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Shaped ultrafast optical pumping for NMR applications

High polarization of nuclear spin systems is essential for quantum information processing using nuclear magnetic resonance and for sensitive spectroscopic measurements. Unfortunately for liquids, the polarization of such systems is terribly small–O(10−5). Continuous Wave (CW) optical pumping can increase the polarization of simple systems. For sufficiently complicated molecules, determining a pumping scheme analytically is intractable. Recent experiments have shown that shaped ultrafast laser pulses controlled by machine learning algorithms has promise for solving previously unapproachable problems in physical chemistry. Shaped light has been used to break specific bonds in molecules and drive chemical reactions. We investigate the potential of enhancing nuclear spin polarization in liquid NMR through the application of shaped ultrafast laser pulses. The excited-singlet → groundtriplet transition intersystem crossing is mediated by spin-orbit coupling of the molecule. Shaped ultrafast pumping has revolutionized control of the wavefunctions of electrons of molecules [Zew00]. The main body of this work is a review of the fields related to shaped ultrafast optical pumping and NMR. Presented here is a proposal for a set of experiments to investigate the usefulness of shaped ultrafast optical pumping for NMR applications. This document begins with a pedagogical review of relevant material. Then proceeds to discuss an experimental exploration of the space around this research trajectory. We then propose a set of experiments to test the feasibility of shaped ultrafast optical pumping, and then present some preliminary results. Thesis Supervisor: Neil Gershenfeld Title: Associate Professor