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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Materials Data on Na4XeO14 by Materials Project

Xe(Na2O7)2 crystallizes in the orthorhombic Pbcn space group. The structure is three-dimensional and consists of four xenon molecules and one Na2O7 framework. In the Na2O7 framework, there are two inequivalent Na sites. In the first Na site, Na is bonded in a 5-coordinate geometry to six O atoms. There are a spread of Na–O bond distances ranging from 2.34–3.03 Å. In the second Na site, Na is bonded in a 4-coordinate geometry to five O atoms. There are a spread of Na–O bond distances ranging from 2.26–2.98 Å. There are eight inequivalent O sites. In the first O site, O is bonded in a bent 120 degrees geometry to two O atoms. There is one shorter (1.35 Å) and one longer (1.38 Å) O–O bond length. In the second O site, O is bonded in a bent 120 degrees geometry to two O atoms. There is one shorter (1.26 Å) and one longer (1.89 Å) O–O bond length. In the third O site, O is bonded in a distorted trigonal planar geometry to two Na and one O atom. In the fourth O site, O is bonded in a distorted T-shaped geometry to two Na and one O atom. The O–O bond length is 1.37 Å. In the fifth O site, O is bonded in a 4-coordinate geometry to two equivalent Na and two equivalent O atoms. In the sixth O site, O is bonded in a distorted see-saw-like geometry to three Na and one O atom. In the seventh O site, O is bonded in a distorted L-shaped geometry to two equivalent Na and two equivalent O atoms. In the eighth O site, O is bonded in a 3-coordinate geometry to two Na and one O atom.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on CuSb2(XeF5)4 by Materials Project

CuSb(Xe2F7)2SbF6 crystallizes in the tetragonal I-4 space group. The structure is one-dimensional and consists of two SbF6 clusters and two CuSb(Xe2F7)2 ribbons oriented in the (0, 0, 1) direction. In each SbF6 cluster, Sb is bonded in an octahedral geometry to six F atoms. There is four shorter (1.92 Å) and two longer (1.93 Å) Sb–F bond length. There are two inequivalent F sites. In the first F site, F is bonded in a single-bond geometry to one Sb atom. In the second F site, F is bonded in a single-bond geometry to one Sb atom. In each CuSb(Xe2F7)2 ribbon, Xe is bonded in a linear geometry to two F atoms. There are one shorter (2.02 Å) and one longer (2.18 Å) Xe–F bond lengths. Cu is bonded to six F atoms to form CuF6 octahedra that share corners with two equivalent SbF6 octahedra. The corner-sharing octahedral tilt angles are 0°. There are four shorter (1.93 Å) and two longer (2.30 Å) Cu–F bond lengths. Sb is bonded to six F atoms to form SbF6 octahedra that share corners with two equivalent CuF6 octahedra. The corner-sharing octahedral tilt angles are 0°. There is four shorter (1.91 Å) and two longer (1.95 Å) Sb–F bond length. There are four inequivalent F sites. In the first F site, F is bonded in a bent 120 degrees geometry to one Xe and one Cu atom. In the second F site, F is bonded in a single-bond geometry to one Xe atom. In the third F site, F is bonded in a single-bond geometry to one Sb atom. In the fourth F site, F is bonded in a linear geometry to one Cu and one Sb atom.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Fe4AgP(XeF3)2 by Materials Project

(Xe)2Fe4AgF4PF2 crystallizes in the tetragonal I-4c2 space group. The structure is zero-dimensional and consists of four difluorophosphine molecules, eight xenon molecules, and four Fe4AgF4 clusters. In each Fe4AgF4 cluster, Fe is bonded in a distorted single-bond geometry to one F atom. The Fe–F bond length is 1.85 Å. Ag is bonded in a 4-coordinate geometry to four equivalent F atoms. All Ag–F bond lengths are 2.40 Å. F is bonded in an L-shaped geometry to one Fe and one Ag atom.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Cluster Dynamics Simulations of Intra-Granular Fission Gas Bubble Size and Pressure Evolution in UO 2

