Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “CF”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Dynamical electron correlation and the chemical bond. II. Recoupled pair bonds in the $a$ 4 Σ - states of CH and CF

We extended our studies of the effect of dynamical electron correlation on the covalent bonds in the AH and AF series (A = B–F) to the recoupled pair bonds in the excited $a$ 4 Σ - states of the CH and CF molecules. Dynamical correlation is energetically less important in the $a$ 4 Σ - states than in the corresponding X 2 Π states for both molecules, which is reflected in smaller changes in bond energies ($D$ e ). Changes in the equilibrium bond distance ($R$ e ) and vibrational frequency ($ω$ e ), on the other hand, are influenced by the changes in the slope and curvature of the dynamical electron correlation energy as a function of the internuclear distance $R$, $E$ DEC ($R$). In the CH($a$ 4 Σ - ) state, these changes are much smaller than in the CH(X 2 Π) state, but in the CF($a$ 4 Σ - ) state, they are larger, reflecting a significant difference in the shapes of $E$ DEC ($R$) curves. At large $R$, the shape of $E$ DEC ($R$) curves for covalent and recoupled pair bonds is similar although different in magnitude. For the CH($a$ 4 Σ - ) state, $E$ DEC ($R$) has a minimum at $R$ = $R$ e + 0.72 Å as the orbitals associated with the formation of the recoupled pair bond switch places. $E$ DEC (R) for the CF($a$ 4 Σ - ) state decreases continuously throughout the bound region of the potential energy curve because the dynamical correlation energy associated with the electrons in the lone pair orbitals is increasing. In conclusion, these results support our earlier conclusion that we still have much to learn about the nature of dynamical electron correlation in molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Secondary scintillation properties of multi-layer THGEMs operated in low-pressure CF 4 and Ar/5%Xe

We present a measurement of the secondary scintillation yield produced by two-layer Thick Gas Electron Multipliers (M-THGEMs) in pure Tetrafluoromethane (CF 4 ) gas and in Ar mixed with 5% Xe in low-pressures down to 20 Torr. The detector was irradiated with 5.49 MeV alpha particles from a low-rate 241-Am source. The secondary scintillation light generated during the gas avalanche process was read out by a Hamamatsu photomultiplier tube (model R8520-406), sensitive to a broad wavelength range (160–650 nm). The avalanche charge was collected on the bottom electrode of M-THGEM and correlated to the scintillation light on an event-by-event basis. We observed that, for both gas types, the value of the photon to electron production ratio (0.4 ph/el in CF 4 and 0.1 ph/el in Ar/5%Xe) increases with the thickness of the M-THGEM electrodes and varies significantly with the pressure, being higher at lower values. The decrease in electroluminescence yield at higher pressures is much more pronounced in the Ar/Xe mixture. In addition, because of a larger gas avalanche volume, the electroluminescence light yield is larger in thicker M-THGEM structures. Presented results are particularly useful for designing the next generation of Optical-readout Time Projection Chambers (O-TPCs) operated at low-pressure CF 4 ; applications include experimental nuclear physics with rare isotope beams, dark matter detection with directional sensitivity and observation of the Migdal effect in a low-pressure Optical TPC.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Campaign 78 - Production of 252 Cf and the Recovery of Curium Feed Material at the Radiochemical Engineering Development Center

The production of californium-252 (Cf-252) has been of interest to the US Department of Energy (DOE) since the 1970s because of its ability to emit neutrons (2.31 x 10 12 neutrons/gram second). Today, Oak Ridge National Laboratory is responsible for the majority of Cf-252 sold around the world. This report aims to provide a complete summary of the chemical processing of the Cf and curium (Cm) from campaign 78 (C78) which started in January 2019.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS2004

A Monte Carlo Sensitivity Analysis of CF2 and CF Radical Densities in a c-C4F8 Plasma

