Optically-detected broadband paramagnetic resonance spectroscopy using NV centers in diamond

Nitrogen-vacancy (NV) centers in diamond provide an excellent platform for high sensitivity nanoscale magnetic resonance (MR) spectroscopy in ambient conditions. We present a broadband approach to detecting paramagnetic resonance that enables spectroscopic studies under diverse conditions of field magnitude and orientation. This easily implementable, relaxation-based protocol requires neither direct microwave manipulation of the NV spins nor spectral overlap between NV and target spin resonances. We demonstrate MR spectroscopy of paramagnetic P1 defect center spins in diamond whose spectra are clearly identifiable by their dispersions and anisotropic hyperfine structure. We propose that the unexpected sensitivity of NV spins to excitation of P1 resonances results from phonon-mediated NV-P1 cross relaxation. Extending our technique to spins outside the diamond would make it particularly effective for broadband studies, characterizing anisotropic materials, and probing dynamical processes at submicron scales.