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Abstract With their optical addressability of individual spins and long coherence time, nitrogen-vacancy (NV) centers in diamond are often called “atom-like solid spin-defects”. As observed with trapped atomic ions, quantum interference mediated by indistinguishable photons was demonstrated between remote NV centers. In high sensitivity DC magnetometry at room temperature, NV ensembles are potentially rivaling with alkali-atom vapor cells. However, local strain induces center-to-center variation of both optical and spin transitions of NV centers. Therefore, advanced engineering of diamond growth toward crystalline perfection is demanded. Here, we report on the synthesis of high-quality HPHT (high-pressure, high-temperature) crystals, demonstrating a small inhomogeneous broadening of the spin transitions, of T 2 * = 1.28 μs, approaching the limit for crystals with natural 13C abundance, that we determine as T 2 * = 1.48 μs. The contribution from strain and local charges to the inhomogeneous broadening is lowered to ~17 kHz full width at half maximum for NV ensemble within a > 10 mm3 volume. Looking at optical transitions in low nitrogen crystals, we examine the variation of zero-phonon-line optical transition frequencies at low temperatures, showing a strain contribution below 2 GHz for a large fraction of single NV centers.

Abstract A recurring challenge in quantum science and technology is the precise control of their underlying dynamics that lead to the desired quantum operations, often described by a set of quantum gates. These gates can be subject to application-specific errors, leading to a dependence of their controls on the chosen circuit, the quality measure and the gate-set itself. A natural solution would be to apply quantum optimal control in an application-oriented fashion. In turn, this requires the definition of a meaningful measure of the contextual gate-set performance. Therefore, we explore and compare the applicability of quantum process tomography, linear inversion gate-set tomography, randomized linear gate-set tomography, and randomized benchmarking as measures for closed-loop quantum optimal control experiments, using a macroscopic ensemble of nitrogen-vacancy centers in diamond as a test-bed. Our work demonstrates the relative trade-offs between those measures and how to significantly enhance the gate-set performance, leading to an improvement across all investigated methods.

Intracellular radicals play important roles in cell signaling and regulation of growth factors, cytokines, transcription, apoptosis, and immunomodulation, among others. To gain a more comprehensive understanding of their biological functions from a spatio-temporal pers­pective, there is a great need for nanoscale sensitive tools that allow real-time detection of these reactive species. Currently, intracellular radical probes are based on chemical reactions that could significantly alter radical levels during detection. Due to the excellent bio­compatibility and favorable photophysical properties of nitrogen-vacancy (NV–) centers in fluorescent nanodiamonds (fNDs), the fNDs can serve as a powerful and chemically inert nanotool for intracellular radical detection. In this study, a positively charged nanogel (NG) coating was prepared to prevent the precipitation of fNDs and promote cellular internalization. After internalization of nanodiamond-nanogels (fND-NGs), different stimulators, namely somatostatin (SST), triphenylphosphonium (TPP), and trans-activator of transcription (TAT) peptide, which are widely used cell- or organelle-targeting ligands in medicine, drug delivery, and diagnostics, were applied to stimulate the cells. In parallel, the intracellular radical changes under stimulation of SST, TPP, and TAT ligands were monitored by fND-NGs in a home-built optically detected magnetic resonance (ODMR) microscope. Our method allows for detecting intracellular radicals in-situ and monitoring their real-time changes during incubation with the targeting ligands in a single living cell. We believe that our method will provide insights into the generation of radical stress in cells, which could improve our fundamental understanding of the pharmacology and signaling pathways of widely used cell- and organelle-targeting ligands associated with free radicals.