A Monte Carlo sensitivity analysis is used to build a plasma chemistry model for octacyclofluorobutane (c-C4F8) which is commonly used in dielectric etch. Experimental data are used both quantitatively and quantitatively to analyze the gas phase and gas surface reactions for neutral radical chemistry. The sensitivity data of the resulting model identifies a few critical gas phase and surface aided reactions that account for most of the uncertainty in the CF2 and CF radical densities. Electron impact dissociation of small radicals (CF2 and CF) and their surface recombination reactions are found to be the rate-limiting steps in the neutral radical chemistry. The relative rates for these electron impact dissociation and surface recombination reactions are also suggested. The resulting mechanism is able to explain the measurements of CF2 and CF densities available in the literature and also their hollow spatial density profiles.

Bose, Deepak↗
NASA NTRSDate not supplied

NASA GEOS-CF: Overview, Applications, Future Direction

Since 2019, the NASA Global Earth Observing System (GEOS) model has been used to generate global, near-real-time estimates and daily five-day forecasts of atmospheric composition at a horizontal resolution of 0.25 degrees (~25 km) from the surface up to the lower mesosphere. This composition forecast system (“GEOS-CF”) combines the GEOS weather forecasting model with the state-of-the-science GEOS-Chem chemistry module to deliver detailed analysis of a wide range of air pollutants, including the policy-relevant species such as ozone, carbon monoxide, nitrogen oxides, sulfur dioxide and fine particulate matter (PM2.5). Because GEOS-CF includes atmospheric levels up through the stratosphere, this system has been leveraged to support the Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite mission and provide stratospheric intrusion alerts to ground-based monitoring stations. We will present recent advances to GEOS-CF which includes assimilation of satellite observations to produce more accurate model analyses. We further discuss our future plans for a composition reanalysis.

K. Emma Knowland↗
DOE OSTI2020

Protonierung von CH 3 N 3 und CF 3 N 3 in Supersäuren: Isolierung und strukturelle Charakterisierung von langlebigen Methyl‐ und Trifluormethylamino‐Diazonium‐Ionen

Abstract Die Methylaminodiazonium‐Kationen [CH 3 N(H)N 2 ] + und [CF 3 N(H)N 2 ] + wurden als ihre bei niedriger Temperatur stabilen [AsF 6 ]‐Salze durch Protonierung von Azidomethan und Azidotrifluormethan in supersauren Systemen hergestellt. Sie wurden durch NMR‐ und Raman‐Spektroskopie charakterisiert. Ein eindeutiger Nachweis der Protonierungsstelle wurde durch die Kristallstrukturen beider Salze erhalten, welche die Bildung der Alkylaminodiazonium‐Ionen bestätigte. Die Lewis‐Addukte CH 3 N 3 ⋅AsF 5 und CF 3 N 3 ⋅AsF 5 wurden ebenfalls hergestellt und durch Tieftemperatur‐NMR‐ und Raman‐Spektroskopie sowie im Falle von CH 3 N 3 ⋅AsF 5 durch Röntgenstrukturbestimmung charakterisiert. Elektronische Strukturberechnungen wurden durchgeführt, um zusätzliche Einblicke zu erhalten. Versuche zur elektrophilen Aminierung von Aromaten wie Benzol und Toluol mit Methyl‐ und Trifluormethylamino‐Diazonium‐Ionen waren erfolglos.

Saal, Thomas↗
DOE OSTI2020

Protonation of CH 3 N 3 and CF 3 N 3 in Superacids: Isolation and Structural Characterization of Long‐Lived Methyl‐ and Trifluoromethylamino Diazonium Ions

Abstract The methylamino diazonium cations [CH 3 N(H)N 2 ] + and [CF 3 N(H)N 2 ] + were prepared as their low‐temperature stable [AsF 6 ] − salts by protonation of azidomethane and azidotrifluoromethane in superacidic systems. They were characterized by NMR and Raman spectroscopy. Unequivocal proof of the protonation site was obtained by the crystal structures of both salts, confirming the formation of alkylamino diazonium ions. The Lewis adducts CH 3 N 3 ⋅AsF 5 and CF 3 N 3 ⋅AsF 5 were also prepared and characterized by low‐temperature NMR and Raman spectroscopy, and also by X‐ray structure determination for CH 3 N 3 ⋅AsF 5 . Electronic structure calculations were performed to provide additional insights. Attempted electrophilic amination of aromatics such as benzene and toluene with methyl‐ and trifluoromethylamino diazonium ions were unsuccessful.

