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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 1,135 records · Page 63
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Resolution effects in the hybrid strong/weak coupling model

Within the context of a hybrid strong/weak coupling model of jet quenching, we study the consequences of the fact that the plasma produced in a heavy ion collision cannot resolve the substructure of a collimated parton shower propagating through it with arbitrarily fine spatial resolution. We introduce a screening length parameter, L res , proportional to the inverse of the local temperature in the plasma, estimating a range for the value of the proportionality constant via comparing weakly coupled QCD calculations and holographic calculations appropriate in strongly coupled plasma. We then modify the hybrid model so that when a parton in a jet shower splits, its two offspring are initially treated as unresolved, and are only treated as two separate partons losing energy independently after they are separated by a distance L res . This modification delays the quenching of partons with intermediate energy, resulting in the survival of more hadrons in the final state with p T in the several GeV range. We analyze the consequences of different choices for the value of the resolution length, L res , and demonstrate that introducing a nonzero L res results in modifications to the jet shapes and jet fragmentations functions, as it makes it more probable for particles carrying a small fraction of the jet energy at larger angles from the jet axis to survive their passage through the quark-gluon plasma. Furthermore, these effects are, however, small in magnitude, something that we confirm via checking for effects on missing- p T observables.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2012

Measurement of the W boson polarization in top quark decays with the ATLAS detector

This paper presents measurements of the polarization ofW bosons in top quark decays, derived from t{bar t} events with missing transverse momentum, one charged lepton and at least four jets, or two charged leptons and at least two jets. Data from pp collisions at a center-of-mass energy of 7 TeV were collected with the ATLAS experiment at the LHC and correspond to an integrated luminosity of 1.04 fb{sup -1}. The measured fractions of longitudinally, left- and right-handed polarization are F{sub 0} = 0.67 {+-} 0.07, F{sub L} = 0.32 {+-} 0.04 and F{sub R} = 0.01 {+-} 0.05, in agreement with the Standard Model predictions. As the polarization of the W bosons in top quark decays is sensitive to the Wtb vertex Lorentz structure and couplings, the measurements were used to set limits on anomalous contributions to the Wtb couplings.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2016

Simulated Temperature Programmed Desorption of Acetaldehyde on CeO 2 (111): Evidence for the Role of Oxygen Vacancy and Hydrogen Transfer

The temperature programmed desorption of acetaldehyde adsorbed on partially reduced CeO 2 (111) has been studied in detail using microkinetic modeling based on self-consistent, periodic density functional theory calculations at the GGA-PW91+U level. Previous experimental studies (Chen et al. J. Phys. Chem. C 115: 3385, 2011; Calaza et al. J. Am. Chem. Soc. 134: 18034, 2012) have shown that, whereas on fully oxidized CeO 2 (111) acetaldehyde desorbs molecularly with a peak temperature of 210 K, the polymerization and enolization of acetaldehyde dominate the surface reactivity on partially reduced CeO 2 (111), resulting in acetaldehyde desorption at higher temperatures. Here we propose a comprehensive reaction mechanism that is consistent with the spectroscopic evidence of the identities of the surface intermediates and with the observed desorption activities, including the formation of ethylene and acetylene. Besides acetaldehyde (CH 3 CHO) and its enolate (CH 2 CHO), several other C 2 H x O species are proposed as key intermediates which are not seen spectroscopically, including ethoxy (CH 3 CH 2 O), ethyleneoxy (CH2CH2O), and formylmethylene (CHCHO). Our study suggests that oxygen vacancies play the critical role of activating the carbonyl bond and thereby facilitating b C–H bond scissions in acetaldehyde, leading to enolization, intermolecular hydrogen transfer, deoxygenation, and potentially C–C coupling reactions.

