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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

IR Laser Control of the Clustering of CF{sub 3}Br Molecules during the Gas-Dynamic Expansion of a CF{sub 3}Br/Ar Mixture: Bromine Isotope Selectivity

The infrared (IR) laser radiation control of the clustering of CF3Br molecules during the gas-dynamic expansion of a CF{sub 3}Br/Ar mixture at the exit from a nozzle is investigated. Prominence is given to studying the possibility of bromine-isotope-selective suppression of the clustering of CF{sub 3}Br molecules due to their resonance vibrational excitation in the gas-dynamic expansion zone near the nozzle. A continuous CO{sub 2} laser is used in experiments to excite molecules and clusters in a beam, and a quadrupole mass spectrometer is used to detect them. The experimental setup and the experimental technique are described. The dependences of the efficiency of molecule clustering suppression on the exciting laser radiation parameters, the gas parameters (composition, pressure) above the nozzle, and the distance from the nozzle exit section to a molecule irradiation zone are obtained. Bromine-isotope-selective suppression of molecule clustering is shown to occur at the exit from the nozzle due to the resonance vibrational excitation of gas-dynamically cooled CF{sub 3}Br molecules. When CF{sub 3}Br/Ar mixtures are used at pressure ratios p(CF{sub 3}Br): p(Ar) = 1: 10 and 1: 30, the enrichment of a cluster beam by bromine isotopes are K{sub enr}({sup 81}Br) ≈ 1.18 ± 0.09 and 1.12 ± 0.07 during the 9R(30) laser line (1084.635 cm{sup –1}) irradiation of a jet. The clustering suppression selectivity is α ≈ 1.18 when the mixture at the pressure ratio p(CF{sub 3}Br): p(Ar) = 1: 10 is used. These results suggest that the proposed method can selectively control the clustering of the molecules containing the heavy element isotopes that have a small isotope shift in IR absorption spectra (OsO{sub 4}, WF{sub 6}, UF{sub 6}).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Suppression of clustering of CF{sub 3}Br molecules with argon atoms by CO{sub 2} laser radiation in gas-dynamic expansion of a CF{sub 3}Br–Ar mixture: bromine isotope selectivity

We present the study of suppressing the clustering of CF{sub 3}Br molecules with argon atoms under gas-dynamic expansion of the CF{sub 3}Br–Ar mixture at a nozzle exit by a cw CO{sub 2} laser. The main attention is paid to the analysis of possibility of implementing the selective control of bromine isotope clustering. The method relies on the vibrational excitation of molecules with the laser radiation, which leads to the suppression of their clustering with argon atoms. The experimental setup and the method of study are briefly described. The results of evaluation of the efficiency and selectivity of suppression of molecular–atomic clustering for different compositions of the gas above the nozzle and separations between the irradiation zone and the nozzle exit section are presented. It is shown that under the resonance vibrational excitation of gas-dynamically cooled CF{sub 3}Br molecules at the nozzle exit one can implement bromine isotope selective suppression of clustering of molecules with argon atoms. It is found that by controlling the clustering of CF{sub 3}Br molecules with argon atoms one can implement considerably higher enrichment and selectivity factors than in the case of controlling the clustering of CF{sub 3}Br molecules with each other. Thus, using the CF{sub 3}Br–Ar mixture (the ratio of pressures 1 : 100 and 1 : 200) the enrichment factors for the bromine isotopes K{sub enr}({sup 81}Br) = 1.50 ± 0.13 and 1.30 ± 0.09, respectively, were obtained under the conditions of irradiating the jet at the 9R(30) line of the laser (ν = 1084.635 cm{sup −1}). The selectivity α of the suppression of clustering of CF{sub 3}Br molecules with argon atoms, achieved in this case, amounted to 4.02 ± 0.19 and 2.31 ± 0.11, respectively. The results show that the method allows one to selectively control the clustering of molecules, comprising isotopes of heavy elements that possess a small isotopic shift in the IR absorption spectra. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Brome isotope selective control of CF{sub 3}Br molecule clustering by IR laser radiation in gas-dynamic expansion of CF{sub 3}Br – Ar mixture