Abstract Background Epigenetic mechanisms are informational cellular processes instructing normal and diseased phenotypes. They are associated with DNA but without altering the DNA sequence. Whereas chemical processes like DNA methylation or histone modifications are well-accepted epigenetic mechanisms, we herein propose the existence of an additional quantum physics layer of epigenetics. Results We base our hypothesis on theoretical and experimental studies showing quantum phenomena to be active in double-stranded DNA, even under ambient conditions. These phenomena include coherent charge transfer along overlapping pi-orbitals of DNA bases and chirality-induced spin selectivity. Charge transfer via quantum tunneling mediated by overlapping orbitals results in charge delocalization along several neighboring bases, which can even be extended by classical (non-quantum) electron hopping. Such charge transfer is interrupted by flipping base(s) out of the double-strand e.g., by DNA modifying enzymes. Charge delocalization can directly alter DNA recognition by proteins or indirectly by DNA structural changes e.g., kinking. Regarding sequence dependency, charge localization, shown to favor guanines, could influence or even direct epigenetic changes, e.g., modification of cytosines in CpG dinucleotides. Chirality-induced spin selectivity filters electrons for their spin along DNA and, thus, is not only an indicator for quantum coherence but can potentially affect DNA binding properties. Conclusions Quantum effects in DNA are prone to triggering and manipulation by external means. By the hypothesis put forward here, we would like to foster research on “Quantum Epigenetics” at the interface of medicine, biology, biochemistry, and physics to investigate the potential epigenetic impact of quantum physical principles on (human) life.

Abstract Diffusion noise is a major source of spectral line broadening in liquid state nano-scale nuclear magnetic resonance with shallow nitrogen-vacancy centres, whose main consequence is a limited spectral resolution. This limitation arises by virtue of the widely accepted assumption that nuclear spin signal correlations decay exponentially in nano-NMR. However, a more accurate analysis of diffusion shows that correlations survive for a longer time due to a power-law scaling, yielding the possibility for improved resolution and altering our understanding of diffusion at the nano-scale. Nevertheless, such behaviour remains to be demonstrated in experiments. Using three different experimental setups and disparate measurement techniques, we present overwhelming evidence of power-law decay of correlations. These result in sharp-peaked spectral lines, for which diffusion broadening need not be a limitation to resolution.

Abstract Precise frequency measurements are important in applications ranging from navigation and imaging to computation and communication. Here we outline the optimal quantum strategies for frequency discrimination and estimation in the context of quantum spectroscopy, and we compare the effectiveness of different readout strategies. Using a single NV center in diamond, we implement the optimal frequency discrimination protocol to discriminate two frequencies separated by 2 kHz with a single 44 μs measurement, a factor of ten below the Fourier limit. For frequency estimation, we achieve a frequency sensitivity of 1.6 µHz/Hz2 for a 1.7 µT amplitude signal, which is within a factor of 2 from the quantum limit. Our results are foundational for discrimination and estimation problems in nanoscale nuclear magnetic resonance spectroscopy.

Abstract The characterization of quantum systems is both a theoretical and technical challenge. Theoretical because of the exponentially increasing complexity with system size and the fragility of quantum states under observation. Technical because of the requirement to manipulate and read out individual atomic or photonic elements. Adaptive methods can help to overcome these challenges by optimizing the amount of information each measurement provides and reducing the necessary resources. Their implementation, however, requires fast-feedback and complex processing algorithms. Here, we implement online adaptive sensing with single spins and demonstrate close to photon shot noise limited performance with high repetition rate, including experimental overheads. We further use fast feedback to determine the hyperfine coupling of a nuclear spin to the nitrogen-vacancy sensor with a sensitivity of $$445\,{\mathrm{nT}}{\sqrt{\mathrm{Hz}}}^{- 1}$$ 445 nT Hz − 1 . Our experiment is a proof of concept that online adaptive techniques can be a versatile tool to enable faster characterization of the spin environment.

