This thesis is divided into two parts. The first part involves the study of molecular structure utilizing Ianthanide induced shift (LIS) and lanthanide induced relaxation (LIR) nuclear magnetic resonance (NMR). It the course of these studies, it was found that the trifluoroethoxy group is a good deactivating group towards lanthanide shift reagents (LSR) and can be used to selectively deactivate multifunctional molecules. The second part of the thesis involves the utilization of liquid-liquid intermolecular transfer (LLIT) dynamic nuclear polarization (DNP) to study the microwave power needed to achieve saturation using deuterated and nondeuterated 2,4,6-tri-tert-butylphenoxy and galvinoxyl radicals, and ¹⁴N labelled, nondeuterated and ¹⁴N labelled, deuterated 4-hydroxy-TEMPO radicals. Also, selective ¹H DNP enhancements for taxol in solid-liquid intermolecular transfer (SLIT) DNP low-to-high field transfer experiments were obtained. Finally, the syntheses of compounds with both a LSR moiety and a nitroxide radical moiety in the same molecule were examined. LLIT DNP transfer experiments for the intramolecular LSR-nitroxide radicals molecular system and the intermolecular LSR—radicals systems were studied. Conclusions based on this study provide new insight regarding approaches for new LIS and DNP studies. / Ph. D.