Fission gases such as xenon (Xe) play a critical role in determining the behavior and response of nuclear fuel. Given that Xe has little solubility in UO 2 , it accumulates and forms bubbles, which significantly impact fuel performance. Intra- and inter-granular bubble nucleation and growth can lead to fuel swelling, and once bubbles interconnect at grain boundaries, fission gas can be released into the plenum. At low temperatures, limited uranium vacancy mobility can restrict swelling, therefore causing the bubbles to become highly pressurized. Consequently, this can induce micro-cracking, promote fission gas release (increasing the likelihood of cladding failure), and even lead to fuel pulverization under accident conditions such as a loss of coolant accident. As bubble evolution is strongly influenced by local temperature and fission rate, markedly different behavior occurs across the radial profile of the fuel pellet. Capturing the mechanisms that underpin bubble evolution is therefore important to predict these behaviors in the fuel. Previous models describing important mechanisms informed by lower length scale simulations have been developed under the NEAMS program. These can describe the evolution of a single bubble type (i.e., single value for radius and pressure) at each position in the pellet, for instance using the Centipede cluster dynamic code. However, in reality, a full distribution in bubble sizes and pressures exists within the microstructure at a given position in the pellet. To address this the cluster dynamics code Xolotl, which can predict Xe and vacancy phase space (i.e., bubble distributions) for intra-granular bubbles, has been used before. Prior work benchmarked the Xolotl code against the Centipede cluster dynamics code to ensure compatibility and to verify that mobile defect properties are adequately transferred between the two codes, along with some physics improvements. In this work, we go further by introducing a physics-based set of improvements that will allow us to accurately predict bubble size distributions and internal bubble pressures under representative UO 2 irradiation conditions. The improvements include (i) coupling bubble-defect reaction energies to a virial equation of state (EOS), (ii) including a bubble surface tension contribution, (iii) incorporating radiation-induced re-solution of Xe and vacancies, (iv) enabling pressure-driven dislocation loop punching through an effective emission of interstitial clusters informed by interstitial loop energetics, (v) accounting for radiation induced athermal diffusion of Xe, and (vi) implementing a Booth-type grain boundary sink representation for all mobile defects and defect clusters. After these modifications, we observe good agreement of Xolotl fission gas bubble size and concentration predictions with legacy experimental measurements. Additionally, it allows the distribution of Xe bubble pressures and radius to also be predicted and compared to data produced through the Advanced Fuels Campaign (AFC) program. Here, we have done this by running simulations under conditions similar to the AFC post-irradiation examination (PIE) samples irradiated at North Anna 2 light water reactor (LWR). Our results shows excellent agreement with these experimental measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Integrated Off-gas System: A Preconceptual Design of an Integrated Off-Gas Treatment System

The U.S. has a vested interest in the advancement of nuclear energy to achieve aggressive net-zero goals, with reprocessing and recycling of used nuclear fuels (UNF) playing a vital role. It will not be possible to meet U.S. regulatory requirements without robust off-gas treatment, so it is crucial to advance treatment technologies to facilitate the design of future reprocessing facilities. For many years, teams of researchers across the U.S. Department of Energy (DOE) National Laboratory complex have been investigating off-gas treatment technologies for the capture and removal of volatile radionuclides (i.e., 85 Kr, Xe, 14 C, and 129 I) and oxides of nitrogen (NO X ) that are produced from reprocessing. These investigations have been focused on developing individual technologies for the capture of Kr, Xe, iodine, and CO 2 . Capture technologies for each constituent were tested independently from one another by utilizing nonradioactive surrogates to simulate simplified off-gas streams. The tests have been relatively small, laboratory-scale experiments of up to approximately 1 L/minute total gas flow rate. To increase the readiness of these technologies for deployment, an integrated test system with a larger-scale capacity is needed to bridge the gap between promising bench scale and fully scalable UNF reprocessing off-gas treatment. This document contains the goals, design basis, functional requirements, preconceptual design, and cost estimates for an integrated off-gas demonstration system for the capture and removal of NO x , Kr, Xe, CO 2 , and iodine at 10× higher throughput than earlier laboratory studies. The order-of-magnitude cost estimate for this system is approximately $\$$886,000. Next phases include conceptual design, detailed design, fabrication, and commissioning.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Modeling of fission gas diffusion and release for Gd 2 O 3 doped UO 2