NV centers are among the most promising platforms in the field of quantum sensing. Magnetometry based on NV centers, especially, has achieved concrete development in areas of biomedicine and medical diagnostics. Improving the sensitivity of NV center sensors under wide inhomogeneous broadening and fieldamplitude drift is a crucial issue of continuous concern that relies on the coherent control of NV centers with high average fidelity. Quantum optimal control (QOC) methods provide access to this target; nevertheless, the high time consumption of current methods due to the large number of needful sample points as well as the complexity of the parameter space has hindered their usability. In this paper, we propose the Bayesian estimation phase-modulated (B-PM) method to tackle this problem. In the case of the state transforming of an NV center ensemble, the B-PM method reduced the time consumption by more than 90% compared with the conventional standard Fourier basis (SFB) method while increasing the average fidelity from 0.894 to 0.905. In the AC magnetometry scenario, the optimized control pulse obtained with the B-PM method achieved an eight-fold extension of coherence time T2 compared with the rectangular π pulse. Similar application can be made in other sensing situations. As a general algorithm, the B-PM method can be further extended to the open- and closed-loop optimization of complex systems based on a variety of quantum platforms.

Abstract The negatively charged nitrogen-vacancy ( $$\hbox {NV}^{-}$$ NV - ) center shows excellent spin properties and sensing capabilities on the nanoscale even at room temperature. Shallow implanted $$\hbox {NV}^{-}$$ NV - centers can effectively be protected from surface noise by chemical vapor deposition (CVD) diamond overgrowth, i.e. burying them homogeneously deeper in the crystal. However, the origin of the substantial losses in $$\hbox {NV}^{-}$$ NV - centers after overgrowth remains an open question. Here, we use shallow $$\hbox {NV}^{-}$$ NV - centers to exclude surface etching and identify the passivation reaction of NV to NVH centers during the growth as the most likely reason. Indirect overgrowth featuring low energy (2.5–5 keV) nitrogen ion implantation and CVD diamond growth before the essential annealing step reduces this passivation phenomenon significantly. Furthermore, we find higher nitrogen doses to slow down the NV–NVH conversion kinetics, which gives insight into the sub-surface diffusion of hydrogen in diamond during growth. Finally, nano sensors fabricated by indirect overgrowth combine tremendously enhanced $$T_2$$ T 2 and $$T_2^*$$ T 2 ∗ times with an outstanding degree of depth-confinement which is not possible by implanting with higher energies alone. Our results improve the understanding of CVD diamond overgrowth and pave the way towards reliable and advanced engineering of shallow $$\hbox {NV}^{-}$$ NV - centers for future quantum sensing devices.

Hyperpolarization of nuclear spins enhances nuclear magnetic resonance signals, which play a key role for imaging and spectroscopy in the natural and life sciences. This signal amplification unlocks previously inaccessible techniques, such as metabolic imaging of cancer cells. In this paper, electron spins from the photoexcited triplet state of pentacene-doped naphthalene crystals are used to polarize surrounding protons. As existing strategies are rendered less effective by experimental constraints, they are replaced with optimal control pulses designed with redcrab. In contrast to previous optimal control approaches, which consider one or two effective nuclei, this closed-loop optimization is macroscopic. A 26% improvement in signal and 15% faster polarization rate are observed. Additionally, a strategy called autonomously optimized repeated linear sweep (ARISE) is introduced to efficiently tailor existing hyperpolarization sequences in the presence of experimental uncertainty to enhance their performance. ARISE is expected to be broadly applicable in many experimental settings.

Nanodiamonds (NDs) have high potential as a drug carrier and in combination with nitrogen vacancies (NV centers) for highly sensitive MR-imaging after hyperpolarization. However, little remains known about their physiological properties in vivo. PET imaging allows further evaluation due to its quantitative properties and high sensitivity. Thus, we aimed to create a preclinical platform for PET and MR evaluation of surface-modified NDs by radiolabeling with both short- and long-lived radiotracers. Serum albumin coated NDs, functionalized with PEG groups and the chelator deferoxamine, were labeled either with zirconium-89 or gallium-68. Their biodistribution was assessed in two different mouse strains. PET scans were performed at various time points up to 7 d after i.v. injection. Anatomical correlation was provided by additional MRI in a subset of animals. PET results were validated by ex vivo quantification of the excised organs using a gamma counter. Radiolabeled NDs accumulated rapidly in the liver and spleen with a slight increase over time, while rapid washout from the blood pool was observed. Significant differences between the investigated radionuclides were only observed for the spleen (1 h). In summary, we successfully created a preclinical PET and MR imaging platform for the evaluation of the biodistribution of NDs over different time scales.

