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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Prototype X-ray and Gamma Detection with Cyclotron Radiation Emission Spectroscopy

Cyclotron radiation emission spectroscopy, or CRES, is a novel approach to measuring the energy of an electron. By trapping a free electron in a high magnetic field, it undergoes cyclotron motion and emits radiofrequency (RF) waves. The frequency of this RF radiation is directly related to the energy of the electron. Because many cycles of the RF emission are recorded, the energy resolution of the CRES system is on the order of a single electron volt. To make a CRES system sensitive to photons, a target gas is used to induce a photoelectric effect, producing the electron that is subsequently trapped. By adding the binding energy of the target atom, the energy of the incident photon may be reconstructed. Using a xenon target gas, photoelectric interactions dominate up to approximately 300 keV, covering not only all atomic shell X-rays of the elements, but many low-lying nuclear states as well, including key transuranic elements related to nuclear security. CRES holds the potential of maintaining single-eV resolution up to this 300-keV range, thereby surpassing current state-of-the-art detectors by a factor of 10-100. The instrumental resolution of the system is limited by the uniformity of the applied magnetic field.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Spectroscopy of a sample of unidentified gamma-ray Fermi sources

ABSTRACT The fourth-DR3 version (4FGL-DR3) of the Fermi-LAT catalogue of γ-ray sources contains ∼1000 objects at a galactic latitude |b| > 10° that are not identified with an optical counterpart. We performed a systematic study of these sources, focusing on 190 objects that have a unique X-ray counterpart in the available Swift/XRT observations. Optical counterparts were then selected, and optical spectra were found in the literature for 33 sources. We found that 21 could be classified as BL Lac objects. Among these, we were able to provide the redshift for eight of them, while for two others we established a lower limit to the redshift by detecting intervening absorption. The other 12 objects display optical spectra with prominent emission lines (0.036 < z < 1.65). These spectra are characterized by both broad and narrow emission lines, with the exception of three sources. One of these displays only broad emission lines, while the other two exclusively exhibit narrow lines. On the basis of the radio/optical flux ratio, all BL Lac objects in this study are radio-loud. Four sources out of the 12 with prominent emission lines can be classified as radio-loud, while at least five of the 12 sources with prominent lines are radio-quiet. This is somewhat unexpected, given the radio-loudness distribution of 4FGL-associated blazars.

Ulgiati, Alberto (ORCID:0009000736025276)↗
DOE OSTI2020

Application of Gaussian Bayes classifier to differentiate chlorine-based chemical agents

The Portable Isotopic Neutron Spectroscopy (PINS) is a commercialized system developed by Idaho National Laboratory (INL) to examine chemical warfare agents (CWA) non-destructively, utilizing Prompt Gamma Neutron Activation Analysis (PGNAA) techniques. The PINS system takes advantage of a high-resolution gamma-ray spectrum from a mechanically-cooled high-purity germanium (HPGe) detector. One of the difficult technical challenges is to discriminate the chlorine-based chemical agents. Especially, CN, CNB, CNS and CG have similar chemical compositions to make it hard to discriminate them with a higher confidence. Current identification algorithms for PINS systems with 252-Cf sources have been improved and updated continuously as more field data became available, and new algorithms was studied to complement the current algorithms by adopting the Gaussian Bayes classifier. These new algorithms were intended to be applied to a subset of chlorine-based chemical agents, and their main goal is discriminate CN, CNB, CNS and CG with their ratios of the chlorine neutron inelastic 1763keV peak to the chlorine thermal neutron capture 1959keV peak, which is referred to as the “Cl i/c” or “clic” ratio in this study. The Cl i/c ratios were assumed to follow Gaussian distributions with the means and the standard deviations unique to their corresponding chemical agents. The prior probabilities of these four chemical agents were optimized with a collection of field data to achieve the best performance in terms of precision or positive predictive value (PPV). Finally, their posterior probabilities as functions of the Cl i/c ratio were implemented in the current version of PINS analysis software in order to be tested with more field data.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2026

