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DOE OSTI2023

New methods for trace analysis of gamma-irradiated pentaerythritol tetranitrate

High explosives (HEs) are used in a diverse range of applications in which they could be exposed to various radiation levels that may cause potential chemical changes. This study further evaluated pentaerythritol tetranitrate (PETN) that was previously aged with a low-level 2 kGy dose of gamma irradiation in order to understand chemical changes caused by irradiation. Both unirradiated PETN and gamma-irradiated PETN were analyzed using ultra high-pressure liquid chromatography coupled to quadrupole time of flight mass spectrometry (UHPLC-QTOF). The resulting data were processed in a non-targeted manner using Fisher's ratio analysis and multivariate curve resolution-alternating least squares (MCR-ALS) to aid in discovery and identification of the chemical changes brought about by irradiation without a priori knowledge. The application of using UHPLC-QTOF in combination with chemometric techniques for the analysis of irradiated samples has not previously been performed. Here, in this work, we show how to use this method to provide chemical information that would otherwise not be discernible, such as the discovery of degradation of the various homologues of PETN. Major differences identified with radiolytic aging of the PETN sample included decomposition products that resulted from the degradation of the trigger linkage – the O–NO 2 bonds – resulting in the formation of alcohol and aldehyde groups. Similar degradation was also observed in the PETN homologues as well as interconversion from one homologue to another.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2026

Irradiation-Induced Grain Growth of gamma-Fe2O3 and Fe3O4 at Cryogenic Temperatures

This work reports the first observations of grain growth under irradiation of Fe oxides, specifically maghemite gamma-Fe2O3 and magnetite Fe3O4. The Fe oxide thin films were grown by Pulsed Laser Deposition and irradiated in-situ in a Transmission Electron Microscope at - 223°C using 1 MeV Kr2+ ions up to 8.75 x 10^19 ions/m^2 to study grain growth kinetics under irradiation. Grain growth at such low temperatures appears to follow kinetics that can be accounted for by the thermal spike model developed for metals in the literature. The corresponding activation energies were calculated and compared with other oxides. The results demonstrate that gamma-Fe2O3, despite its larger initial grain size, exhibits surprisingly fast grain growth in comparison with Fe3O4, likely due to the presence of iron vacancies in the crystal structure that facilitate faster atomic diffusion under irradiation.

Kretov, Dmitrii↗

DOE OSTI2024

A lanthanide-rich kilonova in the aftermath of a long gamma-ray burst

Observationally, kilonovae are astrophysical transients powered by the radioactive decay of nuclei heavier than iron, thought to be synthesized in the merger of two compact objects. Over the first few days, the kilonova evolution is dominated by a large number of radioactive isotopes contributing to the heating rate. On timescales of weeks to months, its behaviour is predicted to differ depending on the ejecta composition and the merger remnant. Previous work has shown that the kilonova associated with gamma-ray burst 230307A is similar to kilonova AT2017gfo, and mid-infrared spectra revealed an emission line at 2.15 micrometres that was attributed to tellurium. Here, in this study, we report a multi-wavelength analysis, including publicly available James Webb Space Telescope data and our own Hubble Space Telescope data, for the same gamma-ray burst. We model its evolution up to two months after the burst and show that, at these late times, the recession of the photospheric radius and the rapidly decaying bolometric luminosity (L bol ∝ t −2.7±0.4 , where t is time) support the recombination of lanthanide-rich ejecta as they cool.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Free-moving Quantitative Gamma-ray Imaging

