Louis J. Santodonato

Flexible sample environment for high resolution neutron imaging at high temperatures in controlled atmosphere

High material penetration by neutrons allows for experiments using sophisticated sample environments providing complex conditions. Thus, neutron imaging holds potential for performing in situ nondestructive measurements on large samples or even full technological systems, which are not possible with any other technique. This paper presents a new sample environment for in situ high resolution neutron imaging experiments at temperatures from room temperature up to 1100 °C and/or using controllable flow of reactive atmospheres. The design also offers the possibility to directly combine imaging with diffraction measurements. Design, special features, and specification of the furnace are described. In addition, examples of experiments successfully performed at various neutron facilities with the furnace, as well as examples of possible applications are presented. This covers a broad field of research from fundamental to technological investigations of various types of materials and components.

A new apparatus design for high temperature (up to 950 °C) quasi-elastic neutron scattering in a controlled gaseous environment

A design for a sample cell system suitable for high temperature Quasi-Elastic Neutron Scattering (QENS) experiments is presented. The apparatus was developed at the Spallation Neutron Source in Oak Ridge National Lab where it is currently in use. The design provides a special sample cell environment under controlled humid or dry gas flow over a wide range of temperature up to 950 °C. Using such a cell, chemical, dynamical, and physical changes can be studied in situ under various operating conditions. While the cell combined with portable automated gas environment system is especially useful for in situ studies of microscopic dynamics under operational conditions that are similar to those of solid oxide fuel cells, it can additionally be used to study a wide variety of materials, such as high temperature proton conductors. The cell can also be used in many different neutron experiments when a suitable sample holder material is selected. The sample cell system has recently been used to reveal fast dynamic processes in quasi-elastic neutron scattering experiments, which standard probes (such as electrochemical impedance spectroscopy) could not detect. In this work, we outline the design of the sample cell system and present results demonstrating its abilities in high temperature QENS experiments.

Characterization of Crystallographic Structures Using Bragg-Edge Neutron Imaging at the Spallation Neutron Source

Over the past decade, wavelength-dependent neutron radiography, also known as Bragg-edge imaging, has been employed as a non-destructive bulk characterization method due to its sensitivity to coherent elastic neutron scattering that is associated with crystalline structures. Several analysis approaches have been developed to quantitatively determine crystalline orientation, lattice strain, and phase distribution. In this study, we report a systematic investigation of the crystal structures of metallic materials (such as selected textureless powder samples and additively manufactured (AM) Inconel 718 samples), using Bragg-edge imaging at the Oak Ridge National Laboratory (ORNL) Spallation Neutron Source (SNS). Firstly, we have implemented a phenomenological Gaussian-based fitting in a Python-based computer called iBeatles. Secondly, we have developed a model-based approach to analyze Bragg-edge transmission spectra, which allows quantitative determination of the crystallographic attributes. Moreover, neutron diffraction measurements were carried out to validate the Bragg-edge analytical methods. These results demonstrate that the microstructural complexity (in this case, texture) plays a key role in determining the crystallographic parameters (lattice constant or interplanar spacing), which implies that the Bragg-edge image analysis methods must be carefully selected based on the material structures.

Spontaneous imbibition of water and determination of effective contact angles in the Eagle Ford Shale Formation using neutron imaging

Understanding of fundamental processes and prediction of optimal parameters during the horizontal drilling and hydraulic fracturing process results in economically effective improvement of oil and natural gas extraction. Although modern analytical and computational models can capture fracture growth, there is a lack of experimental data on spontaneous imbibition and wettability in oil and gas reservoirs for the validation of further model development. In this work, we used neutron imaging to measure the spontaneous imbibition of water into fractures of Eagle Ford shale with known geometries and fracture orientations. An analytical solution for a set of nonlinear second-order differential equations was applied to the measured imbibition data to determine effective contact angles. The analytical solution fit the measured imbibition data reasonably well and determined effective contact angles that were slightly higher than static contact angles due to effects of in-situ changes in velocity, surface roughness, and heterogeneity of mineral surfaces on the fracture surface. Additionally, small fracture widths may have retarded imbibition and affected model fits, which suggests that average fracture widths are not satisfactory for modeling imbibition in natural systems.