A scheme of optical four-level pulse amplitude modulation (PAM-4) is proposed based on phase-dependent electromagnetic-induced transparency (EIT) in nitrogen-vacancy (NV) centers. For a closed structure, its transmission depends on the relative phase of applied fields. Based on EIT, the PAM-4 may be achieved by encoding the relative phase and decoding the amplitude of the transmission field. Simulation results show that the differential nonlinearity and the integral nonlinearity of the proposed scheme could be reduced by two orders of magnitude compared with that based on Mach–Zehnder modulator scheme, and the ratio of level separation mismatch is closer to the ideal value 1. Furthermore, the improvement of the system at different probe field detunings and coupling field strengths is investigated.

Fluorescent nanodiamonds (NDs) are carbon‐based nanoparticles with various outstanding magneto−optical properties. After preparation, NDs have a variety of different surface groups that determine their physicochemical properties. For biological applications, surface modifications are crucial to impart a new interface for controlled interactions with biomolecules or cells. Herein, a straightforward synthesis concept denoted “adsorption−crosslinking” is applied for the efficient modification of NDs, which sequentially combines fast noncovalent adsorption based on electrostatic interactions and subsequent covalent crosslinking. As a result, a very thin and uniform nanogel (NG) coating surrounding the NDs is obtained, which imparts reactive groups as well as high colloidal stability. The impact of the reaction time, monomer concentration, molecular weight, structure of the crosslinker on the resulting NG shell, the availability of reactive chemical surface functions, and the quantum sensing properties of the coated NDs are assessed and optimized. Postmodification of the NG‐coated NDs is achieved with phototoxic ruthenium complexes yielding ND‐based probes suitable for photodynamic applications. The adsorption−crosslinking ND functionalization reported herein provides new avenues toward functional probes and traceable nanocarriers for high‐resolution bioimaging, nanoscale sensing, and photodynamic applications.

The Hen's Egg Test Chorioallantoic Membrane (HET-CAM) of fertilized chick eggs represents a unique model for biomedical research. With its steadily increasing use, non-invasive in ovo imaging for longitudinal direct quantification of the biodistribution of compounds or monitoring of surrogate markers has been introduced. The full range of imaging methods has been applied to the HET-CAM model. From the current perspective, Magnetic Resonance Imaging (MRI) and Positron Emission Tomography (PET) appear promising techniques, providing detailed anatomical and functional information (MRI) and excellent sensitivity (PET). Especially by combining both techniques, the required sensitivity and anatomical localization of the signal source renders feasible. In the following, a review of recent applications of MRI and PET for in ovo imaging with a special focus on techniques for imaging xenotransplanted tumors on the CAM will be provided.

State-of-the-art methods for sensing weak AC fields are only efficient in the low frequency domain. Here, Stark et al. demonstrate a sensing scheme that is capable of probing high frequencies through continuous dynamical coupling by applying it to a nitrogen-vacancy centre in diamond.

Here Jeskeet al. show both theoretical and experimental evidence for stimulated emission from negatively charged nitrogen vacancy centres using light in the phonon sidebands around 700 nm, demonstrating its suitability as a laser medium.

Qudi is a general, modular, multi-operating system suite written in Python 3 for controlling laboratory experiments. It provides a structured environment by separating functionality into hardware abstraction, experiment logic and user interface layers. The core feature set comprises a graphical user interface, live data visualization, distributed execution over networks, rapid prototyping via Jupyter notebooks, configuration management, and data recording. Currently, the included modules are focused on confocal microscopy, quantum optics and quantum information experiments, but an expansion into other fields is possible and encouraged. Keywords: Python 3, Qt, Experiment control, Automation, Measurement software, Framework, Modular

