Nanoscale Vector Electric Field Imaging Using a Single Electron Spin.

The ability to perform nanoscale electric field imaging of elementary charges at ambient temperatures will have diverse interdisciplinary applications. While the nitrogen-vacancy (NV) center in diamond is capable of high-sensitivity electrometry, demonstrations have so far been limited to macroscopic field features or detection of single charges internal to the diamond itself. In this work, we greatly extend these capabilities by using a shallow NV center to image the electric field of a charged atomic force microscope tip with nanoscale resolution. This is achieved by measuring Stark shifts in the NV spin-resonance due to AC electric fields. We demonstrate a near single-charge sensitivity of ηe = 5.3 charges/√Hz and subelementary charge detection (0.68e). This proof-of-concept experiment provides the motivation for further sensing and imaging of electric fields using NV centers in diamond.

Nanomechanical Sensing Using Spins in Diamond.

Nanomechanical sensors and quantum nanosensors are two rapidly developing technologies that have diverse interdisciplinary applications in biological and chemical analysis and microscopy. For example, nanomechanical sensors based upon nanoelectromechanical systems (NEMS) have demonstrated chip-scale mass spectrometry capable of detecting single macromolecules, such as proteins. Quantum nanosensors based upon electron spins of negatively charged nitrogen-vacancy (NV) centers in diamond have demonstrated diverse modes of nanometrology, including single molecule magnetic resonance spectroscopy. Here, we report the first step toward combining these two complementary technologies in the form of diamond nanomechanical structures containing NV centers. We establish the principles for nanomechanical sensing using such nanospin-mechanical sensors (NSMS) and assess their potential for mass spectrometry and force microscopy. We predict that NSMS are able to provide unprecedented AC force images of cellular biomechanics and to not only detect the mass of a single macromolecule but also image its distribution. When combined with the other nanometrology modes of the NV center, NSMS potentially offer unparalleled analytical power at the nanoscale.

Quantum Metrology Enhanced by Repetitive Quantum Error Correction.

We experimentally demonstrate the protection of a room-temperature hybrid spin register against environmental decoherence by performing repeated quantum error correction whilst maintaining sensitivity to signal fields. We use a long-lived nuclear spin to correct multiple phase errors on a sensitive electron spin in diamond and realize magnetic field sensing beyond the time scales set by natural decoherence. The universal extension of sensing time, robust to noise at any frequency, demonstrates the definitive advantage entangled multiqubit systems provide for quantum sensing and offers an important complement to quantum control techniques.

Detection of atomic spin labels in a lipid bilayer using a single-spin nanodiamond probe.

Magnetic field fluctuations arising from fundamental spins are ubiquitous in nanoscale biology, and are a rich source of information about the processes that generate them. However, the ability to detect the few spins involved without averaging over large ensembles has remained elusive. Here, we demonstrate the detection of gadolinium spin labels in an artificial cell membrane under ambient conditions using a single-spin nanodiamond sensor. Changes in the spin relaxation time of the sensor located in the lipid bilayer were optically detected and found to be sensitive to near-individual (4 ± 2) proximal gadolinium atomic labels. The detection of such small numbers of spins in a model biological setting, with projected detection times of 1 s [corresponding to a sensitivity of ∼5 Gd spins per Hz(1/2)], opens a pathway for in situ nanoscale detection of dynamical processes in biology.

Optical depth localization of nitrogen-vacancy centers in diamond with nanometer accuracy.

Precise positioning of nitrogen-vacancy (NV) centers is crucial for their application in sensing and quantum information. Here we present a new purely optical technique enabling determination of the NV position with nanometer resolution. We use a confocal microscope to determine the position of individual emitters along the optical axis. Using two separate detection channels, it is possible to simultaneously measure reflected light from the diamond surface and fluorescent light from the NV center and statistically evaluate both signals. An accuracy of 2.6 nm for shallow NV centers was achieved and is consistent with other techniques for depth determination.

Electronic properties and metrology applications of the diamond NV- center under pressure.

