Developing novel applications of Dynamic Nuclear Polarization in solid-state NMR spectroscopy

Nuclear Magnetic Resonance (NMR) Spectroscopy provides a unique window into the atomic world, revealing information on the structures and dynamics of molecules without altering their properties. However, the intrinsically low sensitivity of NMR imposes significant challenges for its application. Thus, NMR has greatly benefited from the advent of sensitivity enhanced methods. One such method is Dynamic Nuclear Polarization (DNP), a technique specifically used to enhance the signal in solid- and liquid-state NMR as well as MRI. The extension to Magic Angle Spinning (MAS) DNP has made the approach widely applicable to problems in a variety of fields, including structural biology, biophysics, and chemistry.
In this thesis, we aimed to contribute to the further advancement of the DNP technique. These contributions include methodological developments and novel applications of DNP-enhanced solid-state NMR. High-sensitivity NMR approaches are employed on a variety of systems to answer specific questions in life and material science; from in-cell structural studies, where target molecules are probed directly in their natural setting at the atomic level; to zeolite-based catalytic systems, where the distinctive host-guest chemistry between the zeolite and trapped organics during catalysis is investigated. Moreover, strategies to further improve sensitivity at high magnetic fields are described and new biradical polarizing agents are presented, along with an investigation on their potential for biomolecular applications.