Nanostructured diamonds hosting optically active paramagnetic color centers (NV, SiV, GeV, etc.) and hyperfine-coupled with them quantum memory 13C nuclear spins situated in diamond lattice are currently of great interest to implement emerging quantum technologies (quantum information processing, quantum sensing and metrology). Current methods of creation such as electronic-nuclear spin systems are inherently probabilistic with respect to mutual location of color center electronic spin and 13C nuclear spins. A new bottom-up approach to fabricate such systems is to synthesize first chemically appropriate diamond-like organic molecules containing desired isotopic constituents in definite positions and then use them as a seed for diamond growth to produce macroscopic diamonds, subsequently creating vacancy-related color centers in them. In particular, diamonds incorporating coupled NV-13C spin systems (quantum registers) with specific mutual arrangements of NV and 13C can be obtained from anisotopic azaadamantane molecule. Here we predict the characteristics of hyperfine interactions (hfi) for the NV-13C systems in diamonds grown from various isotopically substituted azaadamantane molecules differing in 13C position in the seed, as well as the orientation of the NV center in the post-obtained diamond. We used the spatial and hfi data simulated earlier for the H-terminated cluster C510[NV]-H252. The data obtained can be used to identify (and correlate with the seed used) the specific NV-13C spin system by measuring, e.g., the hfi-induced splitting of the mS = ±1 sublevels of the NV center in optically detected magnetic resonance (ODMR) spectra being characteristic for various NV-13C systems.

Nitrogen vacancy (NV) centers in diamond are a platform for several important quantum technologies, including sensing, communication and elementary quantum processors. In this letter we demonstrate the creation of NV centers by implantation using a deterministic single ion source. For this we sympathetically laser-cool single ${}^{15}\mathrm{N}_{2}^{+}$ molecular ions in a Paul trap and extract them at an energy of 5.9 keV. Subsequently the ions are focused with a lateral resolution of 121(35) nm and are implanted into a diamond substrate without any spatial filtering by apertures or masks. After high-temperature annealing, we detect the NV centers in a confocal microscope and determine a conversion efficiency of about 0.6%. The ^15 NV centers are characterized by optically detected magnetic resonance on the hyperfine transition and coherence time.

We propose a scheme for sensing of an oscillating field in systems with large inhomogeneous broadening and driving field variation by applying sequences of phased, adiabatic, chirped pulses. These act as a double filter for dynamical decoupling, where the adiabatic changes of the mixing angle during the pulses rectify the signal and partially remove frequency noise. The sudden changes between the pulses act as instantaneous π pulses in the adiabatic basis for additional noise suppression. We also use the pulses' phases to correct for other errors, e.g., due to nonadiabatic couplings. Our technique improves significantly the coherence time in comparison to standard XY8 dynamical decoupling in realistic simulations in NV centers with large inhomogeneous broadening. Beyond the theoretical proposal, we also present proof-of-principle experimental results for quantum sensing of an oscillating field in NV centers in diamond, demonstrating superior performance compared to the standard technique.

Quantum metrology is a powerful tool for explorations of fundamental physical phenomena and applications in material science and biochemical analysis. While in principle the sensitivity can be improved by increasing the density of sensing particles, in practice this improvement is severely hindered by interactions between them. Here, using a dense ensemble of interacting electronic spins in diamond, we demonstrate a novel approach to quantum metrology to surpass such limitations. It is based on a new method of robust quantum control, which allows us to simultaneously suppress the undesired effects associated with spin-spin interactions, disorder, and control imperfections, enabling a fivefold enhancement in coherence time compared to state-of-the-art control sequences. Combined with optimal spin state initialization and readout directions, this allows us to achieve an ac magnetic field sensitivity well beyond the previous limit imposed by interactions, opening a new regime of high-sensitivity solid-state ensemble magnetometers.

