Addressing Single Nuclear Spins Quantum Memories by a Central Electron Spin.

Nuclei surrounding single electron spins are valuable resources for quantum technology. For application in this area, one is often interested in weakly coupled nuclei with coupling strength on the order of a few 10-100 kHz. In this paper, we compare methods to address single nuclear spins with this type of hyperfine coupling to a single electron spin. To achieve the required spectral resolution, we specifically focus on two methods, namely dynamical decoupling and correlation spectroscopy. We demonstrate spectroscopy of two single nuclear spins and present a method to derive components of their hyperfine coupling tensor from those measurements.

Quantum error correction in a solid-state hybrid spin register.

Error correction is important in classical and quantum computation. Decoherence caused by the inevitable interaction of quantum bits with their environment leads to dephasing or even relaxation. Correction of the concomitant errors is therefore a fundamental requirement for scalable quantum computation. Although algorithms for error correction have been known for some time, experimental realizations are scarce. Here we show quantum error correction in a heterogeneous, solid-state spin system. We demonstrate that joint initialization, projective readout and fast local and non-local gate operations can all be achieved in diamond spin systems, even under ambient conditions. High-fidelity initialization of a whole spin register (99 per cent) and single-shot readout of multiple individual nuclear spins are achieved by using the ancillary electron spin of a nitrogen-vacancy defect. Implementation of a novel non-local gate generic to our electron-nuclear quantum register allows the preparation of entangled states of three nuclear spins, with fidelities exceeding 85 per cent. With these techniques, we demonstrate three-qubit phase-flip error correction. Using optimal control, all of the above operations achieve fidelities approaching those needed for fault-tolerant quantum operation, thus paving the way to large-scale quantum computation. Besides their use with diamond spin systems, our techniques can be used to improve scaling of quantum networks relying on phosphorus in silicon, quantum dots, silicon carbide or rare-earth ions in solids.

Nanoscale Spin Manipulation with Pulsed Magnetic Gradient Fields from a Hard Disc Drive Writer.

The individual and coherent control of solid-state based electron spins is important covering fields from quantum information processing and quantum metrology to material research and medical imaging. Especially for the control of individual spins in nanoscale networks, the generation of strong, fast, and localized magnetic fields is crucial. Highly engineered devices that demonstrate most of the desired features are found in nanometer size magnetic writers of hard disk drives (HDD). Currently, however, their nanoscale operation in particular comes at the cost of excessive magnetic noise. Here, we present HDD writers as a tool for the efficient manipulation of single as well as multiple spins. We show that their tunable gradients of up to 100 µT/nm can be used to spectrally address individual spins on the nanoscale. Their gigahertz bandwidth allows one to switch control fields within nanoseconds, faster than characteristic time scales such as Rabi and Larmor periods, spin-spin couplings, or optical transitions, thus extending the set of feasible spin manipulations. We used the fields to drive spin transitions through nonadiabatic fast passages or to enable the optical readout of spin states in strong misaligned fields. Building on these techniques, we further apply the large magnetic field gradients for microwave selective addressing of single spins and show its use for the nanoscale optical colocalization of two emitters.

Microwave-Assisted Cross-Polarization of Nuclear Spin Ensembles from Optically Pumped Nitrogen-Vacancy Centers in Diamond.

The ability to optically initialize the electronic spin of the nitrogen-vacancy (NV) center in diamond has long been considered a valuable resource to enhance the polarization of neighboring nuclei, but efficient polarization transfer to spin species outside the diamond crystal has proven challenging. Here we demonstrate variable-magnetic-field, microwave-enabled cross-polarization from the NV electronic spin to protons in a model viscous fluid in contact with the diamond surface. Further, slight changes in the cross-relaxation rate as a function of the wait time between successive repetitions of the transfer protocol suggest slower molecular dynamics near the diamond surface compared to that in bulk. This observation is consistent with present models of the microscopic structure of a fluid and can be exploited to estimate the diffusion coefficient near a solid-liquid interface, of importance in colloid science.

Superresolution Microscopy of Single Rare-Earth Emitters in YAG and H3 Centers in Diamond.