In-Situ Imaging of Liquid Phase Separation in Molten Alloys Using Cold Neutrons

Understanding the liquid phases and solidification behaviors of multicomponent alloy systems becomes difficult as modern engineering alloys grow more complex, especially with the discovery of high-entropy alloys (HEAs) in 2004. Information about their liquid state behavior is scarce, and potentially quite complex due to the presence of perhaps five or more elements in equimolar ratios. These alloys are showing promise as high strength materials, many composed of solid-solution phases containing equiatomic CoCrCu, which itself does not form a ternary solid solution. Instead, this compound solidifies into highly phase separated regions, and the liquid phase separation that occurs in the alloy also leads to phase separation in systems in which Co, Cr, and Cu are present. The present study demonstrates that in-situ neutron imaging of the liquid phase separation in CoCrCu can be observed. The neutron imaging of the solidification process may resolve questions about phase separation that occurs in these alloys and those that contain Cu. These results show that neutron imaging can be utilized as a characterization technique for solidification research with the potential for imaging the liquid phases of more complex alloys, such as the HEAs which have very little published data about their liquid phases. This imaging technique could potentially allow for observation of immiscible liquid phases becoming miscible at specific temperatures, which cannot be observed with ex-situ analysis of solidified structures.

Investigation of a Lithium Indium Diselenide detector for neutron transmission imaging

The development of a thermal neutron imaging sensor constructed with semiconducting lithium indium diselenide is presented. Both a computational and experimental investigation were conducted. In the computational investigation, it is shown that the imaging potential of Lithium Indium Diselenid (LISe) is excellent, even when using a large pixel pitch through the use of super sampling. In the experimental investigation, it was found that a single pixel LISe detector using detector super sampling shows a spatial variation in the count rate, which is a clear sign of imaging capability. However, a good image was not obtained in the first experiment and may be caused by a variety of experimental conditions. Finally, a search is still underway to find a suitable contact metal with good mechanical adhesion for wedge bonding.

Feasibility Study of Making Metallic Hybrid Materials Using Additive Manufacturing

A metallic hybrid structure, consisting of an Inconel-718 matrix and a Co-Cr internal structure, was successfully manufactured using laser direct energy deposition process. Characterizations were performed using energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), neutron-computed tomography (nCT), and electron back-scatter diffraction (EBSD) to verify the interfaces between Co-rich and Ni-rich phases. nCT revealed the internal structures to be continuous without cracking or significant intermixing due to inter-diffusion of Co and Ni (i.e., dissolved boundaries between the two structures). Minor porosity was detected. EBSD confirmed a good bond at the granular level. No precipitate phases were detected with XRD. EDS revealed dilution/intermixing between the Co and Ni interfaces presumably due to melt-pool overlay between the matrix and the internal structures.

Advanced Characterization Techniques

This chapter first provides a brief introduction to some advanced microstructure characterization tools, such as three-dimensional (3D) atom probe tomography, high-resolution transmission electron microscopy, and neutron scattering. Applications of these techniques to characterize high-entropy alloys (HEAs) are illustrated in model alloys. Utilization of these advanced techniques can provide extremely useful structural and chemical information at the nanoscale. For example, the identification of nano-twins in the fracture-toughness crack region of an HEA may explain the anomalous increases in strength and ductility at cryogenic temperatures. Another striking feature of HEAs is the large local strain among neighboring atoms, which, in general, are arranged in a crystal structure with long-range order. Our understanding of these types of features, and their effect on material properties, will increase as the microstructural characterization techniques described here are further developed and applied to HEA research.

TEMPERATURE CONTROL DIAGNOSTICS FOR SAMPLE ENVIRONMENTS

In a scientific laboratory setting, standard equipment such as cryocoolers are often used as part of a custom “sample environment” system designed to regulate temperature over a wide range. The end user may be more concerned with precise sample temperature control than with base temperature. Cryogenic systems, however, tend to be specified mainly in terms of cooling capacity and base temperature. Technical staff at scientific user facilities (and perhaps elsewhere) often wonder how to best specify and evaluate temperature control capabilities. Here we describe test methods and give results obtained at a user facility that operates a large sample environment inventory. Although this inventory includes a wide variety of temperature, pressure, and magnetic field devices, the present work focuses on cryocooler‐based systems.