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DOE OSTI2025

Low-Energy Backgrounds in Solid-State Phonon and Charge Detectors

Solid-state phonon and charge detectors probe the scattering of weakly interacting particles, such as dark matter and neutrinos, through their low recoil thresholds. Recent advancements have pushed sensitivity to eV-scale energy depositions, uncovering previously unseen low-energy excess backgrounds. While some arise from known processes such as thermal radiation, luminescence, and stress, others remain unexplained. This review examines these backgrounds, their possible origins, and parallels to low-energy effects in solids, an understanding of which is essential for interpreting particle interactions at and below the eV scale.

coherent neutrino–nucleus scattering↗

DOE OSTI2022

PVcircuit [SWR-22-26]

The software contains objects that are building blocks for PV modeling and interactive data fitting based on: Optoelectronic models for tandem/multijunction solar cells including resistive and luminescent coupling; simulation of modules composed of 2T, 3T, and 4T tandem solar cells; and energy yield analysis of PV systems composed of tandem solar cells.

Geisz, John↗

DOE OSTI2022

PVcircuit v0.0.6 [SWR-22-26]

Geisz, John↗

DOE OSTI2025

Synergistic effects of Al, Ga, and In doping on ZnO nanorod arrays grown via citrate-assisted hydrothermal technique for highly efficient and fast scintillator screens

To be used as efficient alpha particle scintillator in the fields of nuclear security, nuclear nonproliferation and high-energy physics, scintillator screens must have high light output and fast decay properties. While there has been a great deal of progress in scintillation efficiency, achieving fast decay time properties are still a challenge. In this work, the near band edge (NBE) UV luminescence and alpha particle induced scintillation properties of vertically aligned densely packed ZnO nanorods (NRs) doped with Al, Ga, and In have been thoroughly investigated. The high crystalline hexagonal wurtzite structure with a strong orientation through the c -axis plane (002) and aspect ratios in the range 13–22 have been observed for all ZnO NRs. Electron paramagnetic resonance (EPR) analysis exhibited paramagnetic signals at g ≈ 1.96 for all ZnO NRs. A cost effective green hydrothermal synthesis technique was employed to grow well-aligned NRs. Using citrate as an additive acting as a strong reducing agent in the solution during the crystal growth, defects on the surface are significantly suppressed, thereby enhancing the NBE UV emission. Significantly higher NBE UV emission was observed from the top surface of ZnO NRs in cathodoluminescence (CL) microscopy. Results show that citrate assisted donor doping of ZnO NRs not only reduces the defect emission and NBE self-absorption, but also induces fast decay time (~ 600–700 ps), which makes ZnO NRs a good candidate for fast alpha particle scintillator screens used in associated particle imaging for time and direction tagging of individual neutrons generated in D–T and D–D neutron generators.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Lasofoxifene as a potential treatment for therapy-resistant ER-positive metastatic breast cancer