We demonstrate superresolution imaging of single rare-earth emitting centers, namely, trivalent cerium, in yttrium aluminum garnet crystals by means of stimulated emission depletion (STED) microscopy. The achieved all-optical resolution is ≈50 nm. Similar results were obtained on H3 color centers in diamond. In both cases, STED resolution is improving slower than the conventional inverse square-root dependence on the depletion beam intensity. In the proposed model of this effect, the anomalous behavior is caused by excited state absorption and the interaction of the emitter with nonfluorescing crystal defects in its local surrounding.

Optically controlled switching of the charge state of a single nitrogen-vacancy center in diamond at cryogenic temperatures.

In this Letter, the photoinduced switching of the single nitrogen-vacancy (NV) center between two different charge states, negative (NV(-)) and neutral (NV(0)), is studied under resonant excitation at liquid helium temperature. We show that resonant conversion of NV(0) to NV(-) significantly improves spectral stability of the NV(-) defect and allows high fidelity initialization of the spin qubit. Based on density functional theory calculations a novel mechanism involving an Auger ionization of NV(-) and charge transfer of an electron from the valence band to NV(0) is discussed. This study provides further insight into the charge dynamics of the NV center, which is relevant for quantum information processing based on an NV(-) defect in diamond.

High-dynamic-range imaging of nanoscale magnetic fields using optimal control of a single qubit.

We present a novel spectroscopy protocol based on optimal control of a single quantum system. It enables measurements with quantum-limited sensitivity (η(ω)[proportionality](1/√[T(2)(*)]), T(2)(*) denoting the system's coherence time) but has an orders of magnitude larger dynamic range than pulsed spectroscopy methods previously employed for this task. We employ this protocol to image nanoscale magnetic fields with a single scanning nitrogen-vacancy center in diamond. Here, our scheme enables quantitative imaging of a strongly inhomogeneous field in a single scan without closed-loop control, which has previously been necessary to achieve this goal.

Quantum nonlinear spectroscopy of single nuclear spins.

Conventional nonlinear spectroscopy, which use classical probes, can only access a limited set of correlations in a quantum system. Here we demonstrate that quantum nonlinear spectroscopy, in which a quantum sensor and a quantum object are first entangled and the sensor is measured along a chosen basis, can extract arbitrary types and orders of correlations in a quantum system. We measured fourth-order correlations of single nuclear spins that cannot be measured in conventional nonlinear spectroscopy, using sequential weak measurement via a nitrogen-vacancy center in diamond. The quantum nonlinear spectroscopy provides fingerprint features to identify different types of objects, such as Gaussian noises, random-phased AC fields, and quantum spins, which would be indistinguishable in second-order correlations. This work constitutes an initial step toward the application of higher-order correlations to quantum sensing, to examining the quantum foundation (by, e.g., higher-order Leggett-Garg inequality), and to studying quantum many-body physics.

Violation of a temporal bell inequality for single spins in a diamond defect center.

Quantum nonlocality has been experimentally investigated by testing different forms of Bell's inequality, yet a loophole-free realization has not been achieved up to now. Much less explored are temporal Bell inequalities, which are not subject to the locality assumption, but impose a constraint on the system's time correlations. In this Letter, we report on the experimental violation of a temporal Bell's inequality using a nitrogen-vacancy (NV) defect in diamond and provide a novel quantitative test of quantum coherence. Such a test requires strong control over the system, and we present a new technique to initialize the electronic state of the NV with high fidelity, a necessary requirement also for reliable quantum information processing and/or the implementation of protocols for quantum metrology.

Dark states of single nitrogen-vacancy centers in diamond unraveled by single shot NMR.

The nitrogen-vacancy (NV) center in diamond is supposed to be a building block for quantum computing and nanometer-scale metrology at ambient conditions. Therefore, precise knowledge of its quantum states is crucial. Here, we experimentally show that under usual operating conditions the NV exists in an equilibrium of two charge states [70% in the expected negative (NV-) and 30% in the neutral one (NV0)]. Projective quantum nondemolition measurement of the nitrogen nuclear spin enables the detection even of the additional, optically inactive state. The nuclear spin can be coherently driven also in NV0 (T1≈90 ms and T2≈6 µs).

Strong coupling of a spin ensemble to a superconducting resonator.

We report the realization of a quantum circuit in which an ensemble of electronic spins is coupled to a frequency tunable superconducting resonator. The spins are nitrogen-vacancy centers in a diamond crystal. The achievement of strong coupling is manifested by the appearance of a vacuum Rabi splitting in the transmission spectrum of the resonator when its frequency is tuned through the nitrogen-vacancy center electron spin resonance.