Saal, Thomas↗
DOE OSTI2025

Evaluation of the performance of event reconstruction algorithms in the JSNS 2 experiment using a 252 Cf calibration source

JSNS 2 investigates short-baseline neutrino oscillations using a 24-meter baseline and a 17-tonne Gd-loaded liquid scintillator target. Accurate event-reconstruction algorithms are crucial for analyzing experimental data. The algorithms undergo meticulous validation through calibration with a 252 Cf source. This paper outlines the methodology and evaluates the reconstruction performance, focusing on neutrino interactions up to approximately 50 MeV for sterile neutrino searches. Both 252 Cf and Michel electron events are studied to evaluate reconstruction accuracy. The analysis concludes that the uncertainty of the fiducial volume, with an appropriate correction, is much less than the requirement of JSNS 2 requirement (10%). Furthermore, the energy resolution is measured to be 3.3 ± 0.1% for the Michel electron endpoint and 4.3 ± 0.1% for the n-Gd peak in the central region.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Molecular Dynamics and Free Energy Calculations of Dicyclohexano-18-crown-6 Diastereoisomers with Sm 2+ , Eu 2+ , Dy 2+ , Yb 2+ , Cf 2+ , and Three Halide Salts in Tetrahydrofuran and Acetonitrile Using the AMOEBA Force Field

With the continual development of lanthanides (Ln) in current technological devices, an efficient separation process is needed that can recover greater amounts of these rare elements. Dicyclohexano-18-crown-6(DCH18C6) is a crown ether that may be a promising candidate for Ln separation, but additional research is required. As such, molecular dynamics(MD) simulations have been performed on four divalent lanthanide halide salts(Sm 2+ , Eu 2+ , Dy 2+ , and Yb 2+ ) and one divalent actinide halide salt (Cf 2+ ) bound to three diastereoisomers of DCH18C6. Dy 2+ , Yb 2+ , Cf 2+ , DCH18C6, and tetrahydrofuran (THF) solvent were parameterized for the AMOEBA polarizable force field for the first time, whereas existing parameters for Sm 2+ and Eu 2+ were utilized from our previous efforts. A coordination number (CN) of six for Ln 2+ /An 2+ –O solvated in THF indicated that the cations interacted almost entirely with the oxygens of the polyether ring. A CN of one for Ln 2+ /An 2+ -N solvated in acetonitrile for systems containing iodide suggested that theN atom of acetonitrile was competitive with I – for cation interactions. Fluctuation between five and six CNs for Dy 2+ and Yb 2+ suggested that although the cations remained in the polyether ring, the size of the ring may not be an ideal fit as these cations possess comparatively smaller ionic radii. Gibbs binding free energies of Sm 2+ in all DCH18C6 diastereoisomers solvated in THF were calculated. The binding free energy of the cis-syn-cis diastereoisomer was the most favorable, followed by cis-anti-cis, and then trans-anti-trans. Lastly, two major types of conformation were observed for each diastereoisomer that were related to the electrostatic interactions and charge density of the cations.

