Electric Field Assisted Sintering (EFAS, also referred to as spark plasma sintering) is a powerful technology for the consolidation of powder materials. The high heating rate during the sintering process is critical for minimizing energy consumption, but it can also cause microstructure heterogeneities in sintered parts, such as spatially varied porosity. The examination of localized porosity usually requires the use of a scanning electron microscope with a carefully prepared surface. In this paper, photothermal radiometry is used to measure local thermal diffusivity and extract localized porosity of EFAS-sintered parts by using a percolation-threshold model. Applying this approach, we identified the radial position-dependent porosity variation in EFAS parts, which is likely formed due to the large temperature gradient during the sintering process. This approach has a unique advantage because it can measure samples with minimal or no surface preparation, enabling the possibility of in situ characterization in EFAS with proper system modification. Necessary modifications on the measurement approach for EFAS deployment and in situ characterization are also discussed.

An experimental methodology using photothermal radiometry is developed for the accurate measurement of bulk thermal diffusivity of nuclear fuels and materials irradiated to high doses. Under these conditions, nuclear fuels, such as uranium oxide, and moderator materials, such as graphite, become friable, which requires characterization techniques that can accommodate irregularly shaped fragments. Photothermal radiometry, a good candidate for this application, involves locally heating a sample by using a laser and measuring the temperature field by monitoring blackbody radiation. The interaction volume for this study, less than a millimeter, is carefully chosen to sample a statistically significant number of large-scale structural features, such as pores and gas filled bubbles, and is small enough that the sample fragments can be treated as a thermal half-space. The thermal diffusivity standards considered in this study cover a range of thermal diffusivities representative of both fresh and spent nuclear fuels. We also consider a sample having a porous microstructure representative of large-scale structures found in materials irradiated to high doses. Our measurement methodology circumvents complex thermal wave models that address optical diffraction, nonlinear transfer function associated with blackbody radiation, and finite sample size effects. Consequently, the large measurement uncertainty associated with modeling these effects can be avoided. While the emphasis here is on nuclear fuels and materials, this measurement approach is well suited to measure thermal transport in a variety of technologically important materials associated with advanced synthesis techniques. Examples range from small, exotic single crystals grown using hydrothermal growth techniques to additively manufactured components having complex geometries.

We report on a laser-based square pulse thermoreflectance (SPTR) technique for the measurement of thermal properties for a wide range of materials. SPTR adopts the pump-probe thermoreflectance principle to monitor the evolution of local temperature after square pulse excitation. The technique features a compact setup, high spatial resolution, and fast data collection. By comparing the acquired SPTR signals with a continuum heat transfer model, material thermal properties can be obtained. Taking advantage of various spot sizes and modulation frequencies, SPTR can measure both the thermal diffusivity and thermal conductivity of poorly to moderately conductive materials and the thermal conductivity of conductive materials with satisfactory accuracy, with potential to be applied to more conductive materials. The technique was validated on three materials: fused silica, single crystal CaF 2 and single crystal nickel (with conductivities ranging from 1 W·m −1 ·K −1 to 100 W·m −1 ·K −1 ) with typical measurement errors of 5 % to 20 %. The leading sources of error have been identified by Monte Carlo simulations, and the primary limitations of SPTR are discussed. The compact, fiberized platform we describe here will allow instruments based on this methodology to be deployed in complex, multi-analytical environments for the type of high-throughput correlative analyses that are key to materials design and discovery.

Picosecond ultrasonics has been demonstrated on a tristructural isotropic (TRISO) fuel compact to measure the elastic properties of each compact layer. This technique utilizes an ultrashort pump laser pulse to excite vibrations in a gold transducer film covering the surface of each component and a second probe laser pulse to record the resulting acoustic strain induced change in optical reflectance. From the damping of this film vibration, the acoustic reflection coefficient, which couples the elastic properties of the transducer film and the sample, can be obtained, enabling a calculation of the sample's acoustic velocity and elastic modulus. Results obtained from this method are consistent with known values of elastic moduli, namely that the SiC coating is the stiffest component of the compact while the carbonaceous matrix is the most compliant. Nanoindentation was conducted as a benchmark technique on the same sample and shows satisfactory agreement with the results of picosecond ultrasonics. Compared to other methods like nanoindentation, picosecond ultrasonics is multimodal with a capability of measuring several key properties simultaneously and has potentials to be coupled into optical fibers for remote sensing. Thus, these demonstration measurements reveal the methodology to be a promising candidate for in-situ and high-throughput optical characterizations of nuclear materials. (C) 2021 Elsevier B.V. All rights reserved.