Evidence for an isomeric {pi}½{sup +}[411] state in {sup 183}Ta

We report on the identification of a new isomeric state in Ta populated via the ground-state -decay of Hf. The experiment was performed at the KISS setup at RIKEN, where neutron-rich hafnium isotopes were produced via multi-nucleon transfer (MNT) reactions, followed by laser ionization of hafnium atoms, mass separation, and detection using an electron-gamma coincidence system. Isomeric spectroscopy was carried out by gating on different electron-gamma time correlations. A 459.1 keV -ray transition was identified in delayed spectra, and a half-life of μ was extracted through time-distribution fitting. The 459.1 keV state in Ta is known from previous work and has been assigned a Nilsson orbital configuration of , while a proposed new isomeric state above it is interpreted as a configuration that decays to via a low-energy, unobserved E2 transition. This is consistent with the systematic trends in neighbouring odd-A nuclei and transition rate calculations. Similar content being viewed by others

Doshi, S.↗
DOE OSTI2023

Defects of perovskite semiconductor CsPbBr3 investigated via photoluminescence and thermally stimulated current spectroscopies

Halide perovskites are essential materials for hard radiation detectors at ambient temperature. To improve detector performance, charge transport must be investigated and optimized. Using photoluminescence (PL) and thermally stimulated current (TSC) spectroscopies, we investigate photogenerated charge carriers in Bridgman-grown CsPbBr3 single crystals to understand the nature of charge transport. PL spectroscopy of these halide perovskites revealed the presence of strong emission bands at the band edge, which were attributed to free or bound excitons. It is shown that a wide broadening of the excitonic linewidth in these halide perovskites arises from strong exciton–phonon coupling, which is substantially dominated by longitudinal optical phonons via Fröhlich interaction. An additional contribution due to the presence of ionized impurities was also observed. Crystals with a detectable sensitivity to high-energy gamma radiation are characterized by a higher intensity and a narrower linewidth of the principal PL peak at 2.326 eV. Defect states beyond 2.214 eV have a negative impact on detector sensitivity to high-energy gamma radiation. TSC spectroscopy reveals an array of trap levels spanning 0.15–0.70 eV, attributed to intrinsic point defects and multiple extrinsic defects involving dopants or impurities. Defects identified included Cs and Br vacancies, as well as Pb interstitials with concentrations in the 1011–1016 cm−3 range. Understanding how the synthesis process impacts the types and concentrations of the defects present is currently under investigation. Elimination or suppression of the defect/trap states should result in halide perovskite materials with longer carrier diffusion lengths and improved detector characteristics.

Physics↗
DOE OSTI2022

Characterizing Radiation-Induced Chromium Redox Chemistry

The redox behavior of Cr(III) and Cr(VI) in nuclear environments were studied by analyzing aqueous irradiated chromium ions using UV-Visible spectroscopy. The formation of different chromium oxidation states can occur through gamma radiolysis of chromium solutions. Characterization of radiation-induced chromium is not well understood, and yet important as chromium can make its way into the primary coolant of reactors because of the corrosion of stainless steel reactor components. Furthermore, Cr(VI) is toxic and not suitable for environmental release, therefore Cr speciation is important. Fricke dosimetry was performed to collect doses rates, specific extinction coefficients were obtained from various analytical methods for the two oxidation states of chromium. Chromium samples--conditioned at various pH's and concentration to understand the effects--were then irradiated using a Coblat-60 gamma irradiator. Three optical spectroscopy analytical methods were used , including direct oxidation state measurements and complexation by either EDTA or DPC. Complexation by EDTA was found to not be a reliable method. Radiolytic oxidation of Cr(III) to Cr(VI), and reduction of Cr(VI) to Cr(III) were clearly seen, except for Cr(III) samples were a pH less than or equal to 2, where no change occurred.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Experimental study of the S 38 excited level scheme