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

Probing Conformational Evolution and Associated Dynamics of Mg(N(SO 2 CF 3 ) 2 ) 2 ·Dimethoxyethane Adduct Using Solid-State 19 F and 1 H NMR

Bis(trifluoromethanesulfonimide) or TFSI is widely used as a counter anion in electrolyte design due to its structural flexibility and chemical stability. Here we studied the conformational variations and associated dynamics of TFSI in adduct of Mg(TFSI) 2 with dimethoxyethane (DME), a solvate crystalline material using solid-state 1 H and 19 F NMR. TFSI molecular motion in this solvate structure falls within the timescale of the 19 F NMR experiment, yielding spectroscopic signatures for unique TFSI conformers under the coordination environment of Mg 2+ cation. Within the temperature range of -5 to 82 °C, we observe nine distinct TFSI sites in both crystalline and disordered regions using 19 F NMR, reflecting complexity of structural and dynamics of TFS1 anions within solvate structure. The four distinguishable sites in the disordered region for the two CF 3 groups of the same TFSI molecule are identified using chemical shift analysis. The exchange rate constants from site to site are calculated through variable temperature 19 F NMR and two-dimensional (2D) exchange spectroscopy (EXSY) experiments, along with respective activation enthalpies using Eyring's formulation. The flip rate of CF 3 around the S-C bond is estimated as ~ 15 s -1 at 8 °C with ΔH ≠ ~ 22 kJ/mol, but the rotation of the entire TFSI is 4.8 s -1 at 8 °C with a significantly greater ΔH ≠ = 98 ± 10 kJ/mol. Furthermore, the slow conversion of trans to cis conformers at a lower temperature (T ≤ 1 °C) in the crystalline region is monitored, with a conversion rate of ~ 2 x 10 -5 s -1 at -5 °C. Density functional theory (DFT)-based calculations were performed to support further the assignment of experimental chemical shifts, and the activation energy E a = 21.1 kJ/mol obtained for the cis to trans transition is consistent with experimental values. The combined set of 19 F and 1 H under both one-dimensional (1D) and 2D NMR methods demonstrated here can be further used for examining electrode-electrolyte interfaces to probe the motions of various constituents that can enable detailed studies of interfacial processes and dynamics. Ultimately, such studies will aid in the design and discovery of interfacial constructs in which directed defect chemistry, chemical moiety distribution, and nanostructure are employed to drive efficient charge transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

First-principles investigation of high capacity, rechargeable CF x cathode batteries based on graphdiyne and “holey” graphene carbon allotropes

Batteries composed of CF x cathodes have high theoretical specific capacities (>860 mA h g -1 ). Attempts at realizing such batteries coupled with Li anodes have failed to deliver on this promise, however, due to a discharge voltage plateau below the theoretical maximum lowering the realized energy density and difficulties with recharging the system. Here, in this study, we use first-principles calculations to investigate novel carbon allotropes for these battery systems: graphdiyne and “holey” graphene. We first identify stable flourination structures and calculate their band gaps. We demonstrate that the holes in these carbon allotropes can induce the formation of an amorphous LiF network within the carbon and that this formation may, in fact, be kinetically favored. For structures where amorphous LiF forms within the carbon, we predict it is easier to recharge and higher discharge voltages can be achieved. If the LiF forms outside the carbon product, however, it will be crystalline in form and lead to lower discharge voltages and more difficulty in recharging the systems. Finally, we simulate XPS spectra of representative cases, demonstrating an experimental pathway for determining the reaction pathway of these systems. Our work suggests CF x allotropes with holes in them as potential targets for high capacity, rechargeable cathodes for Li batteries, provided they lead to the formation of amorphous LiF within the C structure.

25 ENERGY STORAGE↗
DOE OSTI2024

Alternatives to NIST Cf-252 Iirradiations for Transfer Calibration of S-32 Neutron Monitors

Gas-flow proportional counting systems are used by the Radiation Metrology Laboratory (RML) at Sandia National Laboratories for reactor fluence monitoring with the 32 S(n,p) 32 P reaction. Calibration of these systems has traditionally been accomplished by fluence-transfer irradiations at the NIST 252 Cf facility. Such calibrations have become increasingly difficult as the NIST 252 Cf source decayed to unusable levels. To minimize the risk to the testing programs from an inability to properly calibrate these systems, the RML has developed two alternative calibration techniques: 1) development and implementation of certified 32 P sources for activity calibrations and subsequent calculation of neutron fluence, and 2) direct counting of non-certified reactor-irradiated sulfur pellets by liquid scintillation counting to determine 32 P activity for the subsequent calibration of gas-flow proportional counters. Preliminary comparisons show that the several calibration methods are capable of overall uncertainties within about 5 percent.

