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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Cumulative short-lived photofission product yields for nuclear forensic application

Experiments have long been carried out with linear accelerator (linac) produced bremsstrahlung X-rays to study high-energy photon-induced fission, known as “photofission”. One benefit of photofission, when compared with neutron-induced fission, is the ability to investigate fundamental physics of fission at excitation energies lower than what is possible with neutrons [1]. Absorption of an incident neutron results in a compound nucleus with an excitation energy at least equal to the neutron binding energy; thus, the lowest energy region of the fission barrier cannot be studied. Fission product yield distributions are dependent on the incident particle energy and the target nucleus mass. They are generally represented by a double-humped curve, with low and high mass “peaks” and an intermediate mass “valley”. As incident particle energy increases, the excitation energy of the nucleus increases, thereby increasing the overall yield of isotopes in the valley with respect to the two maxima or peaks of the fission product curve [3]. Photofission is most probable for incident photons around 14 MeV due to the giant dipole resonance. Induced photofission around this energy results in a fission product yield distribution that resembles 14 MeV DT neutron fission more than thermal or fast (500 keV) neutron fission. In post-detonation nuclear forensics, the peak-to-valley ratio of the fission product yield curve could be used for characterizing device type by providing an indication of the neutron energy spectrum that had induced fission (e.g., 500 keV vs. 14 MeV). The goal of this work is to improve nuclear data for isotopes of interest in nuclear forensics and special nuclear material (SNM) detection, specifically the fission product yield data via photofission experiments for the isotopes of 238U and 232Th. Photofission has been proposed as a less costly and more flexible production method for the valley isotopes that are representative of DT neutron fission product yield distributions, which would benefit nuclear forensics exercises in testing for analysis techniques. Natural uranium and thorium targets were irradiated with bremsstrahlung photons (nominal endpoint energies of 8, 14, and 20 MeV), generated via impingement of high-energy electrons on a tungsten electron-to-photon radiator. Gamma-ray spectroscopy was used to observe and identify the decay of the resulting fission products. The photofission yields of 102 fission products were measured for the set of the 238U and 232Th targets at the three bremsstrahlung X-ray endpoint energies 8, 14, and 20 MeV. These fragments included masses ranging from A=84 to A=144, with half-lives as short as 1.07 seconds.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2020

Neutron-Neutron Correlations in the Photofission of 238U

Background: In the fission of actinides, the nearly back-to-back motion of the fission fragments has a strong effect on the kinematics of fission neutrons. This leads to a favoring of opening angles near 0? and 180? in the neutron-neutron (n-n) opening angle distributions of correlated neutron pairs from the same fission event. Purpose: To measure the n-n opening angle and energy correlations in the photofission of 238U. As of this writing, measurements of correlated n-n opening angle distributions have been reported only for the spontaneous and neutron-induced fission of actinides. This work is the first to report such a measurement using photofission and will provide useful experimental input for photofission models used in codes such as MCNP and FREYA. Method: Fission is induced using bremsstrahlung photons produced via a low duty factor, pulsed, linear electron accelerator. The bremsstrahlung photon beam impinges upon a 238U target that is surrounded by a large neutron scintillation detection system capable of measuring particle position and time of flight, from which n-n opening angle and energy are measured. Neutron-neutron angular correlations are determined by taking the ratio between a correlated neutron distribution and an uncorrelated neutron distribution formed by the pairing of neutrons produced during different beam pulses. This analysis technique greatly diminishes effects due to detector efficiencies, acceptance, and experimental drifts. Results: The angular correlation of neutrons from the photofission of 238U shows a high dependence on neutron energy as well as a dependence on the angle of the emitted neutrons with respect to the incoming photon beam. Angular correlations were also measured using neutrons from the spontaneous fission of 252Cf, showing good agreement with past measurements. Conclusions: The measured angular correlations reflect the underlying back-to-back nature of the fission fragments. An anomalous decline in n-n yield was observed for opening angles near 180? for 238U.