Zhao, Chuanlin↗
DOE OSTI2020

Global error analysis of the Chebyshev rational approximation method

The Chebyshev rational approximation method (CRAM) has become a widely adopted method for solving nuclear depletion problems. Therefore, understanding CRAM’s accuracy is important for the safe operation of nuclear power plants. This article performs a global error analysis of CRAM and finds that, as the length of the time step approaches zero, the relative error measured between the exact and CRAM solutions at a fixed end time approaches one and infinity for even and odd orders, respectively; for intermediate time step sizes, a minimum in relative error is observed. Finally, we show that the reason for CRAM’s behavior is that the method is inconsistent. Two best practices for using CRAM, derived from these results, are: (1) use CRAM order 16 or higher, (2) if necessary, increase the CRAM order when multiphysics coupling requires smaller time steps.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2018

Theoretical Approaches to Describing the Oxygen Reduction Reaction Activity of Single-Atom Catalysts

Single-atom catalysts have recently emerged as promising low-cost alternatives to Pt for the oxygen reduction reaction (ORR). Given the unique properties that distinguish these systems from traditional transition-metal electrocatalysts, it is essential to benchmark and establish appropriate computational approaches to study these novel materials. Herein, we employ multiple levels of theory, including wave function methods, density functional theory (DFT), and classical simulations, to investigate Cu-modified covalent triazine framework catalysts (Cu/CTF). We consider three major aspects of treating this system computationally. First, we present a step-wise approach to predict the ORR mechanism and adsorbate coverages on Cu/CTF. We then benchmark various DFT methods to coupled-cluster theory with the domain-based local pair natural orbital approximation, which indicates that HSE06 and PBE0 hybrid functionals most accurately describe the adsorption energies of ORR adsorbates on Cu/CTF. We finally employ thermodynamic integration and other techniques to consider solvation effects, which play significant roles in predicting the energies of reaction intermediates and the overall ORR pathway. Lastly, our findings indicate that accurate descriptions of both the electronic structure and solvation are necessary to understand the ORR activity of Cu/CTF.

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

Structures of the intermediates of Kok’s photosynthetic water oxidation clock

Inspired by the period-four oscillation in flash-induced oxygen evolution of photosystem II discovered by Joliot in 1969, Kok performed additional experiments and proposed a five-state kinetic model for photosynthetic oxygen evolution, known as Kok’s S-state clock or cycle. The model comprises four (meta)stable intermediates (S 0 , S 1 , S 2 and S 3 ) and one transient S 4 state, which precedes dioxygen formation occurring in a concerted reaction from two water-derived oxygens bound at an oxo-bridged tetra manganese calcium (Mn 4 CaO 5 ) cluster in the oxygen-evolving complex. This reaction is coupled to the two-step reduction and protonation of the mobile plastoquinone QB at the acceptor side of PSII. Here in this paper, using serial femtosecond X-ray crystallography and simultaneous X-ray emission spectroscopy with multi-flash visible laser excitation at room temperature, we visualize all (meta)stable states of Kok’s cycle as high-resolution structures (2.04–2.08 Å). In addition, we report structures of two transient states at 150 and 400 µs, revealing notable structural changes including the binding of one additional ‘water’, Ox, during the S 2 →S 3 state transition. Our results suggest that one water ligand to calcium (W3) is directly involved in substrate delivery. The binding of the additional oxygen Ox in the S 3 state between Ca and Mn1 supports O–O bond formation mechanisms involving O5 as one substrate, where Ox is either the other substrate oxygen or is perfectly positioned to refill the O5 position during O 2 release. Thus, our results exclude peroxo-bond formation in the S 3 state, and the nucleophilic attack of W3 onto W2 is unlikely.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

Landau damping effects on the scattering spin-asymmetry and channel preference in election-hole plasmas

The scattering spin-asymmetry and spin channel preference in electron collisions are investigated in electron-hole plasmas. It is found that the Landau damping effect enhances the scattering channel preference for the spin-singlet electron scattering and suppresses the spin-triplet electron scattering except the scattering angle {theta}={pi}/2. It is also found that the spin-singlet electron scattering decreases with an increase of the quantum shielding distance. In addition, the Landau damping effect on the spin-asymmetry parameter is found to be more significant in the intermediate domain of the quantum Debye length.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2013

Optical properties of three-layer metal-organic nanoparticles with a molecular J-aggregate shell