The thermal properties of tristructural isotropic (TRISO) particle coatings have been measured using laser based thermoreflectance methods from room temperature to 900 degrees C. At room temperature the pyrocarbon coatings have comparable thermal conductivities below 10 Wmiddotm(-1).K-1, whereas the SiC coating has a thermal conductivity around 90 W.(-1).K-1. The thermal diffusivities of all coatings display significant reduction with increasing temperature. The thermal conductivity of SiC decreases by more than 25% above 800 degrees C and the thermal conductivities of pyrocarbons increase moderately with the temperature, displaying similar changes to that of amorphous graphite at elevated temperatures. (C) 2022 Elsevier B.V. reseverd.

Laser-generated ultrasound was used to monitor microstructure evolution during thermal processing of as-cast, polycrystalline binary uranium-zirconium metallic fuel alloys with compositions of U-20wt.%Zr (U-20Zr), U-50wt.%Zr (U-50Zr) and U-80wt.%Zr (U-80Zr). Ultrasonic waveforms were recorded during heating and cooling the samples from room temperature to >973 K and back. A phase transition temperature for all three compositions was estimated from the temperature at which an abrupt and rapid reduction in ultrasonic velocities was observed. Microstructural features on the length scale of tens of micrometers were inferred from the observation of scattering of ultrasonic waves by elastic heterogeneities above ~823 K in U-20Zr, while a hysteresis in the ultrasonic velocities of U-80Zr upon cooling was attributed to a partial retention of the high temperature phase following thermal annealing. The U-50Zr alloy exhibited a reversible viscoelastic response above 933 K, as evidenced by the observation of high frequency attenuation of the shear component of the waveforms at high temperature. Ultrasonic measurements were supplemented by in situ transmission electron microscopy (TEM). The TEM images revealed that the δ-U-Zr matrix in the three compositions underwent a spinodal decomposition above ~823 K into nanoscale regions. The ultrasonic measurements revealed larger, micron-scale structure evolution in the U-20Zr alloy at the same temperature. This large-scale structure is associated with heterogeneous regions having different Zr content. Our findings show the potential heating rate dependence of microstructural evolution in U-Zr alloys and highlight differences in the thermomechanical response and associated length scales during thermal annealing between single- and dual-phase compositions. These results demonstrate the utility of laser ultrasonics to rapidly and efficiently scan phase boundaries and monitor micrometer-scale structure evolution in metallic fuel alloys.

Microstructure evolution due to irradiation in a nuclear reactor can have a dramatic effect on material properties. A better understanding of this evolution is necessary for developing improved nuclear fuels and materials. In the current scoping study we evaluate the influence of irradiation induced defects on the recrystallization temperature of a single component fuel surrogate.

Laser-based techniques have become an appealing option for determining the thermal diffusivities (D) and conductivities (k) of nuclear materials that would otherwise prove too hazardous or difficult to measure otherwise. These techniques have enabled non-destructive and non-contact thermal transport measurements with micron level spatial resolution. In this study, a new thermoreflectance technique known as square-pulse transient thermoreflectance (SPTR) is described and used to determine D values of both uranium sesquisilicide (U3Si2) and uranium nitride (UN) phases in a composite fuel. An extensive sensitivity analysis was conducted that identified the optimal measurement parameters of standard materials with a range of thermal transport properties comparable to those of various fuel types. The standards were measured using both SPTR as well as a spatial-domain thermoreflectance technique (SDTR). Several U3Si2 and UN phase regions of polished UN/U3Si2 (70/30 vol%) samples were measured using both methods, and the resulting calculated D and k values are reported, with both techniques showing excellent agreement between samples. Finally, the ability to use the technique for local diffusivity mapping was demonstrated over a multiphase region, and could be used to determine thermal transport properties in precipitates, secondary phases, and irradiation-damaged regions of postirradiated fuel samples. (C) 2019 Elsevier B.V. All rights reserved.