Burggraf, Jeff↗
DOE OSTI2023

Prompt Photofission Neutron Detection in Depleted Uranium

The detection of prompt photofission neutrons during active interrogation is a strong indication of the presence of special nuclear materials. However, the high-energy photons used for interrogation create a very challenging radiation environment for the detection of prompt fission signatures. These challenges include detector saturation and pulse pile-up. Additionally, there is an elevated neutron background that further challenges the detection of prompt fission neutrons. This background is produced because of (γ, Xn) photonuclear reactions in the surrounding high-Z materials. Here, we demonstrate the detection of prompt photofission neutrons in these challenging environments. Depleted uranium (DU) and lead targets are interrogated with bremsstrahlung photons produced by a 9-MV electron linear accelerator. Fast neutrons are detected with trans-stilbene organic detectors, and scintillation pulses are analyzed using a previously developed and demonstrated artificial neural network system. We observe a 5 times higher photoneutron count rate when the lead target is replaced with the DU target. Additionally, we observe a difference in the photoneutron light-output distributions of lead and DU. Here, this difference in the measured distributions is due to the difference in the photoneutron-energy spectra; DU photoneutrons are emitted with (γ, n) and watt-energy spectra, whereas lead photoneutrons are emitted with only the (γ, n) spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Detection of uranium-photofission neutrons with a 4 He scintillation detector

The use of photon active interrogation to detect special nuclear material has held significant theoretical promise, as the interrogating source particles, photons, are fundamentally different from one of the main signatures of special nuclear material: neutrons produced in nuclear fission. However, neutrons produced by photonuclear reactions in the accelerator target, collimator, and environment can obscure the fission neutron signal. These (γ, n) neutrons could be discriminated from fission neutrons by their energy spectrum, but common detectors sensitive to the neutron spectrum, like organic scintillators, are typically hampered by the intense photon background characteristic of photon-based active interrogation. In contrast, high-pressure 4 ⁢He-based scintillation detectors are well-suited to photon active interrogation, as they are similarly sensitive to fast neutrons and can measure their spectrum, but show little response to gamma rays. Here, in this work, a photon active interrogation system utilizing a 4 ⁢He scintillation detector and a 9 MeV linac-bremsstrahlung x-ray source was experimentally evaluated. The detector was shown to be capable of operating in intense gamma-ray environments and detecting photofission neutrons from 238 ⁢U when interrogated by this x-ray source. The photofission neutrons show clear spectral separation from (γ, n) neutrons produced in lead, a common shielding material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2021

Short-lived photofission product yields from 238 U and 232 Th at Bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV for nuclear forensics isotope production applications

The existing photofission product yield data sets are often based on nuclear models, and limited experimental measurements of these fission product yields have been performed. These experiments resulted in measured cumulative fission product yields (CFPYs) for 238 U and 232 Th for the bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV. The half-lives of the reported fission products range from 1.07–40.8 s. This work is motivated by a demonstrated need for novel isotope production methods for nuclear forensics and improved nuclear data to support the nonproliferation community. A high-purity germanium detector and a pneumatic transfer system were employed for measurements of short-lived fission products, collecting data between cycles of accelerator irradiation and measurement.

07 ISOTOPE AND RADIATION SOURCES↗
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 OSTI2025

Measurements of short-lived fission product yields from photofission of 238 U using 13.0 MeV monoenergetic photons

Photon-induced fission product yield (FPY) measurements were conducted on the isotope 238U. Fission was induced using Eγ = 13.0 MeV monoenergetic photons produced by the Triangle Universities Nuclear Laboratory’s (TUNL’s) High Intensity γ-ray Source (HIγS) facility. Short-lived FPYs were measured by performing cyclic activation of the sample using a rapid target transfer system. Following activation, the 238U target was rapidly (0.4 s) transferred to a counting station consisting of two well-shielded high-purity germanium (HPGe) detectors. The irradiation-counting cycle was repeated until the summed data had sufficient statistical accuracy. Twenty-eight unique fission products with half-lives ranging from 1 s to 450 s were identified, and their cumulative FPYs determined. Furthermore, the results are compared with previous independent FPY measurements using inverse kinematics. Good agreement between the data sets is found despite the different excitation energy distributions of the fissioning nucleus in the experiments.

