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The imaging of nanostructures with novel x-ray methods

Abstract

The use of x-rays to probe matter is an ever increasing popular technique due to their short wavelength that can achieve better than atomic resolution; chemical selectivity that permit the separation of material contributions; and tunable interaction strength allowing a wide class of materials to be probed including interfaced and bulk structures. As more powerful sources of x-rays have become available in the form of synchrotrons and linear accelerators, new and inventive experimental method have emerged to access the unknown. In this dissertation, three novel uses of x-rays are advanced to study a wide class materials. Since the next generation of x-ray sources will feature highly brilliant x-ray beams, they will enable the imaging of local nanoscale structures with unprecedented resolution. A general formalism to predict the achievable spatial resolution in coherent diffractive imaging (CDI), based solely on diffracted intensities, is provided. The coherent dose necessary to reach atomic resolution depends significantly on the atomic scale structure, where amorphous materials or disordered materials require less dose than crystalline materials. A reduction in dose can be larger than three-orders of magnitude as compared to the expected scaling for uniform density materials. Additionally, dose reduction for crystalline materials are predicted at certain resolutions based only on their unit cell dimensions and structure factors. An extension of dichroic coherent diffractive imaging of thin films with perpendicular magnetic anisotropy is made from a uniform case to one that contains charge contributions. With the use of linear polarized x-rays near resonant edges, the charge and magnetic scattering can be reconstructed. First, an approximate manual separation is made before reconstruction to obtain the magnetic domains of a Au patterned GdFe multilayer thin film. This is then compared to a direct reconstruction using the two coherent modes contributed by the right-hand and left-hand circular polarization. These methods lead to very similar results for the magnetic domain reconstruction, proving the viability of this technique. Thus, dichroic CDI may be applied to a much wider class of materials than was previously possible. Finally, persistent photocoductivity was induced during nano-diffraction. The resistivity of vanadium dioxide (VO₂) decreased by over one-order of magnitude upon localized illumination with x-rays at room temperature. Despite this reduction, the structure remained in the monoclinic phase and had no signature of the high-temperature tetragonal phase that is usually associated with the lower resistance. Once illumination ceased, relaxation to the insulating state took tens of hours near room temperature. However, a full recovery of the insulating state was achieved within minutes by thermal cycling. This behavior is consistent with random local-potential fluctuations and random distribution of discrete recombination sites used to model residual photoconductivity

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