Browsing Theses and Dissertations by Subject "Xps"
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ELECTRON TUNNELING STUDIES OF MATERIALS FOR SUPERCONDUCTING RADIO FREQUENCY APPLICATIONSRadio frequency (RF) cavities are the foundational infrastructure which facilitates much of the fundamental research conducted in high energy particle physics. These RF cavities utilize their unique shape to produce resonant electromagnetic fields used to accelerate charged particles. Beside their core role in fundamental physics research, RF cavities have found application in other disciplines including material science, chemistry and biology which take advantage of their unique light sources. Industry has been keen on taking advantage of accelerator technology for a multitude of applications. Particle accelerators like the one found at Jefferson Lab’s Continuous Electron Beam Accelerator Facility must produce stable beams of high energy particles which is an incredibly costly endeavor to pursue. With the gargantuan size of these facilities, the cost of high-quality beam production is a matter of great importance. The quest to find highly efficient RF cavities has resulted in the widespread use of superconducting radio frequency (SRF) cavities which are the most efficient resonators that exploit a superconductor’s incredibly low AC surface resistance. While metals like Cu are up to the demanding job of RF cavity particle acceleration, their efficiency at transferring RF power to the particle beam is low when they are compared with SRF Nb cavities. Nb is the standard material for all SRF cavity technology particularly for its reproducibly low surface resistance, comparatively high transition temperature and thermodynamic critical field. Using superconducting Nb is not without its drawbacks. Keeping hundreds of Nb cavities in their superconducting state under extreme RF conditions is quite a daunting task. It requires the normal state not nucleate during operation. This is achieved by producing high-quality cavities with as few defects and impurities as possible while also keeping the cavities at low temperature, usually 2K. Again, due to the sheer scale of the facilities, hundred million-dollar cryogenic plants are required to handle the heat loads during SRF cavity operation. This means even small increases in maximum accelerating gradients or decrease in cavity surface resistance results in a sizably reduced operation cost. Considerable effort has been put forth to increase the efficiency of Nb cavities toward and even beyond the theoretical maximum accelerating gradients and quality factor for a clean superconductor. Recently, a new method to produce high quality factor cavities has emerged that involves nitrogen doping the cavity. The mechanism by which N doping causes the improvement is still not well understood, but the experimental research described in this dissertation shines some light into the mechanisms behind such a drastic improvement. These insights are universal for all superconductors and may prove useful for SRF cavities beyond Nb. With Nb approaching its fundamental limits, new materials are being proposed to increase the performance of future SRF cavities which MgB2 finds itself among. MgB2 is a two-band superconductor that possesses many properties that are very attractive for the next generation of SRF cavities. One of the most important properties is MgB2’s comparatively large critical temperature which in part predicts it will have a lower surface resistance than Nb at higher operating temperatures. Such behavior of MgB2 may unlock the possibility of using cryocoolers instead of costly liquid helium plants for large scale industrial use. This dissertation starts with an introduction to superconductivity, its theory, and application to SRF cavities as well as the open questions that can be addressed in Nb and the next generation of SRF materials. A description of the experimental techniques of scanning tunneling microscopy, X-ray photoelectron spectroscopy, and atomic force microscopy is presented. Our experimental investigation into Nb SRF cavity cutouts starts with a discussion of the material’s limitations for SRF applications with an emphasis on the proximity effect which arises at the surface of this material due to its myriad of naturally forming oxides. The results of our scanning tunneling microscopy measurements for typically prepared Nb and nitrogen doped Nb follows and comparisons are made which show that the surface oxides are fundamentally different between these samples likely resulting in the profound enhancement of the cavity’s quality factor. Experimental investigation into the native oxide of hot spot nitrogen doped Nb shows a degraded oxide and superconducting properties as compared with the cold spot. The dissertation continues with a brief introduction to MgB2, followed by our scanning tunneling and electron tunneling insights into MgB2. The dissertation is concluded with a summary of our investigations and broader impact of our research on the SRF community.
