Exciton spectroscopy using non-resonant X-ray Raman scattering

Core electron excitations in solids have long been of interest in condensed matter physics. The state of the low-energy photoelectron is dominated by many-body effects from screening by valence electrons and interactions with the core-hole. In some insulators, these interactions create a localized state for the photoelectron core-hole pair, namely a core-exciton. In this dissertation, we use q-dependent non-resonant x-ray Raman scattering together with ab initio simulations to extend exciton spectroscopy to probe the angular characteristics of the near-edge exciton. The transferred momentum q acts as an extra parameter and provides new information about the projected density of states which is inaccessible to traditional core-excitation spectroscopies, such as x-ray absorption spectroscopy and electron energy loss spectroscopy. In several cases, we find that the angular characteristics of the exciton are strongly connected with the local atomic structure and symmetry. This is illustrated by a study on hexagonal boron nitride, in which a dominantly Y₁₀-type exciton was identified necessarily due to the reflection symmetry about the basal plane at every boron site. This new understanding of the relationship between the exciton type and local symmetry has helped solve a site-substitution disorder problem in the icosahedral boron carbide B₄C system, where a p -type exciton was identified due to dominant boron occupation at the center of a three-atom chain in the unit cell, the only site with the inversion symmetry. This exciton spectroscopy using q-dependent x-ray Raman scattering may have wide applications in the future, such as in geophysical studies in high pressure diamond anvil cells.