UC Berkeley

The work in this dissertation revolves around the use and evolution of methods and molecular contrast agents for 129Xe nuclear magnetic resonance (NMR) techniques. A general overview of the scope of this work is provided in Chapter 1. An overview of the basic principles of magnetic resonance, the manipulation of magnetization in an NMR experiment, and the ways data from NMR experiments can be treated is provided in Chapter 2. Chapter 3 introduces hyperpolarized 129Xe NMR and describes the theoretical background and current applications of hyperpolarized xenon as they apply to biosensing, including the functionalization of xenon for molecular detection using macromolecular hosts and the principles of the hyperpolarized gas chemical exchange saturation transfer (hyperCEST) technique. Practical technical considerations involved with hyperpolarized 129Xe gas generation and delivery are provided in Chapter 4. The following three chapters each expound upon a completely different type of 129Xe sensor explored as a part of this thesis work: a cryptophane derivative (Chapter 5), a cucurbit[6]uril rotaxane (Chapter 6), and a targeted cucurbit[7]uril (Chapter7), while Chapter 8 introduces a new device that enables examination of hyperpolarized 129Xe in viscous and orienting media. Chapter 9 synthesizes all the components of previous chapters to explore the use of orienting media to further enhance molecular detection. This dissertation concludes in Chapter 10 with a clear direction for the next steps toward sensitive analysis of unprocessed biological samples with 129Xe NMR.