Wide-band nanoscale magnetic resonance spectroscopy using quantum relaxation of a single spin in diamond

We demonstrate an all-optical approach of nanoscale magnetic resonance (MR) spectroscopy whereby quantum relaxation (T1) of a single probe spin in diamond is monitored during a precise static magnetic field sweep to construct a spectrum of the surrounding spin environment. The method is inherently noninvasive as it involves no driving fields, and instead relies on the natural resonance between the quantum probe and target spins. As a proof of concept, we measure the T1-MR spectra across a wide band [megahertz (MHz) to gigahertz (GHz)] of a small ensemble of N14 impurities surrounding a single probe spin, providing information on both electron spin transitions (in the GHz range) and nuclear spin transitions (in the MHz range) of the N14 spin targets. Analysis of the T1-MR spectrum reveals that the electron spin transitions are probed via dipole interactions with the probe, while the relatively weak nuclear spin resonances are dramatically enhanced by hyperfine coupling in an electron-mediated process. With a projected sensitivity to external single-proton spins, this work establishes T1-MR as a powerful noninvasive wide-band technique for nanoscale MR spectroscopy.