The stainless steel chamber was specifically conceived and designed for housing an interferometer controlled scanning transmission x-ray microscope (STXM). The construction of the chamber is such that internal components of the microscope rest within the chamber and are fixed to a 4 inch stainless steel belly band. The integral and most important part of the chamber is the belly band, which serves to isolate high frequency vibrations (e.g., floor surroundings, people traffic) from the sensitive measurements performed using the microscope. In addition, the chamber effectively acts as a sound barrier to the nanometer measurements conducted within. The assembled chamber (and microscope) are readily adjustable at the micron level using strut members external to the chamber but fixed to the belly band and a stand made of polymer concreate.

Tricalcium aluminate (cement clinker phase), gypsum, katoite, ettringite, and calcium monosulfoaluminate hydrate (abbreviated as kuzelite) are the major minerals in the hydration reaction of tricalcium aluminate in the presence of gypsum and have critical impacts on the kinetics and thermodynamics of early-age cement hydration mechanisms. Here, spectroscopic analysis of these minerals is conducted using scanning transmission X-ray microscopy (STXM). Their Ca L2,3-edge near edge X-ray absorption fine structure (NEXAFS) spectra are measured and correlated to the known Ca coordination environments. The results indicate that these minerals have unique Ca environments that can be differentiated from one another based on the intensities and positions of the absorption peaks at 346.5-348.5 and 350.5-351.5 eV. It is concluded that Ca in tricalcium aluminate (cubic and orthorhombic polymorphs) and katoite is in cubic-like coordination with negative 10Dq, whereas Ca is in an octahedral-like coordination with positive 10Dq in ettringite, gypsum, and kuzelite. For tricalcium aluminate, the Ca atoms in both polymorphs are in similar chemical environments with slightly more distortion in the orthorhombic polymorph. As a common issue in STXM experiments, absorption saturation of NEXAFS spectra is also investigated. It is demonstrated that the optical density difference between pre- and post-edge absorption levels provides a reliable indication of the sample thickness in the systems studied. The present work provides a reference for the STXM study of the calcium (sulfo)aluminate reactions in cement hydration and natural aqueous environments, and in the former case, provides a more complete understanding of a system that may serve as a low-C alternative to Portland cement.

We have developed an experimental system to simultaneously measure surface structure, morphology, composition, chemical state, and chemical activity for samples in gas phase environments. This is accomplished by simultaneously measuring x-ray photoelectron spectroscopy (XPS) and grazing incidence x-ray scattering in gas pressures as high as the multi-Torr regime while also recording mass spectrometry. Scattering patterns reflect near-surface sample structures from the nano-scale to the meso-scale, and the grazing incidence geometry provides tunable depth sensitivity of structural measurements. Scattered x rays are detected across a broad range of angles using a newly designed pivoting-UHV-manipulator for detector positioning. At the same time, XPS and mass spectrometry can be measured, all from the same sample spot and under ambient conditions. To demonstrate the capabilities of this system, we measured the chemical state, composition, and structure of Ag-behenate on a Si(001) wafer in vacuum and in O₂ atmosphere at various temperatures. These simultaneous structural, chemical, and gas phase product probes enable detailed insights into the interplay between the structure and chemical state for samples in gas phase environments. The compact size of our pivoting-UHV-manipulator makes it possible to retrofit this technique into existing spectroscopic instruments installed at synchrotron beamlines. Because many synchrotron facilities are planning or undergoing upgrades to diffraction limited storage rings with transversely coherent beams, a newly emerging set of coherent x-ray scattering experiments can greatly benefit from the concepts we present here.

High-resolution X-ray microscopy is used to investigate the sequence of lithiation in LiFePO4 porous electrodes. For electrodes with homogeneous interparticle electronic connectivity via the carbon black network, the smaller particles lithiate first. For electrodes with heterogeneous connectivity, the better-connected particles preferentially lithiate. Correlative electron and X-ray microscopy also reveal the presence of incoherent nanodomains that lithiate as if they are separate particles.

Oxygen migration in tantalum oxide, a promising next-generation storage material, is studied using in operando X-ray absorption spectromicroscopy. This approach allows a physical description of the evolution of conduction channel and eventual device failure. The observed ring-like patterns of oxygen concentration are modeled using thermophoretic forces and Fick diffusion, establishing the critical role of temperature-driven oxygen migration.