Manifestations of broken symmetry: The surface phases of calcium-strontium ruthenate

The discovery of superconductivity in Sr2RuO4 has renewed vigor in the study of correlated electron systems. The evolution of a p-wave superconducting state from a paramagnetic 2-dimensional Fermi liquid shows the ruthenate superconductivity is anything but conventional. Sr 2RuO4 is isostructural with La2CuO4, the parent compound for the high temperature superconducting family La 2-xSrxRuO 4. The substitution of Ca2+ for Sr2+ generates a different structure involving a static rotation and tilt of the RuO 6 octahedral, however, the antiferromagnetic insulating ground state of Ca2RuO4 is more akin to the cuprate parent. The generation of Ca2-xSrxRuO 4 has offered a new family of compounds where the evolution from an antiferromagnetic insulator to a superconductor can be studied. Bulk studies have demonstrated how the intricate couplings between structural, orbital, electronic, and magnetic degrees of freedom are responsible for the exotic phases of the system. The layered perovskite structure which plays a key role in the properties observed also makes the crystals amenable to cleaving. Breaking symmetry by the creation of a surface on a quasi 2-dimensional system offers an opportunity to gain insight into the role of structure and symmetry on the properties of the system and offers a new avenue to discover new physics. Inelastic neutron scattering has been utilized to reveal the structural instability against the RuO6 tilt. While the sum4 phonon mode involving the octahedral tilt shows classic soft phonon mode behavior across a tetragonal to orthorhombic phase transition, a new anomalous mode is discovered and its origin is explored. Surface phonon dynamics have been investigated across a Mott metal-to-insulator transition utilizing High Resolution Electron Energy Loss Spectroscopy where it is revealed the surface electronic transition temperature is significantly lower than the bulk. Low Energy Electron Diffraction has been employed to investigate the surface structure and structural transitions on the surface. Results show surface relaxations inhibit the RuO6 tilt dramatically altering the ensuing orthorhombic phase transition near a quantum critical point at xc = 0.5. It is also revealed that structural distortions accompanying the bulk metal-to-insulator transition are simply nonexistent on the surface. Physical manifestations from breaking symmetry in a correlated electron system are revealed.