Uranium dioxide (UO 2 ) is the primary nuclear fuel in light water reactors, and its excess neutronic reactivity can be controlled by adding burnable absorbers, such as Gd 2 O 3 . This burnable absorber has a large neutron absorption cross-section, lowering the high reactivity of the reactor's initial fuel load. However, there needs to be more understanding of how added Gd 2 O 3 influences the properties of UO 2 under irradiation. To understand the behavior of defects and fission gas in the UO 2 /Gd 2 O 3 system under irradiation, we use cluster dynamics modeling supported by density functional theory calculations. First, we calculate the formation energies of Gd point and cluster defects, and evaluate the temperature-dependent defect concentrations using the defect formation energies and entropies. We show that Gd is soluble in UO 2 , introducing a negative charge in the system. Using this information, we adapted the cluster dynamics code Centipede to model the influence of Gd on U self-diffusion and Xe diffusion in UO 2 with 10 wt% Gd 2 O 3 . Also, we analyzed the Xe diffusion as a function of Gd 2 O 3 concentration, showing that the Xe diffusivity is decreased, which means that the athermal diffusivity due to electronic stopping persists at higher temperatures. In conclusion, the decrease in Xe diffusion means that more Xe stays in the matrix, decreasing the Xe release, and lowering its influence of fission gas release on the thermomechanical properties of UO 2 .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Fission gas diffusion and release for Cr 2 O 3 -doped UO 2 : From the atomic to the engineering scale

Here, the anticipated benefits of large grains in Cr 2 O 3 -doped UO 2 pellets include improved mechanical and fission gas retention properties. To support the assessment of fission gas release (FGR) from doped pellets, the impact of doping on fission gas diffusivity for in-reactor conditions must be understood. In this work, we tackle this issue by informing the fission gas model within the BISON fuel performance code using material models developed at the atomic scale. The investigation of intra-granular fission gas diffusivity in Cr 2 O 3 -doped UO 2 is carried out by adapting a cluster dynamics model that, accounting for UO 2 thermochemistry, is capable of describing Xe diffusion under irradiation in undoped UO 2 as the starting point. Using a thermodynamic analysis, it is shown that in stoichiometric UO 2 with additions of Cr 2 O 3 the oxygen potential is defined by the Cr-Cr 2 O 3 two-phase equilibrium. Using the cluster dynamics model, the predicted Xe diffusivity in doped UO 2 was significantly increased in both the intrinsic and irradiation-enhanced regimes compared to undoped UO 2 as a result of higher concentrations of uranium and oxygen vacancies, respectively. This is a consequence of the more oxidizing conditions at high temperature, and more reducing conditions at low temperature, as a result of doping. Arrhenius functions have been fitted to the cluster dynamics results to enable implementation of the new diffusivities in the BISON fission gas behavior model. BISON simulations were carried out, showing the competing effects of the enlarged grains and the new fission gas diffusivity model, which act to suppress and enhance fission gas release, respectively. The new physics-informed model was validated against in-reactor experimental measurements under normal operation. Additionally, benchmarking was carried out for power ramp conditions. The predicted fission gas release agreed well with the experimental data, showing noticeable improvements over the standard UO 2 model.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Matrix-formation dynamics dictate methyl nitrite conformer abundance

