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arXiv:1610.05675 · Nature Communications

Nonvolatile nuclear spin memory enables sensor-unlimited nanoscale spectroscopy of small spin clusters

Matthias Pfender, Nabeel Aslam, Hitoshi Sumiya, Shinobu Onoda, Philipp Neumann, Junichi Isoya, Carlos A. Meriles, Jörg Wrachtrup

Published Oct 4, 2017• 81 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1038/s41467-017-00964-z

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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.
Abstract The Nitrogen-Vacancy (NV) defect in diamond is a unique quantum system that offers precision sensing of nanoscale physical quantities at room temperature beyond the current state-of-the-art. The benchmark parameters for nanoscale magnetometry applications are sensitivity, spectral resolution, and dynamic range. Under realistic conditions the NV sensors controlled by conventional sensing schemes suffer from limitations of these parameters. Here we experimentally show a new method called dynamical sensitivity control (DYSCO) that boost the benchmark parameters and thus extends the practical applicability of the NV spin for nanoscale sensing. In contrast to conventional dynamical decoupling schemes, where π pulse trains toggle the spin precession abruptly, the DYSCO method allows for a smooth, analog modulation of the quantum probe’s sensitivity. Our method decouples frequency selectivity and spectral resolution unconstrained over the bandwidth (1.85 MHz–392 Hz in our experiments). Using DYSCO we demonstrate high-accuracy NV magnetometry without |2π| ambiguities, an enhancement of the dynamic range by a factor of 4 · 103, and interrogation times exceeding 2 ms in off-the-shelf diamond. In a broader perspective the DYSCO method provides a handle on the inherent dynamics of quantum systems offering decisive advantages for NV centre based applications notably in quantum information and single molecule NMR/MRI.
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.
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.
Abstract 2D nuclear magnetic resonance (NMR) is essential in molecular structure determination. The nitrogen vacancy (NV) center in diamond is proposed and developed as an outstanding quantum sensor to realize NMR in nanoscale. In this work, a scheme for 2D nanoscale NMR spectroscopy is developed based on quantum controls on an NV center. A proof‐of‐principle experiment on a target of two coupled nuclear spins in diamond is carried out. A correlation spectroscopy (COSY) like sequence is used to acquire the data on time domain, which is then converted to frequency domain with the fast Fourier transform. With the 2D NMR spectrum, the structure and location of the set of nuclear spin are resolved. This work marks a fundamental step toward resolving the structure of a single molecule.
Quantum technologies are expected to significantly change our world in the next decades and the possible applications are diverse – ranging from quantum computation and encryption to metrology with unprecedented sensitivity. This thesis focuses on quantum sensing and imaging based on single nitrogen-vacancy (NV) centres in diamond to measure magnetic fields. Its electronic spin qualifies this point defect as a highly sensitive quantum sensor and its atomic size offers nanoscale spatial resolution. The simple optical initialisation and readout, together with the relatively long coherence time at ambient conditions, make NV centres promising candidates for biological applications and in particular for nuclear magnetic resonance (NMR) on the nanoscale. Recording the spectral information on the nanoscale allows to determine the structure of single or just a few molecules. However, the current main problems and challenges include insufficient spectral resolution, artificial signals and overall poor performance. In this thesis new spectroscopic techniques which tackle these issues are presented. First, it is shown that by randomisation of control pulse phases spurious harmonic signals can be suppressed, which otherwise complicate spectrum interpretation and can lead to false signal identification. At the same time the effects of pulse imperfections are mitigated. Furthermore, a protocol allowing to measure with a coherence independent spectral resolution is presented. It is demonstrated that linewidths below 1mHz are possible, which is an improvement of more than seven orders of magnitude compared to traditional methods. Due to its simple implementation, the protocol is relevant for many applications. Initially developed to measure signals oscillating up to several megahertz, it is further shown that modifications allow to extend the frequency range into the gigahertz domain. Finally, quantum frequency discrimination with the task to differentiate between two frequency distributions using a quantum sensor is analysed. An optimised protocol is introduced and the influences of different readout strategies are discussed with respect to the probability to make an incorrect decision. These findings are useful for diagnostic tests in NMR.
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.