This paper examines the optical properties of two types of spherical three-component nanoparticles: (1) particles comprising a metallic core, outer organic dye J-aggregate shell and passive intermediate layer and (2) metallic nanoshells having an insulator or semiconductor core and coated with a molecular J-aggregate layer. The two types of nanoparticles are shown to differ significantly in the behaviour of electromagnetic fields and photoabsorption spectra. As a result of additional possibilities to control the magnitude and nature of the coupling between Frenkel excitons and localised surface plasmons in these systems, the spectral properties of the three-layer particles have radically new inherent features in comparison with earlier studied metal/J-aggregate bilayer particles. In the case of J-aggregate-coated metallic nanoshells, particular attention is paid to the strong plasmon – exciton coupling regime, which takes place when the plasmon resonance frequency of the nanoshell approaches the centre frequency of the J-band of the dye forming the outer layer of the particle. (optics of nanoparticles)

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2011

Development of the ANL Plant Dynamics Code and Control Strategies for the Supercritical Carbon Dioxide Brayton Cycle and Code Validation with Data from the Sandia Small-Scale Supercritical Carbon Dioxide Brayton Cycle Test Loop

Significant progress has been made in the ongoing development of the Argonne National Laboratory (ANL) Plant Dynamics Code (PDC), the ongoing investigation and development of control strategies, and the analysis of system transient behavior for supercritical carbon dioxide (S-CO 2 ) Brayton cycles. Several code modifications have been introduced during FY2011 to extend the range of applicability of the PDC and to improve its calculational stability and speed. A new and innovative approach was developed to couple the Plant Dynamics Code for S-CO 2 cycle calculations with SAS4A/SASSYS-1 Liquid Metal Reactor Code System calculations for the transient system level behavior on the reactor side of a Sodium-Cooled Fast Reactor (SFR) or Lead-Cooled Fast Reactor (LFR). The new code system allows use of the full capabilities of both codes such that whole-plant transients can now be simulated without additional user interaction. Several other code modifications, including the introduction of compressor surge control, a new approach for determining the solution time step for efficient computational speed, an updated treatment of S-CO 2 cycle flow mergers and splits, a modified enthalpy equation to improve the treatment of negative flow, and a revised solution of the reactor heat exchanger (RHX) equations coupling the S-CO 2 cycle to the reactor, were introduced to the PDC in FY2011. All of these modifications have improved the code computational stability and computational speed, while not significantly affecting the results of transient calculations. The improved PDC was used to continue the investigation of S-CO 2 cycle control and transient behavior. The coupled PDC-SAS4A/SASSYS-1 code capability was used to study the dynamic characteristics of a S-CO 2 cycle coupled to a SFR plant. Cycle control was investigated in terms of the ability of the cycle to respond to a linear reduction in the electrical grid demand from 100% to 0% at a rate of 5%/minute. It was determined that utilization of turbine throttling control below 50% load improves the cycle efficiency significantly. Consequently, the cycle control strategy has been updated to include turbine throttle valve control. The new control strategy still relies on inventory control in the 50%-90% load range and turbine bypass for fine and fast generator output adjustments, but it now also includes turbine throttling control in the 0%-50% load range. In an attempt to investigate the feasibility of using the S-CO 2 cycle for normal decay heat removal from the reactor, the cycle control study was extended beyond the investigation of normal load following. It was shown that such operation is possible with the extension of the inventory and the turbine throttling controls. However, the cycle operation in this range is calculated to be so inefficient that energy would need to be supplied from the electrical grid assuming that the generator could be capable of being operated in a motoring mode with an input electrical energy from the grid having a magnitude of about 20% of the nominal plant output electrical power level in order to maintain circulation of the CO 2 in the cycle. The work on investigation of cycle operation at low power level will be continued in the future. In addition to the cycle control study, the coupled PDC-SAS4A/SASSYS-1 code system was also used to simulate thermal transients in the sodium-to-CO 2 heat exchanger. Several possible conditions with the potential to introduce significant changes to the heat exchanger temperatures were identified and simulated. The conditions range from reactor scram and primary sodium pump failure or intermediate sodium pump failure on the reactor side to pipe breaks and valve malfunctions on the S-CO 2 side. It was found that the maximum possible rate of the heat exchanger wall temperature change for the particular heat exchanger design assumed is limited to ±7 C/s for less than 10 seconds. Modeling in the Plant Dynamics Code has been compared with available data from the Sandia National Laboratories (SNL) small-scale S-CO 2 Brayton cycle demonstration that is being assembled in a phased approach currently at Barber-Nichols Inc. and at SNL in the future. The available data was obtained with an earlier configuration of the S-CO 2 loop involving only a single-turbo-alternator-compressor (TAC) instead of two TACs, a single low temperature recuperator (LTR) instead of both a LTR and a high temperature recuperator (HTR), and fewer than the later to be installed full set of electric heaters. Due to the absence of the full heating capability as well as the lack of a high temperature recuperator providing additional recuperation, the temperature conditions obtained with the loop are too low for the loop conditions to be prototypical of the S-CO 2 cycle.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
NASA NTRS1980

