We investigate nuclear spin hyperpolarization from nitrogen vacancy centers in isotopically enriched diamonds with C concentrations up to 100%. C enrichment leads to hyperfine structure of the nitrogen vacancy electron spin resonance spectrum and as a result the spectrum of dynamic nuclear polarization. We show that strongly-coupled C spins in the first shell surrounding a nitrogen vacancy center generate resolved hyperfine splittings, but do not act as an intermediary in the transfer of hyperpolarization of bulk nuclear spins. High levels of C enrichment are desirable to increase the efficiency of hyperpolarizaiton for magnetic resonance signal enhancement, imaging contrast agents, and as a platform for quantum sensing and many-body physics.

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