NEUTRON STUDIES ON RARE-EARTH AND DOUBLE PEROVSKITE MAGNETIC OXIDES WITH FRUSTRATED TETRAHEDRAL ARCHITECTURES

Abstract

Magnetic frustration is the underpinning theme to all of the magnetic oxide systems explored in this dissertation. The materials studied in this thesis belong to two topical families of interest in modern condensed matter physics, namely, the rare-earth titanates R2Ti2O7 and the double perovskites A2BB'O6. Chapter 1 provides the theoretical background necessary to understand the crystalline systems studied in this thesis. Chapter 2 explains the necessity of utilizing neutron scattering and x-ray experiments to tease out the key signatures which were essential to formulating the conclusions made in each study. Chapter 3 outlines the neutron scattering techniques which were employed to investigate the crystal systems. The first objective of this thesis is to understand effect of “stuffing” on the ground state anisotropy of the quantum spin liquid candidate Yb2Ti2O7 via an investigation of the crystal-field excitations in intentionally stuffed samples. The pentultimate study was performed on the monoclinic crystal systems, La2LiRuO6 and La2LiOsO6, to discern the effect of lattice distortions on the spin-orbit induced magnetic ground state of 4d3 and 5d3 double perovskites based on Ru and Os magnetic ions. The final investigation involves an inelastic neutron scattering investigation of magnetic ground states in three d2 double perovskites, Ba2CaOsO6, Ba2MgOsO6 and Ba2ZnOsO6. Here, we make the case for novel octupolar order below their respective transition temperatures T* of 50 K, 49 K and 30 K based on information provided by neutron scattering, heat capacity, muon spin relaxation and synchrotron x-ray diffraction studies.