Vehar, David W.↗
DOE OSTI2025

Transmission spectroscopy of CF 4 molecules in intense x-ray fields

The nonlinear interaction of x rays with matter is at the heart of understanding and controlling ultrafast molecular dynamics from an atom-specific viewpoint, providing new scientific and analytical opportunities to explore the structure and dynamics of small quantum systems. At increasingly high x-ray intensity, the sensitivity of ultrashort x-ray pulses to specific electronic states and emerging short-lived transient intermediates is of particular relevance for our understanding of fundamental multiphoton absorption processes. In this work, intense x-ray free-electron laser (XFEL) pulses at the European XFEL are combined with a gas cell and grating spectrometer for a high-intensity transmission spectroscopy study of multiphoton-induced ultrafast molecular fragmentation dynamics in CF 4 . This approach unlocks the direct intrapulse observation of transient fragments, including neutral atoms, by their characteristic absorption lines in the transmitted broadband x-ray spectrum. The dynamics with and without initially producing fluorine 𝐾-shell holes are studied by tuning the central photon energy. The absorption spectra are measured at different FEL intensities to observe nonlinear effects. Transient isolated fluorine atoms and ions are spectroscopically recorded within the ultrashort pulse duration of a few tens of femtoseconds. An isosbestic point that signifies the correlated transition between intact neutral CF 4 molecules and charged atomic fragments is observed near the fluorine 𝐾 edge. The dissociation dynamics and the multiphoton absorption-induced dynamics encoded in the spectra are theoretically interpreted. Overall, this study demonstrates the potential of high-intensity x-ray transmission spectroscopy to study ultrafast molecular dynamics with sensitivity to specific intermediate species and their electronic structure.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Structure of Nd 155 and Gd 163 from Cf 252 spontaneous fission

Background: A puzzle has arisen recently caused by the apparent shift in maximum deformation from the expected 66 Dy isotopic chain to the Nd 60 isotopic chain in the 82 155 Nd and 163 Gd, useful for constraining parameters in models that seek to answer the six proton shift in maximum deformation. Method: Data from the spontaneous fission of 252 Cf were taken by the Gammasphere detector array at Lawrence Berkeley National Laboratory to observe the excited states of 155 Nd and 163 Gd. Results: The structure of 163 Gd has been expanded with the addition of two new levels and three new γ rays, which are found to be consistent with previously published calculations and the structure of 165 Dy. In 155 Nd, nine new levels and 12 new γ rays are observed. The spins and parities of the previously known levels in 155 Nd have been reassigned from a ν3/2 - [521] ground state configuration to a ν5/2 + [642] isomeric configuration by comparison of these newly observed levels with levels in 153 Nd and 155 Sm. Conclusion: Further experimentation is required to determine the energy of the newly reassigned ν5/2+[642] level in 155 Nd with respect to the suspected ν3/2-[521] ground state. Additionally, more experiments should be conducted to further determine the structure of neutron rich nuclei, rarely produced in the spontaneous fission of 252 Cf, such as 163 Gd.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Ising-CF: A Pathbreaking Collaborative Filtering Method Through Efficient Ising Machine Learning

Due to Ising models’ strong expressivity and Ising machines’ unique computational power, it is highly desired if Ising-based learning can be used in real-world applications. Unfortunately, the challenges in learning Ising models and gaps between the practical accuracy of Ising machines and the theoretical accuracy of Ising models impede the realization of Ising machines’ potential. Hence, we propose an Ising Machine Learning framework, Ising-CF, for collaborative filtering, a widely-used recommendation method. Specifically, Ising-CF uses Linear Neural Networks with Besag’s pseudo-likelihood and voltage polarization for fast, accurate Ising model learning and an Ising-specific logarithmic quantization for ns-level Ising machine inference with near-theoretical accuracy, 7.3% over SOTA.

