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Synchrotron radiation spectromicroscopy provides a combination of submicron spatial resolution and chemical sensitivity that is well-suited to analysis of heterogeneous nuclear materials. The chemical and physical characteristics determined by scanning transmission X-ray microscopy (STXM) are complementary to information obtained from standard radiochemical analysis methods. In addition, microscopic quantities of radioactive material can be characterized rapidly by STXM with minimal sample handling and intrusion, especially in the case of particulate materials. The STXM can accommodate a diverse range of samples including wet materials, complex mixtures, and small quantities of material contained in a larger matrix. In these cases, the inventory of species present in a sample is likely to carry information on its process history; STXM has the demonstrated capability to identify contaminants and sample matrices. Operating in the soft X-ray regime provides particular sensitivity to the chemical state of specimens containing low-Z materials, via the K-edges of light elements. Here, recent developments in forensics-themed spectromicroscopy, sample preparation, and data acquisition methods at the Molecular Environmental Science Beamline 11.0.2 of the Advanced Light Source are described. Results from several initial studies are presented, demonstrating the capability to identify the distribution of the species present in heterogeneous uranium-bearing materials. Future opportunities for STXM forensic studies and potential methodology development are discussed.

We report the development of a laboratory-based Rowland-circle monochromator that incorporates a low power x-ray (bremsstrahlung) tube source, a spherically bent crystal analyzer, and an energy-resolving solid-state detector. This relatively inexpensive, introductory level instrument achieves 1-eV energy resolution for photon energies of ∼5 keV to ∼10 keV while also demonstrating a net efficiency previously seen only in laboratory monochromators having much coarser energy resolution. Despite the use of only a compact, air-cooled 10 W x-ray tube, we find count rates for nonresonant x-ray emission spectroscopy comparable to those achieved at monochromatized spectroscopy beamlines at synchrotron light sources. For x-ray absorption near edge structure, the monochromatized flux is small (due to the use of a low-powered x-ray generator) but still useful for routine transmission-mode studies of concentrated samples. These results indicate that upgrading to a standard commercial high-power line-focused x-ray tube or rotating anode x-ray generator would result in monochromatized fluxes of order 10(6)-10(7) photons/s with no loss in energy resolution. This work establishes core technical capabilities for a rejuvenation of laboratory-based hard x-ray spectroscopies that could have special relevance for contemporary research on catalytic or electrical energy storage systems using transition-metal, lanthanide, or noble-metal active species.

Core-shell X-ray emission spectroscopy (XES) is a valuable complement to X-ray absorption spectroscopy (XAS) techniques. However, XES in the hard X-ray regime is much less frequently employed than XAS, often as a consequence of the relative scarcity of XES instrumentation having energy resolutions comparable with the relevant core-hole lifetimes. To address this, a family of inexpensive and easily operated short-working-distance X-ray emission spectrometers has been developed. The use of computer-aided design and rapid prototype machining of plastics allows customization for various emission lines having energies from ∼3 keV to ∼10 keV. The specific instrument described here, based on a coarsely diced approximant of the Johansson optic, is intended to study volume collapse in Pr metal and compounds by observing the pressure dependence of the Pr Lα emission spectrum. The collection solid angle is ∼50 msr, roughly equivalent to that of six traditional spherically bent crystal analyzers. The miniature X-ray emission spectrometer (miniXES) methodology will help encourage the adoption and broad application of high-resolution XES capabilities at hard X-ray synchrotron facilities.

We present a short working distance miniature x-ray emission spectrometer (miniXES) based on the cylindrical von Hamos geometry. We describe the general design principles for the spectrometer and detail a specific implementation that covers Kβ and valence level emission from Fe. Large spatial and angular access to the sample region provides compatibility with environmental chambers, microprobe, and pump/probe measurements. The primary spectrometer structure and optic is plastic, printed using a 3-dimensional rapid-prototype machine. The spectrometer is inexpensive to construct and is portable; it can be quickly set up at any focused beamline with a tunable narrow bandwidth monochromator. The sample clearance is over 27 mm, providing compatibility with a variety of environment chambers. An overview is also given of the calibration and data processing procedures, which are implemented by a multiplatform user-friendly software package. Finally, representative measurements are presented. Background levels are below the level of the Kβ(2, 5) valence emission, the weakest diagram line in the system, and photometric analysis of count rates finds that the instrument is performing at the theoretical limit.