The negatively charged nitrogen-vacancy (NV-) center in diamond has realized new frontiers in quantum technology. Here, the optical and spin resonances of the NV- center are observed under hydrostatic pressures up to 60 GPa. Our results motivate powerful new techniques to measure pressure and image high-pressure magnetic and electric phenomena. Additionally, molecular orbital analysis and semiclassical calculations provide insight into the effects of compression on the electronic orbitals of the NV- center.

Plasmonic lenses formed by two-dimensional nanometric cross-shaped aperture arrays for Fresnel-region focusing.

We present the experimental demonstration of what are to our knowledge the first two-dimensional planar plasmonic lenses formed by an array of spatially varying cross-shaped apertures in a metallic film for Fresnel-region focusing. The design utilizes localized surface plasmon resonances occurring inside the apertures, accompanied by an aperture geometry dependent phase shift, to achieve the desired spatial phase modulation in the transmitted field. The performance of lenses with different design configurations was evaluated using a confocal scanning optical microscope, and the effects of diffraction on the optical response of these microscale devices are discussed.

NV center based nano-NMR enhanced by deep learning.

The growing field of nano nuclear magnetic resonance (nano-NMR) seeks to estimate spectra or discriminate between spectra of minuscule amounts of complex molecules. While this field holds great promise, nano-NMR experiments suffer from detrimental inherent noise. This strong noise masks to the weak signal and results in a very low signal-to-noise ratio. Moreover, the noise model is usually complex and unknown, which renders the data processing of the measurement results very complicated. Hence, spectra discrimination is hard to achieve and in particular, it is difficult to reach the optimal discrimination. In this work we present strong indications that this difficulty can be overcome by deep learning (DL) algorithms. The DL algorithms can mitigate the adversarial effects of the noise efficiently by effectively learning the noise model. We show that in the case of frequency discrimination DL algorithms reach the optimal discrimination without having any pre-knowledge of the physical model. Moreover, the DL discrimination scheme outperform Bayesian methods when verified on noisy experimental data obtained by a single Nitrogen-Vacancy (NV) center. In the case of frequency resolution we show that this approach outperforms Bayesian methods even when the latter have full pre-knowledge of the noise model and the former has none. These DL algorithms also emerge as much more efficient in terms of computational resources and run times. Since in many real-world scenarios the noise is complex and difficult to model, we argue that DL is likely to become a dominant tool in the field.

Blueprint for nanoscale NMR.

Nitrogen vacancy (NV) centers in diamond have been used as ultrasensitive magnetometers to perform nuclear magnetic resonance (NMR) spectroscopy of statistically polarized samples at 1-100 nm length scales. However, the spectral linewidth is typically limited to the kHz level, both by the NV sensor coherence time and by rapid molecular diffusion of the nuclei through the detection volume which in turn is critical for achieving long nuclear coherence times. Here we provide a blueprint supported by detailed theoretical analysis for a set-up that combines a sensitivity sufficient for detecting NMR signals from nano- to micron-scale samples with a spectral resolution that is limited only by the nuclear spin coherence, i.e. comparable to conventional NMR. Our protocol detects the nuclear polarization induced along the direction of an external magnetic field with near surface NV centers using lock-in detection techniques to enable phase coherent signal averaging. Using the NV centers in a dual role of NMR detector and optical hyperpolarization source to increase signal to noise, and in combination with Bayesian inference models for signal processing, nano/microscale NMR spectroscopy can be performed on sample concentrations in the micromolar range, several orders of magnitude better than the current state of the art.

Quantum measurement of a rapidly rotating spin qubit in diamond.