Quantitative nanoscale MRI with a wide field of view.

Novel magnetic sensing modalities using quantum sensors or nanoscale probes have drastically improved the sensitivity and hence spatial resolution of nuclear magnetic resonance imaging (MRI) down to the nanoscale. Recent demonstrations of nuclear magnetic resonance (NMR) with paramagnetic colour centres include single molecule sensitivity, and sub-part-per-million spectral resolution. Mostly, these results have been obtained using well-characterised single sensors, which only permit extended imaging by scanning-probe microscopy. Here, we enhance multiplexed MRI with a thin layer of ensemble spin sensors in an inhomogeneous control field by optimal control spin manipulation to improve ensemble sensitivity and field of view (FOV). We demonstrate MRI of fluorine in patterned thin films only 1.2 nm in thickness, corresponding to a net moment of 120 nuclear spins per sensor spin. With the aid of the NMR signal, we reconstruct the nanoscale depth distribution of the sensor spins within the substrate. In addition, we exploit inhomogeneous ensemble control to squeeze the point spread function of the imager to about 100 nm and show that localisation of a point-like NMR signal within 40 nm is feasible. These results pave the way to quantitive NMR ensemble sensing and magnetic resonance microscopy with a resolution of few ten nanometers.

Diffusion behavior of gap junction hemichannels in living cells.

Due to its non-invasive character, fluorescence correlation spectroscopy (FCS) is particularly suited for the investigation of diffusion behavior of proteins in living cells. In this study we have investigated the diffusion properties of CFP-labeled gap junction hemichannels in the plasma membrane of living HeLa cells. Gap junction hemichannels or connexons are the precursors for the cell-cell- or gap junction channels that form large plaques at the contact areas between two adjacent cells. It has been proposed that new channels are recruited into a gap junction structure from a pool of hemichannels that can freely diffuse over the entire plasma membrane. The statistical approach shows that the geometry of the membrane within the focus is the most important property for the form of the autocorrelation curve and in turn for the determination of the diffusion coefficient. On the other hand binding-unbinding events which lead to anomalous diffusion have only a minor effect to the position and shape of the correlation curve compared to the geometry of the membrane.

Nanoscale nuclear magnetic imaging with chemical contrast.

Scanning probe microscopy is one of the most versatile windows into the nanoworld, providing imaging access to a variety of electronic, dielectric, magnetic and topographic sample properties, depending on the probe used. Here, we demonstrate a scanning probe imaging method that extends the range of accessible quantities to label-free imaging of chemical species while operating on arbitrary samples--including insulating materials--under ambient conditions. Moreover, its sensitivity extends below the surface of a sample, allowing for imaging of subsurface features. We achieve these results by recording NMR signals from a sample surface with a recently introduced scanning probe, a single nitrogen-vacancy centre in diamond. We demonstrate NMR imaging with 10 nm resolution and achieve chemically specific contrast by separating fluorine from hydrogen-rich regions. Our result opens the door to scanning probe imaging of the chemical composition and molecular structure of arbitrary samples. A method with these abilities will find widespread application in materials science, even on biological specimens down to the level of single macromolecules.

Probing molecular dynamics at the nanoscale via an individual paramagnetic centre.

We demonstrate a protocol using individual nitrogen-vacancy centres in diamond to observe the time evolution of proton spins from organic molecules located a few nanometres from the diamond surface. The protocol records temporal correlations among the interacting protons, and thus is sensitive to the local dynamics via its impact on the nuclear spin relaxation and interaction with the nitrogen vacancy. We gather information on the nanoscale rotational and translational diffusion dynamics by analysing the time dependence of the nuclear magnetic resonance signal. Applying this technique to liquid and solid samples, we find evidence that liquid samples form a semi-solid layer of 1.5-nm thickness on the surface of diamond, where translational diffusion is suppressed while rotational diffusion remains present. Extensions of the present technique could be exploited to highlight the chemical composition of molecules tethered to the diamond surface or to investigate thermally or chemically activated dynamical processes such as molecular folding.

A diamond-based scanning probe spin sensor operating at low temperature in ultra-high vacuum.