The safe and efficient operation of nuclear reactors require accurate knowledge of peak temperatures in the fuel assemblies. The temperature profiles are governed by the thermal transport properties of the fuel, namely the thermal conductivities (k) and thermal diffusivities (D). These properties can be very difficult to measure as they can vary considerably from the measured bulk values of the fresh fuel, and quickly degrade with increasing burnup [1-3]. Laser-based techniques have been effectively used for nondestructive and non-contact thermal transport measurements of a wide variety of materials, including nuclear materials [4-6] that would otherwise prove too hazardous or difficult to measure otherwise. In this study, a new thermoreflectance technique known as square-pulse transient thermoreflectance (SPTR) is

Microstructure evolution due to irradiation in a nuclear reactor can have a dramatic effect on material properties. A better understanding of this evolution is necessary for developing improved nuclear fuels and materials. The ability to measure such changes in real time is extremely challenging due to high temperatures, high radiation fields, and limited access of the reactor environment. Through carefully designed experiments, measurement of elastic properties can be tied directly to microstructure. We present an instrument that has been developed to monitor in-pile changes in grain microstructure. The measurement approach involves optically exciting and detecting flexural waves in a thin cantilever beam. An instrument capsule based on this technique was fabricated and underwent an irradiation test in the TREAT reactor in May 2019. Analyses of the test results are presented in this report. Scoping studies on the expected impact of radiation on similar tests are also presented.

the development of a bench-top photothermal radiometry (PTR) system to measure the thermal diffusivity of solid samples, and the preliminary design of a fiber-based PTR instrument to measure the real-time, in-pile thermal diffusivity of nuclear fuels. The PTR technique measures the local temperature response from a modulated heat source by detecting the sample radiation heat flux. Initially a well-developed thermal wave analytical model was fit to the data to obtain the thermal diffusivity. However, systematic errors from the diffraction effect and non-linearity issues resulted in thermal diffusivity measurements higher than literature values. These effects have been studied and an improved analytical model has been developed, and the physics behind the phenomena are still under investigation. A procedure for optimizing measurements from the bench-top system has been provided. The experiences from the bench top measurement were then used to guide the fiber-based system.

Under a Department of Energy Office of Nuclear Energy (DOE-NE) initiative to develop in-pile instrumentation, an activity has been initiated to develop an infrared thermography (IRT) approach for in-reactor monitoring of fuel behaviors. The project will focus on leveraging mature, mainstream IRT techniques for use on nuclear fuel systems inside a nuclear reactor through unique adaptations for remote applications – an extremely challenging engineering and measurement objective – never before accomplished in-pile. To this end, some of the most important issues to be addressed include identifying an optimal IRT configuration (of many possible) and components for detecting specific structural evolutions such as fuel cracking and fuel void formation and migration; developing a long distance imaging system to transmit high resolution infrared images from a small specimen surface in the harsh environment of a reactor core to a IR camera or other detector array; and ultimately, integrating a complete experimental system to create a full in-reactor experiment. This document provides an overview of potential in-pile applications of IRT, a brief overview of IRT techniques, a detailed research plan and schedule for the project, and a summary of activities that have been initiated in the closing months of fiscal year 2017.

The scope of the FY17 milestone involved entering the TCM into stage one mockup at the Materials and Fuels Complex (MFC) and completing initial testing. While the TCM head was designed and partially fabricated in FY16, the ancillary equipment and software for standalone operation at the IMCL still required development. The tasks required to prepare the TCM for stage one mockup included: 1 – develop cell feedthroughs for both optical and electrical signals, 2 – design and construction of a film thickness monitor, 3 – drafting an equipment qualification plan, 4 – develop an integrated equipment rack to house lasers and instrumentation, and 5 – develop coding instrumentation software for controlling the TCM.

Simultaneous measurement of local thermal diffusivity and conductivity is demonstrated on a range of ceramic samples. This was accomplished by measuring the temperature field spatial profile of samples excited by an amplitude modulated continuous wave laser beam. A thin gold film is applied to the samples to ensure strong optical absorption and to establish a second boundary condition that introduces an expression containing the substrate thermal conductivity. The diffusivity and conductivity are obtained by comparing the measured phase profile of the temperature field to a continuum based model. A sensitivity analysis is used to identify the optimal film thickness for extracting the both substrate conductivity and diffusivity. Proof of principle studies were conducted on a range of samples having thermal properties that are representatives of current and advanced accident tolerant nuclear fuels. It is shown that by including the Kapitza resistance as an additional fitting parameter, the measured conductivity and diffusivity of all the samples considered agreed closely with the literature values. A distinguishing feature of this technique is that it does not require a priori knowledge of the optical spot size which greatly increases measurement reliability and reproducibility.

