Quantitative x-ray microanalysis in an AEM: instrumental considerations and applications to materials science

There are a wide variety of instrumental problems which are present to some degree in all AEM instruments. The nature and magnitude of these artifacts can in some instances preclude the simple quantitative interpretation of the recorded x-ray emission spectrum using a thin-film electron excitation model; however, by judicious modifications to the instrument these complications can be effectively eliminated. The specific operating conditions of the microscope necessarily vary from one analysis to another depending on the type of specimen and experiment being performed. In general, however, the overall performance of the AEM system during x-ray analysis is optimized using the highest attainable incident electron energy; selecting the maximum probe diameter and probe current consistent with experimental limitations; and positioning the x-ray detector in a geometry such that it records information from the electron entrance surface of the specimen

Nanometer-scale sharpness in corner-overgrown heterostructures

A corner-overgrown GaAs/AlGaAs heterostructure is investigated with transmission and scanning transmission electron microscopy, demonstrating self-limiting growth of an extremely sharp corner profile of 3.5 nm width. In the AlGaAs layers we observe self-ordered diagonal stripes, precipitating exactly at the corner, which are regions of increased Al content measured by an XEDS analysis. A quantitative model for self-limited growth is adapted to the present case of faceted MBE growth, and the corner sharpness is discussed in relation to quantum confined structures. We note that MBE corner overgrowth maintains nm-sharpness even after microns of growth, allowing the realization of corner-shaped nanostructures.Comment: 4 pages, 3 figure

Precise determination of atom configuration in partially disordered spinel compounds by HARECSX.

Electron channeling enhanced x-ray spectroscopy has been being widely used to determine ordered arrangement of component atoms in multinary inorganic or metallic crystals. Recent theoretical advancements in the modeling of characteristic x-ray emission by inelastic scattering of incident electrons under dynamical diffraction conditions has achieved remarkable progress, and it has enabled scientists to analyze the experimental intensity of x-ray emission in precise detail. In this study, the ion configuration in magnesium aluminate spinel (MgO{center_dot}nAl{sub 2}O{sub 3}) has been examined by measurements of characteristic x-ray emission as a function of incident electron beam direction at high angular resolution, a technique which we have termed HARECXS (high angular resolution electron channeling x-ray spectroscopy). This paper reports the results and emphasizes the applicability of HARECXS to partially disordered materials

HVEM-Tandem and EELS study of radiation damage in zirconolite

Zirconolite (CaZrTi{sub 2}O{sub 7}) is the major host phase for actinides in Synroc, a promising waste form for the immobilization of high-level radioactive waste. The effect of radiation damage on the structure and durability of zirconolite are important to predictive modeling of zirconolite`s behavior in the repository environment and risk assessment. In this study, radiation damage effects in zirconolite were investigated by irradiating samples with 1.5 MeV Kr{sup +} ions using the HVEM-Tandem at Argonne National Laboratory (ANL) and energy loss electron spectroscopy (EELS). The HVEM-Tandem consists of a modified AEI high voltage transmission electron microscope interfaced to a 2 MV tandem ion accelerator. EELS spectra were collected using a Philips 420 TEM, operated at 120 kV, fitted with a Gatan Model 607 Serial EELS. EELS data were recorded at resolutions of {approximately} 1.0 eV and at a dispersion of about {approximately} 0.25 eV. Selected area diffraction patterns (SADs) of individual grains of various zirconolites were monitored as a function of dose to establish the critical dose for amorphization (D{sub c}). The authors found that (1) D{sub c}(zirconolite) is independent of the atomic weight of dopants in zirconolite and the mean atomic weight of the sample and that (2) the Bragg reflections in SAD patterns which persist to the highest doses are firstly those resulting from the fluorite sublattice and secondly the four (110)-type reflections which lie on the innermost of the two diffuse rings representative of amorphous zirconolite

Temperature Dependence of Ion Irradiation Induced Amorphization of Zirconolite

Zirconolite is one of the major host phases for actinides in various wasteforms for immobilizing high level radioactive waste (HLW). Over time, zirconolite's crystalline matrix is damaged by {alpha}-particles and energetic recoil nuclei recoil resulting from {alpha}-decay events. The cumulative damage caused by these particles results in amorphization. Data from natural zirconolites suggest that radiation damage anneals over geologic time and is dependant on the thermal history of the material. Proposed HLW containment strategies rely on both a suitable wasteform and geologic isolation. Depending on the waste loading, depth of burial, and the repository-specific geothermal gradient, burial could result in a wasteform being exposed to temperatures of between 100--450 C. Consequently, it is important to assess the effect of temperature on radiation damage in synthetic zirconolite. Zirconolite containing wasteforms are likely to be hot pressed at or below 1,473 K (1,200 C) and/or sintered at or below 1,623 K (1,350 C). Zirconolite fabricated at temperatures below 1,523 K (1,250 C) contains many stacking faults. As there have been various attempts to link radiation resistance to structure, the authors decided it was also pertinent to assess the role of stacking faults in radiation resistance. In this study, they simulate {alpha}-decay damage in two zirconolite samples by irradiating them with 1.5 MeV Kr{sup +} ions using the High Voltage Electron Microscope-Tandem User Facility (HTUF) at Argonne National Laboratory (ANL) and measure the critical dose for amorphization (D{sub c}) at several temperatures between 20 and 773 K. One of the samples has a high degree of crystallographic perfection, the other contains many stacking faults on the unit cell scale. Previous authors proposed a model for estimating the activation energy of self annealing in zirconolite and for predicting the critical dose for amorphization at any temperature. The authors discuss their results and earlier published data in relation to that model