Probing electronic, magnetic and structural heterogeneity in advanced materials and Nanostructures with x-ray imaging, scattering and spectroscopic techniques.In this dissertation, we have used a combination of synchrotron-based x-ray spectroscopic, scattering and imaging techniques to investigate the electronic, magnetic and structural properties of materials and material systems which exhibit natural as well as engineered nanoscale structural distortions. In order to investigate the interplay between the above-mentioned degrees of freedom with spatial and depth resolution, we have utilized non-destructive techniques, such as x-ray absorption spectroscopy (XAS), polarization-dependent photoemission electron microscopy (PEEM), nanoscale scanning x-ray diffraction microscopy (nano-SXDM) and standing-wave x-ray photoemission spectroscopy (SW-XPS). The results were compared to several types of state-of-the-art first-principles theoretical calculations. In the first part of the dissertation, we have investigated the nanoscale magneto-elastic structure of the Fe3Ga magnetic alloy, which was recently reported to exhibit non-volume conserving magnetostriction. As the result of our combined PEEM and nano-SXDM study, we have discovered the structural basis for this phenomenon – periodic long-wavelength (~269 nm) elastic domain walls, with domains (regions of zero-strain) existing as narrow transition regions. Atto-scale elastic gradients and self-strain across the elastic domain walls were quantitatively measured and imaged by nano-SXDM. Our measurements revealed that the gradients inside the elastic walls are accommodated by gradually increasing/decreasing inter-planar spacing resembling a longitudinal wave. Our element-specific polarization-dependent PEEM measurements revealed that the magnetic structure of the crystal modulates with similar periodicity (~255 nm), and the resulting magneto-elastic coupling produces a ‘giant’ field-induced bulk deformation, which is equal to the measured self-strain of the elastic domain wall. In the second part of this dissertation, we utilized a combination of soft x-ray standing-wave photoemission spectroscopy (SW-XPS), hard x-ray photoemission spectroscopy (HAXPES) and scanning transmission electron microscopy (STEM) to probe the depth-dependent and single-unit-cell resolved electronic structure of isovalent manganite superlattices (Eu0.7Sr0.3MnO3/La0.7Sr0.3MnO3)15 wherein the electronic and magnetic properties are intentionally modulated with depth via engineered O octahedral rotations and A-site displacements. Standing-wave-excited spectroscopy of the Mn 2p and O 1s core-levels confirmed the isovalent nature of the Mn ions in the superlattice and revealed significant depth-dependent variations in the local chemical and electronic environment around the O atoms, consistent with the state-of-the-art theoretical calculations. Furthermore, it was shown that a surface relaxation and orbital reconstruction in the several top Eu0.7Sr0.3MnO3 atomic layers produces substantial changes in the observed electronic structure, which, according to the first-principles theoretical calculations, occur due to the establishment of orbital stripe order in the top unit cell. In summary, we have used synchrotron-based x-ray spectroscopic and microscopic techniques, in conjunction with high-resolution electron microscopy, to study the electronic, magnetic and structural properties of advanced functional materials exhibiting strong nanoscale heterogeneity. We discovered a strong coupling between the nanoscale structural and magnetic properties in the non-conventional magnetostrictive Fe3Ga single crystal. Our results suggest that this coupling provides the fundamental basis for the non-conventional magnetostriction phenomenon in this material. We have also discovered that the electronic properties of the Eu0.7Sr0.3MnO3/La0.7Sr0.3MnO3 superlattices can be epitaxially tuned via engineered A-site cation displacement, which is a result of the strong interfacial coupling between the Eu0.7Sr0.3MnO3 and La0.7Sr0.3MnO3 layers. This suggests a new way of tailoring and spatially-confining electronic and ferroic behavior in complex oxide heterostructures and creating novel ordered surface-reconstruction effects.