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Nuclear magnetic resonance (NMR) imaging with shallow nitrogen-vacancy (NV)centers in diamond offers an exciting route toward sensitive and localizedchemical characterization at the nanoscale. Remarkable progress has been madeto combat the degradation in coherence time and stability suffered bynear-surface NV centers using suitable chemical surface termination. However,approaches that also enable robust control over adsorbed molecule density,orientation, and binding configuration are needed. We demonstrate a diamondsurface preparation for mixed nitrogen- and oxygen-termination thatsimultaneously improves NV center coherence times for emitters <10-nm-deep andenables direct and recyclable chemical functionalization via amine-reactivecrosslinking. Using this approach, we probe single NV centers embedded innanopillar waveguides to perform $^{19}\mathrm{F}$ NMR sensing of covalentlybound trifluoromethyl tags in the ca. 50-100 molecule regime. This worksignifies an important step toward nuclear spin localization and structureinterrogation at the single-molecule level.

Single Nitrogen-Vacancy-NMR of Amine-Functionalized Diamond Surfaces