ArXiv · 2026
Nuclear hyperpolarization from optically pumped color centers in solids offers an alternative to conventional microwave-driven dynamic nuclear polarization (DNP). Diamond can host the nitrogen vacancy (NV) center, whose ground spin state can be readily polarized by light at room temperature, making diamond a candidate platform for nuclear hyperpolarization. We report ¹³rm C nuclear hyperpolarization in randomly oriented diamond particles with sizes ranging from 0.2 to 2 μm, both at natural ¹³rm C abundance (1.1 %) and at 20 % isotopic enrichment, at magnetic fields of 7.1 T and 9.4 T. The protocol combines optical illumination with magic angle spinning (MAS) and does not require microwave irradiation. By investigating the nuclear polarization as a function of the MAS frequency between 0 and 6 kHz at the magnetic field of 7.1 T, we find maximum light-induced polarization enhancements of 280-fold for the isotopically enriched sample and 411-fold for the natural abundance sample. Under continuous illumination, steady-state absolute ¹³rm C polarization levels above 0.1 % are reached. A model involving optical pumping of NV centers and spin dynamics near level anticrossings (LACs) in three-spin clusters formed by NV, a substitutional nitrogen (P1) and ¹³rm C is used to describe these findings. The protocol strongly mitigates the effect of the anisotropy of the NV spin Hamiltonian, allowing more than 99.9% of NV orientations to participate in the polarization transfer process. These results represent a first step toward transferring nuclear polarization from diamond particles to external nuclei, with potential applications in sensitive and high-resolution NMR at room temperature.
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