High-Resolution NMR Spectroscopy at Large Fields with Nitrogen Vacancy Centers.

Ensembles of nitrogen-vacancy (NV) centers are used as sensors to detect nuclear magnetic resonance signals from micron-sized samples at room temperature. In this scenario, the regime of large magnetic fields is especially interesting as it leads to a large nuclear thermal polarization-thus, to a strong sensor response even in low concentration samples-while chemical shifts and J couplings become more accessible. Nevertheless, this regime remains largely unexplored owing to the difficulties of coupling NV-based sensors with high-frequency nuclear signals. In this Letter, we circumvent this problem with a method that maps the relevant energy shifts in the amplitude of an induced nuclear spin signal that is subsequently transferred to the sensor. This stage is interspersed with free-precession periods of the sample nuclear spins where the sensor does not participate. Thus, our method leads to high spectral resolutions ultimately limited by the coherence of the nuclear spin signal.