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Grain Boundary Plane Measurement Using Transmission Electron Microscopy Automated Crystallographic Orientation Mapping for Atom Probe Tomography Specimens

Abstract Grain boundaries are critical in determining the properties of materials, including mechanical stability, conductivity, and corrosion resistance. The specific properties of materials depend not only on the misorientation of the crystals, the three most commonly characterized parameters, but also on the angle of the grain boundary plane between the two crystals, the final two parameters in the five-parameter macroscopic description of the grain boundary. The method presented here allows for the direct measurement of all five parameters of the grain boundary in a transmission electron microscopy specimen of various morphologies. This is especially applicable to atom probe specimens, where only a single-tilt axis is generally available, allowing the crystallographic description to be matched to the detailed chemical data available in the atom probe tomography. This method provides a platform for efficient grain boundary analysis in unique samples, saving operator time and allowing for ease of acquisition and interpretation in comparison with traditional electron diffraction methods.

Materials Science↗

Orientation mapping of semicrystalline polymers using scanning electron nanobeam diffraction

Here, we demonstrate a scanning electron nanobeam diffraction technique that can be used for mapping the size and distribution of nanoscale crystalline regions in a polymer blend. In addition, it can map the relative orientation of crystallites and the degree of crystallinity of the material. The model polymer blend is a 50:50 w/w mixture of semicrystalline poly(3-hexylthiophene-2,5-diyl) (P3HT) and amorphous polystyrene (PS). The technique uses a scanning electron beam to raster across the sample and acquires a diffraction image at each probe position. Through image alignment and filtering, the diffraction image dataset enables mapping of the crystalline regions within the scanned area and construction of an orientation map.

36 MATERIALS SCIENCE↗

Automated Crystal Orientation Mapping in py4DSTEM using Sparse Correlation Matching

Crystalline materials used in technological applications are often complex assemblies composed of multiple phases and differently oriented grains. Robust identification of the phases and orientation relationships from these samples is crucial, but the information extracted from the diffraction condition probed by an electron beam is often incomplete. We have developed an automated crystal orientation mapping (ACOM) procedure which uses a converged electron probe to collect diffraction patterns from multiple locations across a complex sample. We provide an algorithm to determine the orientation of each diffraction pattern based on a fast sparse correlation method. We demonstrate the speed and accuracy of our method by indexing diffraction patterns generated using both kinematical and dynamical simulations. We have also measured orientation maps from an experimental dataset consisting of a complex polycrystalline twisted helical AuAgPd nanowire. From these maps we identify twin planes between adjacent grains, which may be responsible for the twisted helical structure. All of our methods are made freely available as open source code, including tutorials which can be easily adapted to perform ACOM measurements on diffraction pattern datasets.

36 MATERIALS SCIENCE↗

Nano-scale orientation mapping of graphite in cast irons

A diametrical section of a graphite spheroid from a ductile iron sample was prepared using the focused ion beam-lift out technique. Characterization of this section was carried out through automated crystal orientation mapping in a transmission electron microscope. This new technique automatically collects electron diffraction patterns and matches them with precalculated templates. The results of this investigation are crystal orientation and phase maps of the specimen, which bring new light to the understanding of growth mechanisms of this peculiar graphite morphology. This article shows that mapping the orientation of carbon-based materials such as graphite, which is difficult to achieve with conventional techniques, can be performed automatically and at high spatial resolution using automated crystal orientation mapping in a transmission electron microscope. - Highlights: • ACOM/TEM can be used to study the crystal orientation of carbon-based materials. • A spheroid is formed by conical sectors radiating from a central nuclei. • Misorientations exist within the conical sectors, defining various orientation domains.

36 MATERIALS SCIENCE↗

Point-group sensitive orientation mapping of non-centrosymmetric crystals

We demonstrate polarity-sensitive orientation mapping of non-centrosymmetric phases by Electron Backscatter Diffraction (EBSD). The method overcomes the restrictions of kinematic orientation determination by EBSD, which is limited to the centro-symmetric Laue-groups according to Friedel's rule. Using polycrystalline GaP as an example, we apply a quantitative pattern matching approach based on simulations using the dynamical theory of electron diffraction. This procedure results in a distinct assignment of the local orientation according to the non-centrosymmetric point group of the crystal structure under investigation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Comparison of Orientation Mapping in SEM and TEM

In this work, multiple experimental configurations for performing nanoscale orientation mapping are compared to determine their fidelity to the true 3D microstructure of a sample. Transmission Kikuchi Diffraction (TKD) experiments in an SEM and nanobeam diffraction (NBD) experiments in a TEM were performed on thin electrodeposited hard Au films with two different microstructures. The Au samples either have a grain size that is >50 nm or <20 nm. The same regions of the samples were measured with TKD apparatuses at 30 kV in an SEM with detectors in the horizontal and vertical configurations and in the TEM at 300 kV. Under the proper conditions, we demonstrate all three configurations can produce data of equivalent quality.Each method has strengths and challenges associated with its application and representation of the true microstructure. The conditions needed to obtain high-quality data for each acquisition method and the challenges associated with each will be discussed.