Physics - Nuclear physics and radiation physics↗
DOE OSTI2022

High-fidelity photoneutron detection via neutron activation analysis

To interdict illicit radioactive sources and prevent nuclear terror, governments have deployed portal monitor systems at ports of entry. Such portal monitors rely upon the detection of spontaneously-emitted radiation signatures, however, detection scenarios become more challenging for highly enriched uranium, which emits relatively few spontaneous radiation signatures. Photon active interrogation techniques can augment current cargo inspection scenarios and improve detection capabilities for illicit nuclear material. A high-energy photon interrogation source can induce photofission in nuclear material, producing strong radiation signatures for detection. Prompt fission signals are of specific interest because prompt neutrons are greater than 99% of the fission signal. When using detectors capable of spectroscopy, e.g., pulse shape discrimination-capable organic scintillators, the intense interrogating source often will cause pulse pile-up, degrading particle classification. In this work, we demonstrate photoneutron detection via neutron activation of aluminum and iron. The experiments rely upon nuclear reactions that can only be induced by neutrons, and are robust against pile-up, thereby providing high-confidence neutron rates. In this work, we apply neutron activation analysis for the detection of high-energy neutrons produced by high-energy photon irradiation; the depleted uranium sample was irradiated with a 9-MeV bremsstrahlung beam. We find that the irradiated depleted uranium produced an aluminum activation flux of 1.77 × 10 5 n cm –2 s –1 and an iron-56 activation flux of 1.05 × 10 5 n cm –2 s –1 . Furthermore, the ability to detect radioactivity induced by neutrons created in (, n) and photofission reactions demonstrates a new approach for photon active interrogation to identify nuclear materials.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Clinical 6 MV X-Ray Facility Photo-Neutron/Fission Interrogations with TMFD Sensors

Detection of several targets (U, Be, D2O) of interest to national security has been achieved at Purdue University’s 6 MV (~104 R/h) X-Ray clinical linear accelerator (CLINAC), from photoneutron/fission induced neutron signatures using a Centrifugally Tensioned Metastable Fluid Detector (CTMFD). Traditional neutron detection schemes were saturated and ineffective under the intense (to ~104 R/h) photon environment; however, the CTMFD sensor technology was capable of measuring the relatively insignificant (~10-12x lower intensity) neutron field produced from 6 MeV-end point X-Ray beam interactions with the CLINAC components and surroundings. This is in stark contrast to published results based on conventional belief for immeasurable neutron dose in 6 MV CLINAC facilities. Photoneutron and photofission neutron production rates were detected and analyzed at various standoffs from the isocenter, with and without special nuclear material (SNM) related targets ranging in mass from 5 g of Be, to ~0.6 kg of UO2. It was confirmed that 6 MV X-Ray photons do result in measurable neutron dose above normal cosmic background. Additionally, in threshold mode, the CTMFD operating under a tensioned metastable pressure of -5bar, enabled conclusive rejection of background photoneutrons, while enabling the rapid detection of: Be, D2O, C and U targets within seconds to minutes while operating in and around 104 R/h photon fields.

Ozerov, Stepan↗
DOE OSTI2020

12 C(p,p') 12 C Reaction ( E p =19.5–30 MeV) for Active Interrogation of Special Nuclear Material

Passive detection of special nuclear material (SNM) is challenging due to its inherently low rate of spontaneous emission of penetrating radiation, the relative ease of shielding, and the fluctuating and frequently overwhelming background. Active interrogation, the use of external radiation to increase the emission rate of characteristic radiation from SNM, has long been considered to be a promising method to overcome those challenges. Current active-interrogation systems that incorporate radiography tend to use bremsstrahlung beams, which can deliver high radiation doses. Low-energy ion-driven nuclear reactions that produce multiple monoenergetic photons may be used as an alternative. The 12 C ( p , p ' ) 12 C reaction is one such reaction that could produce large yields of highly penetrating 4.4- and 15.1-MeV gamma rays. This reaction does not directly produce neutrons below the approximately 19.7 MeV threshold, and the 15.1-MeV gamma-ray line is well matched to the photofission cross section of 235 U and 238 U . In this article, we report the measurements of thick-target gamma-ray yields at 4.4 and 15.1 MeV from the 12 C ( p , p ' ) 12 C reaction at proton energies of 19.5, 25, and 30 MeV. Measurements are made with two 3 -in. EJ-309 cylindrical liquid scintillation detectors and thermoluminescent dosimeters placed at 0 ° and 90 ° , with an additional 1.5 -in. Na I ( Tl ) cylindrical scintillation detector at 0 ° . We estimate the highest yields of the 4.4- and 15.1-MeV gamma rays of 1.65 × 10 10 and 4.47 × 10 8 sr - 1 μ C - 1 at a proton energy of 30 MeV, respectively. The yields in all experimental configurations are greater than in a comparable deuteron-driven reaction that produces the same gamma-ray energies— 11 B ( d , n γ ) 12 C . However, a significant increase of the neutron radiation dose accompanies the proton energy increase from 19.5 to 30 MeV.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2023

Erratum: Monoenergetic photon-induced fission cross-section ratio measurements for U 235 , U 238 , and Pu 239 from 9.0 to 17.0 MeV

