Alex L. Melendez, Ruotian Gong, Guanghui He, Yan Wang, Yueh‐Chun Wu, Thomas Poirier, Steven Randolph, Sujoy Ghosh, Liangbo Liang, Stephen Jesse, An-Ping Li, Joshua T. Damron, Benjamin Lawrie, James H. Edgar, Ivan Vlassiouk, Chong Zu, Huan Zhao
Abstract Spin defects in solids offer promising platforms for quantum sensing and memory due to their long coherence times and optical addressability. Here, we integrate a single nitrogen-vacancy (NV) center in diamond with scanning probe microscopy to detect, read out, and spatially map spin-based quantum sensors at the nanoscale. Using the boron vacancy ( $${{{{\rm{V}}}}}_{{{{\rm{B}}}}}^{-}$$ V B − ) center in hexagonal boron nitride—an emerging two-dimensional spin system—as a model, we detect its electron spin resonance indirectly via changes in the spin relaxation time ( T 1 ) of a nearby NV center, eliminating the need for optical excitation or fluorescence detection of the $${{{{\rm{V}}}}}_{{{{\rm{B}}}}}^{-}$$ V B − . Cross-relaxation between NV and $${{{{\rm{V}}}}}_{{{{\rm{B}}}}}^{-}$$ V B − ensembles significantly reduces NV T 1 , enabling quantitative nanoscale mapping of defect densities beyond the optical diffraction limit and clear resolution of hyperfine splitting in isotopically enriched h 10 B 15 N. Our method demonstrates interactions between spin sensors in 3D and 2D materials, establishing NV centers as versatile probes for characterizing otherwise inaccessible spin defects.