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arXiv:1806.02181 · Nature Communications

High-resolution spectroscopy of single nuclear spins via sequential weak measurements

Matthias Pfender, Ping Wang, Hitoshi Sumiya, Shinobu Onoda, Wen Yang, Durga Bhaktavatsala Rao Dasari, Philipp Neumann, Xinyu Pan, Junichi Isoya, Ren‐Bao Liu, Jörg Wrachtrup

Published Feb 5, 2019• 94 citations
arXivHTMLPDF

Abstract

Abstract Nuclear magnetic resonance (NMR) of single spins have recently been detected by quantum sensors. However, the spectral resolution has been limited by the sensor’s relaxation to a few kHz at room temperature. This can be improved by using quantum memories, at the expense of sensitivity. In contrast, classical signals can be measured with exceptional spectral resolution by using continuous measurement techniques, without compromising sensitivity. When applied to single-spin NMR, it is critical to overcome the impact of back action inherent of quantum measurement. Here we report sequential weak measurements on a single 13C nuclear spin. The back-action causes the spin to undergo a quantum dynamics phase transition from coherent trapping to coherent oscillation. Single-spin NMR at room-temperature with a spectral resolution of 3.8 Hz is achieved. These results enable the use of measurement-correlation schemes for the detection of very weakly coupled single spins.

DOI
10.1038/s41467-019-08544-z

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Abstract Nuclear magnetic resonance (NMR) of single spins have recently been detected by quantum sensors. However, the spectral resolution has been limited by the sensor’s relaxation to a few kHz at room temperature. This can be improved by using quantum memories, at the expense of sensitivity. In contrast, classical signals can be measured with exceptional spectral resolution by using continuous measurement techniques, without compromising sensitivity. When applied to single-spin NMR, it is critical to overcome the impact of back action inherent of quantum measurement. Here we report sequential weak measurements on a single 13C nuclear spin. The back-action causes the spin to undergo a quantum dynamics phase transition from coherent trapping to coherent oscillation. Single-spin NMR at room-temperature with a spectral resolution of 3.8 Hz is achieved. These results enable the use of measurement-correlation schemes for the detection of very weakly coupled single spins.
Nuclear magnetic resonance (NMR) spectroscopy is a powerful technique for analyzing the structure and function of molecules, and for performing three-dimensional imaging of the spin density. At the heart of NMR spectrometers is the detection of electromagnetic radiation, in the form of a free induction decay (FID) signal, generated by nuclei precessing around an applied magnetic field. While conventional NMR requires signals from 1e12 or more nuclei, recent advances in sensitive magnetometry have dramatically lowered this number to a level where few or even individual nuclear spins can be detected. It is natural to ask whether continuous FID detection can still be applied at the single spin level, or whether quantum back-action modifies or even suppresses the NMR response. Here we report on tracking of single nuclear spin precession using periodic weak measurements. Our experimental system consists of carbon-13 nuclear spins in diamond that are weakly interacting with the electronic spin of a nearby nitrogen-vacancy center, acting as an optically readable meter qubit. We observe and minimize two important effects of quantum back-action: measurement-induced decoherence and frequency synchronization with the sampling clock. We use periodic weak measurements to demonstrate sensitive, high-resolution NMR spectroscopy of multiple nuclear spins with a priori unknown frequencies. Our method may provide the optimum route for performing single-molecule NMR at atomic resolution.
Nuclear magnetic resonance (NMR) spectroscopy is a powerful technique for analyzing the structure and function of molecules, and for performing three-dimensional imaging of the spin density. At the heart of NMR spectrometers is the detection of electromagnetic radiation, in the form of a free induction decay (FID) signal, generated by nuclei precessing around an applied magnetic field. While conventional NMR requires signals from 1e12 or more nuclei, recent advances in sensitive magnetometry have dramatically lowered this number to a level where few or even individual nuclear spins can be detected. It is natural to ask whether continuous FID detection can still be applied at the single spin level, or whether quantum back-action modifies or even suppresses the NMR response. Here we report on tracking of single nuclear spin precession using periodic weak measurements. Our experimental system consists of a 13C nuclear spin in diamond that is weakly interacting with the electronic spin of a nearby nitrogen-vacancy center, acting as an optically readable meter qubit. We observe and minimize two important effects of quantum back-action: Measurement-induced decoherence and frequency synchronization with the sampling clock. We use weak measurements to demonstrate nanoscale NMR spectroscopy with a simultaneous enhancement of the signal-to-noise ratio (SNR), frequency bandwidth and spectral resolution. Our method may provide the optimum route for performing single-molecule NMR at atomic resolution.
Abstract We realize a two-qubit sensor designed for achieving high-spectral resolution in quantum sensing experiments. Our sensor consists of an active “sensing qubit” and a long-lived “memory qubit”, implemented by the electronic and the nitrogen-15 nuclear spins of a nitrogen-vacancy center in diamond, respectively. Using state storage times of up to 45 ms, we demonstrate spectroscopy of external ac signals with a line width of 19 Hz (∼2.9 ppm) and of carbon-13 nuclear magnetic resonance signals with a line width of 190 Hz (∼74 ppm). This represents an up to 100-fold improvement in spectral resolution compared to measurements without nuclear memory.
We realize a two-qubit sensor designed for achieving high spectral resolution in quantum sensing experiments. Our sensor consists of an active "sensing qubit" and a long-lived "memory qubit", implemented by the electronic and the nitrogen-15 nuclear spins of a nitrogen-vacancy center in diamond, respectively. Using state storage times of up to 45 ms, we demonstrate spectroscopy of external ac signals with a line width of 19 Hz (~2.9 ppm) and of carbon-13 nuclear magnetic resonance (NMR) signals with a line width of 190 Hz (~ 74 ppm). This represents an up to 100-fold improvement in spectral resolution compared to measurements without nuclear memory.
In nanoscale metrology, dissipation of the sensor limits its performance. Strong dissipation has a negative impact on sensitivity, and sensor-target interaction even causes relaxation or dephasing of the latter. The weak dissipation of nitrogen-vacancy (NV) sensors in room temperature diamond enables detection of individual target nuclear spins, yet limits the spectral resolution of nuclear magnetic resonance (NMR) spectroscopy to several hundred Hertz, which typically prevents molecular recognition. Here, we use the NV intrinsic nuclear spin as a nonvolatile classical memory to store NMR information, while suppressing sensor back-action on the target using controlled decoupling of sensor, memory, and target. We demonstrate memory lifetimes up to 4 min and apply measurement and decoupling protocols, which exploit such memories efficiently. Our universal NV-based sensor device records single-spin NMR spectra with 13 Hz resolution at room temperature.Dissipation of the sensor is a limiting factor in metrology. Here, Pfender et al. suppress this effect employing the nuclear spin of an NV centre for robust intermediate storage of classical NMR information, allowing then to record single-spin NMR spectra with 13 Hz resolution at room temperature.
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.