Methyl nitrite has two stable conformational isomers resulting from rotation about the primary C–O–N–O dihedral angle: cis-CH 3 ONO and trans-CH 3 ONO, with cis being more stable by ∼5 kJ/mol. Here, the barrier to rotational interconversion (∼45 kJ/mol) is too large for isomerization to occur under ambient conditions. This paper presents evidence of a change in conformer abundance when dilute CH 3 ONO is deposited onto a cold substrate; the relative population of the freshly deposited cis conformer is seen to increase compared to its gas-phase abundance, measured by in situ infrared spectroscopy. We observe abundance changes depending on the identity of the bath gas (N 2 , Ar, and Xe) and deposition angle. The observations indicate that the surface properties of the growing matrix influence conformer abundance—contrary to the widely held assumption that conformer abundance in matrices reflects gas-phase abundance. We posit that differences in the angle-dependent host-gas deposition dynamics affect the growing surfaces, causing changes in conformer abundances. Quantum chemistry calculations of the binding energies between CH 3 ONO and a single bath-gas component reveal that significant energetic stabilization is not observed in 1:1 complexes of N 2 :CH 3 ONO, Ar:CH 3 ONO, or Xe:CH 3 ONO. From our results, we conclude that the growing surface plays a significant role in trapping cis-CH 3 ONO more effectively than trans-CH 3 ONO, likely because cis-CH 3 ONO is more compact. Taken together, the observations highlight the necessity for careful characterization of conformers in matrix-isolated systems, emphasizing a need for further study into the deposition dynamics and surface structure of chemically inert matrices.

Hockey, Emily K.↗
DOE OSTI2022

A dry ancient plume mantle from noble gas isotopes

Primordial volatiles were delivered to terrestrial reservoirs during Earth’s accretion, and the mantle plume source is thought to have retained a greater proportion of primordial volatiles compared with the upper mantle. This study shows that mantle He, Ne, and Xe isotopes require that the plume mantle had low concentrations of volatiles like Xe and H 2 O at the end of accretion compared with the upper mantle. A lower extent of mantle processing alone is not sufficient to explain plume noble gas signatures. Ratios of primordial isotopes are used to determine proportions of solar, chondritic, and regassed atmospheric volatiles in the plume mantle and upper mantle. The regassed Ne flux exceeds the regassed Xe flux but has a small impact on the mantle Ne budget. Pairing primordial isotopes with radiogenic systems gives an absolute concentration of 130 Xe in the plume source of ∼1.5 × 10 7 atoms 130 Xe/g at the end of accretion, ∼4 times less than that determined for the ancient upper mantle. A record of limited accretion of volatile-rich solids thus survives in the He-Ne-Xe signatures of mantle rocks today. A primordial viscosity contrast originating from a factor of ∼4 to ∼250 times lower H 2 O concentration in the plume mantle compared with the upper mantle may explain (a) why giant impacts that triggered whole mantle magma oceans did not homogenize the growing planet, (b) why the plume mantle has experienced less processing by partial melting over Earth’s history, and (c) how early-formed isotopic heterogeneities may have survived ∼4.5 Gy of solid-state mantle convection.

58 GEOSCIENCES↗
DOE OSTI2021

Sensitivity of the NEXT experiment to Xe-124 double electron capture

Double electron capture by proton-rich nuclei is a second-order nuclear process analogous to double beta decay. Despite their similarities, the decay signature is quite different, potentially providing a new channel to measure the hypothesized neutrinoless mode of these decays. The Standard-Model-allowed two-neutrino double electron capture (2$\nu$EC EC) has been predicted for a number of isotopes, but only observed in 78 Kr, 130 Ba and, recently, 124 Xe. The sensitivity to this decay establishes a benchmark for the ultimate experimental goal, namely the potential to discover also the lepton-number-violating neutrinoless version of this process, 0$\nu$EC EC. Here we report on the current sensitivity of the NEXT-White detector to 124 Xe 2$\nu$EC EC and on the extrapolation to NEXT-100. Using simulated data for the 2$\nu$EC EC signal and real data from NEXT-White operated with 124 Xe-depleted gas as background, we define an optimal event selection that maximizes the NEXT-White sensitivity. We estimate that, for NEXT-100 operated with xenon gas isotopically enriched with 1 kg of 124 Xe and for a 5-year run, a sensitivity to the 2$\nu$EC EC half-life of 6 × 10 22 y (at 90% confidence level) or better can be reached.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Improved sampling technique to collect natural gas from hydrate-bearing pressure cores

