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Short, Michael

Publications and source records attributed to Short, Michael.

Measuring Very Low Radiation Doses in PTFE for Nuclear Forensic Enrichment Reconstruction

Every country that has made nuclear weapons has used uranium enrichment. Despite the centrality of this technology to international security, there is still no reliable physical marker of past enrichment that can be used to perform forensic verification of historically produced weapons. We show that the extremely low radioactivity from uranium alpha emissions during enrichment leaves detectable and irreversible calorimetric signatures in the common enrichment gasket material PTFE, allowing for historical reconstruction of past enrichment activities at a sensitivity better than one weapon's quantity of highly enriched uranium. Fast scanning calorimetry also enables the measurement of recrystallization enthalpies of sequentially microtomed slices, confirming the magnitude and the type of radiation exposure while also providing a detection of tampering and a method for analyzing field samples useful for treaty verification. This work opens the door for common items to be turned into precise dosimeters to detect the past presence of radioactivity, nuclear materials, and related activities with high confidence.

Connick, Rachel↗

Detecting Thermally Induced Spinodal Decomposition with Picosecond Ultrasonics in Cast Austenitic Stainless Steels

Given the existential climate crisis faced by mankind and the world, the lifetime and sustainability of nuclear reactors as a carbon-free source of renewable energy depend on the susceptibility of their structural components to environmental degradation. In particular, critical components for light water reactors (LWRs) evolve over decades in service, losing ductility and toughness due to thermal and irradiation aging. Techniques to monitor their health cannot be easily applied in the field due to their destructive, expensive, or immobile nature. Thus, non-destructive evaluation (NDE) methods are sought to monitor and evaluate the health of major LWR components such as core barrels, steam generator tubes, or primary coolant pipes and are often required by policy, such as NRC policy #10-CFR-50.65. In this work we demonstrate the use of gigahertz, non-contact ultrasonics to gauge the state of cast austenitic stainless steels (CASS), used in some of the largest components in LWR primary systems. We do so by linking changes in their surface acoustic wave (SAW) characteristics using transient grating spectroscopy (TGS) to transmission electron microscopy (TEM)-verified evidence of spinodal decomposition and G-phase precipitation. In this thesis, thermal aging is shown to induce SAW peak splitting in spinodally decomposed CASS alloys, correlated strongly with lowered toughness and decreased ductility. Furthermore, statistical testing on the number of SAW peak splits observed show that the second SAW peak significantly appears more frequently and is significantly different in frequency in comparison to counts and frequencies measured in unaged specimens. The ability of this technique to non-destructively detect microstructural degradation at a distance in a predictive manner in the case of CASS motivates extending gigahertz ultrasonics to detect other LWR material degradation modes as an in-vessel inspection technique, such as reactor pressure vessel (RPV) embrittlement. This allows for the greater use of NDE techniques for confident monitoring of LWR structural material health to 80 years and beyond, saving costs by minimizing structural replacements until needed and maximizing energy production by preventing early decommission until necessary.

36 MATERIALS SCIENCE↗

CRUD Source Term Assessment and Development for VERA

In pressurized water reactors, corrosion of primary loop materials is an ongoing process, as primary loop components (steam generator, hot leg, cold leg, and core) are constantly exposed to the coolant. As a result of this corrosion, primary loop materials are released into the coolant in the form of aqueous metal ions and particulate oxides. These corrosion products are the source of materials that form crud deposits on fuel rod clad surfaces. The mass of corrosion products available to create crud will limit the rate and extent of crud buildup that occurs. This is commonly referred to as the crud “source term”. The major contribution to the source term mass comes from the steam generator, due to the large surface area exposed to the coolant. Steam generators are not identical; the wetted area exposed to the coolant and the alloy used in the steam generator tubes vary. Different alloys corrode at different rates; Inconel 690 corrodes at approximately one-third of the rate of corrosion of Inconel 600. The mass of corrosion products released from the steam generator also varies by the area exposed to the coolant. The release of these corrosion products depends on the local environmental factors within the primary loop, including temperature, pH, local fluid conditions, electrochemical potential, and thermodynamic solubilities of the species present within this system. As such, each PWR will have a different crud source term based on these plant-specific parameters. In order to accurately model and predict crud growth and issues that arise from the presence of crud (CIPS, CILC), the source of these corrosion product materials must be accurately modeled in a system mass balance. These models should be mechanistic, representative of the underlying physics phenomena, and account for the effects of the plant-specific design and operating parameters, including the alloys used, local temperatures, and fluid flow conditions.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Advanced surface plasma nitriding for development of corrosion resistant and accident tolerant fuel cladding: Final Report

