The 229mTh isomeric state holds much promise as the reference for a clock of incredi-bly high precision and accuracy. This dissertation discusses the first direct excitation of the 229Th isomer in a LiSrAlF6 environment, and the laser system that was used for excitation spectroscopy. In addition, we discuss two other efforts towards determina- tion of the energy of the isomeric transition. The first involved the implantation of 229mTh into a superconducting nanowire single-photon imager (SNSPI). The second was towards the first instance of laser-based conversion electron M¨ossbauer spec- troscopy (CEMS) in a ThO2 sample. The results of these efforts will be discussed, as well as possible improvements that would enable detection of the isomeric transition within these environments.