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Nanodiamond (ND) hosting nitrogen-vacancy (NV) centers is a promisingplatform for quantum sensing applications. Sensitivity of the applicationsusing NV centers in NDs is often limited due to presence of paramagneticimpurity contents near the ND surface. Here, we investigate near-surfaceparamagnetic impurities in NDs. Using high-frequency (HF) electron paramagneticresonance spectroscopy, the near-surface paramagnetic impurity within the shellof NDs is probed and its g-value is determined to be 2.0028(3). Furthermore, HFelectron-electron double resonance-detected nuclear magnetic resonancespectroscopy and a first principle calculation show that a possible structureof the near-surface impurity is the negatively charged vacancy V-. Theidentification of the near-surface impurity by the present investigationprovides a promising pathway to improve the NV properties in NDs and theNV-based sensing techniques.

Investigation of Near-Surface Defects of Nanodiamonds by High-Frequency EPR and DFT Calculation