Although various surface coating techniques have been proposed to increase oxidation and corrosion resistance of fuel cladding materials, the de-bonding of the coating layer with the original cladding matrix under exposure to coolants makes such approaches unsuitable for reactor applications. Furthermore, the feasibility of techniques for large scale processing on cladding tubes remains another technological bottleneck. This project aims to develop a hollow cathode plasma nitriding technique to solve the above issues. Starting with alloys of DOE interest, the team will apply an advanced surface plasma nitriding technique to convert alloy surface layers into nitride layers for better structural integrity and compatibility with both coolants and nuclear fuels. The technique can form uniform nitride layers on both inner and outer surfaces of cylindrical hollow tubes. Both treated and untreated samples will be irradiated by using Fe self ions or dual beams of Fe ions and He ions. Various microstructural characterizations and mechanical property measurements will be performed. For outside surfaces, samples will be tested in high temperature water and liquid molten salt to evaluate their corrosion resistance and compatibility with coolants for LWR and fast reactor applications. For inside surfaces, solid-to-solid diffusion couple experiments will be used to study interface reactions of nitrided samples with uranium, to test whether a nitrided layer can slow down fuel-cladding interactions. The project will impact both the development of advanced methods for manufacturing and the development of advanced reactor in-core structural materials. The proposed technique can form nitride layers on alloys of irregular shapes without an edging effect - an issue encountered in traditional plasma nitriding processes, and is suitable for surface processing of other in-core components.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nanotube/Nanowire as Effective Defect Sinks in Metals—Atomistic Simulations and In Situ Ion Radiation Transmission Electron Microscopy

The accumulation of defects during irradiation leads to material property degradation modes such as embrittlement and swelling, eventually causing material failure. Effective and efficient removal of defects is of crucial importance to design radiation damage-tolerant materials. Here, by biasing defect migration pathways via carbon nanotube (CNT) infiltration, we present a greatly enhanced damage-tolerant Al-CNT composite with defect storage measured to be one order of magnitude lower than that in pure, irradiated Al. Furthermore, extreme-value statistics (largest size) of defect clusters are significantly changed in the presence of CNT. In situ ion irradiation transmission electron microscopy (TEM) experiments and atomistic simulations together reveal the dynamic evolution and convergent diffusion of radiation-induced defects to CNTs, facilitating defect recombination and enhancing radiation tolerance. The occurrence of CNT-biased defect convergent migration is tuned by the thermodynamic driving force of stress gradient in Al matrix due to the CNT phase transformation. This approach to controlling defect migration using 1D interface engineering creates a new opportunity to enhance the properties of nuclear materials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Multiphysics modeling of two-phase film boiling within porous corrosion deposits

Porous corrosion deposits on nuclear fuel cladding, known as CRUD, can cause multiple operational problems in light water reactors (LWRs). CRUD can cause accelerated corrosion of the fuel cladding, increase radiation fields and hence greater exposure risk to plant workers once activated, and induce a downward axial power shift causing an imbalance in core power distribution. In order to facilitate a better understanding of CRUD's effects, such as localized high cladding surface temperatures related to accelerated corrosion rates, we describe an improved, fully-coupled, multiphysics model to simulate heat transfer, chemical reactions and transport, and two-phase fluid flow within these deposits. Our new model features a reformed assumption of 2D, two-phase film boiling within the CRUD, correcting earlier models' assumptions of single-phase coolant flow with wick boiling under high heat fluxes. This model helps to better explain observed experimental values of the effective CRUD thermal conductivity. Finally, we propose a more complete set of boiling regimes, or a more detailed mechanism, to explain recent CRUD deposition experiments by suggesting the new concept of double dryout specifically in thick porous media with boiling chimneys. - Highlights: • A two-phase model of CRUD's effects on fuel cladding is developed and improved. • This model eliminates the formerly erroneous assumption of wick boiling. • Higher fuel cladding temperatures are predicted when accounting for two-phase flow. • Double-peaks in thermal conductivity vs. heat flux in experiments are explained. • A “double dryout” mechanism in CRUD is proposed based on the model and experiments.

