Developing Laboratory-Based X-ray Spectroscopies for Energy and Materials Research spectroscopy
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Advanced x-ray spectroscopies interrogate a material’s electronic structure in an element-specific manner. Traditionally, X-ray absorption fine structure (XAFS) and X-ray emission spectroscopy (XES) studies are performed at synchrotron X-ray light sources. These facilities serve to push the forefront of science and, thus, operate under an access model which necessarily excludes projects requiring routine analytical characterization, rapid feedback for prototyping, or regular access. In response to this deficit, my dissertation presents a laboratory-based XAFS and XES spectrometer of high energy resolution, reproducibility, and efficiency, along with other improvements in instrumentation, especially as pertains to the utilized crystal analyzer. A range of basic and applied materials problems were addressed with this and similar instrumentation. Select applied research studies include operando XAFS analysis of a prototype lithium-ion battery’s state-of-charge and state-of-health and an XES-based method for the quantification of hexavalent chromium in manufactured plastics that is being developed into a standard test method. Basic research spanned a study of photoexcitation dynamics in Ni metal and time-dependent density functional theory interpretations of valence-to-core XES spectra collected from a series of vanadium oxide and vanadyl phosphate energy storage materials candidates. This thesis provides strong evidence that laboratory-based X-ray spectroscopy instrumentation can serve as a powerful tool for increasing productivity and understanding in the fields of chemistry and materials science.
- Physics