Optical coupling enables intermediate- and long-range interactions between distant quantum emitters. Such interaction may be the basic element in bottom-up approaches of coupled spin systems or for integrated quantum photonics and quantum plasmonics. Here, we prepare nanodiamonds carrying single, negatively-charged silicon-vacancy centers for evanescent optical coupling with access to all degrees of freedom by means of atomic force nanomanipulation. The color centers feature excellent optical properties, comparable to silicon-vacancy centers in bulk diamond, resulting in a resolvable fine structure splitting, a linewidth close to the Fourier-Transform limit under resonant excitation and a good polarization contrast. We determine the orbital relaxation time T _1 of the orbitally split ground states and show that all optical properties are conserved during translational nanomanipulation. Furthermore, we demonstrate the rotation of the nanodiamonds. In contrast to the translational operation, the rotation leads to a change in polarization contrast. We utilize the change in polarization contrast before and after nanomanipulation to determine the rotation angle. Finally, we evaluate the likelihood for indistinguishable, single photon emission of silicon-vacancy centers located in different nanodiamonds. Our work enables ideal evanescent, optical coupling of distant nanodiamonds containing silicon-vacancy centers with applications in the realization of quantum networks, quantum repeaters or complex quantum systems.

We demonstrate the coupling of single color centers in diamond to plasmonic and dielectric photonic structures to realize novel nanophotonic devices. Nanometer spatial control in the creation of single color centers in diamond is achieved by implantation of nitrogen atoms through high-aspect-ratio channels in a mica mask. Enhanced broadband single-photon emission is demonstrated by coupling nitrogen–vacancy centers to plasmonic resonators, such as metallic nanoantennas. Improved photon-collection efficiency and directed emission is demonstrated by solid immersion lenses and micropillar cavities. Thereafter, the coupling of diamond nanocrystals to the guided modes of micropillar resonators is discussed along with experimental results. Finally, we present a gas-phase-doping approach to incorporate color centers based on nickel and tungsten, in situ into diamond using microwave-plasma-enhanced chemical vapor deposition. The fabrication of silicon–vacancy centers in nanodiamonds by microwave-plasma-enhanced chemical vapor deposition is discussed in addition.

Within the last two decades, quantum technologies (QT) have made tremendous progress, moving from Nobel Prize award-winning experiments on quantum physics (1997: Chu, Cohen-Tanoudji, Phillips; 2001: Cornell, Ketterle, Wieman; 2005: Hall, Hänsch-, Glauber; 2012: Haroche, Wineland) into a cross-disciplinary field of applied research. Technologies are being developed now that explicitly address individual quantum states and make use of the ‘strange’ quantum properties, such as superposition and entanglement. The field comprises four domains: quantum communication, where individual or entangled photons are used to transmit data in a provably secure way; quantum simulation, where well-controlled quantum systems are used to reproduce the behaviour of other, less accessible quantum systems; quantum computation, which employs quantum effects to dramatically speed up certain calculations, such as number factoring; and quantum sensing and metrology, where the high sensitivity of coherent quantum systems to external perturbations is exploited to enhance the performance of measurements of physical quantities. In Europe, the QT community has profited from several EC funded coordination projects, which, among other things, have coordinated the creation of a 150-page QT Roadmap ( http://qurope.eu/h2020/qtflagship/roadmap2016 ). This article presents an updated summary of this roadmap.

The simultaneous control of the number and position of negatively charged nitrogen-vacancy (NV) centers in diamond was achieved. While single near-surface NV centers are known to exhibit outstanding capabilities in external spin sensing, trade-off relationships among the accuracy of the number and position, and the coherence of NV centers have made the use of such engineered NV centers difficult. Namely, low-energy nitrogen implantation with lithographic techniques enables the nanoscale position control but results in degradation of the creation yield and the coherence property. In this paper, we show that low-energy nitrogen ion implantation to a ^12 C (99.95%)-enriched homoepitaxial diamond layer using nanomask is applicable to create shallow NV centers with a sufficiently long coherence time for external spin sensing, at a high creation yield. Furthermore, the NV centers were arranged in a regular array so that 40% lattice sites contain single NV centers. The XY8- k measurements using the individual NV centers reveal that the created NV centers have depths from 2 to 12 nm, which is comparable to the stopping range of nitrogen ions implanted at 2.5 keV. We show that the position-controlled NV centers are capable of external spin sensing with a ultra-high spatial resolution.

