Quantum Heterodyne Sensing of Nuclear Spins via Double Resonance

Nanoscale nuclear magnetic resonance (NMR) signals can be measured through hyperfine interaction to paramagnetic electron sensor spins. A heterodyne approach is widely used to overcome the electron spin lifetime limit in spectral resolution. It uses a series of modified Hahn echo pulse sequences applied coherently with precession signal resulting in a subsampled NMR signal. Due to challenges with applying high electron Rabi frequencies its application is limited to low fields, thus the full potential of the method is not yet exploited at high magnetic fields, beneficial for NMR. Here we present heterodyne detection utilizing a series of phase coherent electron nuclear double resonance sensing blocks which extends nanoscale NMR protocols to arbitrary magnetic fields. We demonstrate this principle on a single NV center, both with an intrinsic $^{14}$N and a weekly coupled $^{13}$C nuclear spin in the bath surrounding single NV centres. We compare our protocol to existing heterodyne protocols and discuss its prospects. This work paves the way towards high field nanoscale heterodyne NMR protocols with NV centres which is crucial for reducing sample volumes and improving chemical resolution.