The Nitrogen-Vacancy (NV) defect in diamond is a unique quantum system that offers precision sensing of nanoscale physical quantities beyond the current state-of-the-art. Here we present a method to controllably encode the interactions in the population of the spin states, thereby introducing a way to control the sensitivity of a single spin as a continuum in contrast to free-evolution based methods. By adopting this feature we demonstrate high-accuracy NV magnetometry without 2pi ambiguities, enhance the dynamic range by a factor of 4*10^3 achieve interaction times exceeding 2 ms in off-the-shelf diamond. We perform nuclear spin-noise spectroscopy in the frequency domain by dynamically controlling the NV spins sensitivity piecewise and in a smooth manner thereby precluding harmonic artefacts and undesired interactions. On a broader perspective dynamical sensitivity control provides an elegant handle on the inherent dynamics of quantum systems, while offering decisive advantages for NV centre applications notably in quantum controls and single molecule NMR/MRI.
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