The ability to map and estimate the activity of radiological source distributions in unknown three-dimensional environments has applications in the prevention and response to radiological accidents or threats as well as the enforcement and verification of international nuclear non-proliferation agreements. Such a capability requires well-characterized detector response functions, accurate time-dependent detector position and orientation data, a digitized representation of the surrounding 3D environment, and appropriate image reconstruction and uncertainty quantification methods. We have previously demonstrated 3D mapping of gamma-ray emitters with free-moving detector systems on a relative intensity scale using a technique called Scene Data Fusion (SDF). Here we characterize the detector response of a multi-element gamma-ray imaging system using experimentally benchmarked Monte Carlo simulations and perform 3D mapping on an absolute intensity scale. We present experimental reconstruction results from hand-carried and airborne measurements with point-like and distributed sources in known configurations, demonstrating quantitative SDF in complex 3D environments.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Determination of electron-hole pair creation energy in Cd 0.9 Zn 0.1 Te 0.98 Se 0.02 quaternary semiconductor for room-temperature gamma-ray detection

We report the first-time measurement of the electron-hole pair (ehp) creation energy (W ehp ) in novel Cd 0.9 Zn 0.1 Te 0.98 Se 0.02 (CZTS) quaternary semiconductor. CZTS in single crystalline form is poised to be the future of large-volume room-temperature gamma-ray detectors due to its excellent compositional homogeneity with highly reduced defects, high-Z (atomic number) constituents, wide bandgap (1.6 eV), and superior charge transport properties. Despite a great deal of study of the material and device properties since its inception, the W ehp in CZTS has not been measured experimentally. Accurate determination of W ehp is essential for calibration of the spectrometer and other theoretical calculations. In this study we have used an absolute calibration approach, which is based on an iterative approach that yields the Wehp as the best-fit parameter. Using a 241 Am alpha emitting radioisotope and a planar CZTS detector, the Wehp in CZTS was calculated to be 4.47 eV. The obtained value has been validated by accurately predicting the peak energy for gamma rays emitted by a 137 Cs source and read by a CZTS detector with different dimensions. The dependences of the calculated W ehp value on the detector dimensions, type of interaction, and effect of charge trapping are also discussed.

42 ENGINEERING↗

DOE OSTI2022

Upgrades to the gamma ray imager on DIII-D enabling access to high flux hard x-ray measurements during the runaway electron plateau phase (invited)

The Gamma Ray Imager (GRI) is a pinhole camera providing 2D imaging of MeV hard x-ray (HXR) bremsstrahlung emission from runaway electrons (REs) over the poloidal cross section of the DIII-D tokamak. We report a series of upgrades to the GRI expanding the access to RE scenarios from the diagnosis of a trace amount of REs to high flux HXR measurements during the RE plateau phase. We present the implementation of novel gamma ray detectors based on LYSO and YAP crystals coupled to multi-pixel photon counters, enabling a count rate in excess of 1 MHz. Finally, we highlight new insights into the RE physics discovered during the current quench and RE plateau phase experiments as the result of these upgrades.

Lvovskiy, A. (ORCID:0000000236491169)↗

DOE OSTI2025

Compact in-vacuum gamma-ray spectrometer for high-repetition rate PW-class laser–matter interaction

With the advent of high repetition rate laser facilities, novel diagnostic tools compatible with these advanced specifications are required. This paper presents the design of an active gamma-ray spectrometer intended for these high repetition rate experiments, with particular emphasis on functionality within a PW level laser-plasma interaction chamber’s extreme conditions. The spectrometer uses stacked scintillators to accommodate a broad range of gamma-ray energies, demonstrating its adaptability for various experimental setups. In addition, it has been engineered to maintain compactness, electromagnetic pulse resistance, and ISO-5 cleanliness requirements while ensuring high sensitivity. The spectrometer has been tested in real conditions inside the PW-class level interaction chamber at the BELLA center, LBNL. The paper further details the calibration process, which utilizes a 60 Co radioactive source, and describes the unfolding technique implemented through a stochastic minimization method.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

A cryogenic white light absorption spectroscopy setup with in situ gamma irradiation and thermo-optical annealing for optical fiber radiation-induced attenuation characterization

