| Summary: | This thesis represents two bodies of work: a detailed look at what angle- resolved photoemission spectroscopy (ARPES) measures, as well as ARPES and circularly polarized photon spin- and angle-resolved photoemission spectroscopy (CPS-ARPES) measurements on the unconventional superconductor Sr₂RuO₄.
In the first part I present a study of both established methods of ARPES analysis and some new variations on model spectral functions. This modelling was done in a realistic regime, yet far from the limits often assumed. Away from these limits I show that any "effective coupling" inferred from quasiparticle renormalizations differs drastically and unpredictably from the true coupling. Conversely, I show that perturbation theory retains good predictive power where expected, that the momentum dependence of the self-energy can be revealed via the relationship between velocity renormalization and quasiparticle strength, and that it is often possible to infer the self-energy and bare electronic structure through lineshape analysis.
In the second part I present experimental ARPES and CPS-ARPES data on Sr₂RuO₄. Newly discovered and unexplained ARPES features are characterized and compared with a variety of different possible structural distortions through bulk and slab local-density approximation (LDA) band structure calculations. I thereby rule out phases driven by electronic interaction, such as Dirac- or Rashba-type surface states, and instead find that there exists a progressive structural modulation whereby both the surface and (at a minimum) sub-surface layers exhibit a (√2 x √2)R45° reconstruction.
Through CPS-ARPES on Sr₂RuO₄ I also directly demonstrate that the effects of spin-orbit (SO) coupling are not limited to a modification of the band structure, but fundamentally entangle the spin and spatial parts of the wave-function. This must drive the superconducting state in Sr₂RuO₄ to be even more unconventional than is generally assumed, with mixing between singlet and triplet states that varies around the Fermi surface, and thereby offers a possible resolution to a number of experiments that clash with the categorization of Sr₂RuO₄ as a hallmark spin-triplet chiral p-wave superconductor. === Science, Faculty of === Physics and Astronomy, Department of === Graduate
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