We report the results of research on the experimental control of CF{sub 3}Br molecule clustering under gas-dynamic expansion of the CF{sub 3}Br – Ar mixture at a nozzle exit by using IR laser radiation. A cw CO{sub 2} laser is used for exciting molecules and clusters in the beam and a time-of-flight mass-spectrometer with laser UV ionisation of particles for their detection. The parameters of the gas above the nozzle are determined (compositions and pressure) at which intensive molecule clustering occurs. It is found that in the case of the CF{sub 3}Br gas without carrier when the pressure P{sub 0} above the nozzle does not exceed 4 atm, molecular clusters actually are not generated in the beam. If the gas mixture of CF{sub 3}Br with argon is used at a pressure ratio 1 : N, where N ⩾ 3, and the total pressure above the nozzle is P{sub 0} ⩾ 2 atm, then there occurs molecule clustering. We study the dependences of the efficiency of suppressing the molecule clustering on parameters of the exciting pulse, gas parameters above the nozzle, and on a distance of the molecule irradiation zone from the nozzle exit section. It is shown that in the case of resonant vibrational excitation of gas-dynamically cooled CF{sub 3}Br molecules at the nozzle exit one can realise isotope-selective suppression of molecule clustering with respect to bromine isotopes. With the CF{sub 3}Br – Ar mixtures having the pressure ratio 1 : 3 and 1 : 15, the enrichment factors obtained with respect to bromine isotopes are k{sub enr} ≈ 1.05 ± 0.005 and k{sub enr} ≈ 1.06 ± 0.007, respectively, under jet irradiation by laser emission in the 9R(30) line (1084.635 cm{sup −1}). The results obtained let us assume that this method can be used to control clustering of molecules comprising heavy element isotopes, which have a small isotopic shift in IR absorption spectra. (paper)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2019

Infrared laser-induced isotope-selective dissociation of mixed (CF{sub 3}Br){sub m}Ar{sub n} van der Waals clusters

The paper presents the results of studies of IR laser-induced bromine-isotope-selective dissociation of small mixed (CF{sub 3}Br){sub m}Ar{sub n} van der Waals clusters (m = 1, 2 and 1 ≤ n ≤ 5 is the number of molecules and atoms in the clusters, respectively). The experiments used a pulsed CO{sub 2} laser to excite clusters and a quadrupole mass spectrometer to detect a molecular cluster beam. The research method is based on the selective vibrational excitation of clusters by IR laser radiation, leading to their predissociation. The possibilities of implementing bromine-isotope-selective dissociation of clusters are considered. The experimental setup and research method are briefly described. The results of determining the cluster dissociation efficiency and selectivity as functions of the energy and frequency of laser radiation are presented. It is shown that resonant vibrational excitation of clusters makes it possible to induce their isotope-selective dissociation. Thus, using a CF{sub 3}Br/Ar mixture with a pressure ratio of 1/200, the enrichment factors of the {sup 79}Br isotope are found to be K{sub enr}({sup 79}Br) = 1.15 ± 0.04 and 0.95 ± 0.03 under cluster irradiation conditions on the 9R(30) (ν = 1084.635 cm{sup −1}) and 9R(24) (ν = 1081.087 cm{sup −1}) lines, respectively The achieved dissociation selectivities for the clusters are, respectively, 1.16 ± 0.05 and 0.95 ± 0.04. The results obtained suggest that this method can be used to separate isotopes in molecules containing isotopes of heavy elements, which have a slight isotopic shift in the IR absorption spectra. (laser isotope separation)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Total absorption γ -ray spectroscopy of the β -delayed neutron emitters Br 87 , Br 88 , and Rb 94

In this paper, we investigate the decay of 87,88 Br and 94 Rb using total absorption γ-ray spectroscopy. These important fission products are β-delayed neutron emitters. Our data show considerable βγ intensity, so far unobserved in high-resolution γ-ray spectroscopy, from states at high excitation energy. We also find significant differences with the β intensity that can be deduced from existing measurements of the β spectrum. We evaluate the impact of the present data on reactor decay heat using summation calculations. Although the effect is relatively small it helps to reduce the discrepancy between calculations and integral measurements of the photon component for 235 U fission at cooling times in the range 1-100 s. We also use summation calculations to evaluate the impact of present data on reactor antineutrino spectra. We find a significant effect at antineutrino energies in the range of 5 to 9 MeV. In addition, we observe an unexpected strong probability for γ emission from neutron unbound states populated in the daughter nucleus. The γ branching is compared to Hauser-Feshbach calculations, which allow one to explain the large value for bromine isotopes as due to nuclear structure. However the branching for 94 Rb, although much smaller, hints of the need to increase the radiative width Γ γ by one order of magnitude. Finally, this increase in Γ γ would lead to a similar increase in the calculated (n, γ) cross section for this very neutron-rich nucleus with a potential impact on r process abundance calculations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1975

Krypton and xenon in Apollo 14 samples - Fission and neutron capture effects in gas-rich samples

Gas-rich Apollo 14 breccias and trench soil are examined for fission xenon from the decay of the extinct isotopes Pu-244 and I-129, and some samples have been found to have an excess fission component which apparently was incorporated after decay elsewhere and was not produced by in situ decay. Two samples have excess Xe-129 resulting from the decay of I-129. The excess is correlated at low temperatures with excess Xe-128 resulting from neutron capture on I-127. This neutron capture effect is accompanied by related low-temperature excesses of Kr-80 and Kr-82 from neutron capture on the bromine isotopes. Surface correlated concentrations of iodine and bromine are calculated from the neutron capture excesses.