Information on the 38 S level scheme was expanded through experimental work utilizing a fusion-evaporation reaction and in-beam γ-ray spectroscopy. Prompt γ-ray transitions were detected by the Gamma-Ray Energy Tracking Array (GRETINA) and recoiling 38 S residues were selected by the Fragment Mass Analyzer (FMA). Tools based on machine-learning techniques were developed and deployed for the first time in order to enhance the unique selection of 38S residues and identify any associated γ-ray transitions. The new level information, including the extension of the even-spin yrast sequence through J π =8( + ), was interpreted in terms of a basic single-particle picture as well shell-model calculations which incorporated the empirically derived FSU interaction. A comparison between the properties of the yrast states in the even-Z, N = 22 isotones from Z = 14 to 20, and for 36 Si– 38 S in particular, was also presented with an emphasis on the role and influence of the neutron 1 p 3/2 orbital on the structure in the region.

20 ≤ A ≤ 38↗
DOE OSTI2020

New, low-energy excitations in 107 Mo and 109 Mo

New ground-state level with spin-parity 1/2 + is established in 109 Mo, 69.8 keV below the previously reported 5/2(+) ground state in this nucleus, based on precise spectroscopy measurements of gamma radiation following spontaneous fission of 248 Cm performed using the Eurogam2 array of anti-Compton spectrometers. Analogous measurement of gamma radiation following spontaneous fission of 252 Cf, performed using the Gammasphere array, confirms the new 1/2 + ground state of 107 Mo, proposed recently and establishes the isomeric character of the 5/2 + first excited state in 107 Mo. Two beta-decaying isomers are suggested in 111 Mo nucleus based on regular energy systematics, supporting previous predictions. Low-energy excitations in Mo isotopes are interpreted and compared to calculations reported in the literature. The results suggest shape transition from prolate to oblate deformation at N >= 67.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Steam-Assisted Ammonolysis of MoO2 as a Synthetic Pathway to Oxygenated δ-MoN

A common route for the synthesis of molybdenum nitrides is through the temperature-programmed reaction of molybdenum oxides with NH3, or ammonolysis. In this work, the role of precursor phase, gas phase chemistry (impact of H2O), and temperature profile on the reaction outcome (700 °C) was examined, which resulted in varying amounts of MoO2, H2MoO5, and the nitride phases—cubic γ (nominally Mo2N) and hexagonal δ (nominally MoN). The phase fraction of the δ phase increased with precursor in the sequence MoO2 > MoO3 > H2MoO5. Steam in the reaction gas also favored the production of δ over γ, but with too much steam, MoO2 was obtained in the product. Synthesis conditions for obtaining nearly phase-pure δ were identified: MoO2 as the precursor, 2% H2O in the gas stream, and a moderate heating rate (3 °C/min). In situ X-ray diffraction provided insights into the reaction pathway. Extensive physico-chemical analysis of the δ phase, including synchrotron X-ray and neutron diffraction, electron microscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy, and prompt gamma activation analysis, revealed its stoichiometry to be MoO0.108(8)N0.892(8)H0.012(5), indicating non-trivial oxygen incorporation. The presence of N/O ordering and an impurity phase Mo5N6 were also revealed, detectable only by neutron diffraction. Notably, a computationally predicted MoON phase (doi: 10.1103/PhysRevLett.123.236402), of interest due to its potential to display a metal-insulator transition, did not appear under any reaction condition examined.

Pandey, Shobhit↗
DOE OSTI2020

Study of CdZnTeSe Gamma-Ray Detector under Various Bias Voltages

Cadmium zinc telluride selenide (CdZnTeSe) is a new semiconductor material for gamma-ray detection and spectroscopy applications at room temperature. It has very high crystal quality compared to similar materials such as cadmium telluride and cadmium zinc telluride. The consistency of peak position in radiation detection devices is important to practical applications. In this paper, we have characterized a CdZnTeSe planar detector for bias voltages in the range of -20 V to -200 V and amplifier shaping time of 2, 3 and 6 μs. The peak position of the 59.6-keV gamma line of 241 Am becomes more stable as the absolute value of the applied voltage increases. The best energy resolution of 8.5% was obtained for the 59.6-keV gamma peak at -160 V bias voltage and 3-μs shaping time. The energy resolution was relatively stable in the -120 V to -200 V range for a 6-μs shaping time. Future work will be focused on the study of the peak position and energy resolution over time.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Identification and time evolution of thionyl chloride (SOCl 2 ) radiolysis products