Background: Endocrine therapy remains the mainstay of treatment for estrogen receptor-positive (ER+) breast cancer. Constitutively active mutations in the ligand binding domain of ERα render tumors resistant to endocrine agents. Breast cancers with the two most common ERα mutations, Y537S and D538G, have low sensitivity to fulvestrant inhibition, a typical second-line endocrine therapy. Lasofoxifene is a selective estrogen receptor modulator with benefits on bone health and breast cancer prevention potential. This study investigated the anti-tumor activity of lasofoxifene in breast cancer xenografts expressing Y537S and D538G ERα mutants. The combination of lasofoxifene with palbociclib, a CDK4/6 inhibitor, was also evaluated. Methods: Luciferase-GFP tagged MCF7 cells bearing wild-type, Y537S, or D538G ERα were injected into the mammary ducts of NSG mice (MIND model), which were subsequently treated with lasofoxifene or fulvestrant as single agents or in combination with palbociclib. Tumor growth and metastasis were monitored with in vivo and ex vivo luminescence imaging, terminal tumor weight measurements, and histological analysis. Results: As a monotherapy, lasofoxifene was more effective than fulvestrant at inhibiting primary tumor growth and reducing metastases. Adding palbociclib improved the effectiveness of both lasofoxifene and fulvestrant for tumor suppression and metastasis prevention at four distal sites (lung, liver, bone, and brain), with the combination of lasofoxifene/palbociclib being generally more potent than that of fulvestrant/palbociclib. X-ray crystallography of the ERα ligand binding domain (LBD) shows that lasofoxifene stabilizes an antagonist conformation of both wild-type and Y537S LBD. The ability of lasofoxifene to promote an antagonist conformation of Y537S, combined with its long half-life and bioavailability, likely contributes to the observed potent inhibition of primary tumor growth and metastasis of MCF7 Y537S cells. Conclusions: We report for the first time the anti-tumor activity of lasofoxifene in mouse models of endocrine therapy-resistant breast cancer. The results demonstrate the potential of using lasofoxifene as an effective therapy for women with advanced or metastatic ER+ breast cancers expressing the most common constitutively active ERα mutations.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2020

Accurate calibration of thermophotovoltaic efficiency

Abstract The new record efficiency in Thermophotovoltaics relies upon a highly reflective rear mirror. The excellent rear mirror boosts voltage by enhancing the luminescence extraction, and separately also reflects low energy photons, which would otherwise be useless in thermophotovoltaics. The reflected low energy photons reheat the thermal emitter, and regenerate above-bandgap energy photons. The efficiency calibration for such regenerative thermophotovoltaics depends on several factors, yet predominantly on the accurate measurement of the rear mirror reflectivity. Here, we report on the technique for accurate measurement of mirror reflectivity, and of record thermophotovoltaic efficiency 29.1 ± 0.6%, at 1207 °C.

14 SOLAR ENERGY↗

DOE OSTI2022

Raman Spectroscopy Characterization of Nuclear Materials and Soot from High Explosives

Vibrational and luminescence spectroscopy were used in the investigation of U and Pu-bearing compounds and soot from high explosives testing. Key spectroscopic signatures of UF4 and its hydrates, PuO 2 , and soot from different explosives will be presented. The United States Government retains and the publisher, by accepting this article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for United States Government purposes.

Villa-Aleman, Eliel↗

DOE OSTI2025

All-optical control of charge-trapping defects in rare-earth doped oxides

Abstract Charge-trapping defects in crystalline solids play important roles in applications ranging from microelectronics, optical storage, sensing and quantum technologies. On one hand, depleting trapped charges in the host matrix reduces charge noise and enhances coherence of solid-state quantum emitters. On the other hand, stable charge traps can enable high-density optical storage systems. Here we report all-optical control of charge-trapping defects via optical charge trapping (OCT) spectroscopy of a rare-earth ion doped oxide (Y 2 O 3 ). Charge trapping is realized by low intensity optical excitation in the 200–375 nm range. Charge detrapping or depletion is carried out by optically stimulated luminescence (OSL) under 532 nm stimulation. Using a Pr-doped Y 2 O 3 polycrystalline ceramic host matrix, we observe charging pathways via the inter-band optical absorption of Y 2 O 3 and via the 4f-5d transitions of Pr 3+ . We demonstrate effective control of the density of trapped charges within the Y 2 O 3 matrix at ambient environment. These results point to a viable method for controlling the local charge environment in rare-earth doped crystals via all-optical means, and pave the way for further development of efficient optical storage technologies with ultrahigh storage capacity, as well as for the localized control of quantum coherence in rare-earth doped solids.