Color centers in diamond are important quantum emitters for a broad range of applications ranging from quantum sensing to quantum optics. Understanding the internal energy level structure is of fundamental importance for future applications. We experimentally investigate the level structure of an ensemble of few negatively charged silicon-vacancy (SiV ^− ) and germanium-vacancy (GeV ^− ) centers in bulk diamond at room temperature by photoluminescence (PL) and excitation (PLE) spectroscopy over a broad wavelength range from 460 to $650\,\mathrm{nm}$ and perform power-dependent saturation measurements. For SiV ^− our experimental results confirm the presence of a higher energy transition at $\sim 2.31\,\mathrm{eV}$ . By comparison with detailed theoretical simulations of the imaginary dielectric function we interpret the transition as a dipole-allowed transition from ${}^{2}{E}_{g}$ -state to ${}^{2}{A}_{2u}$ -state where the corresponding a _2 _u -level lies deeply inside the diamond valence band. Therefore, the transition is broadened by the diamond band. At higher excitation power of $10\,\mathrm{mW}$ we indicate signs of a parity-conserving transition at $\sim 2.03\,\mathrm{eV}$ supported by saturation measurements. For GeV ^− we demonstrate that the PLE spectrum is in good agreement with the mirror image of the PL spectrum of the zero-phonon line. Experimentally we do not observe a higher lying energy level up to a transition wavelength of $460\,\mathrm{nm}$ . The observed PL spectra are identical, independent of excitation wavelength, suggesting a rapid decay to ${}^{2}{E}_{u}$ excited state and followed by optical transition to ${}^{2}{E}_{g}$ ground state. Our investigations convey important insights for future quantum optics and quantum sensing experiments based on SiV ^− -center and GeV ^− -center in diamond.

The sensitivity of magnetic resonance imaging (MRI) depends strongly on nuclear spin polarisation and, motivated by this observation, dynamical nuclear spin polarisation has recently been applied to enhance MRI protocols (Kurhanewicz et al 2011 Neoplasia http://dx.doi.org/10.1593/neo.101102 13 http://dx.doi.org/10.1593/neo.101102 ). Nuclear spins associated with the ^13 C carbon isotope (nuclear spin I = 1/2) in diamond possess uniquely long spin lattice relaxation times (Reynhardt and High 2011 Prog. Nucl. Magn. Reson. Spectrosc. http://dx.doi.org/10.1016/s0079-6565(00)00025-x 38 http://dx.doi.org/10.1016/s0079-6565(00)00025-x ). If they are present in diamond nanocrystals, especially when strongly polarised, they form a promising contrast agent for MRI. Current schemes for achieving nuclear polarisation, however, require cryogenic temperatures. Here we demonstrate an efficient scheme that realises optically induced ^13 C nuclear spin hyperpolarisation in diamond at room temperature and low ambient magnetic field. Optical pumping of a nitrogen-vacancy centre creates a continuously renewable electron spin polarisation which can be transferred to surrounding ^13 C nuclear spins. Importantly for future applications we also realise polarisation protocols that are robust against an unknown misalignment between magnetic field and crystal axis.

Colour centres in nanodiamonds are an important resource for applications in quantum sensing, biological imaging, and quantum optics. Here we report unprecedented narrow optical transitions for individual colour centres in nanodiamonds smaller than 200 nm. This demonstration has been achieved using the negatively charged silicon vacancy centre, which has recently received considerable attention due to its superb optical properties in bulk diamond. We have measured an ensemble of silicon-vacancy centres across numerous nanodiamonds to have an inhomogeneous distribution of 1.05 nm at 5 K. Individual spectral lines as narrower than 360 MHz were measured in photoluminescence excitation, and correcting for apparent spectral diffusion yielded an homogeneous linewidth of about 200 MHz which is close to the lifetime limit. These results indicate the high crystalline quality achieved in these nanodiamond samples, and advance the applicability of nanodiamond-hosted colour centres for quantum optics applications.