The US Department of Energy sponsors the Advanced Test Reactor (ATR) National Scientific User Facility (NSUF) program to promote U.S. research in nuclear science and technology. By attracting new research users - universities, laboratories, and industry - the ATR NSUF facilitates basic and applied nuclear research and development, advancing U.S. energy security needs. A key component of the ATR NSUF effort is to design, develop, and deploy new in-pile instrumentation techniques that are capable of providing real-time measurements of key parameters during irradiation. This paper describes the strategy developed by the Idaho National Laboratory (INL) for identifying instrumentation needed for ATR irradiation tests and the program initiated to obtain these sensors. New sensors developed from this effort are identified; and the progress of other development efforts is summarized. As reported in this paper, INL staff is currently involved in several tasks to deploy real-time length and flux detection sensors, and efforts have been initiated to develop a crack growth test rig. Tasks evaluating 'advanced' technologies, such as fiber-optics based length detection and ultrasonic thermometers are also underway. In addition, specialized sensors for real-time detection of temperature and thermal conductivity are not only being provided to NSUF reactors, but are also being provided to several international test reactors.

A laser ultrasonic source just below the ablation regime is examined by recording an epicentral waveform in a high purity tungsten sample. Using pulse energy as a parameter, a slight delay in the shear wave arrival time is observed upon transition to the melting regime. This phenomenon is attributed to a change in character of the ultrasonic source. In the thermoelastic regime, shear waves are generated by mode conversion at the sample surface of longitudinal waves emanating from subsurface sources. Just above the melting threshold, a molten pool forms in the center of the generation volume. Shear waves are not supported by the molten pool. As a result, shear waves generated from off-axis thermoelastic sources are weighted more heavily. This results in a delay of the shear wave arrival time.

In-reactor measurement of material properties is required for a better understanding of radiation effects on materials. We present an optical fiber based technique for measuring changes in elastic properties which involves exciting and measuring flexural vibrations in a thin cantilever beam. By exciting the beam and measuring the resonant frequency, changes in the modulus of elasticity can be monitored. The technique is demonstrated by monitoring the elastic property changes of a beam fabricated from copper, as the copper undergoes recrystallization at elevated temperature.

A photothermal technique capable of measuring thermal conductivity with micrometer lateral resolution is presented. This technique involves measuring separately the thermal diffusivity, D, and thermal effusivity, e, to extract the thermal conductivity, k = (e2/D)1/2. To generalize this approach, sensitivity analysis is conducted for materials having a range of thermal conductivities. Application to nuclear fuel is consider by performing experimental validation using two materials (CaF2 and SiO2) having thermal properties representative of fresh and high burnup nuclear fuel. The measured conductivities compare favorably with literature values.

This paper describes the first noncontact elastic vibration measurements of an object in a high gamma radiation field. Using a laser-coupled resonant ultrasound technique, the vibration modes of an Inconel hollow capped cylinder were measured as the gamma radiation field was increased to 10(4) Gy/h. This measurement technique allowed shifts in the resonant frequency of the sample's vibration modes to be tracked over a 170-h period. The vibration mode frequencies changed in a manner consistent with the temperature dependence of the elastic stiffness coefficients of the material. These results demonstrate the efficacy of the laser approach for real-time resonant ultrasound measurements in this severely hostile nuclear environment.

Two-photon excited emission centered at 379–426 nm in photodarkening borosilicate glass doped with CuCl nanocrystalline quantum dots at room temperature has been observed. The emission is detected in the direction of the fundamental near-infrared beam. Time- and frequency-resolved measurements at room temperature and 77 K indicate that the emission is largely coherent light characteristic of second harmonic generation (SHG). An average conversion efficiency of ∼10−10 is obtained for a 2 mm thick sample. The observed SHG can originate in the individual noncentrosymmetric nanocrystals, leading to a bulk-like contribution, and at the nanocrystal-glass interface, leading to a surface contribution. The bulk-like conversion efficiency is estimated using previously reported values of coherence length (5μm) and bulk nonlinear susceptibility. This bulk-like conversion efficiency estimate is found to be smaller than the measured value, suggesting a more prominent surface contribution.