High quality gas compositional data are an important factor in interpreting the genetic source of natural gas hosted in hydrate-bearing sediments and other subsurface systems. In order to accurately characterize the composition of gas samples degassed from hydrate-bearing pressure cores, one must use a reproducible sampling technique that minimizes artifacts of the sampling process. Herein, we review sediment core degassing techniques and compare data obtained from a commonly used degassing approach, which we term the standard quantitative degassing (SQD) technique, to our newly developed modified quantitative degassing (MQD) method designed to minimize atmospheric contamination and gas-water interactions. The SQD method allows sample gas to interact with water in a bubbling chamber, which we hypothesize could alter the gas composition following mixing with water or dissolved gases in the bubbling chamber. Whereas, the MQD method allows for the collection of sample gas prior to the bubbling chamber. To compare the SQD and MQD methods, we performed a side-by-side comparison of noble (He, Ne, Ar, Kr, and Xe), major (H 2 , N 2 , O 2 , and CO 2 ), and hydrocarbon (CH 4 , C 2 H 6 , C 3 H 8 , i-C 4 H 10 , C 4 H 10 , i-C 5 H 12 , C 5 H 12 ) gas concentrations and select isotopic compositions obtained using both sample collection techniques. Gas samples were collected from hydrate-bearing pressure cores recovered and maintained under hydrate stable conditions from the northern Gulf of Mexico during the UT-GOM 2 -1 Expedition. The MQD method displayed significantly lower concentrations of atmospheric gases, higher proportions of hydrocarbon gases, lower ratios of C 1 /C 2 + , and heavier stable carbon and hydrogen isotopes of methane than the SQD method. These results demonstrate that the MQD method reduced air contamination and minimized alteration of the hydrocarbon gases. Finally, we conclude this method may be important for future work that seeks to determine the composition of natural gas from pressure cores using quantitative degassing experiments, especially those seeking to measure major (e.g., N 2 ) and noble gases.

58 GEOSCIENCES↗
DOE OSTI2025

Precision measurement of lifetime and branching ratios of the 4⁢𝑓 13⁡ 5⁢𝑑⁢6⁢𝑠 1 ⁢[5/2] 5/2 state in Yb + ions

We report spectroscopic and time-resolved experimental observations to characterize the [Xe]⁢4⁢𝑓 13 ⁡( 2 𝐹$^𝑜_{5/2}$)⁢5⁢𝑑⁢6⁢𝑠⁡( 1 𝐷)⁢ 1 ⁢[5/2]$^𝑜_{5/2}$ state in 172 Yb + ions. We access this state from the metastable 4⁢𝑓 14 ⁡5⁢𝑑⁡( 2 𝐷 3/2,5/2 ) manifold and observe an unexpectedly long lifetime of 𝜏 = 37.9⁢(9) ⁢µ⁢s that allows visible Rabi oscillations and resolved-sideband spectroscopy. Using a combination of coherent population dynamics, high-fidelity detection and heralded state preparation, and optical pumping methods, we measure the branching ratios to the 2 𝐷 3/2 , 2 𝐷 5/2 , and 2 𝑆 1/2 states to be 0.359⁢(2), 0.639(2), and 0.0023⁢(16), respectively. The branching ratio to the 4⁢𝑓 13⁡ 6⁢𝑠 2 ⁡( 2 𝐹 7/2 ) is compatible with zero within our experimental resolution. We also report measurements of Landé 𝑔-factor of the 1 ⁢[5/2]$^𝑜_{5/2}$ state. Further, the branching ratio of the 2 𝐷 5/2 to 2 𝑆 1/2 decay in 172 Yb + was measured to be 0.188(3), improving its relative uncertainty by an order of magnitude. Our measurements provide experimental benchmarks for better understanding the atomic structure of Yb + ions, which still lacks accurate numerical descriptions, and the use of high-lying excited states for partial detection and qubit manipulation in the omg architecture.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Materials Data on Pd(XeF8)2 by Materials Project

