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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., Comment: 29 pages including methods and extended data figures; for supplementary material, see v1 of this submission

We report on precise localization spectroscopy experiments of individual 13C nuclear spins near a central electronic sensor spin in a diamond chip. By detecting the nuclear free precession signals in rapidly switchable external magnetic fields, we retrieve the three-dimensional spatial coordinates of the nuclear spins with sub-Angstrom resolution and for distances beyond 10 Angstroms. We further show that the Fermi contact contribution can be constrained by measuring the nuclear g-factor enhancement. The presented method will be useful for mapping the atomic-scale structure of single molecules, an ambitious yet important goal of nanoscale nuclear magnetic resonance spectroscopy.

Quantum sensing takes advantage of well controlled quantum systems for performing measurements with high sensitivity and precision. We have implemented a concept for quantum sensing with arbitrary frequency resolution, independent of the qubit probe and limited only by the stability of an external synchronization clock. Our concept makes use of quantum lock-in detection to continuously probe a signal of interest. Using the electronic spin of a single nitrogen vacancy center in diamond, we demonstrate detection of oscillating magnetic fields with a frequency resolution of 70 uHz over a MHz bandwidth. The continuous sampling further guarantees an excellent sensitivity, reaching a signal-to-noise ratio in excess of 10,000:1 for a 170 nT test signal measured during a one-hour interval. Our technique has applications in magnetic resonance spectroscopy, quantum simulation, and sensitive signal detection., Comment: Manuscript resubmitted to Science. Includes Supplementary Materials

We investigate the application of amplitude-shaped control pulses for enhancing the time and frequency resolution of multipulse quantum sensing sequences. Using the electronic spin of a single nitrogen vacancy center in diamond and up to 10,000 coherent microwave pulses with a cosine square envelope, we demonstrate 0.6 ps timing resolution for the interpulse delay. This represents a refinement by over 3 orders of magnitude compared to the 2 ns hardware sampling. We apply the method for the detection of external AC magnetic fields and nuclear magnetic resonance signals of carbon-13 spins with high spectral resolution. Our method is simple to implement and especially useful for quantum applications that require fast phase gates, many control pulses, and high fidelity., Comment: 5 pages, 4 figures, plus supplemental material

We report hyperpolarization of the electronic spins associated with substitutional nitrogen defects in bulk diamond crystal. Hyperpolarization is achieved by optical pumping of nitrogen vacancy centers followed by rapid cross relaxation at the energy level matching condition in a 51 mT bias field. The maximum observed donor spin polarization is 0.9 \% corresponding to an enhancement by 25 compared to the thermal Boltzmann polarization. A further accumulation of polarization is impeded by an anomalous optical saturation effect that we attribute to charge state conversion processes. Hyperpolarized nitrogen donors may form a useful resource for increasing the efficiency of diamond-based dynamic nuclear polarization devices., Comment: 15 pages, 4 figures

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., Comment: 4 pages with 5 figures. Supplemental material is included

We report on Fourier spectroscopy experiments performed with near-surface nitrogen-vacancy centers in a diamond chip. By detecting the free precession of nuclear spins rather than applying a multipulse quantum sensing protocol, we are able to unambiguously identify the NMR species devoid of harmonics. We further show that by engineering different Hamiltonians during free precession, the hyperfine coupling parameters as well as the nuclear Larmor frequency can be selectively measured with high precision (here 5 digits). The protocols can be combined to demonstrate two-dimensional Fourier spectroscopy. The technique will be useful for mapping nuclear coordinates in molecules en route to imaging their atomic structure., Comment: 5 pages, 5 figures

Multipulse sequences based on Carr-Purcell decoupling are frequently used for narrow-band signal detection in single spin magnetometry. We have analyzed the behavior of multipulse sensing sequences under real-world conditions, including finite pulse durations and the presence of detunings. We find that these non-idealities introduce harmonics to the filter function, allowing additional frequencies to pass the filter. In particular, we find that the XY family of sequences can generate signals at the 2fac, 4fac and 8fac harmonics and their odd subharmonics, where fac is the ac signal frequency. Consideration of the harmonic response is especially important for diamond-based nuclear spin sensing where the NMR frequency is used to identify the nuclear spin species, as it leads to ambiguities when several isotopes are present., Comment: 6 pages, 7 figures

We present nanofabrication and mechanical measurements of single-crystal diamond cantilevers with thickness down to 85 nm, thickness uniformity better than 20 nm, and lateral dimensions up to 240 um. Quality factors exceeding one million are found at room temperature, surpassing those of state-of-the-art single-crystal silicon cantilevers of similar dimensions by roughly an order of magnitude. Force sensitivities of a few hundred zeptonewtons result for the best cantilevers at millikelvin temperatures. Single-crystal diamond could thus directly improve existing force and mass sensors by a simple substitution of resonator material, and lead to quantum nanomechanical devices with exceptionally low energy dissipation.