A controlled qubit in a rotating frame opens new opportunities to probe fundamental quantum physics, such as geometric phases in physically rotating frames, and can potentially enhance detection of magnetic fields. Realizing a single qubit that can be measured and controlled during physical rotation is experimentally challenging. We demonstrate quantum control of a single nitrogen-vacancy (NV) center within a diamond rotated at 200,000 rpm, a rotational period comparable to the NV spin coherence time T2. We stroboscopically image individual NV centers that execute rapid circular motion in addition to rotation and demonstrate preparation, control, and readout of the qubit quantum state with lasers and microwaves. Using spin-echo interferometry of the rotating qubit, we are able to detect modulation of the NV Zeeman shift arising from the rotating NV axis and an external DC magnetic field. Our work establishes single NV qubits in diamond as quantum sensors in the physically rotating frame and paves the way for the realization of single-qubit diamond-based rotation sensors.

Submillihertz magnetic spectroscopy performed with a nanoscale quantum sensor.

Precise timekeeping is critical to metrology, forming the basis by which standards of time, length, and fundamental constants are determined. Stable clocks are particularly valuable in spectroscopy because they define the ultimate frequency precision that can be reached. In quantum metrology, the qubit coherence time defines the clock stability, from which the spectral linewidth and frequency precision are determined. We demonstrate a quantum sensing protocol in which the spectral precision goes beyond the sensor coherence time and is limited by the stability of a classical clock. Using this technique, we observed a precision in frequency estimation scaling in time T as T-3/2 for classical oscillating fields. The narrow linewidth magnetometer based on single spins in diamond is used to sense nanoscale magnetic fields with an intrinsic frequency resolution of 607 microhertz, which is eight orders of magnitude narrower than the qubit coherence time.

Stimulated emission from nitrogen-vacancy centres in diamond.

Stimulated emission is the process fundamental to laser operation, thereby producing coherent photon output. Despite negatively charged nitrogen-vacancy (NV-) centres being discussed as a potential laser medium since the 1980s, there have been no definitive observations of stimulated emission from ensembles of NV- to date. Here we show both theoretical and experimental evidence for stimulated emission from NV- using light in the phonon sidebands around 700 nm. Furthermore, we show the transition from stimulated emission to photoionization as the stimulating laser wavelength is reduced from 700 to 620 nm. While lasing at the zero-phonon line is suppressed by ionization, our results open the possibility of diamond lasers based on NV- centres, tuneable over the phonon sideband. This broadens the applications of NV- magnetometers from single centre nanoscale sensors to a new generation of ultra-precise ensemble laser sensors, which exploit the contrast and signal amplification of a lasing system.

Scalable fabrication of high-quality, ultra-thin single crystal diamond membrane windows.

High quality, ultra-thin single crystal diamond (SCD) membranes that have a thickness in the sub-micron range are of extreme importance as a materials platform for photonics, quantum sensing, nano/micro electro-mechanical systems (N/MEMS) and other diverse applications. However, the scalable fabrication of such thin SCD membranes is a challenging process. In this paper, we demonstrate a new method which enables high quality, large size (∼4 × 4 mm) and low surface roughness, low strain, ultra-thin SCD membranes which can be fabricated without deformations such as breakage, bowing or bending. These membranes are easy to handle making them particularly suitable for fabrication of optical and mechanical devices. We demonstrate arrays of single crystal diamond membrane windows (SCDMW), each up to 1 × 1 mm in dimension and as thin as ∼300 nm, supported by a diamond frame as thick as ∼150 µm. The fabrication method is robust, reproducible, scalable and cost effective. Microwave plasma chemical vapour deposition is used for in situ creation of single nitrogen-vacancy (NV) centers into the thin SCDMW. We have also developed SCD drum head mechanical resonator composed of our fully clamped and freely suspended membranes.

Near-surface spectrally stable nitrogen vacancy centres engineered in single crystal diamond.

A method for engineering thin (<100 nm) layers of homoepitaxial diamond containing high quality, spectrally stable, isolated nitrogen-vacancy (NV) centres is reported. The photoluminescence excitation linewidth of the engineered NVs are as low as 140 MHz, at temperatures below 12 K, while the spin properties are at a level suitable for quantum memory and spin register applications. This methodology of NV fabrication is an important step toward scalable and practical diamond based photonic devices suitable for quantum information processing.