França, Leonardo V. S. [Pritzker School of Molecul↗

DOE OSTI2020

Rugged nanoparticle tracers for mass tracking in explosive events

Tracing the flow of solid matter during an explosion requires a rugged tag that can be measured by a unique identifiable signature. Silica-covered semiconductor quantum dots (QDs) provide a unique and tunable photoluminescent signature that emits from within a sacrificial outer layer. Five types of silica-covered zinc sulfide QDs were synthesized and covalently bound to commercial luminescent powders. The combination of five dots and five powders enables a matrix of 25 unique tags. The tracers are shown to be tolerant of environments associated with chemical explosives and provides a unique tag to evaluate debris fields.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2021

Parameters of fast and high-yield InAs/GaAs quantum dot semiconductor scintillator

InAs quantum dots (QDs) embedded into a waveguiding GaAs semiconductor matrix may produce scintillation detectors with exceptional speed and yield, making them valuable for nuclear security, medical imaging, and high energy physics applications. In this work, we developed thick (~25 μm) epitaxial heterostructres with high luminescence efficiency composed of self-assembled nano-engineered InAs QDs grown by molecular beam epitaxy. Here, the bulk GaAs acts as a stopping material for incident particles and as a waveguide when layer-transferred onto a low-index substrate. Waveguiding and self-absorption (< 1 cm –1 ) were studied using photoluminescence with scanning laser excitation and modeled with ray optics approximation and geometrical coupling of high-index waveguide to a collection fiber. Scintillating signals from α-particles were analyzed with an external photodiode (PD) and an integrated PD which provided an improved optical coupling. The mean charge collected by the integrated PD corresponded to 3 × 10 4 photoelectrons per 1 MeV of deposited energy, or ~13% of the theoretically achievable light yield. Combined with the previously measured QD scintillation time of 0.3-0.6 ns, this makes the InAs/GaAs QD heterostructures the fastest high yield scintillation material reported.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Effects of delta ray electrons on measurement uncertainties of harp system

A harp system, which is a multi-wire beam profile monitoring (MWPM) system, is planned upstream of the spallation target to make in situ calibration of beam current density configuration on the target along with beam imaging from luminescent coating on the beam entrance window at the Second Target Station (STS) of the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory (ORNL). This beam interception-based beam diagnostics system on the target will be used to ensure that the maximum beam loads on the target are within the design range during neutron production. Current design of the harp consists of three layers of measurement wires each of which is sandwiched between voltage biasing wire planes. The signal obtained from each measurement wire layer is disturbed by secondary electrons (SE) and delta rays produced by beam-matter interactions in neighboring wires and ionization of residual gases in accelerator vacuum. While the backgrounds from SE can be suppressed by voltage biasing, the delta-ray electrons with kinetic energies above keV ranges overcome the electric potential bias. In this paper, we study the effects of delta-rays on the measurement uncertainties of MWPM using the particle transport simulation code FLUKA. Furthermore, the cases where the harp system is installed in the proximity of a large delta ray sources such as proton beam window or in the core vessel filled with sub-atmospheric gas have been studied.

Lee, Yong Joong↗

DOE OSTI2023

Dark matter searches and energy accumulation and release in materials

Efforts to identify dark matter by detecting nuclear recoils produced by dark matter particles reveal low-energy backgrounds of unknown origin in different types of detectors. In many cases, energy accumulation and delayed burst-like releases of stored energy could provide an explanation. These dynamics follow Prigogine’s ideas on systems with energy flow and the general Self-Organized Criticality scenario. We compare these models with properties of excess backgrounds in cryogenic solid-state detectors, relaxation processes in glasses and crystals, our observations of delayed luminescence in NaI(Tl), and make predictions for more phenomena present in these systems and in superconducting photon detectors and qubits. Experiments to create accurate phenomenological models are needed.