Pd(XeF8)2 crystallizes in the orthorhombic Pca2_1 space group. The structure is zero-dimensional and consists of four Pd(XeF8)2 clusters. there are two inequivalent Xe sites. In the first Xe site, Xe is bonded in a 5-coordinate geometry to six F atoms. There are a spread of Xe–F bond distances ranging from 1.99–2.45 Å. In the second Xe site, Xe is bonded in a 5-coordinate geometry to six F atoms. There are a spread of Xe–F bond distances ranging from 1.99–2.47 Å. Pd is bonded in an octahedral geometry to six F atoms. There are a spread of Pd–F bond distances ranging from 1.94–1.97 Å. There are sixteen inequivalent F sites. In the first F site, F is bonded in a single-bond geometry to one Pd atom. In the second F site, F is bonded in a single-bond geometry to one Xe atom. In the third F site, F is bonded in a single-bond geometry to one Xe atom. In the fourth F site, F is bonded in a single-bond geometry to one Xe atom. In the fifth F site, F is bonded in a single-bond geometry to one Xe atom. In the sixth F site, F is bonded in a single-bond geometry to one Xe atom. In the seventh F site, F is bonded in a single-bond geometry to one Xe atom. In the eighth F site, F is bonded in a distorted single-bond geometry to one Pd atom. In the ninth F site, F is bonded in a single-bond geometry to one Xe atom. In the tenth F site, F is bonded in a single-bond geometry to one Pd atom. In the eleventh F site, F is bonded in a single-bond geometry to one Pd atom. In the twelfth F site, F is bonded in a single-bond geometry to one Xe atom. In the thirteenth F site, F is bonded in a distorted bent 150 degrees geometry to one Xe and one Pd atom. In the fourteenth F site, F is bonded in a single-bond geometry to one Xe atom. In the fifteenth F site, F is bonded in a distorted bent 150 degrees geometry to one Xe and one Pd atom. In the sixteenth F site, F is bonded in a single-bond geometry to one Xe atom.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Re4Xe3(O5F7)2 by Materials Project

Xe3Re4(O5F7)2 crystallizes in the triclinic P-1 space group. The structure is zero-dimensional and consists of one Xe3Re4(O5F7)2 cluster. there are two inequivalent Xe sites. In the first Xe site, Xe is bonded in a linear geometry to two equivalent O atoms. Both Xe–O bond lengths are 2.22 Å. In the second Xe site, Xe is bonded in a linear geometry to one O and one F atom. The Xe–O bond length is 2.06 Å. The Xe–F bond length is 2.43 Å. There are two inequivalent Re sites. In the first Re site, Re is bonded to two O and four F atoms to form distorted corner-sharing ReO2F4 octahedra. The corner-sharing octahedral tilt angles are 21°. There is one shorter (1.71 Å) and one longer (1.72 Å) Re–O bond length. There are a spread of Re–F bond distances ranging from 1.88–2.08 Å. In the second Re site, Re is bonded to two O and four F atoms to form distorted corner-sharing ReO2F4 octahedra. The corner-sharing octahedral tilt angles are 21°. There is one shorter (1.70 Å) and one longer (1.72 Å) Re–O bond length. There are a spread of Re–F bond distances ranging from 1.89–2.28 Å. There are five inequivalent O sites. In the first O site, O is bonded in a single-bond geometry to one Re atom. In the second O site, O is bonded in a single-bond geometry to one Re atom. In the third O site, O is bonded in a single-bond geometry to one Re atom. In the fourth O site, O is bonded in a bent 120 degrees geometry to two Xe atoms. In the fifth O site, O is bonded in a single-bond geometry to one Re atom. There are seven inequivalent F sites. In the first F site, F is bonded in a distorted bent 150 degrees geometry to one Xe and one Re atom. In the second F site, F is bonded in a bent 150 degrees geometry to two Re atoms. In the third F site, F is bonded in a single-bond geometry to one Re atom. In the fourth F site, F is bonded in a single-bond geometry to one Re atom. In the fifth F site, F is bonded in a single-bond geometry to one Re atom. In the sixth F site, F is bonded in a single-bond geometry to one Re atom. In the seventh F site, F is bonded in a single-bond geometry to one Re atom.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Boosted Dark Matter Search with the ICARUS Detector at the Gran Sasso Underground National Laboratory