Silica optical fiber sensors offer a fast, distributed measurement solution in various cryogenic and radiation environments, such as magnets for fusion power. Under these conditions, light-absorbing point defects limit lifetime via radiation-induced attenuation (RIA). To support RIA kinetics prediction, we present an in situ, broadband absorption spectroscopy setup combining gamma irradiation with liquid nitrogen cooling. The apparatus enables continuous monitoring of narrowband RIA levels and the use of secondary optical annealing light sources, alongside broadband spectrum measurements to characterize RIA defects through spectrum decomposition. Initial results confirm the inevitable photobleaching effect of the probe light source, which must be accounted for. In addition, we report RIA kinetics during cycles of gamma irradiation at 77 K and isochronal thermal annealing steps from liquid nitrogen to room temperature, showcasing the setup’s ability to replicate real fiber operation scenarios. These instruments form an ideal platform to further study the kinetics of RIA coupled with thermal and optical annealing.

Absorption spectroscopy↗

DOE OSTI2024

Applying simulation-based inference to spectral and spatial information from the Galactic Center gamma-ray excess

Abstract The two most favored explanations of theFermiGalactic Center gamma-ray excess (GCE) are millisecond pulsars and self annihilation of the smooth dark matter halo of the galaxy. In order to distinguish between these possibilities, we would like to optimally use all information in the available data, including photon direction and energy information.To date, analyses of the GCE have generally treated directional and energy information separately, or have ignored one or the other completely.Here, we develop a method for analyzing the GCE that relies on simulation-basedinference with neural posterior models to jointly analyze photon directional and spectral information while correctly accounting for the spatial and energy resolution of the telescope, here assumed to be theFermiLarge Area Telescope (LAT).Our results also have implications for analyses of the diffuse gamma-ray background, which we discuss.

Astronomy & Astrophysics↗

DOE OSTI2020

The evolution of gamma-ray burst jet opening angle through cosmic time

ABSTRACT Jet opening angles of long gamma-ray bursts (lGRBs) appear to evolve in cosmic time, with lGRBs at higher redshifts being on average more narrowly beamed than those at lower redshifts. We examine the nature of this anticorrelation in the context of collimation by the progenitor stellar envelope. First, we show that the data indicate a strong correlation between gamma-ray luminosity and jet opening angle, and suggest this is a natural selection effect – only the most luminous GRBs are able to successfully launch jets with large opening angles. Then, by considering progenitor properties expected to evolve through cosmic time, we show that denser stars lead to more collimated jets; we argue that the apparent anticorrelation between opening angle and redshift can be accounted for if lGRB massive star progenitors at high redshifts have higher average density compared to those at lower redshifts. This may be viable for an evolving initial mass function (IMF) – under the assumption that average density scales directly with mass, this relationship is consistent with the form of the IMF mass evolution suggested in the literature. The jet angle–redshift anticorrelation may also be explained if the lGRB progenitor population is dominated by massive stars at high redshift, while lower redshift lGRBs allow for a greater diversity of progenitor systems (that may fail to collimate the jet as acutely). Overall, however, we find both the jet angle–redshift anticorrelation and jet angle–luminosity correlation are consistent with the conditions of jet launch through, and collimation by, the envelope of a massive star progenitor.

Lloyd-Ronning, Nicole↗

DOE OSTI2021

Variational study of the Kitaev-Heisenberg-Gamma model

Here we compute the low-energy excitation spectrum and the dynamical spin structure factor of the Kitaev-Heisenberg-Gamma model through a variational approach based on the exact fractionalized excitations of the pure Kitaev honeycomb model. This novel approach reveals the physical reason for the asymmetric stability of the Kitaev spin liquid phases around the ferromagnetic and antiferromagnetic Kitaev limits. Moreover, we demonstrate that the fractionalized excitations form bound states in specific regions of each Kitaev spin liquid phase and that certain phase transitions induced by Heisenberg and Gamma interactions are driven by the condensation of such a bound state. Remarkably, this bound state appears as a sharp mode in the dynamical spin structure factor, while its condensation patterns at the appropriate phase transitions provide a simple explanation for the magnetically ordered phases surrounding each Kitaev spin liquid phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Sequential versus Simultaneous Aging of XLPE Nuclear Cable Insulation Subjected to Elevated Temperature and Gamma Radiation