We investigate phonon induced electronic dynamics in the ground and excited states of the negatively charged silicon-vacancy ( ${\rm Si}{{{\rm V}}^{-}}$ ) centre in diamond. Optical transition line widths, transition wavelength and excited state lifetimes are measured for the temperature range 4 K–350 K. The ground state orbital relaxation rates are measured using time-resolved fluorescence techniques. A microscopic model of the thermal broadening in the excited and ground states of the ${\rm Si}{{{\rm V}}^{-}}$ centre is developed. A vibronic process involving single-phonon transitions is found to determine orbital relaxation rates for both the ground and the excited states at cryogenic temperatures. We discuss the implications of our findings for coherence of qubits in the ground states and propose methods to extend coherence times of ${\rm Si}{{{\rm V}}^{-}}$ qubits.

Fast and accurate quantum operations of a single spin in room-temperature solids are required in many modern scientific areas, for instance in quantum information, quantum metrology, and magnetometry. However, the accuracy is limited if the Rabi frequency of the control is comparable with the transition frequency of the qubit due to the breakdown of the rotating wave approximation (RWA). We report here an experimental implementation of a control method based on quantum optimal control theory which does not suffer from such restriction. We demonstrate the most commonly used single qubit rotations, i.e. $\pi /2$ - and π -pulses, beyond the RWA regime with high fidelity $F_{\pi /2}^{{\rm exp} }=0.95\pm 0.01$ and $F_{\pi }^{{\rm exp} }=0.99\pm 0.016$ , respectively. They are in excellent agreement with the theoretical predictions, $F_{\pi /2}^{{\rm theory}}=0.9545$ and $F_{\pi }^{{\rm theory}}=0.9986$ . Furthermore, we perform two basic magnetic resonance experiments both in the rotating and the laboratory frames, where we are able to deliberately ‘switch’ between the frames, to confirm the robustness of our control method. Our method is general, hence it may immediately find its wide applications in magnetic resonance, quantum computing, quantum optics, and broadband magnetometry.

The silicon-vacancy centre ( ${\rm Si}{{{\rm V}}^{-}}$ ) in diamond has exceptional spectral properties for single-emitter quantum information applications. Most of the fluorescence is concentrated in a strong zero phonon line (ZPL), with a weak phonon sideband extending for 100 nm that contains several clear features. We demonstrate that the ZPL position can be used to reliably identify the silicon isotope present in a single ${\rm Si}{{{\rm V}}^{-}}$ centre. This is of interest for quantum information applications since only the ^29 Si isotope has nuclear spin. In addition, we show that the sharp 64 meV phonon peak is due to a local vibrational mode of the silicon atom. The presence of a local mode suggests a plausible origin of the measured isotopic shift of the ZPL.

The detection of a nuclear spin in an individual molecule represents a key challenge in physics and biology whose solution has been pursued for many years. The small magnetic moment of a single nucleus and the unavoidable environmental noise present the key obstacles for its realization. In this paper, we demonstrate theoretically that a single nitrogen-vacancy center in diamond can be used to construct a nano-scale single-molecule spectrometer that is capable of detecting the position and spin state of a single nucleus and can determine the distance and alignment of a nuclear or electron spin pair. The proposed device would find applications in single-molecule spectroscopy in chemistry and biology, for example in determining the protein structure or in monitoring macromolecular motions, and can thus provide a tool to help unravel the microscopic mechanisms underlying bio-molecular function.

We investigate the performance of inhomogeneously broadened spin ensembles as quantum memories under continuous dynamical decoupling. The role of the continuous driving field is twofold: firstly, it decouples individual spins from magnetic noise; secondly, and more importantly, it suppresses and reshapes the spectral inhomogeneity of spin ensembles. We show that a continuous driving field, which itself may also be inhomogeneous over the ensemble, can considerably enhance the decay of the tails of the inhomogeneous broadening distribution. This fact enables a spin-ensemble-based quantum memory to exploit the effect of cavity protection and achieve a much longer storage time. In particular, for a spin ensemble with a Lorentzian spectral distribution, our calculations demonstrate that continuous dynamical decoupling has the potential to improve its storage time by orders of magnitude for the state-of-the-art experimental parameters.