In this erratum we report a correction to the previously published photofission cross-section ratio data. The actinide fission-chamber foils utilized in this work were extensively characterized during a new campaign using α- and γ-ray spectroscopy, and 2π alpha counting. These three techniques agreed, resulting in an improved accuracy of the fission-chamber foil masses used in the original experiment. The foil masses measured by α spectroscopy are detailed in Table I. All foils were counted on the same α spectrometer, using an identical geometry, which reduces the systematic uncertainty in the calculated mass ratios since the α spectrometer efficiency cancels out in the ratio. This results in a relative uncertainty on the mass ratio of 1.0% for 235 U/ 238 U, 0.62% for 239 Pu/ 235 U, and 1.1% for 239 Pu/ 238 U. The published cross-section ratio data are re-calculated to reflect the updated target masses and uncertainties. The new mass values cause a 2.40% decrease for the σ( 235 U(γ, f)/ 238 U(γ, f)) ratio, a 5.10% decrease for the σ( 235 U(γ, f)/ 239 Pu(γ, f)) ratio, and a 2.77% decrease for the σ( 238 U(γ, f)/ 239 Pu(γ, f)) ratio. The updated cross-section ratios are presented in Tables II, III, and IV, which are corrected versions of Tables III, IV, and V in Ref. [1]

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Fission with Exotic Nuclei (Abbreviated Report)

Nuclear fission is a key mechanism involved in the synthesis of heavy elements in the Cosmos and is the primary explanation for the stability of superheavy elements. Nevertheless, our knowledge of fission remains extremely fragmented. Most experiments have been conducted only on a tiny number of stable actinide nuclei and are often incomplete, leading to gaps in our basic understanding of the process. For many radioactive isotopes, basic fission data such as the charge or mass distribution of the fragments is unknown. These gaps cannot always be filled by simulation alone. Common fission models contain too many free parameters and lack predictive power. In contrast, the fundamental theory of fission under development at LLNL is much more predictive, but its current computational cost is too high to be used extensively for data evaluations. A unique window of opportunity to resolve these limitations has recently opened: the U.S. nuclear science community is ramping up major experimental programs at the Facility for Rare Isotope Beams (FRIB, the DOE flagship facility in low-energy nuclear science), and techniques from machine learning have shown great potential to simplify the use of a fundamental, quantum-mechanical theory of fission. This project has two components. On the experimental side, we acquired and deployed at the HIGS facility a new dual Frisch-Grid ionization chamber to measure correlated fragment-mass, kinetic energy, and angular distributions of fission fragments from induced fission. This new device was used to perform measurements of charge, mass and total kinetic energy of fission fragments in the photofission of 238 U and eight gamma-ray beam energies between 6.2 and 13 MeV, which allowed extracting high-precision independent yields for this reaction. The device was also used to perform measurements of the same quantities in the neutron-induced fission of 234 U with monoenergetic beams of energy between 5 and 8 MeV. In parallel, we collaborated with a team at Commissariat à l’énergie atomique et aux énergies alternatives (CEA) to perform a series of measurements of fission yields in inverse kinematics for the two isotopes of 236 U and 240 Pu. The experiment took place at the Grand Accélérateur National d’Ions Lourds in France in June 2023. The deployment of the VAMOS spectrometer with a new array called PISTA allowed determining the excitation energy of the fissioning system within 1 Mega-electronvolts. The second component of the project involved using deep neural networks to build fast and reliable emulators of our current fission models. In an invited paper published in Frontier in Physics, we showed that autoencoders could successfully compress nuclear wavefunctions in nuclear density functional theory. We achieved a dimensionality reduction of the order of two orders of magnitude while keeping the error in the total energy to less than 0.01%. In a second paper submitted to Physical Review Letters in June 2023 with our collaborators at CEA, we showed that variational autoencoders can learn the collective degrees of freedom driving the fission process.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1985

Cosmological constraints on the lifetime of massive particles

Particles with masses more than a few MeV, decaying into photons or electrons, can cause destruction by photofission of cosmologically produced light elements. A previous calculation of this effect is corrected and extended, and used to derive maximum lifetimes for massive neutrinos; these range from a few thousand seconds upward, depending on the particle mass. Some approximate expressions are given that enable lifetime limits to be obtained for other particles, with different masses and abundances, such as gravitinos. These limits are generally stronger than previously determined constraints, such as distortion of the microwave background by energetic photons.

Lindley, D.↗