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arXiv:2604.09310

Coherent Control of Nanoscale Nuclear Spin Ensembles in the Spin Noise Regime

Ana Martin, Roberto Rizzato, Carlos Munuera-Javaloy, Dileep Singh, Dominik B. Bucher, Jorge Casanova

quant-phcond-mat.mes-hallSubmitted Apr 10, 2026• Announced Apr 13, 2026
arXivHTMLPDF

Abstract

Spin defects in solids, such as the nitrogen-vacancy (NV) center in diamond, have emerged as a key tool for detecting nuclear spins at the nanoscale. While active nuclear spin control via radio-frequency (RF) irradiation is often unnecessary for standard spin-noise detection, it becomes essential for advanced protocols like multidimensional nanoscale NMR. In this work, we investigate nuclear spin control using correlation spectroscopy techniques. We demonstrate, both theoretically and experimentally, that the resulting nuclear spin dynamics depend critically on the initial RF phase and its orientation relative to the NV crystalline axis. Depending on these parameters, identical nuclear rotations can yield full, partial, or even vanishing contrast in the NV readout. These findings highlight a previously underappreciated aspect of spin manipulation in the spin-noise regime: the link between the phase and direction of the applied RF field and its direct impact on correlation-based experiments. Consequently, imperfect calibration of these parameters can lead to ambiguous signal contrasts and misinterpretation of the underlying nuclear spin dynamics. Our results provide deeper insight into nanoscale spin control and pave the way toward reliable multidimensional spin resonance experiments.

Comments
5 pages, 2 figures and 3 appendices

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Spin defects in solids, such as the nitrogen-vacancy (NV) center in diamond, have emerged as a key tool for detecting nuclear spins at the nanoscale. While active nuclear spin control via radio-frequency (RF) irradiation is often unnecessary for standard spin-noise detection, it becomes essential for advanced protocols like multidimensional nanoscale NMR. In this work, we investigate nuclear spin control using correlation spectroscopy techniques. We demonstrate, both theoretically and experimentally, that the resulting nuclear spin dynamics depend critically on the initial RF phase and its orientation relative to the NV crystalline axis. Depending on these parameters, identical nuclear rotations can yield full, partial, or even vanishing contrast in the NV readout. These findings highlight a previously underappreciated aspect of spin manipulation in the spin-noise regime: the link between the phase and direction of the applied RF field and its direct impact on correlation-based experiments. Consequently, imperfect calibration of these parameters can lead to ambiguous signal contrasts and misinterpretation of the underlying nuclear spin dynamics. Our results provide deeper insight into nanoscale spin control and pave the way toward reliable multidimensional spin resonance experiments.
Nuclear magnetic resonance (NMR) spectroscopy is widely used in fields ranging from chemistry, materials science to neuroscience. Nanoscale NMR spectroscopy using Nitrogen-vacancy (NV) centers in diamond has emerged as a promising platform due to an unprecedented sensitivity down to the single spin level. At the nanoscale, high nuclear spin polarization through spin fluctuations (statistical polarization) far outweighs thermal polarization. However, until now efficient NMR detection using coherent averaging techniques could not be applied to the detection of statistical polarization, leading to long measurement times. Here we present two protocols to enable coherent averaging of statistically oscillating signals through rectification. We demonstrate these protocols on an artificial radiofrequency signal detected with a single NV center at 2.7 T. The signal-to-noise scaling with number of measurements 𝑁 increases from 𝑁0.5 to 𝑁1, improving the measurement time significantly. The relevance of rectification for the detection of statistically polarized nuclear spins using ensembles of NV centers is outlined, paving the way for efficient nanoscale NMR spectroscopy.
Nuclear magnetic resonance (NMR) spectroscopy is widely used in fields ranging from chemistry and materials science to neuroscience. Nanoscale NMR spectroscopy using nitrogen-vacancy (NV) centers in diamond has emerged as a promising platform due to an unprecedented sensitivity down to the single spin level. At the nanoscale, high nuclear spin polarization through spin fluctuations (statistical polarization) far outweighs thermal polarization. However, until now efficient NMR detection using coherent averaging techniques could not be applied to the detection of statistical polarization, leading to long measurement times. Here we present two protocols to enable coherent averaging of stochastic oscillatory signals through rectification. We demonstrate these protocols on an artificial radio frequency signal detected with a single NV center at 2.7 T. The signal-to-noise scaling with number of measurements N increases from N^{0.5} to N^{1}, improving the measurement time significantly. The relevance of rectification for the detection of statistically polarized nuclear spins using ensembles of NV centers is outlined, paving the way for efficient nanoscale NMR spectroscopy.
Nuclear magnetic resonance spectroscopy with solid-state spin sensors is a promising pathway for the detection of nuclear spins at the micro- and nanoscale. Although many nanoscale experiments rely on a single sensor spin for the detection of the signal, leveraging spin ensembles can enhance sensitivity, particularly in cases in which the signal merely originates from statistically polarized nuclear spins. In this Letter, we introduce multipoint correlation spectroscopy, which combines the advantages of two well-established methods-correlation spectroscopy and quantum heterodyne detection-to enable temporally efficient measurements of statistically polarized samples at the nanoscale with spin ensembles. We present a theoretical framework for this approach and demonstrate an experimental proof of concept with a nitrogen vacancy center in diamond. We achieve single hertz uncertainty in the estimated signal frequency, highlighting the potential applications of the technique for nanoscale nuclear magnetic resonance.
Two-dimensional Nuclear Magnetic Resonance (NMR) is essential in molecular structure determination. The Nitrogen-Vacancy (NV) center in diamond has been proposed and developed as an outstanding quantum sensor to realize NMR in nanoscale. In this work, we develop a scheme for two-dimensional nanoscale NMR spectroscopy based on quantum controls on an NV center. We carry out a proof of principle experiment on a target of two coupled 13^{13}13C nuclear spins in diamond. A COSY-like sequences is used to acquire the data on time domain, which is then converted to frequency domain with the fast Fourier transform (FFT). With the two-dimensional NMR spectrum, the structure and location of the set of nuclear spin are resolved. This work marks a fundamental step towards resolving the structure of a single molecule.
Nuclear magnetic resonance (NMR) schemes can be applied to micron-, and nanometer-sized samples by the aid of quantum sensors such as nitrogen vacancy (NV) color centers in diamond. These minute devices allow for magnetometry of nuclear spin ensembles with high spatial and frequency resolution at ambient conditions, thus having a clear impact in different areas such as chemistry, biology, medicine, and material sciences. In practice, NV quantum sensors are driven by microwave (MW) control fields with a twofold objective: On the one hand, MW fields bridge the energy gap between NV and nearby nuclei which enables a coherent and selective coupling among them while, on the other hand, MW fields remove environmental noise on the NV leading to enhanced interrogation time. In this work we review distinct MW radiation patterns, or dynamical decoupling techniques, for nanoscale NMR applications.
Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically active electron, nuclear spins can be rapidly polarized, controlled, and read via lasers and radio-frequency (rf) fields. Possessing typical coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. In this work, we demonstrate optical nuclear-spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at 1kHz1\phantom{\rule{0.16em}{0ex}}\mathrm{kHz}1kHz, faster than the nuclear-spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in the presence of a large, time-varying magnetic field that makes an angle of more than ${100}^{\ensuremath{\circ}}$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation. We combine continuous dynamical decoupling with feed-forward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.