Electrical cables constitute a critical component of nuclear power generation. The aging behavior of electrical cable insulation under combined exposure to thermal and radiation stress is not additive, complicating lifetime prediction of cable performance based on sequential accelerated aging. In this work we explore the relative effects of simultaneous and sequential thermal and gamma radiation aging on cross-linked polyethylene (XLPE), which is commonly found in commercial nuclear power plants in the United States. Samples of XLPE were subjected to up to 320 kGy of gamma irradiation at a dose rate of 300 Gy/hr in two heating scenarios. In the first, simultaneously-aged samples were heated at 150°C during irradiation. In the second, sequentially aged samples were heated at 150°C for designated durations followed by corresponding periods of irradiation without heating. The mass, total color difference, and density were characterized to quantify aging of the insulation polymer. Sequential aging is hypothesized to be more damaging to XLPE insulation due to an increased trend in mass gain, total color difference, and density.

Cross-linked polyethylene, XLPE, nuclear cable, ac↗

DOE OSTI2020

Modeling Aerial Gamma-Ray Backgrounds Using Non-negative Matrix Factorization

Airborne gamma-ray surveys are useful for many applications, ranging from geology and mining to public health and nuclear security. In all these contexts, the ability to decompose a measured spectrum into a linear combination of background source terms can provide useful insights into the data and lead to improvements in the techniques that use spectral energy windows. Multiple methods for the linear decomposition of spectra exist but are subject to various drawbacks, such as allowing negative photon fluxes or requiring detailed Monte Carlo modeling. In this work, we propose using non-negative matrix factorization (NMF) as a data-driven approach to spectral decomposition. Using aerial surveys that include flights over water, we demonstrate that the mathematical approach of NMF finds physically relevant structure in the aerial gamma-ray background, namely, that measured spectra can be expressed as the sum of nearby terrestrial emission, distant terrestrial emission, and radon and cosmic emission. Furthermore, these NMF background components are compared with the background components obtained by noise-adjusted singular value decomposition (NASVD), which contain negative photon fluxes and, thus, do not represent the emission spectra in as straightforward a way. Finally, we comment on the potential areas of research that are enabled by NMF decompositions, such as new approaches to spectral anomaly detection and data fusion.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

A gamma-ray pulsar timing array constrains the nanohertz gravitational wave background

We report after large galaxies merge, their central supermassive black holes are expected to form binary systems. Their orbital motion should generate a gravitational wave background (GWB) at nanohertz frequencies. Searches for this background use pulsar timing arrays, which perform long-term monitoring of millisecond pulsars at radio wavelengths. We used 12.5 years of Fermi Large Area Telescope data to form a gamma-ray pulsar timing array. Results from 35 bright gamma-ray pulsars place a 95% credible limit on the GWB characteristic strain of 1.0 × 10 -14 at a frequency of 1 year –1 . The sensitivity is expected to scale with t obs , the observing time span, as t$^{-13/6}_{obs}$. This direct measurement provides an independent probe of the GWB while offering a check on radio noise models.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

A Variational Inference Approach to Inverse Problems with Gamma Hyperpriors

Hierarchical models with gamma hyperpriors provide a flexible, sparse-promoting framework to bridge L 1 and L 2 regularizations in Bayesian formulations to inverse problems. Despite the Bayesian motivation for these models, existing methodologies are limited to maximum a posteriori estimation. The potential to perform uncertainty quantification has not yet been realized. This paper introduces a variational iterative alternating scheme for hierarchical inverse problems with gamma hyperpriors. The proposed variational inference approach yields accurate reconstruction, provides meaningful uncertainty quantification, and is easy to implement. In addition, it lends itself naturally to conduct model selection for the choice of hyperparameters. Here, we illustrate the performance of our methodology in several computed examples, including a deconvolution problem and sparse identification of dynamical systems from time series data.