Drozd, R.↗
DOE OSTI2020

Strong mutual increase in the efficiency of isotope-selective laser IR dissociation of molecules under nonequilibrium thermodynamic conditions of the compression shock under irradiation in a bimolecular mixture

We have revealed a strong (by a factor of 2 to 5) mutual increase in the yield of IR molecular dissociation (by the example of CF{sub 2}HCl and CF{sub 3}Br) and a significant (by a factor of 1.5 to 3) lowering of dissociation thresholds in the nonequilibrium thermodynamic conditions of compression shock in the irradiation of the molecules by resonance IR laser radiation in the bimolecular mixture in comparison with their individual irradiation. This opens up the possibility to perform efficient isotope-selective IR dissociation of molecules at lower excitation energy densities (Φ ⩽ 1.5 – 2.0 J cm{sup −2}) and thereby to improve the dissociation selectivity. This was demonstrated by the example of chlorine- and bromine-isotope selective dissociation of the specified molecules, which are characterised by quite small (less than 0.25 cm{sup −1}) isotope shifts in the IR vibrational absorption spectra excited by laser radiation. The enrichment coefficients K {sub enr}({sup 35}Cl / {sup 37}Cl) = 0.90 ± 0.05 in the residual CF{sub 2}HCl gas and K {sub enr}({sup 79}Br / {sup 81}Br) in the resultant Br{sub 2} product are obtained when the CF{sub 2}HCl : CF{sub 3}Br = 1 : 1 molecular mixture and CF{sub 3}Br molecules, respectively, are irradiated by the 9R(30) CO{sub 2} laser line (frequency, 1084.635 cm{sup −1}) at an energy density Φ ≈ 1.3 J cm{sup −2}. (laser isotope separation)

36 MATERIALS SCIENCE↗
DOE OSTI2017

Novel Concepts of MS-Cleavable Cross-linkers for Improved Peptide Structure Analysis

The chemical cross-linking/mass spectrometry (MS) approach is gaining increasing importance as an alternative method for studying protein conformation and for deciphering protein interaction networks. This study is part of our ongoing efforts to develop innovative cross-linking principles for a facile and efficient assignment of cross-linked products. We evaluate two homobifunctional, amine-reactive, and MS-cleavable cross-linkers regarding their potential for automated analysis of cross-linked products. We introduce the bromine phenylurea (BrPU) linker that possesses a unique structure yielding a distinctive fragmentation pattern on collisional activation. Moreover, BrPU delivers the characteristic bromine isotope pattern and mass defect for all cross-linker-decorated fragments. We compare the fragmentation behavior of the BrPU linker with that of our previously described MS-cleavable TEMPO-Bz linker (which consists of a 2,2,6,6-tetramethylpiperidine-1-oxy moiety connected to a benzyl group) that was developed to perform free-radical-initiated peptide sequencing. Comparative collisional activation experiments (collision-induced dissociation and higher-energy collision-induced dissociation) with both cross-linkers were conducted in negative electrospray ionization mode with an Orbitrap Fusion mass spectrometer using five model peptides. As hypothesized in a previous study, the presence of a cross-linked N-terminal aspartic acid residue seems to be the prerequisite for the loss of an intact peptide from the cross-linked products. As the BrPU linker combines a characteristic mass shift with an isotope signature, it presents a more favorable combination for automated assignment of cross-linked products compared with the TEMPO-Bz linker. .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Expanded Coverage of Phytocompounds by Mass Spectrometry Imaging Using On-Tissue Chemical Derivatization by 4-APEBA

Probing the entirety of any species metabolome is an analytical grand challenge, especially at a cellular scale. Where spatial metabolomics, completed primarily by matrix-assisted laser desorption/ionization (MALDI), has limited molecular coverage for several reasons. To expand the scope of spatial metabolomics, we developed an on-tissue chemical derivatization (OTCD) workflow using 4-APEBA for confident identification of several dozen elusive phytocompounds, including several phytohormones, which have various roles within stress responses and cellular communication. Superiority of 4-APEBA is established in comparison to other derivatization agents with (1) broad specificity towards carbonyls, (2) low background, and (3) introduction of bromine isotopes, where the latter two facilitate confident bioinformatics. In conclusion, the outlined workflow trailblazes a path towards spatial hormonomics within plant samples, enhancing detection of carboxylates, aldehydes, ketones, and plausibly phenols.

