Robust optical polarization of nuclear spin baths using Hamiltonian engineering of nitrogen-vacancy center quantum dynamics

Dynamic nuclear polarization (DNP) is an important technique that uses polarization transfer from electron to nuclear spins to achieve nuclear hyperpolarization. Combining efficient DNP with optically polarized nitrogen-vacancy (NV) centers offers promising opportunities for novel technological applications, including nanoscale nuclear magnetic resonance spectroscopy of liquids, hyperpolarized nanodiamonds as magnetic resonance imaging contrast agents, and the initialization of nuclear spin-based diamond quantum simulators. However, none of the current realizations of polarization transfer are simultaneously robust and sufficiently efficient, making the realization of the applications extremely challenging. We introduce the concept of systematically designing polarization sequences by Hamiltonian engineering, resulting in polarization sequences that are robust and fast. We theoretically derive sequences and experimentally demonstrate that they are capable of efficient polarization transfer from optically polarized NV centers in diamond to the surrounding C-13 nuclear spin bath even in the presence of control errors, making the above mentioned novel applications possible.