Parallel Accelerated Electron Paramagnetic Resonance Spectroscopy Using Diamond Sensors

The nitrogen-vacancy (NV) center can serve as a magnetic sensor for electron paramagnetic resonance (EPR) measurements. Benefiting from its atomic size, the diamond chip can integrate a tremendous amount of NV centers to improve the magnetic-field sensitivity. However, EPR spectroscopy using NV ensembles is less efficient due to inhomogeneities in both sensors and targets. Spectral line broadening induced by ensemble averaging is even detrimental to spectroscopy. Here we show a kind of cross-relaxation EPR spectroscopy at zero field, where the sensor is tuned by an amplitude-modulated control field to match the target. The modulation makes detection robust to the sensors inhomogeneity, while zero-field EPR is naturally robust to the targets inhomogeneity. We demonstrate an efficient EPR measurement on an ensemble of ∼30 000 NV centers. Our method shows the ability to not only acquire unambiguous EPR spectra of free radicals, but also monitor their spectroscopic dynamics in real time.