The quest to discover dark matter is one of the most pressing topics in modern physics. Evidence of gravitational anomalies is present at different cosmological scales, spanning the stability and rotation of galaxies to the overall density profile of the entire observable Universe. Due to the discrepancy between the mass measured and the gravitational influence on the mass, if General Relativity is to correctly describe gravity at different scales, extra electromagnetically invisible matter termed dark matter must exist. In recent decades, many experiments have been performed to detect dark matter with masses that span many orders of magnitude, from Mass Compact Halo Objects (MACHOs) with masses several orders of magnitude that of our sun to very light particles on the order of $\sim\mu$eV. However, experiments have only been able to constrain the possible parameter space of dark matter models and, in general, probe dark matter models with single constituent dark matter like Weakly Interacting Massive Particles (WIMPs). In the Boosted Dark Matter (BDM) paradigm, there are four particles in the dark sector: $\chi_0$, $\chi_1$, $\chi_2$, and the dark photon $X$. WIMP-like properties are ascribed to $\chi_0$ to describe the physics of the gravitational anomalies, while relativistic components are assigned to $\chi_1$ and $\chi_2$. The inelastic boosted dark matter (iBDM) channel $\chi_1 e^-\rightarrow \chi_2 e^-\rightarrow \chi_1 Xe^-\rightarrow \chi_1 (e^+ e^- ) e^-$, where $\chi_2$ is an excited state of $\chi_1$, has a unique signature that is distinguishable from neutrino interactions, making neutrino experiments a viable search environment for BDM. Using data collected by the ICARUS collaboration with ICARUS T-600 Liquid Argon Time Projection Chamber (LArTPC) during its operation at the Gran Sasso Underground Laboratory (LNGS), the first-ever LArTPC dark matter search using the ICARUS detector is presented. With a total detector exposure of 0.13 kton$\cdot$year, a total of 4 iBDM candidate events were identified by several stages of data scanning. All were rejected due to defined selection criteria and a wire-by-wire $dE/dx$ evaluation, giving a null result. Exclusion plots at 90\%C.L. for the dark photon ($m_X$, $\epsilon$) parameter space for fixed ($m_0,m_1,m_2$) DM mass sets are presented, setting new limits on the dark photon visible decay parameter space.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Improving the laser performance of ion beam sputtered dielectric thin films through the suppression of nanoscale defects by employing a xenon sputtering gas

Laser damage-prone precursors in high index materials such as hafnia are believed to be the primary limiter in the performance of dielectric multilayer films to advance ultra-high power and energy laser applications. Removing or suppressing these precursors is the key to fabricating laser damage resistant thin films for the enabling technologies. Early work has revealed that nanobubbles formed by entrapped argon (Ar) working gas in ion beam sputtering (IBS) produced hafnia films are primarily responsible for the onset of laser damage upon exposure to UV, ns-laser pulses. In this study, we demonstrate that the UV ns-laser damage onset of IBS produced hafnia films can be improved to 3.1 +/- 0.2 J/cm 2 by substituting the conventional Ar working gas with xenon (Xe), a nearly 1 J/cm 2 increase from that of the Ar produced hafnia films. In addition to the suppression of the overall point-defect density of the hafnia films, the reduction of the Xe entrapment eliminates the nanobubbles and the generation of plasmas that initiates the laser damage. The defect suppression and its correlation to the increase in laser damage threshold is revealed by the combined analysis of Rutherford backscattering spectroscopy, electron paramagnetic resonance spectroscopy, transmission electron microscopy, and laser damage testing. Monte Carlo simulations suggest a much smaller entrapment of Xe gas by comparison to Ar, which is attributed to the significant difference in the energy of the reflected neutrals (3X) which are likely to be implanted. These results provide an effective process route with a fundamental understanding for producing high laser damage resistant dielectric films for high power and high energy laser applications.

36 MATERIALS SCIENCE↗