42 ENGINEERING↗

Applications of Transient Grating Spectroscopy to Radiation Materials Science

Radiation damage is an inherently multi-scale phenomenon, with much of the key material evolution occurring at the mesoscale. Current techniques for the direct interrogation of material property changes due to irradiation either function with very small volumes, such as in-situ TEM, cannot cover the full range of defect populations produced, such as in positron annihilation spectroscopy, or requires destruction of the test material, such as in standard or micromechanical testing. In addition, the ultimate quantities of interest to radiation materials scientists are the changes in key material properties with irradiation. These include stiffness, ductility, and thermal conductivity for structural materials, and optical properties such as index of refraction or changes in transmittance spectra for optically active materials. The latter of these are often correlated directly to stress- or thermally-induced changes, themselves a function of the specific defect populations responsible for their change. The rapid study of such a mesoscale phenomenon requires an inherently mesoscale technique, where multiple quantities of interest can be accurately measured in very short times. Determining the sensitivity of any technique with known certainly is of critical importance to qualifying a new technique to measure in-situ material property changes during irradiation. In this paper, we present the new applicability of an existing technique, known as transient grating (TG) spectroscopy, to rapidly and accurately study key problems in radiation materials science. Results quantifying the absolute sensitivity of the technique are presented, alongside molecular dynamics (MD) simulations of the TG spectroscopy process to gauge direct agreement between theory, simulation, and experiment. An example problem of interest is demonstrated as an illustration of what is possible, showing elastic and thermal changes in irradiated silicon carbide (SiC) films. Finally, future work to quantify the effects of experimentally-simulated radiation defects is proposed, in support of building a database to use TG spectroscopy to deconvolve irradiated material property changes in-situ in terms of the defect populations responsible for their evolution. The application of the TG spectroscopy technique to in-situ radiation materials science has the potential to answer long-standing questions in the field, relating to ion beam rastering, the onset of void swelling, and direct measurement of radiation-created point defect concentrations. Before it can do so, the technique must carefully be analyzed and tuned to increase its sensitivity, the certainty of its results, and the ability to predict radiation-induced changes by simulations must be developed. Making such measurements in-situ with the aid of predictive MD simulations has the potential to elucidate mechanisms of radiation damage accumulation, as well as more rapidly qualify radiation-resistant alloys for service in nuclear systems. Work is underway to build this database of experimentally-simulated radiation-produced defects, which will be combined and compared with actual irradiated materials for eventual in-situ deconvolution of the TG signal into the defect populations responsible for irradiation-induced microstructural change. (authors)

36 MATERIALS SCIENCE↗

A Raman cell based on hollow core photonic crystal fiber for human breath analysis

Purpose: Breath analysis has a potential prospect to benefit the medical field based on its perceived advantages to become a point-of-care, easy to use, and cost-effective technology. Early studies done by mass spectrometry show that volatile organic compounds from human breath can represent certain disease states of our bodies, such as lung cancer, and revealed the potential of breath analysis. But mass spectrometry is costly and has slow-turnaround time. The authors’ goal is to develop a more portable and cost effective device based on Raman spectroscopy and hollow core-photonic crystal fiber (HC-PCF) for breath analysis. Methods: Raman scattering is a photon-molecular interaction based on the kinetic modes of an analyte which offers unique fingerprint type signals that allow molecular identification. HC-PCF is a novel light guide which allows light to be confined in a hollow core and it can be filled with a gaseous sample. Raman signals generated by the gaseous sample (i.e., human breath) can be guided and collected effectively for spectral analysis. Results: A Raman-cell based on HC-PCF in the near infrared wavelength range was developed and tested in a single pass forward-scattering mode for different gaseous samples. Raman spectra were obtained successfully from reference gases (hydrogen, oxygen, carbon dioxide gases), ambient air, and a human breath sample. The calculated minimum detectable concentration of this system was ∼15 parts per million by volume, determined by measuring the carbon dioxide concentration in ambient air via the characteristic Raman peaks at 1286 and 1388 cm{sup −1}. Conclusions: The results of this study were compared to a previous study using HC-PCF to trap industrial gases and backward-scatter 514.5 nm light from them. The authors found that the method presented in this paper has an advantage to enhance the signal-to-noise ratio (SNR). This SNR advantage, coupled with the better transmission of HC-PCF in the near-IR than in the visible wavelengths led to an estimated seven times improvement in the detection sensitivity. The authors’ prototype device also demonstrated a 100-fold improvement over a recently reported detection limit of a reflective capillary fiber-based Raman cell for breath analysis. Continued development is underway to increase the detection sensitivity further to reach practical clinical applications.

60 APPLIED LIFE SCIENCES↗