The nitrogen-vacancy (N-V) center in diamond has emerged as a candidate to noninvasively hyperpolarize nuclear spins in molecular systems to improve the sensitivity of nuclear magnetic resonance (NMR) experiments. Several promising proof-of-principle experiments have demonstrated small-scale polarization transfer from single N-V centers to hydrogen spins outside the diamond. However, the scaling up of these results to the use of a dense N-V ensemble, which is a necessary prerequisite for achieving realistic NMR sensitivity enhancement, has not yet been demonstrated. In this work, we present evidence for a polarizing interaction between a shallow N-V ensemble and external nuclear targets over a micrometer scale, and characterize the challenges in achieving useful polarization enhancement. In the most favorable example of the interaction with hydrogen in a solid-state target, a maximum polarization transfer rate of approximately 7500 spins per second per N-V is measured, averaged over an area containing order 10(6) N-V centers. Reduced levels of polarization efficiency are found for liquid-state targets, where molecular diffusion limits the transfer. Through analysis via a theoretical model, we find that our results suggest that implementation of this technique for NMR sensitivity enhancement is feasible following realistic diamond material improvements.
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