We present the design and performance of an ultra-high vacuum (UHV) low temperature scanning probe microscope employing the nitrogen-vacancy color center in diamond as an ultrasensitive magnetic field sensor. Using this center as an atomic-size scanning probe has enabled imaging of nanoscale magnetic fields and single spins under ambient conditions. In this article we describe an experimental setup to operate this sensor in a cryogenic UHV environment. This will extend the applicability to a variety of molecular systems due to the enhanced target spin lifetimes at low temperature and the controlled sample preparation under UHV conditions. The instrument combines a tuning-fork based atomic force microscope (AFM) with a high numeric aperture confocal microscope and the facilities for application of radio-frequency (RF) fields for spin manipulation. We verify a sample temperature of <50 K even for strong laser and RF excitation and demonstrate magnetic resonance imaging with a magnetic AFM tip.

Coherent properties of single rare-earth spin qubits.

Rare-earth-doped crystals are excellent hardware for quantum storage of photons. Additional functionality of these materials is added by their waveguiding properties allowing for on-chip photonic networks. However, detection and coherent properties of rare-earth single-spin qubits have not been demonstrated so far. Here we present experimental results on high-fidelity optical initialization, efficient coherent manipulation and optical readout of a single-electron spin of Ce(3+) ion in a yttrium aluminium garnet crystal. Under dynamic decoupling, spin coherence lifetime reaches T2 = 2 ms and is almost limited by the measured spin-lattice relaxation time T1 = 4.5 ms. Strong hyperfine coupling to aluminium nuclear spins suggests that cerium electron spins can be exploited as an interface between photons and long-lived nuclear spin memory. Combined with high brightness of Ce(3+) emission and a possibility of creating photonic circuits out of the host material, this makes cerium spins an interesting option for integrated quantum photonics.

Nuclear magnetic resonance spectroscopy on a (5-nanometer)3 sample volume.

Application of nuclear magnetic resonance (NMR) spectroscopy to nanoscale samples has remained an elusive goal, achieved only with great experimental effort at subkelvin temperatures. We demonstrated detection of NMR signals from a (5-nanometer)(3) voxel of various fluid and solid organic samples under ambient conditions. We used an atomic-size magnetic field sensor, a single nitrogen-vacancy defect center, embedded ~7 nanometers under the surface of a bulk diamond to record NMR spectra of various samples placed on the diamond surface. Its detection volume consisted of only 10(4) nuclear spins with a net magnetization of only 10(2) statistically polarized spins.

Magnetic spin imaging under ambient conditions with sub-cellular resolution.

The detection of small numbers of magnetic spins is a significant challenge in the life, physical and chemical sciences, especially when room temperature operation is required. Here we show that a proximal nitrogen-vacancy spin ensemble serves as a high precision sensing and imaging array. Monitoring its longitudinal relaxation enables sensing of freely diffusing, unperturbed magnetic ions and molecules in a microfluidic device without applying external magnetic fields. Multiplexed charge-coupled device acquisition and an optimized detection scheme permits direct spin noise imaging of magnetically labelled cellular structures under ambient conditions. Within 20 s we achieve spatial resolutions below 500 nm and experimental sensitivities down to 1,000 statistically polarized spins, of which only 32 ions contribute to a net magnetization. The results mark a major step towards versatile sub-cellular magnetic imaging and real-time spin sensing under physiological conditions providing a minimally invasive tool to monitor ion channels or haemoglobin trafficking inside live cells.

Optical detection of a single rare-earth ion in a crystal.

Rare-earth-doped laser materials show strong prospects for quantum information storage and processing, as well as for biological imaging, due to their high-Q 4f↔4f optical transitions. However, the inability to optically detect single rare-earth dopants has prevented these materials from reaching their full potential. Here we detect a single photostable Pr(3+) ion in yttrium aluminium garnet nanocrystals with high contrast photon antibunching by using optical upconversion of the excited state population of the 4f↔4f optical transition into ultraviolet fluorescence. We also demonstrate on-demand creation of Pr(3+) ions in a bulk yttrium aluminium garnet crystal by patterned ion implantation. Finally, we show generation of local nanophotonic structures and cell death due to photochemical effects caused by upconverted ultraviolet fluorescence of praseodymium-doped yttrium aluminium garnet in the surrounding environment. Our study demonstrates versatile use of rare-earth atomic-size ultraviolet emitters for nanoengineering and biotechnological applications.