Pereverzev, Sergey↗

DOE OSTI2020

Evaluation and Demonstration of Intrusion Detection for Spent Fuel Storage Facilities

The IAEA recommends dual containment and surveillance (C/S) systems for difficult to access or difficult to measure spent fuel storage areas. However, many storage areas have limitations that prevent traditional secondary C/S systems, such as radiation levels too high for inspectors to apply individual Tamper Indicating Devices (TID) or have physical impedances to the use of TIDs. Recent developments in C/S technology include Laser Curtain for Containment (LCCT) technology implemented at Atucha-1 power plant in Argentina. The LCCT is a new approach to perimeter-wide C/S and the IAEA has granted provisional approval for its use as one of two required C/S systems. This proposal focuses on investigating and testing new and evolving completely passive (or ultra-low power) tamper indicating systems that will provide backup C/S to the LCCT even during power outages. An investigation of Commercial Off The Shelf (COTS) technology will be conducted to identify readily available options. Optically Stimulated Luminescence (OSL) fibers will also be investigated. OSL fibers are a passive technology that can measure radiation dose by knocking an electron into a metastable state where it remains until the fiber is interrogated with light. The goal of this project would be to investigate COTS technologies that can be used in low or no power scenarios for radiation detection as well as test and evaluate OSL technology, which can operate passively in no power scenarios. Limitations for each technology will be determined and documented in an effort to determine the best technology for spent fuel storage monitoring.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

Synthesis and Single Crystals of Refractory Oxides of Lanthanides and Thorium

At the completion of this program, we can report that we developed a considerable degree of technical improvements in our ability to perform hydrothermal reactions at high temperatures and pressures. We can now routinely perform reactions at 700-750°C and 200 MPa. Currently we are in the process of exploiting this new technology synthesizing a range of exotic new materials investigating relatively poorly understood materials. Our initial efforts focused on the chemistry of rare earth oxides with tetravalent and pentavalent oxides. We recently published a study of the lanthanides with Nb 5+ and Ta 5+ ions, where we grew oxides such as RENdO 4 and RETaO 4 as high quality single crystals. These compounds were targeted as potential hosts for luminescent and scintillation materials, particularly given that they are among the densest oxide hosts and hence have good potential as absorbers for high energy radiation like X-rays and gamma rays. We also isolated a range of unusual new rare earth tantalates with very complex structures. indicating that the chemistry is very sensitive to conditions. We performed some fairly comprehensive examinations of the solid-state chemistry of rare earth ions with various tetravalent metal ions especially Si 4+ , Ge 4+ , Sn 4+ and Ti 4+ . Given the potential role of rare earth silicates in immobilizing radioactive waste elements in long-term storage, and the similarity of our hydrothermal fluids with known geological conditions, this chemistry continues to be relevant. We prepared an extensive series of new lanthanide germanates (e.g. RE 13 Ge 6 O 31 (OH), BaRE 10 (GeO 4 ) 4 O 8 ). and found that there is there is almost no overlap between the chemistry of the rare earth silicates. Stannic oxide (SnO 2 ) is much more refractory and requires higher temperatures and of mineralizer concentrations. One significant result is the growth of RE 2 Sn 2 O 7 pyrochlore single crystals. These are of interest because the rare earth stannate pyrochlores are known to display a wide range of magnetic frustration such as spin ice behavior. We grew high quality single crystals of rare earth germanate and stannate pyrochlores and this led to a collaboration with Professor Kate Ross at Colorado State. Preliminary measurements, indicate that the crystals contain no detectable defects or site disorder. Initial neutron diffraction on single crystals was performed at Oak Ridge, and more detailed experiments involving the Ross group are underway at both NIST and ORNL. This particular chemistry has turned out to be the most potentially significant work on this project and the collaborative effort with Prof. Ross is the topic of a DoE renewal project on quantum materials. Our initial foray into the hydrothermal chemistry of rare earth titanates has also been very promising and a range of cubic and polar ferroic phases of the light rare earths RE 2 Ti 2 O 7 (RE = La - Pr) in the P2 1 phase. We also discovered an interesting new phase Ce 2 Ti 4 O 11 that can have implications in heavy metal immobilization and storage. along with a series of new rare earth titanates (La 5 Ti 4 O 15 (OH) Sm 3 TiO 5 (OH) 3 and Lu 5 Ti 2 O 11 (OH) with exceptionally complex structures. One interesting sidelight has been high temperature hydrothermal chemistry terbium, including the growth of large crystals of TbO(OH). This is not a new compound but it is the first time it has been grown as large single crystals. The Tb atom density is almost as high as that in Tb 2 O 3 and has a very high Verdet constant (ca. 70), making it a very attractive candidate as a Faraday rotator. Unfortunately it is not in a cubic structure but he material is hard, stable, pure and inexpensive, so should still be an attractive Faraday oscillator. We recently received a patent on this material. We also synthesized K 2 Tb(Ge 2 O 7 ) containing stable octahedral Tb 4+ ions, which appears to be the first example of a well-characterized Tb 4+ complex. Given that Tb 4+ has been proposed as a benign surrogate for more treacherous tetravalent ions such as Cf 4+ and Bk 4+ , we think that Tb 4+ silicates can be a particularly useful study for actinide immobilization and related work. We also began reaction studies with rare earths and both ReO 2 and RuO 2 . These resulted in large single crystals of species like RE 5 Ru 2 O 12 , RE 4 Re 2 O 11 , REReO 4 and RE 2 ReO 5 . Several of these samples have already been sent to ORNL for magnetic and neutron diffraction studies.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Time Domain Thermoreflectance (TDTR) Studies of Microstructural Characterization of as-Fabricated and/or Irradiated TPBAR Components

