Asymmetric Rowland circle geometries for spherically bent crystal analyzers in laboratory and synchrotron applications

• Published in: Journal of analytical atomic spectrometry 2024-05, Vol.39 (5), p.1375-1387
• Main Authors: Gironda, Anthony J, Abramson, Jared E, Chen, Yeu, Solovyev, Mikhail, Sterbinsky, George E, Seidler, Gerald T
• Format: Article
• Language: English
• Subjects: Analyzers; Asymmetry; Configurations; Crystals; Emission; Energy resolution; Fine structure; Raman spectra; Rowland circles; X ray absorption
• ISSN: 0267-9477; 1364-5544
• DOI: 10.1039/d3ja00437f

Spherically bent crystal analyzers (SBCAs) are the dominant high-resolution hard X-ray optic in the ongoing rebirth of laboratory-based X-ray absorption fine structure (XAFS) and X-ray emission spectroscopy (XES) as well as in synchrotron methods such as high energy resolution fluorescence detection (HERFD) and non-resonant X-ray Raman scattering (XRS). In the overwhelming majority of cases, SBCAs are implemented in a 'symmetric' configuration on the Rowland circle, wherein the diffracting crystal plane is nominally coincident with the analyzer surface. We report here comprehensive investigations of 'asymmetric' operation of SBCA on the Rowland circle, wherein the diffracting crystal plane is not coincident with the optical surface of the analyzer. First, we have developed a laboratory spectrometer for XAFS and XES that is specialized for asymmetric SBCA operation. We find several benefits, including the capacity to use a single SBCA over a very wide energy range via ' hkl hopping' and the frequent ability to eliminate Johann error, the most prevalent energy-broadening mechanism when using SBCA symmetrically on the Rowland circle. Second, we expand these ideas to synchrotron facilities with a demonstration study of HERFD and XRS where asymmetric operation also provided advantage. Our results suggest that large-array systems for HERFD augmented with an additional mechanical degree of freedom could streamline user operation and also indicate benefits to XRS in the asymmetric configuration, where larger solid angle, larger sample-to-detector distance, and decreased Johann error can be achieved simultaneously. We show that asymmetric operation of spherically bent crystal analyzers is an underutilized opportunity that can improve x-ray spectrometer performance and user operations in both the laboratory and synchrotron environments.