Bayesian shrinkage↗

DOE OSTI2021

Measurement of the helicity asymmetry E for the reaction $$ \gamma p\rightarrow \pi ^0 p$$: The CBELSA/TAPS Collaboration

Abstract A measurement of the double-polarization observable E for the reaction $$\gamma p\rightarrow \pi ^0 p$$ γ p → π 0 p is reported. The data were taken with the CBELSA/TAPS experiment at the ELSA facility in Bonn using the Bonn frozen-spin butanol (C $$_4$$ 4 H $$_9$$ 9 OH) target, which provided longitudinally-polarized protons. Circularly-polarized photons were produced via bremsstrahlung of longitudinally-polarized electrons. The data cover the photon energy range from $$E_\gamma =600$$ E γ = 600 to 2310 MeV and nearly the complete angular range. The results are compared to and have been included in recent partial wave analyses.

Gottschall, M.↗

DOE OSTI2023

Measurement of the helicity asymmetry $${\mathbb {E}}$$ for the $$\vec {\gamma }\vec {p} \rightarrow p \pi ^0$$ reaction in the resonance region: The CLAS Collaboration

Abstract The double-spin-polarization observable $${\mathbb {E}}$$ E for $$\vec {\gamma }\vec {p}\rightarrow p\pi ^0$$ γ → p → → p π 0 has been measured with the CEBAF Large Acceptance Spectrometer (CLAS) at photon beam energies $$E_\gamma $$ E γ from 0.367 to $$2.173~\textrm{GeV}$$ 2.173 GeV (corresponding to center-of-mass energies from 1.240 to $$2.200~\textrm{GeV}$$ 2.200 GeV ) for pion center-of-mass angles, $$\cos \theta _{\pi ^0}^{c.m.}$$ cos θ π 0 c . m . , between $$-$$ - 0.86 and 0.82. These new CLAS measurements cover a broader energy range and have smaller uncertainties compared to previous CBELSA data and provide an important independent check on systematics. These measurements are compared to predictions as well as new global fits from The George Washington University, Mainz, and Bonn-Gatchina groups. Their inclusion in multipole analyses will allow us to refine our understanding of the single-pion production contribution to the Gerasimov-Drell-Hearn sum rule and improve the determination of resonance properties, which will be presented in a future publication.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

A new way to unravel the $^{12}$C($\alpha $,$\gamma $)$^{16}$O cross section components using neural networks

The $^{12}$C($\alpha $,$\gamma $)$^{16}$O reaction rate is crucial in determining the carbon-to-oxygen abundance ratio in stellar nucleosynthesis. Measuring this reaction’s cross section at stellar energies is challenging due to its extremely small value, approximately 10 -17 barn at E c.m. = 300 keV. To address this, R-matrix calculations are employed to extrapolate data to lower energies, requiring a comprehensive understanding of each contribution to the cross section. The dominant contributions to the cross section at stellar energies arise from electric dipole (E1) and electric quadrupole (E2) transitions to the ground state of 16 O, along with a significant cascade contribution. Traditionally, these contributions have been separated using the γ-ray angular distribution. In this work, we propose a novel technique using the energy distribution of the 16 O recoils at the focal plane. This method involves a neural network trained on detailed Monte Carlo simulations of the energy distribution of recoils transported through the recoil mass separator ERNA. This approach enables the simultaneous determination of all three contributions with errors around 10% in the energy range E c.m. = 1.0–2.2 MeV. In conclusion, by employing this new technique, we aim to significantly improve the accuracy of determining the cross section of the $^{12}$C($\alpha $,$\gamma $)$^{16}$O reaction at astrophysical energies.

Astrochemistry↗