Paddock et al. demonstrated for the first-time the measurement of thermal diffusivity from thin metal films using picosecond transient thermoreflectance in 1986. This project attempted to use a similar experimental setup based on a femtosecond time domain thermoreflectance (TDTR) to measure the damage to the crystal lattice of LiAlO 2 from irradiation in the reactor and production of tritium and helium. The TDTR is based on a pump-probe laser configuration where the pump laser is used to heat the sample and the probe laser is used to follow the thermal evolution created by the pump laser. The goal for this project is to measure the differences in thermal diffusivity between LiAlO 2 and the irradiated Li AIO 2 sample in a reactor. Unfortunately, COVID-19 restricted laboratory research time and the availability of researchers capable to conduct TDTR work. In addition, the ultrafast laser (Astrella 35fs laser) required to conduct the work was inoperable making this particulate work impossible to conduct in FY20 and FY21. The purpose of the thermal diffusion measurements with a TDTR setup is to probe the damage and disorder to the crystal lattice of pristine and irradiated samples. Since TDTR was not available for this work, a different approach using Raman and luminescence spectroscopy was used to characterize the crystal lattice damage in LiAlO 2 from irradiation.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2023

Hybrid Tandem Photovoltaics

Tandem solar cell structures are the only strategy demonstrated to surpass the detailed balance efficiency limit of high-quality single-junction solar cells. To continue to improve the efficiencies of cost-effective terrestrial solar power, hybrid tandems of dissimilar subcells are being considered by many around the world, especially designs that incorporate silicon solar cells as a bottom subcell. In this project, we studied a wide variety of tandem design possibilities including those with three-terminal (3T) and four-terminal (4T) configurations. The use of 3T and 4T designs could be useful for efficient and economical hybrid tandem designs that utilize the best available subcell materials such as emerging perovskite materials. Three-terminal configurations, in particular, have not been sufficiently studied previously. We have laid the foundational groundwork in this project for understanding the operation of 3T tandems: developing a taxonomy for naming, a methodology for measuring and interconnecting, and models for simply characterizing 3T tandems. Electrical and optical subcell coupling between the subcells was also measured and modeled. An important part of this work was the fabrication of novel example tandem structures, including 4T GaAs/Si, 3T GaInP/Si, 3T GaAs/Si, and 3T GaInP/GaAs devices. Using these high-quality tandem cells, we have been able to clearly demonstrate the achievability of high-efficiencies, and subtle physical effects such as photon recycling and luminescent coupling. We have developed and demonstrated essential building-block tools such as transparent conductive adhesives (TCA) and 3T silicon bottom cells with interdigitated back contacts (IBC) that can also be used in many other tandem designs. We have tested the reliability of these tools and devices under standardized testing and outdoor measurements. We have found 4T GaAs/Si tandems to be relatively straightforward to fabricate and robust in real-world outdoor conditions. While we have demonstrated working hybrid 3T III-V/TCA/Si IBC tandems, we experienced low yields even with our best process flows yet. Further work is still needed to improve the processing yield of these devices. We therefore also created tandem cells using an all-III-V 3T tandem process which was very robust with high yields, allowing for the creation of voltage-matched strings in many different configurations using 8 nearly identical 