Liu, Zhuo↗
DOE OSTI2026

Development of a deep potential model for F and CF 2 etching of Si and SiO 2

An understanding of plasma-surface interactions at increasingly smaller scales is invaluable for the development of novel technologies and processing techniques. Molecular dynamics (MD) simulations can provide insights into atomic-scale interactions, though they are restricted by the availability of interatomic potentials. Machine learning methods, such as Deep Potential Molecular Dynamics (DeepMD), provide a systematic framework for the development of accurate and flexible ab initio-based models. In this work, we develop DeepMD models for the ion-enhanced etching of Si and SiO 2 by F and CF 2 radicals. We employ an active learning process to expand the data set on which the model is trained and demonstrate its effect on the model accuracy. The DeepMD results are compared to data from classical MD simulations and experiments. Physical sputtering yields of SiO 2 by Ar + ions show good agreement with previous simulation results using conventional interatomic potentials, though the predicted depth profiles are different. Etching yields are calculated as a function of ion energy and neutral to ion flux ratio for the Ar + ion-enhanced etching of SiO 2 and Si by F atoms, as well as for etching of SiO 2 by CF 2 radicals, showing reasonable agreement with experimental data. Finally, an ion-enhanced surface kinetic model is fitted to the DeepMD etch yields, and the fitted parameters are compared to quantities computed directly from DeepMD simulations. This study illustrates how molecular dynamics simulations using machine learning potentials can provide an accurate model of etching processes relevant to device manufacturing.

Kounis-Melas, Andreas [Princeton Univ., NJ (United↗
DOE OSTI2020

Production of Cf-252 and other transplutonium isotopes at Oak Ridge National Laboratory

In 1957 Glenn T. Seaborg conceived and advocated for the construction of the High Flux Isotope Reactor (HFIR) and the Transuranium Processing Plant (since then renamed the Radiochemical Engineering Development Center, or REDC) at Oak Ridge National Laboratory. There, heavily shielded hot cells, glove boxes, and laboratories allow recovery of transuranium elements produced in substantial quantities. Seaborg’s vision of HFIR and REDC producing milligram quantities of berkelium, californium, and einsteinium has been fulfilled beginning in 1966 through May 2019 with 78 production campaigns yielding a cumulative totals of 1.2 g of 249 Bk, 10.2 g of 252 Cf, 39 mg of 253 Es, and 15 pg of 257 Fm. Notably, 252 Cf is a neutron source used in many industrial applications including oil exploration; process control systems for the cement industry, coal analysis, and power production; sources to start nuclear reactors and perform nondestructive materials analyses; homeland security and national defense detection devices; and medical research. Isotopes made available through transplutonium production at HFIR/REDC have enabled scientists to study the nuclear properties and reactions, chemical properties, optical properties, and solid-state properties of transplutonium elements. Long-lived isotopes have served as targets in heavy ion accelerators to produce heavier elements leading to the discovery of 104 Rf, 105 Db, 106 Sg, 113 Nh, 114 Fl, 115 Mc, 116 Lv, 117 Ts, and 118 Og. This paper reviews the evolution of the processing flowsheets to produce, separate, and purify transplutonium isotopes, which have evolved over 50 years of operation at HFIR and REDC, and summarizes directions of future work to improve the efficiency of the production operations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Measurement Plan for Uncertainty Contributions to 252 Cf Waste Measurements

This measurement plan establishes the methodology for performing and analyzing mock-up measurements of Building 7930 Cell G Cf waste generated from 252 Cf product preparation to better determine the measurement uncertainty contributors. Understanding the uncertainty contributors will establish the total measurement uncertainty. This is critical because it will impact the administrative threshold at which personnel can discriminate between low-level waste (LLW) and transuranic (TRU) waste.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