Hyperpolarization of nuclear spins: Polarization blockade

Abstract

Efficient hyperpolarization of nuclear spins via optically active defect centers, such as the nitrogen vacancy (NV) center in diamond, has great potential for enhancing NMR-based quantum information processing and nanoscale magnetic resonance imaging. Recently, pulse-based protocols have been shown to efficiently transfer optically induced polarization of the electron defect spin to surrounding nuclear spins—at particular resonant pulse intervals. In this work, we investigate the performance of these protocols, both analytically and experimentally, with the electronic spin of a single NV defect. We find that whenever polarization resonances of nuclear spins are near degenerate with a “blocking” spin, which is single spin with stronger off-diagonal coupling to the electronic central spin, they are displaced out of the central resonant region—without, in general, significant weakening in the rate of polarization. We analyze the underlying physical mechanism and obtain a closed-form expression for the displacement. We propose that spin blocking represents a common but overlooked effect in hyperpolarization of nuclear spins and suggest solutions for improved protocol performance in the presence of (naturally occurring) blocking nuclear spins.