3T tandems. Using these robust 3T tandem examples, we were able measure and precisely characterize 3T tandem behaviors to predict their operation under changing spectrum and temperature. The optoelectronic equivalent-circuit model was shown to be very general and applicable to hybrid tandems, and encompassed the operation 3T Si IBC cells. This general model has been distributed to the public in as open-source Python-based software called PVcircuit. We have calculated the implications of these new tandem device designs on the real-world energy production and shown how the relative performance of different tandem configurations is situational and can be engineered using the tools developed here.

14 SOLAR ENERGY↗

DOE OSTI2024

Manufacturing Supply Chain Development for Modular Solar-Thermochemical Conversion Platform [Abstract]

We will develop a tunable pulsed electron source capable of generating variable intensity highly-focused electron pulses at high repetition rates. Specifically, we need to demonstrate a high-speed variable electron gun capable of generating a variable intensity electron pulse containing between 102 and 105 electrons with an accelerating voltage of 1kV focused into a spot size <100nm in diameter at with a pulse rate >10MHz (with path to 300MHz). This combined performance cannot be achieved by commercially available electron sources. The primary technology path selected for this work will be to use a photocathode approach, where an easily modulated UV laser is used to stimulate electron emission. The approach utilizes the advances made in the development of the Dynamic TEM (DTEM), though this project will be simpler in that the pulse intensity is lower and there is no requirement for coherency. Alternate paths, including using a traditional electron beam modulated using a v-shaped slit and electrostatically deflecting the beam to adjust intensity; will also be considered for future capabilities. The electron source will then be used generate optically stimulated luminescence (OSL) in lithium fluoride (LiF) substrates to demonstrate the potential for OSL to serve as a basis technology for next generation data storage systems.

42 ENGINEERING↗

DOE OSTI2024

Surface Tagging of Al 6061-T6 using Photoluminescent Oxides

The goal of tagging nuclear fuels (or related materials, such as fuel cladding) is to provide a persistent marker, traceable to the fuel manufacturer, that can be detected after some length of time, likely after the fuel has been lost, rerouted, or partially destroyed. Ideally, the tag is complicated enough to encode data pertaining to the provenance (manufacturer, date or time, constituents, etc.) and robust enough to survive in-pile exposure and/or further destruction. The taggant should not change the behavior or performance of the fuel in any meaningful way. Photoluminescent tagging was an attractive solution to many of these challenges, as it is undetectable under normal lighting conditions, visible to the naked eye under specific lighting conditions, does not require a significant quantity of material to be photoluminescent, observable with simple commercial detection tools, and is versatile and robust in application. In FY23, the team focused on embedding photoluminescent taggants onto the replicate fuel cladding surface using welding. From a welding standpoint, photoluminescent taggants, in the form of oxides, are a viable option for tagging because the taggants have high melting points, and thus likely to survive welding temperatures (i.e., remain as a secondary phase particle and maintain luminescent properties). Additionally, these taggants have the potential to act as a metal matrix composite which may increase the strength-to-weight ratio, stiffness, and ductility of the base material, all beneficial to cladding and fuel performance.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