Blanket technology workshop report

The solar array blanket, defined as a substrate covered with interconnected and glassed solar cells, but excluding the necessary support structure, deployment, and orientation devices is considered. The interactions between the blanket and the structure that is used to package, deploy, support and, if necessary restow it, are addressed along with systems constraints such as spacecraft configuration, size, and payload requirements. The influence on blanket design is emphasized. The three main mission classes considered are low Earth orbital (LEO), intermediate, or LEO to GEO transfer, and geosynchronous (GEO). Although interplanetary missions could be considered to be a separate class, their requirements, primarily power per unit mass, are generally close enough to geosynchronous missions to allow this mission class to be included within the third type. Examination of the critical elements of each class coupled with considerations of the shuttle capabilities is used to define the type of blanket technology most likely required to support missions that will be flown starting in 1990.

Scott-Monck, J. A.↗
NASA NTRS2010

Biasable, Balanced, Fundamental Submillimeter Monolithic Membrane Mixer

This device is a biasable, submillimeter-wave, balanced mixer fabricated using JPL s monolithic membrane process a simplified version of planar membrane technology. The primary target application is instrumentation used for analysis of atmospheric constituents, pressure, temperature, winds, and other physical and chemical properties of the atmospheres of planets and comets. Other applications include high-sensitivity gas detection and analysis. This innovation uses a balanced configuration of two diodes allowing the radio frequency (RF) signal and local oscillator (LO) inputs to be separated. This removes the need for external diplexers that are inherently narrowband, bulky, and require mechanical tuning to change frequency. Additionally, this mixer uses DC bias-ability to improve its performance and versatility. In order to solve problems relating to circuit size, the GaAs membrane process was created. As much of the circuitry as possible is fabricated on-chip, making the circuit monolithic. The remainder of the circuitry is precision-machined into a waveguide block that holds the GaAs circuit. The most critical alignments are performed using micron-scale semiconductor technology, enabling wide bandwidth and high operating frequencies. The balanced mixer gets superior performance with less than 2 mW of LO power. This can be provided by a simple two-stage multiplier chain following an amplifier at around 90 GHz. Further, the diodes are arranged so that they can be biased. Biasing pushes the diodes closer to their switching voltage, so that less LO power is required to switch the diodes on and off. In the photo, the diodes are at the right end of the circuit. The LO comes from the waveguide at the right into a reduced-height section containing the diodes. Because the diodes are in series to the LO signal, they are both turned on and off simultaneously once per LO cycle. Conversely, the RF signal is picked up from the RF waveguide by the probe at the left, and flows rightward to the diodes. Because the RF is in a quasi- TEM (suspended, microstrip-like) mode, it impinges on the diodes in an anti-parallel mode that does not couple to the waveguide mode. This isolates the LO and RF signals. This operation is similar to a cross-bar mixer used at low frequencies, except the RF signal enters through the back-short end of the waveguide rather than through the side. The RF probe also conveys the down-converted intermediate frequency (IF) signal out to an off-chip circuit board through a simple LC low-pass filter to the left as indicated. The bias is brought to the diodes through a bypass capacitor at the top.