In this study, innovative solutions are needed to reduce the amount of high-level waste generated by used nuclear fuel recycling strategies to support the widespread adoption of sustainable nuclear fission energy technologies. To this end, a new sulfur chloride-based process has been developed to recycle zirconium alloy-based materials, which make up a significant fraction of high-level radioactive waste. To support the continued development of this process, we present new data on the potential reaction pathways over time of the products arising from the gamma and electron beam radiolysis of neat thionyl chloride (SOCl 2 ). Interrogation of the gamma irradiated liquid by Raman spectroscopy provided more conclusive identification of the SOCl 2 degradation products, specifically sulfur dichloride (SCl 2 ), molecular chlorine (Cl 2 ), sulfur dioxide (SO 2 ), and sulfuryl chloride (SO 2 Cl 2 ). In comparison, the high dose rate (~10 7 Gy s -1 ) electron beam irradiations formed significantly more degradation products. For both cobalt-60 gamma and electron beam irradiations, the observed degradation products were found to evolve as a function of time post-irradiation via the same reaction pathways, with indication of a solvent regeneration mechanism. These findings are fortuitous for process development, as such a mechanism would be beneficial for process longevity and cost effectiveness.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2021

Structure of high-lying levels populated in the 96 Y → 96 Zr β decay

The nature of the high-lying final levels of the 96 Y gs β decay, one of the three most important contributors to the high-energy reactor antineutrino spectrum, has been investigated in high-resolution γ-ray spectroscopy following the β decay as well as in a campaign of inelastic photon scattering experiments. The comprehensive approach establishes 1 - levels associated with the Pygmy Dipole Resonance as high-lying final levels in the β decay. Branching ratios extracted from β decay complement photon scattering and allow the absolute E1 excitation strength to be determined for levels populated in both reactions. The combined data represents a comprehensive approach to the wavefunction of the 1 - levels below the Qβ value, which are investigated in the Quasiparticle Phonon Model. The calculations reveal that the components populated in β decay contribute only with small amplitudes to the complex wavefunction of these 1 - levels. A comparison of the β decay results to data from total absorption γ -ray spectroscopy demonstrates a good agreement between both measurements.

Pygmy dipole resonance↗
DOE OSTI2023

Characterization of D-T Generator Neutron Flux Spectrum for Cyclic Neutron Activation Analysis Experiments

Improving nuclear data for short-lived fission product yields will further our fundamental understanding of fission, which is needed across various scientific fields and applications. One method of attaining the needed product yield data is through cyclic neutron activation, which allows a target to be irradiated in a neutron environment and then transported for counting of the radionuclides produced, typically via g spectroscopy. Recently, such a system has been constructed and commissioned at Pacific Northwest National Laboratory. Targets are shuttled between the head of a D-T neutron generator and a counting station with a transit time of 2 seconds. As part of the characterization of this system, the neutron flux was studied using two activation targets. The neutron flux from the deuterium-tritium fusion generator was determined to be 9.95(33) x10^8 n/cm2-s with a peak energy of 14.9 MeV and a spread of approximately 4 decades between the epithermal and 14 MeV peak group flux.

cyclic neutron activation, gamma-ray spectroscopy,↗
DOE OSTI2021

Measurements of Short-Lived Isomers from Photofission as a Method of Active Interrogation for Special Nuclear Materials

