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Dynamic nuclear polarisation, which transfers the spin polarisation ofelectrons to nuclei, is routinely applied to enhance the sensitivity of nuclearmagnetic resonance; it is also critical in spintronics, particularly when spinhyperpolarisation can be produced and controlled optically or electrically.Here we show the complete polarisation of nuclei located near theoptically-polarised nitrogen-vacancy (NV) centre in diamond. When approachingthe ground-state level anti-crossing condition of the NV electron spins, 13Cnuclei in the first-shell are polarised in a pattern that depends sensitivelyand sharply upon the magnetic field. Based on the anisotropy of the hyperfinecoupling and of the optical polarisation mechanism, we predict and observe acomplete reversal of the nuclear spin polarisation with a few-mT change in themagnetic field. The demonstrated sensitive magnetic control of nuclearpolarisation at room temperature will be useful for sensitivity-enhanced NMR,nuclear-based spintronics, and quantum computation in diamond.

Sensitive Magnetic Control of Ensemble Nuclear Spin Hyperpolarisation in Diamond