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High-Pressure NMR Enabled by Diamond Nitrogen-Vacancy Centers

The integration of NMR and high pressure technique brings unique opportunities to study electronic, structural and dynamical properties under extreme conditions. Despite a great degree of success has been achieved using coil-based schemes, the contradictory requirement on sample volume of these two techniques remains an outstanding challenge. In this letter, we introduce diamond nitrogen-vacancy (NV) centers, as the source and probe of in-situ nuclear spin polarization, to address the sample volume issue. We demonstrate hyperpolarization and coherent control of $^{14}$N nuclear spins under high pressures. NMR spectra of a micro-diamond are measured up to 16.6 GPa, and unexpected pressure shift of the $^{14}$N nuclear quadrupole and hyperfine coupling terms are observed. Our work contributes to quantum sensing enhanced spectrometry under extreme conditions.