Isomeric fission products, such as 134m Te (T 1/2 = 164 ns) and 136m Xe (T 1/2 = 2.95 μs), are proposed as a signature of special nuclear materials in active interrogation applications. To test this conjecture, monoenergetic 9, 11, and 13 MeV photons from the HIγS facility are used to induce fission of 235 U, 238 U, and 239 Pu targets. The de-excitation γ rays of the isomers are measured using time-gated spectroscopy with high-purity germanium detectors. The 134m Te and 136m Xe isomers are detected and identified by the energy and decay half-life of their characteristic γ-ray transitions. The ratio of yields for these two signature γ rays, corresponding to 134m Te/( 136m Xe + 136 I), is found to be strongly correlated with the identity of the fissioning nuclei. These results show that fission-product isomers may be used in active interrogation to detect and identify special nuclear materials, even providing information on the isotopic enrichment. In conclusion, the feasibility of an active interrogation scenario using a bremsstrahlung beam is discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Decay spectroscopy of the blocked fission product 130 $\mathrm{I}$

We report numerous applications rely on the identification and quantification of fission products with the activation technique, where γ-rays emitted in the decay are used to estimate the initial activity of the radionuclide of interest. 130 I is a so-called blocked fission product, which can be produced only directly through fission, a property that makes it particularly attractive for nuclear forensics. A source of 130 I was produced using a (p,n) reaction on enriched 130 Te at the Brookhaven Tandem Van de Graaff and its decay was studied with Gammasphere at Argonne National Laboratory. Two new levels were identified, and over 25 transitions were added, removed or re-placed in the level scheme, with intensity measurements made down to I γ = 0.00066 per 100 decays. The uncertainty on the intensities of the strongest transitions, those that are commonly used to quantify the activity of the radionuclide, was improved by a factor of 2 compared to the previous best assessment and discrepancies in the literature values were resolved. A detailed angular correlation analysis further permitted the determination of a number of spin assignments for excited levels and mixing ratios for γ-ray transitions

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Level structure of the T z = –1 nucleus 34 Ar and its relevance for nucleosynthesis in ONe novae

The 24 Mg+ 12 C fusion reaction was used to perform a detailed γ-ray spectroscopy study of the astrophysically important nucleus 34 Ar. In particular, an experimental setup, coupling the advanced γ-ray tracking array GRETINA with the well-established Argonne fragment mass analyzer (FMA), was employed to obtain excitation energies and spin-parity assignments for excited states in 34 Ar, both above and below the proton separation energy. For the first time, an angular distribution analysis of in-beam γ rays from fusion-evaporation reactions, using a tracking array, has been performed and Coulomb energy differences of analog states in the T = 1, A = 34 mirror system, explored from 0 to 6 MeV. Lastly, we present a comprehensive discussion of the astrophysical 33 Cl(p,γ) stellar reaction rate, together with implications for the identification of nova presolar grains from sulfur isotopic abundances.

20 ≤ A ≤ 38↗
DOE OSTI2025

Characterizing hole trap production due to proton irradiation in germanium cross-strip detectors

We present an investigation into the effects of high-energy proton damage on charge trapping in germanium cross-strip detectors with the goal of accomplishing three important measurements. First, we calibrated and characterized the spectral resolution of a spare COSI-balloon detector in order to determine the effects of intrinsic trapping, finding that electron trapping due to impurities dominates over hole trapping in the undamaged detector. Second, we performed two rounds of proton irradiation of the detector in order to quantify, for the first time, the rate at which charge traps are produced by proton irradiation. We find that the product of the hole trap density and cross-sectional area, [nσ] h , follows a linear relationship with the proton fluence, F p , with a slope of (5.4 ± 0.4) x 10 -11 cm/p + . Third, by utilizing our measurements of physical trapping parameters, we performed calibrations which corrected for the effects of trapping and mitigated degradation to the spectral resolution of the detector.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

A New Measurement of the 60 keV Emission from Am-241 Using Metallic Magnetic Calorimeters

Here, we report a new measurement of the 60 keV transition from 241 Am. It uses a metallic magnetic calorimeter gamma-ray detector calibrated in the region around 60 keV by four accurately known X-rays and gamma rays from the decay of 169 Yb. We determine an energy of 59,539.3 ± 0.3 (stat) ± 0.3 (syst) eV, which is 1.6 ± 0.4 eV lower than the current literature value of 59,540.9 ± 0.1 eV. We discuss the sources of this uncertainty and approaches to address them.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