Author ORCID Identifier
Year of Publication
Doctor of Philosophy (PhD)
Arts and Sciences
Physics and Astronomy
Dr. Ambrose Seo
The 5d transition metal oxides have drawn substantial interest for predictions of being suitable candidates for hosting exotic electronic and magnetic states, including unconventional superconductors, magnetic skyrmions, topological insulators, and Weyl semimetals. In addition to the electron-electron correlation notable in high-temperature 3d transition metal superconductors, the 5d oxides contain a large spin-orbit interaction term in their ground state, which is largely responsible for the intricate phase diagram of these materials. Iridates, or compounds containing 5d iridium bonded with oxygen, are of particular interest for their spin-orbit split Jeff = 1/2 state, which is partially filled without the presence of any additional electron correlation. However, the comparable energetics between a small, finite electron correlation energy and the spin-orbit interaction make the band structure of iridates amenable to small perturbations of the crystalline lattice and ideal for exploring the interplay between these two interactions.
While altering the spin-orbit interaction strength of iridium is tenably not feasible, the electron correlation energy can be tuned using a variety of experimental techniques. In this dissertation, the electronic and magnetic properties of iridates at various electron correlation energies are studied by altering the epitaxial lattice strain, dimensionality, and the radius size of the A-site cation. These parameters tune the effective electronic bandwidth of the system, which is inversely proportional to the effective electron correlation energy. The lattice strain and the cationic radius size achieve this by altering the Ir-O-Ir bond angle between nearest neighbor Ir ions. In the case of dimensionality tuning, the effective bandwidth is controlled via the coordination number of each Ir ion.
In the first study, a metal-to-insulator transition is observed in thin films of the semi-metallic SrIrO3 as in-plane compressive lattice strain is increased. This observation is consistent with the expectation of compressive lattice strain increasing the effective correlation energy; however, optical spectroscopy spectra reveal the increase is not sufficient for opening an insulating Mott gap. In the second part, the effective correlation energy is adjusted using a dimensional confinement of the layered iridate Sr2IrO4. Here, the coordination number of each Ir ion is reduced using an a-axis oriented superlattice of one-dimensional IrO2 quantum stripes, where several emergent features are revealed in its insulating Jeff = 1/2 state. In the final study, the effective correlation is tuned in a series of mixed-phase pyrochlore iridate thin films, where the Ir atoms take a corner-shared tetrahedral configuration. Here, a transition between conducting to insulating magnetic domain walls is revealed as the correlation energy is increased via A-site chemical doping. Each of these studies sheds light on the pronounced role the effective correlation energy plays in determining the local subset of phases predicted for iridates and related systems featuring strong spin-orbit interactions.
Digital Object Identifier (DOI)
Gruenewald, John H., "TUNING THE EFFECTIVE ELECTRON CORRELATION IN IRIDATE SYSTEMS FEATURING STRONG SPIN-ORBIT INTERACTION" (2017). Theses and Dissertations--Physics and Astronomy. 51.