36 MATERIALS SCIENCE↗

Energy-resolved neutron imaging and diffraction including grain orientation mapping using event camera technology

Time-of-flight neutron diffraction and energy-resolved imaging each provide unique perspectives into material properties. Neutron diffraction is useful for assessing microstructural parameters such as phase composition, texture, and dislocation densities, though it typically provides averaged data over the sampled volume. Energy-resolved imaging, on the other hand, offers both spatial and spectral information by detecting Bragg edges and neutron absorption resonances, which enables detailed mapping of microstructure and isotopic composition. When combined, these techniques have the potential to enrich our understanding of material behavior across different scales, enhancing our understanding of complex materials. Traditionally, these modalities are conducted on separate instruments, which is time-consuming and poses challenges for data integration. Here, we report the integration of the LumaCam, an event-mode energy-resolved neutron imaging camera with the HIPPO time-of-flight diffractometer at LANSCE. This integration enables simultaneous diffraction and imaging across the full spectrum, with analysis optimized for diffraction and Bragg-edge imaging in the thermal range (0.45–10 Å) and resonance imaging in the epithermal range (0.5–3000 eV), facilitating comprehensive multi-modal analysis. We demonstrate its capabilities through case studies, including spatial mapping of grain orientations in a steel sample and accurate thickness estimations for irregular samples including a depleted uranium cylinder and a natural silver-containing mineral specimen. The combined setup enhances real-time sample alignment and provides comprehensive data for crystal structure, texture, and isotopic composition analysis. This approach opens new possibilities for advanced applications in nuclear engineering, archaeology, and materials science.

36 MATERIALS SCIENCE↗

High-resolution 3D strain and orientation mapping within a grain of a directed energy deposition laser additively manufactured superalloy

The industrialization of Laser Additive Manufacturing (LAM) is challenged by the undesirable microstructures and high residual stresses originating from the fast and complex solidification process. Non-destructive assessment of the mechanical performance controlling deformation patterning is therefore critical. Here, we use Dark Field X-ray Microscopy (DFXM) to map the 3D subsurface intragranular orientation and strain variations throughout a surface-breaking grain within a directed energy deposition nickel superalloy. DFXM results reveal a highly heterogenous 3D microstructure in terms of the local orientation and lattice strain. The grain comprises ≈ 5 μm-sized cells with alternating strain states, as high as 5 x10 -3 , and orientation differences <0.5°. The DFXM results are compared to Electron Backscatter Diffraction measurements of the same grain from its cut-off surface. Here, we discuss the microstructure developments during LAM, rationalising the development of the deformation patterning from the extreme thermal gradients during processing and the susceptibility for solute segregation.

36 MATERIALS SCIENCE↗

Orbital orientation mapping of V 2 O 5 thin films

We report the effects of growth methods on the orbital orientation in vanadium pentoxide (V 2 O 5 ) thin films, an important factor to consider when selecting growth techniques for highly selective catalysts and devices. Thermal evaporation and sol-gel methods were used to synthesize the V 2 O 5 films. The surface morphology, roughness, and orientation of the films were characterized by atomic force microscopy and x-ray diffraction. Surface electronic properties and oxidation states were assessed by x-ray photoemission spectroscopy. Polarized x-ray absorption spectroscopy demonstrated that the thermally evaporated film [which was in the (001) orientation] exhibited greater anisotropy than the (100) oriented sol-gel film. The observed increase in anisotropy agrees well with computational findings which revealed that more vanadyl bonds are present at the surface of the thermally evaporated film than at the surface of the sol-gel film. The same computational study also found that the orientation of these bonds is more parallel to the film surface in the thermally evaporated film than in the sol-gel film. Finally, the data suggest that the method of growth may be used as a controlled variable to select key film characteristics for potential applications.

36 MATERIALS SCIENCE↗

Composition and automated crystal orientation mapping of rapid solidification products in hypoeutectic Al-4 at.%Cu alloys

Rapid solidification can produce metastable phases and unusual microstructure modifications in multi-component alloys during additive manufacturing or laser beam welding. Composition and phase mapping by transmission electron microscopy have been used in this paper to characterize the morphologically distinct zones developing in hypoeutectic Al-4 at.% Cu alloy after pulsed laser melting for different crystal growth rate regimes. Deviations of the compositions of the alloy phases from equilibrium predictions and unique orientation relationships between the solidification transformation products have been determined. Specifically, for the columnar growth zone at solidification rates of 0.8 m s - 1 < v < v a = 1.8 m s - 1 , two distinct orientation relationships were established between the concomitantly forming non-equilibrium phases, supersaturated α-Al solid solution and the discontinuously distributed α-Al 2 Cu-based θ'-phase, which can be described as {110} θ ∥ {001} α , [001] θ ∥ [110] α and {001} θ ∥ {001} α , [100] θ ∥ [100] α . These orientation relationships permit formation of coherent interphase interfaces with low interfacial free energy. Finally, this endows a kinetic advantage to the thermodynamically less stable θ'-Al 2 Cu phase relative to the more stable equilibrium θ-Al 2 Cu phase during formation of the morphologically modified eutectic of the columnar growth zone grains, since repeated nucleation is required to establish the discontinuous distribution of θ'-Al 2 Cu phase.

36 MATERIALS SCIENCE↗

Identifying Disadvantaged Communities in the United States: An Energy-Oriented Mapping Tool that Aggregates Environmental and Socioeconomic Burdens

This paper defines a policy-relevant nationwide composite index to identify communities disproportionately impacted by environmental, energy, and climate injustices in the United States. We review existing vulnerability indicators and indices to assess the tradeoffs of different design parameters, including variable selection, geographic unit, dimensionality reduction, weighting, and aggregation methods. From this methodological review, we create the first nationwide, census tract-level index of cumulative burden that includes energy-relevant indicators alongside climate, social, environmental, and economic indicators, and is flexible to the inclusion of additional data sources. We provide a summary of the sources of inputs used to develop a definition for "disadvantaged communities" that can be used to prioritize energy investments. We discuss use-cases for this index including the implementation of the Justice40 Initiative, which calls for 40% of certain federal clean energy benefits to flow to disadvantaged communities in the United States. We use our results to examine historic allocations of federal energy investments and show that communities that we identify as disadvantaged received about 37% fewer funds per capita than non-disadvantaged communities.

cumulative burden↗