This thesis is for a Doctorate of Philosophy in the field of Condensed Matter. This thesis weaves a common thread which connects together everything I have worked on from 2013-2019. The structure of materials at the atomic level dictates their appearance. Conversely, precise optical experiments performed on these materials can be used to determine details of their structure and chemistry. Multiscale modeling was used to build up from the atomic scale and to test hypotheses of lattice dynamics. This document is (hopefully) a useful reference for those who want to understand how to model complex, dynamic systems over multiple orders of magnitude of length and time.