Temperature dependence of ion irradiation induced amorphization of zirconolite

Zirconolite is one of the major host phases for actinides in various wasteforms for immobilizing high level radioactive waste (HLW). Over time, zirconolite's crystalline matrix is damaged by {alpha}-particles and energetic recoil nuclei recoil resulting from {alpha}-decay events. The cumulative damage caused by these particles results in amorphization. Data from natural zirconolites suggest that radiation damage anneals over geologic time and is dependant on the thermal history of the material. Proposed HLW containment strategies rely on both a suitable wasteform and geologic isolation. Depending on the waste loading, depth of burial, and the repository-specific geothermal gradient, burial could result in a wasteform being exposed to temperatures of between 100--450 C. Consequently, it is important to assess the effect of temperature on radiation damage in synthetic zirconolite. Zirconolite containing wasteforms are likely to be hot pressed at or below 1,473 K (1,200 C) and/or sintered at or below 1,623 K (1,350 C). Zirconolite fabricated at temperatures below 1,523 K (1,250 C) contains many stacking faults. As there have been various attempts to link radiation resistance to structure, the authors decided it was also pertinent to assess the role of stacking faults in radiation resistance. In this study, they simulate {alpha}-decay damage in two zirconolite samples by irradiating them with 1.5 MeV Kr{sup +} ions using the High Voltage Electron Microscope-Tandem User Facility (HTUF) at Argonne National Laboratory (ANL) and measure the critical dose for amorphization (D{sub c}) at several temperatures between 20 and 773 K. One of the samples has a high degree of crystallographic perfection, the other contains many stacking faults on the unit cell scale. Previous authors proposed a model for estimating the activation energy of self annealing in zirconolite and for predicting the critical dose for amorphization at any temperature. The authors discuss their results and earlier published data in relation to that model

Beam-broadening effects in STEM/EDS measurement of radiation-induced segregation in high-purity 304L stainless steel

Radiation-induced segregation (RIS) is the spatial redistribution of elements at defect sinks such as grain boundaries and free surfaces during irradiation. This phenomenon has been studied in a wide variety of alloys and has been linked to irradiation-assisted stress corrosion cracking (IASCC) of nuclear reactor core components. Therefore, accurate determination of the grain boundary composition is important in understanding its effects on environmental cracking. Radiation-induced segregation profiles are routinely measured by scanning-transmission electron microscopy using energy-dispersive X-ray spectroscopy (STEM-EDS) and Auger electron spectroscopy (AES). Because of the narrow width of the segregation profile (typically less than 10-nm full width at half-maximum), the accuracy of grain boundary concentration measurements using STEM/EDS depends on the characteristics of the analyzing instrument, specifically, the excited volume in which x-rays are generated. This excited volume is determined by both electron beam diameter and the primary electron beam energy. Increasing the primary beam energy in STEM/EDS produces greater measured grain boundary segregation, as the reduced electron beam broadening a smaller excited volume. In this work, the effect of beam broadening is assessed on segregation measurements in a 304L stainless steel sample irradiated with 3.2 MeV protons at 400 C to doses of 3.0 and 0.1 dpa. The STEM/EDS measurements are also compared to measurements made using AES

Future Science Needs and Opportunities for Electron Scattering: Next-Generation Instrumentation and Beyond. Report of the Basic Energy Sciences Workshop on Electron Scattering for Materials Characterization, March 1-2, 2007

To identify emerging basic science and engineering research needs and opportunities that will require major advances in electron-scattering theory, technology, and instrumentation

Irradiation-assisted stress corrosion cracking of austenitic stainless steels: Recent progress and new approaches

Irradiation-assisted stress corrosion cracking (IASCC) of several types of BWR field components fabricated from solution-annealed austenitic stainless steels (SSs), including a core internal weld, were investigated by means of slow-strain-rate test (SSRT), scanning electron microscopy (SEM), Auger electron spectroscopy (AES), and field-emission-gun advanced analytical electron microscopy (FEG-AAEM). Based on the results of the tests and analyses, separate effects of neutron fluence, tensile properties, alloying elements and major impurities identified in the American Society for Testing and Materials (ASTM) specifications, minor impurities, water chemistry, and fabrication-related variables were determined. The results indicate strongly that minor impurities not specified by the ASTM-specifications play important roles, probably through a complex synergism with grain-boundary Cr depletion. These impurities, typically associated with steelmaking and component fabrication processes, are very low or negligible in solubility in steels and are the same impurities that have been known to promote intergranular SCC significantly when they are present in water as ions or soluble compounds. It seems obvious that IASCC is a complex integral problem which involves many variables that are influenced strongly by not only irradiation conditions, water chemistry, and stress but also iron and steelmaking processes, fabrication of the component, and joining and welding. Therefore, for high-stress components in particular, it would be difficult to mitigate IASCC problems at high fluence based on the consideration of water chemistry alone, and other considerations based on material composition and fabrication procedure would be necessary as well