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

Decay studies of the 𝛽-delayed neutron emitters 87 Br and 88 Br measured by means of the Modular Total Absorption Spectrometer at ORNL HRIBF

The β decays of 87 Br, 88 Br, and 87 Kr were measured with the Modular Total Absorption Spectrometer (MTAS) at Oak Ridge National Laboratory’s Holifield Radioactive Ion Beam Facility (HRIBF). Both bromine isotopes are β-delayed neutron emitters that have large cumulative fission yields and were identified as top-priority cases for total absorption study by the Nuclear Energy Agency in 2007. Our investigations corroborate that the decay schemes of 87 Br and 88 Br suffer from the so-called pandemonium effect. Unique MTAS properties enable direct neutron measurements. Here, we present MTAS-derived β-delayed neutron spectra, β-delayed neutron emission probabilities of P n ( 87 Br) = 2.36(24)%, and P n ( 88 Br) = 6.4(6)%, and the β-delayed neutron transitions intensity of 4(2)% to the first excited 87 Kr state, populated in the β-neutron decay of 88Br. Incorporating new data into calculations of the electromagnetic decay heat component emitted during thermal neutron fission of 235 U and 239 Pu improves agreement with experimental data up to approximately 80 s after fission. The estimation of the nuclear reactor $\bar{ν}_e$ flux results in changes of up to 1% in the expected $\bar{ν}_e$ interactions with the detector material for 235 U, 238 U, 239Pu, and 241 Pu.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1995

The n1(sub 1) Band of HOBr

The n1 band of HOBr centered at 3614.903 cm-1 has been observed at 0.006 cm-1 resolution. The band is a hybrid type with The spectra of both bromine isotopes have been simultaneously fitted with a single calculation which includes all the previously reported rotational transitions. There appear to be no strong local perturbations to complicate the fitting of the line positions. Precise parameters are reported for the upper states as well as improved parameters for the ground states of both species. There is a prominent Herman-Wallis effect for the b-type transitions which is well described by linear and quadratic terms in Ka. The equilibrium structure has been calculated.

Band of HOBr↗
DOE OSTI2011

Nuclear Data Sheets for A = 93

Nuclear structure data pertaining to all nuclei with mass number A=93 (Se, Br, Kr, Rb, Sr, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag) have been compiled and evaluated and incorporated into the ENSDF data file. This publication for A=93 supersedes the previous publication by C.M. Baglin, Nuclear Data Sheets80, 1 (1997) (literature cutoff date November 1996) and subsequent revisions by C.M. Baglin of the ENSDF files for 93Br and {sup 93}Kr (literature cutoff 26 February 2001) and for {sup 93}Rh (literature cutoff 27 February 2001); it includes all data available prior to 15 December 2010. Significant changes since prior evaluations include the following: 2010Hw03 identified several high-spin states in {sup 93}Kr in {sup 252}Cf SF decay; in addition to the many low-spin levels already known in {sup 93}Rb from {beta}{sup -} decay, several higher-spin states have now been identified in a {sup 252}Cf SF decay study (2009Hw03); this SF decay has also been used to identify additional states in {sup 93}Sr (2003Hw01) and the {sup 238}U({sup 82}Se,X{gamma}) reaction (2007Bu35) has provided new information on {sup 93}Y. (HI,xn{gamma}) reaction studies have expanded our knowledge of the structure of {sup 93}Zr (2002Fo03, 2005Pa48), {sup 93}Nb (2007Wa45), {sup 93}Mo (2005Fu01), {sup 93}Tc (2003Ha22) and {sup 93}Pd (2004So04,2004Ru02). Considerable information on {sup 93}Nb was provided by a (p,2n{gamma}) study (2010Or01, 2006Or09, 2007Or01). The level schemes of {sup 93}Ru, {sup 93}Rh and {sup 93}Pd have undergone the most extensive revision thanks to studies of {sup 93}Rh {epsilon} decay (2004De40), {sup 94}Ag {epsilon}p decay (2004Mu30) and {sup 94}Ag p decay (2005Mu15, 2005Mu30), respectively. The half-life of the Zr member of this chain is of particular interest because of {sup 93}Zr's large contribution to long-term activity of nuclear reactor waste and also due to its potential as a supernova chronometer. During 2010, two new well-documented measurements of T{sub 1/2}({sup 93}Zr) were published (2010Ya01 and 2010Ca01); one agrees well with an earlier, undocumented measurement but, unfortunately, the other is many standard deviations lower for reasons which are not immediately apparent.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Shape evolution at high spin states in Kr and Br isotopes

