Ab initio quantum chemistry provides many benefits to experimental studies through verification and prediction of experimental results. Several examples are given of quantum chemistry methods being used to direct experimental discovery. Through canonical transition state theory, methylamine was found to have greater reactivity with the simplest, anti-methylated, and syn-methylated Criegee intermediates relative to more abundant atmospheric species. This was true for both addition orientations, but the naturally low concentration of methylamine makes it unlikely to be an important contributor to the consumption of Criegee intermediates under typical conditions. The kinetics of pentazole decomposition were also investigated to determine its potential as a high-energy-density material. A decomposition barrier of 18.8 kcal mol-1 makes it unsuitable as an hedm candidate at room temperature. A temperature of 180 K or lower is required to achieve a half-life of 35 years. Anharmonic frequencies were calculated for four In2H2 isomers and their deuterated counterparts. Numerous agreements and some disagreements were found between our results and those of previous studies. Each of these theoretical studies either provided insight for future experimental discovery or sought to verify current data.