This thesis describes the results of angle resolved photoemission spectroscopy experiments on delafossite oxide metals, and theoretical work explaining these observations. The study was motivated by the extraordinarily high conductivity of the non-magnetic delafossites PdCoO2 and PtCoO2, the measurement of whose electronic structure is reported and discussed. Two unexpected effects were observed in the course of the investigation; each is described and analysed in detail. Firstly, a previously unrecognised type of spectroscopic signal, allowing the non-magnetic probe of photoemission to become sensitive to spin-spin correlations, was observed in the antiferromagnetic PdCrO2. Its origin was identified as the Kondo-like coupling of itinerant and Mott insulating electrons. Furthermore, surface states exhibiting an unusually large Rashba-like spin-splitting were observed on the transition metal terminated surfaces of delafossites. The large inversion symmetry breaking energy scale, a consequence of the unusual structure of the surface layer, is identified as the origin of the effect.

This thesis describes in-depth studies of the remarkable electronic transport within the ultrahigh conductivity delafossite metals PtCoO_2 and PdCoO_2 using the tool of focused ion beam (FIB) microstucturing. Despite being first synthesised over 50 years ago, important questions remain regarding both the origin of the unusually high conductivity of these compounds and the consequences of their unique properties for unconventional electronic transport, such as that within the ballistic regime. The thesis explores both these areas. High-energy electron irradiation is used to examine the effects of deliberately introducing point defects into PdCoO_2 and PtCoO_2, demonstrating that the extremely low resistivity of these materials stems from an extreme purity as high as 1 defect in 120,000 atoms, rather than a novel scattering suppression mechanism. In addition, studies of the electronic transport in micron-scale squares of these metals show that their broadly hexagonal Fermi surfaces lead not only to long range ballistic behaviour but novel ballistic regime phenomena which cannot be observed in materials with a higher-symmetry Fermi surface.

This thesis presents pioneering work in the relatively new field of focused ion beam (FIB) sculpting of single crystals to produce bespoke devices and enable the investigation of physics that cannot be studied in bulk samples. It begins with a comprehensive and didactic account of how to achieve this sculpting, revealing the ‘tricks of the trade’ of state-of-the-art FIB microstructuring. In subsequent chapters, the author presents ground-breaking results obtained from microstructures of the delafossite oxide metal PdCoO2 and the heavy fermion superconductor CeIrIn5. In these elegant, forefront experiments, a new form of directional ballistic transport in the ultra-pure delafossites is described and explained. Furthermore, a new way to spatially modulate superconductivity induced by strain is demonstrated with electrical transport measurements that agree well with predictions based on thermoelastic finite element simulations.

This book is devoted to the rapidly developing field of oxide thin-films and heterostructures. Oxide materials combined with atomic-scale precision in a heterostructure exhibit an abundance of macroscopic physical properties involving the strong coupling between the electronic, spin, and structural degrees of freedom, and the interplay between magnetism, ferroelectricity, and conductivity. Recent advances in thin-film deposition and characterization techniques made possible the experimental realization of such oxide heterostructures, promising novel functionalities and device concepts. The book consists of chapters on some of the key innovations in the field over recent years, including strongly correlated oxide heterostructures, magnetoelectric coupling and multiferroic materials, thermoelectric phenomena, and two-dimensional electron gases at oxide interfaces. The book covers the core principles, describes experimental approaches to fabricate and characterize oxide heterostructures, demonstrates new functional properties of these materials, and provides an overview of novel applications.

This book develops the subject from the basic principles of quantum mechanics. The emphasis is on a single statement of the ideas underlying the various approximations that have to be used and care is taken to separate sound arguments from conjecture. This book is written for the student of theoretical physics who wants to work in the field of solids and for the experimenter with a knowledge of quantum theory who is not content to take other people's arguments for granted. The treatment covers the electron theory of metals as well as the dynamics of crystals, including the author's work on the thermal conductivity of crystals which has been previously published in English.