Siegel, Peter↗
DOE OSTI2012

Is the bipyridyl thorium metallocene a low-valent thorium complex? A combined experimental and computational study

Bipyridyl thorium metallocenes [5-1,2,4-(Me3C)3C5H2]2Th(bipy) (1) and [5-1,3-(Me3C)2C5H3]2Th(bipy) (2) have been investigated by magnetic susceptibility and computational studies. The magnetic susceptibility data reveal that 1 and 2 are not diamagnetic, but they behave as temperature independent paramagnets (TIPs). To rationalize this observation, density functional theory (DFT) and complete active space SCF (CASSCF) calculations have been undertaken, which indicated that Cp2Th(bipy) has indeed a Th(IV)(bipy2-) ground state (f0d0 2, S = 0), but the open-shell singlet (f0d1 1, S = 0) (almost degenerate with its triplet congener) is lying only 9.2 kcal/mol higher in energy. Complexes 1 and 2 react cleanly with Ph2CS to give [ 5-1,2,4-(Me3C)3C5H2]2Th[(bipy)(SCPh2)] (3) and [ 5-1,3-(Me3C)2C5H3]2Th[(bipy)(SCPh2)] (4), respectively, in quantitative conversions. Since no intermediates were observed experimentally, this reaction was also studied computationally. Coordination of Ph2CS to 2 in its S = 0 ground state is not possible, but Ph2CS can coordinate to 2 in its triplet state (S = 1) upon which a single electron transfer (SET) from the (bipy2-) fragment to Ph2CS followed by C-C coupling takes place.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Five-body systems with Bethe-Salpeter equations

We extend the Bethe-Salpeter formalism to systems made of five valence particles. Restricting ourselves to two-body interactions, we derive the subtraction terms necessary to prevent overcounting. We solve the five-body Bethe-Salpeter equation numerically for a system of five scalar particles interacting by a scalar exchange boson. To make the calculations tractable, we implement properties of the permutation group S 5 and construct an approximation based on intermediate two- and three-body poles. We extract the five-body ground and excited states along with the spectra obtained from the two-, three-, and four-body equations. In the limit of a massless exchange particle, the two-, three, four- and five-body states coexist within a certain range of the coupling strength, whereas for heavier exchange particles the five-body system becomes Borromean. Our study serves as a building block for the calculation of pentaquark properties using functional methods.

Eichmann, Gernot [Univ. of Graz (Austria)] (ORCID:↗
DOE OSTI2018

Experimental and Theoretical Insights into the Structure of Tellurium Chloride Glasses

Here, the structure of the binary chalcohalide glasses Te 1-x CL x (0.35 <= x <= 0.65) is considered by combining experimental and theoretical results. The structural network properties are influenced by a competition between ionic and covalent bonding in such glasses. At first, a focus is placed on the detailed information available by using the complementary high-energy X-ray and the neutron diffractions in both the reciprocal and real spaces. The main characteristic suggested by the structure factors S(Q) concerns the presence of three length scales in the intermediate range order. The total correlation function T(r) lets us also suppose that the structure of these glasses is more complicated than Te-chain fragments with terminal Cl as demonstrated in crystalline Te 3 Cl 2 . Molecular dynamics simulations were subsequently performed on Te 3 Cl 2 and Te 2 Cl 3 , and coupled with the experimental data, a highly reticulated network of chalcogen atoms, with a fair amount of chlorine atoms bonded in a bridging mode, is proposed. The simulations clearly lead to a glass description that differs markedly from the simple structural model based on only Te atom chains and terminal Cl atoms. Solidstate NMR experiments and NMR parameters calculations allowed validation of the presence of Te highly coordinated with chlorine in these glasses.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Influence of Rigidity–Hydration Coupling on Size-Dependent Diffusion in Hydrated Polymer Membranes

