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arXiv:2503.18930 · Physical Review Letters

Quantum Memory Enhanced Multipoint Correlation Spectroscopy for Statistically Polarized NMR

Tobias Spohn, Nicolas Staudenmaier, Philipp J. Vetter, Timo Joas, Thomas Unden, Ilai Schwartz, Philipp Neumann, Genko T. Genov, Fedor Jelezko

Published Nov 19, 2025• 2 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/1cj2-rxkm

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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.
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 (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 provides unparalleled access to molecular structure and dynamics but is traditionally limited by weak signal strength, requiring large sample volumes and high magnetic fields. Here, we demonstrate nanoscale deuterium (2H) NMR spectroscopy using nitrogen vacancy (NV) centers in diamond, reproducing the characteristic quadrupolar powder line shapes that are present in the conventional bulk NMR spectra. By detecting statistical spin fluctuations from nanometer scale detection volumes, our approach delivers a sensitivity enhancement of six to eight orders of magnitude over inductive detection while operating at magnetic fields two orders of magnitude lower than those used in conventional NMR. Temperature dependent measurements of a deuterated polymer and molecular solid reveal distinct motional averaging and phase transitions with nanoscale sensitivity. Powder-like NV detected 2H NMR establishes a powerful tool for probing molecular dynamics on the nanoscale and, in the ultimate limit, at the single molecule level - capabilities beyond those of most existing spectroscopic techniques.
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.
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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.