam and weaker probe beam, ion trapping, collisional de-trapping, and plasma flow induced by thermal effects are shown to affect the CBET gain. Ion trapping can enhance or detune the CBET resonance [Nguyen et al., Phys. Plasmas 28, 082705 (2021)]. Collisional de-trapping can affect the CBET gain at low seed beam intensity near the onset threshold for ion trapping. Thermal-effects-induced flow can also detune the CBET resonance at a level comparable to that from trapping at low seed beam intensity. As a consequence, the CBET gain is sensitive to collisions and dimensionality at low seed beam intensity where ion trapping is weak but is insensitive to collisions and dimensionality at high seed beam intensity where ion trapping is strong.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Growing neoclassical tearing modes seeded via transient-induced-multimode interactions

Nonlinear extended magnetohydrodynamics simulations demonstrating seeding of neoclassical tearing modes (NTMs) via magnetohydrodynamics-transient-induced multimode interactions are presented. Simulations of NTMs are enabled by two recent NIMROD code developments: the implementation of heuristic neoclassical stresses and the application of transient magnetic perturbations (MPs) at the boundary. NTMs are driven unstable by the inherently pressure driven kinetic bootstrap current, which arises due to collisional viscosity between passing and trapped electrons. These simulations use heuristic closures that model the neoclassical electron and ion stresses. NTM growth requires a seed island, which is generated by a transiently applied MP in simulations. The capability is demonstrated using kinetic-based reconstructions with flow of a DIII-D ITER Baseline Scenario discharge (La Haye et al., in Proceedings IAEA FEC, 2020). The applied MP seeds a 2/1 NTM that grows in two phases: a slow growth phase followed by a faster robust growth phase. Additionally, an evolving sequence of higher order core modes are excited at first. Power transfer analysis shows that nonlinear interactions between the core modes and the 2/1 helps drive the initial slow growth. Once the induced 2/1 magnetic island reaches a critical width, the NTM transitions to faster robust growth, which is well described by the nonlinear modified Rutherford equation. Furthermore, this work highlights the role of nonlinear mode coupling in seeding NTMs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Long‐Range Electron Transport Rates Depend on Wire Dimensions in Cytochrome Nanowires

Abstract The ability to redirect electron transport to new reactions in living systems opens possibilities to store energy, generate new products, or probe physiological processes. Recent work by Huang et al. showed that 3D crystals of small tetraheme cytochromes (STC) can transport electrons over nanoscopic to mesoscopic distances by an electron hopping mechanism, making them promising materials for nanowires. However, fluctuations at room temperature may distort the nanostructure, hindering efficient electron transport. Classical molecular dynamics simulations of these fluctuations at the nano‐ and mesoscopic scales allowed us to develop a graph network representation to estimate maximum electron flow that can be driven through STC wires. In longer nanowires, transient structural fluctuations at protein‐protein interfaces tended to obstruct efficient electron transfer, but these blockages are ameliorated in thicker crystals where alternative electron transfer pathways become more efficient. The model implies that more flexible proteinprotein interfaces limit the required minimum diameter to carry currents commensurate with conventional electronics.

Chemistry↗
DOE OSTI2021

Dependence of the electronic structure of the EuS/InAs interface on the bonding configuration

The EuS/InAs interface has recently attracted attention for the possibility of inducing magnetic exchange correlations in a strong spin-orbit semiconductor, which could be useful for topological quantum devices. We use density functional theory with a machine-learned Hubbard U correction [Yu et al., npj Comput. Mater. 6, 180 (2020)] to elucidate the effect of the bonding configuration at the interface on the electronic structure. For all interface configurations considered here, we find that the EuS valence band maximum (VBM) lies below the InAs VBM. In addition, dispersed states emerge at the top of the InAs VBM at the interface, which do not exist in either material separately. These states are contributed mainly by the InAs layer adjacent to the interface. They are localized at the interface and may be attributed to charge transfer from the EuS to the InAs. The interface configuration affects the position of the EuS VBM with respect to the InAs VBM, as well as the dispersion of the interface states. For all interface configurations studied here, the induced magnetic moment in the InAs is small. Our results suggest that this interface, in its coherent form studied here, may not be promising for inducing equilibrium magnetic properties in InAs.

36 MATERIALS SCIENCE↗
NASA NTRS1998

Fluorescence of Pentavalent Chromium in SiO2 Sol-Gel Glasses

Chromium ions are very attractive to optical spectroscopy and laser physics. It is well known that the first laser in the history is a ruby laser activated with Cr(3+). It was found in early nineties that Cr(4+) was also an interesting lasing ion in the near infrared, and various Cr(4+) lasers have been developed. Very recently, it was reported that Cr(2+) doped in CdSe crystals showed lasing action in the infrared. The above achievement have stimulated an interest in searching for Cr(5+) and investigating its optical properties. Cr(5+) is isoelectronic with Ti(3+) and V(4+), having electron configuration 3d1. Ti(3+) is the active center of commercial cw and femtosecond sapphire lasers, tunable in the range 680-1100 nm. V(4+) doped in YAlO3 and Al2O3 showed broad band emission near 635 nm. Although EPR results of Cr(5+) were reported, the optical properties were less studied. Herren et al. reported an observation of luminescence from Cr doped in SiO2 sol-gel glass. The luminescence spectrum was assigned to pentavalent ions in their first paper, and later it was identified to be the emission from the charge transfer transition of Cr(6+). The first observation of photoluminescence from octahedrally coordinated Cr(5+) in BaCaMg aluminate glasses was reported very recently. In this work, we report luminescence results of Cr doped SiO2 sol-gel glasses. The fluorescence spectra are very different from Herrens' results, and we believe it originates from pentavalent Cr.

Jia, Weiyi↗