Selective ion transport in polymer membranes depends critically on how penetrant motion couples to polymer dynamics and hydration. Yet, the mechanistic interplay between polymer rigidity, water content, and penetrant size remains poorly understood, especially in the regime where the penetrant diameter, polymer Kuhn length, and correlation length are comparable. Here, we employ coarse-grained molecular dynamics simulations to systematically investigate penetrant diffusion in hydrated polymer networks across a broad range of water volume fractions, chain rigidities, and penetrant sizes. The results reveal a transition from a decoupled regime, where small penetrants diffuse nearly independently of polymer relaxation, to a coupled regime in which large penetrants require cooperative polymer motion for transport. Increasing polymer rigidity amplifies the sensitivity of diffusivity to hydration, particularly at low water content, leading to pronounced deviations from Stokes−Einstein scaling. Comparison with scaling theories and free-volume models shows that classical nanoparticle-based frameworks fail to capture this intermediate regime. To address this gap, we extend the Yasuda model to incorporate polymer rigidity through a single parameter that quantifies the dynamic contribution of chain stiffness to free-volume fluctuations. The resulting model collapses diffusivity data across all sizes, water contents, and rigidities, providing a unified description of penetrant transport in hydrated polymer matrices. Furthermore, these findings establish polymer rigidity as a key, tunable determinant of diffusion and offer a framework for interpreting size-dependent transport in ion-selective membranes.

diffusion↗
DOE OSTI2022

The mechanism for acetate formation in electrochemical CO (2) reduction on Cu: selectivity with potential, pH, and nanostructuring

Nanostructured Cu catalysts have increased the selectivities and geometric activities for high value C–C coupled (C 2 ) products (ethylene, ethanol, and acetate) in the electrochemical CO (2) reduction reaction (CO (2) RR). The selectivity among the high-value C 2 products is also altered, where for instance the yield of acetate increases with alkalinity and is dependent on the catalyst morphology. The reaction mechanisms behind the selectivity towards acetate vs. other C 2 products remain controversial. In this work, we elucidate the reaction mechanism for acetate formation by using ab initio simulations, a coupled kinetic-transport model, and loading dependent experiments. We find that trends in acetate selectivity can be rationalized from variations in electrolyte pH and the local mass transport properties of the catalyst and not from changes in Cu's intrinsic activity. The selectivity mechanism originates from the transport of ketene, a stable (closed shell) intermediate, away from the catalyst surface into solution where it reacts to form acetate. While this type of mechanism has not yet been discussed in the CO (2) RR, variants of it may explain similar selectivity fluctuations observed for other stable intermediates like CO and acetaldehyde. Our proposed mechanism suggests that acetate selectivity increases with increasing pH, decreasing catalyst roughness and significantly varies with the applied potential.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Unveiling the role of halide mixing in the crystallization kinetics and charge transfer mechanisms of wide-bandgap organic–inorganic halide perovskites

Understanding the crystallization kinetics of Br–I mixed-halide WBG perovskite films, and their correlation to the crystallographic structure and charge transfer dynamics, is critical for advancing WBG perovskite devices. Despite many efforts to increase the photovoltaic performances of wide-bandgap (WBG, with a Br content above 20%) perovskite solar cells based on bromine–iodine (Br–I) mixed-halide perovskites, understanding the crystallization kinetics of WBG perovskite films, as well as the role of Br mixing in the crystallization kinetics, is still lacking. Furthermore, an overlooked aspect is the correlation of the halide compositions, crystallization kinetics, crystallographic structure, and charge transfer dynamics. Here, we unveil that Br–I mixed-halide WBG perovskite films undergo two intrinsically different crystallization kinetic processes. One is the intermediate solvent-complex phase-assisted growth (I-rich), and the other is top-to-bottom downward growth (Br-rich). Such downward growth (including high Br concentrations) correlates with the formation of a highly vertically oriented perovskite film, which is accompanied by defect formation caused by a dissolving and recrystallization process coupled with halide homogenization. Consequently, Br-rich WBG perovskite films exhibit enhanced charge carrier transport, but are concurrently plagued by non-radiative charge recombination. Addressing this fundamental perspective is critical to precisely tailor Br-related crystallization, which significantly affects the structure and optoelectronic properties of WBG perovskite films and devices.

Li, Nian↗