The high spin states in A = 75, Kr and Br isotopes have been populated via fusion-evaporation reaction at an incident beam energy of 90 MeV. The de-exciting γ-rays were detected utilizing the Indian National Gamma Array (INGA). Lifetime of these excited high spin states were determined by Doppler-shift attenuation method. Experimental results obtained from lifetime measurement are interpreted in the frame work of projected shell-model to get better insight into the evolution of collectivity. Comparison of the calculations of the model with transitional quadrupole moments Q{sub t} of the positive and negative parity bands firmly established their configurations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2011

Digital Electronics For The Versatile Array Of Neutron Detectors At Low Energies

A {chi}{sup 2} minimization algorithm has been developed to extract sub-sampling-time information from digitized waveforms, to be used to instrument the future Versatile Array of Neutron Detectors at Low energies. The algorithm performance has been characterized with a fast Arbitrary Function Generator, obtaining time resolution better than 1 ns for signals of amplitudes between 50 mV and 1V, with negligible walk in the whole range. The proof-of-principle measurement of the beta-delayed neutron emission from {sup 89}Br indicates a resolution of 1 ns can be achieved in realistic experimental conditions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Development of a Computational Framework for Multiphysics Multiphase Species Tracking using NEAMS Tools

This report implements a high-fidelity multiphysics modeling framework using the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program tools to track isotopic species in Molten Salt Reactors (MSRs), with a specific focus on the 91-depletion chain within the Molten Salt Reactor Experiment (MSRE). The model integrates neutronics, thermal-hydraulics, depletion, and thermochemistry to simulate the production, transport, and phase transitions of isotopes under steady-state and transient conditions. The main findings reveal that isotopes such as bromine-91 largely remain in the liquid phase, while others, including krypton-91and yttrium-91, transition to the gas phase, significantly influencing the reactor’s radiological source term. The study also shows that during transients, like a reactivity insertion transient, rapid void formation and the expansion of the liquid-gas interface led to substantial transfers of dissolved isotopes into the gas phase, altering isotope distribution and largely increasing the source term in the off-gas system. Additionally, the research highlights that short-lived isotopes dominate the initial off-gas response during transients, while longer-lived isotopes determine the equilibrium state, underscoring the necessity of dynamic simulations for accurate species tracking and reactor safety analysis. The developed methodology will be applied in the future to the tracking of a larger number of species and introduce other species tracking mechanisms, such as deposition and plating.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1986

The composition of lunar noble gases traped 2.5 AE and 3.5 AE ago

The times when the soils 74001 and 73261 were exposed on the lunar surface were determined by the U-235 - Xe-136 dating method. The isotopic composition of the trapped noble gases in these two soils is compared with that of the surface correlated noble gases in the young soils 12001 and in the present day solar wind. The surface correlated trapped gases are a mixture of implanted solar wind particles and retrapped lunar atmospheric gases. The observed changes are interpreted as a result of decreasing outgassing of radiogenic Ar-40 and perhaps He-4 and of fissiogenic Xe from the lunar crust. The old soils probably also contain surface correlated Kr-80 and Kr-82 produced by secondary cosmic ray neutron capture of adsorbed or retrapped bromine. To some extent the isotopic composition of the trapped gases in old lunar soil may also have been altered due to diffusion loss from material of low retentivity.

Eugster, O.↗
NASA NTRS1972

Exposure ages and neutron capture record in lunar samples from Fra Mauro.

Cosmic-ray exposure ages of Apollo 14 rocks and rock fragments obtained by the Kr81-Kr83 method range from 27 to 700 m.y. Rock 14321, collected near the Cone crater rim, is one of the many approximately 27 m.y. old ejecta which were reported at the Third Lunar Science Conference. All the other rocks have considerably higher exposure ages. Isotopic anomalies from neutron capture in gadolinium, bromine, and barium are used to obtain information on the lunar neutron spectrum at various depths below the lunar surface. The flux ratio of resonance and slow (less than 0.3 eV) neutrons is found to be nearly constant in the topmost approximately 100 g/sq cm.

Lugmair, G. W.↗