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Spins associated to solid-state colour centers are a promising platform for investigating quantum computation and quantum networks. Recent experiments have demonstrated multi-qubit quantum processors, optical interconnects, and basic quantum error correction protocols. One of the key open challenges towards larger-scale systems is to realize high-fidelity universal quantum gates. In this work, we design and demonstrate a complete high-fidelity gate set for the two-qubit system formed by the electron and nuclear spin of a nitrogen-vacancy center in diamond. We use gate set tomography (GST) to systematically optimise the gates and demonstrate single-qubit gate fidelities of up to $99.999(1)\%$ and a two-qubit gate fidelity of $99.93(5) \%$. Our gates are designed to decouple unwanted interactions and can be extended to other electron-nuclear spin systems. The high fidelities demonstrated provide new opportunities towards larger-scale quantum processing with colour-center qubits.

Nitrogen vacancy centres in diamond can be used for vector magnetometry. In this work we present a portable vector diamond magnetometer. Its vector capability, combined with feedback control and robust structure enables operation on moving platforms. While placed on a trolley, magnetic mapping of a room is demonstrated and the magnetometer is also shown to be operational in a moving van with the measured magnetic field shifts for the x, y, and z axes being tagged with GPS coordinates. These magnetic field measurements are in agreement with measurements taken simultaneously with a fluxgate magnetometer., Comment: 25 pages, 32 figures

The decoherence of a central electron spin due to the dynamics of a coupled electron-spin bath is a core problem in solid-state spin physics. Ensemble experiments have studied the central spin coherence in detail, but such experiments average out the underlying quantum dynamics of the bath. Here, we show the coherent back-action of an individual NV center on an electron-spin bath and use it to detect, prepare and control the dynamics of a pair of bath spins. We image the NV-pair system with sub-nanometer resolution and reveal a long dephasing time ($T_2^* = 44(9)$ ms) for a qubit encoded in the electron-spin pair. Our experiment reveals the microscopic quantum dynamics that underlie the central spin decoherence and provides new opportunities for controlling and sensing interacting spin systems.

Spins associated to optically accessible solid-state defects have emerged as a versatile platform for exploring quantum simulation, quantum sensing and quantum communication. Pioneering experiments have shown the sensing, imaging, and control of multiple nuclear spins surrounding a single electron-spin defect. However, the accessible size of these spin networks has been constrained by the spectral resolution of current methods. Here, we map a network of 50 coupled spins through high-resolution correlated sensing schemes, using a single nitrogen-vacancy center in diamond. We develop concatenated double-resonance sequences that identify spin-chains through the network. These chains reveal the characteristic spin frequencies and their interconnections with high spectral resolution, and can be fused together to map out the network. Our results provide new opportunities for quantum simulations by increasing the number of available spin qubits. Additionally, our methods might find applications in nano-scale imaging of complex spin systems external to the host crystal., Comment: 7 pages, 5 figures

Vector magnetometry provides more information than scalar measurements for magnetic surveys utilized in space, defense, medical, geological and industrial applications. These areas would benefit from a mobile vector magnetometer that can operate in extreme conditions. Here we present a scanning fiber-coupled nitrogen vacancy (NV) center vector magnetometer. Feedback control of the microwave excitation frequency is employed to improve dynamic range and maintain sensitivity during movement of the sensor head. Tracking of the excitation frequency shifts for all four orientations of the NV center allow us to image the vector magnetic field of a damaged steel plate. We calculate the magnetic tensor gradiometry images in real time, and they allow us to detect smaller damage than is possible with vector or scalar imaging., Comment: 6 pages, 5 figures

Ensembles of nitrogen vacancy centres (NVCs) in diamond can be employed for sensitive magnetometry. In this work we present a fiber-coupled NVC magnetometer with an unshielded sensitivity of (30 $\pm$ 10) pT/$\sqrt{\textrm{Hz}}$ in a (10 - 500)-Hz frequency range. This sensitivity is enabled by a relatively high green-to-red photon conversion efficiency, the use of a [100] bias field alignment, microwave and lock-in amplifier (LIA) parameter optimisation, as well as a balanced hyperfine excitation scheme. Furthermore, a silicon carbide (SiC) heat spreader is used for microwave delivery, alongside low-strain $^{12}\textrm{C}$ diamonds, one of which is placed in a second magnetically insensitive fluorescence collecting sensor head for common-mode noise cancellation. The magnetometer is capable of detecting signals from sources such as a vacuum pump up to 2 m away, with some orientation dependence but no complete dead zones, demonstrating its potential for use in remote sensing applications., Comment: 21 pages, 19 figures, correction to data analysis

Quantum networks can enable long-range quantum communication and modular quantum computation. A powerful approach is to use multi-qubit network nodes which provide the quantum memory and computational power to perform entanglement distillation, quantum error correction, and information processing. Nuclear spins associated with optically-active defects in diamond are promising qubits for this role. However, their dephasing during entanglement distribution across the optical network hinders scaling to larger systems. In this work, we show that a single 13C spin in isotopically engineered diamond offers a long-lived quantum memory that is robust to the optical link operation of an NV centre. The memory lifetime is improved by two orders-of-magnitude upon the state-of-the-art, and exceeds the best reported times for remote entanglement generation. We identify ionisation of the NV centre as a newly limiting decoherence mechanism. As a first step towards overcoming this limitation, we demonstrate that the nuclear spin state can be retrieved with high fidelity after a complete cycle of ionisation and recapture. Finally, we use numerical simulations to show that the combination of this improved memory lifetime with previously demonstrated entanglement links and gate operations can enable key primitives for quantum networks, such as deterministic non-local two-qubit logic operations and GHZ state creation across four network nodes. Our results pave the way for test-bed quantum networks capable of investigating complex algorithms and error correction.

Solid-state spin qubits are a promising platform for quantum computation and quantum networks. Recent experiments have demonstrated high-quality control over multi-qubit systems, elementary quantum algorithms and non-fault-tolerant error correction. Large-scale systems will require using error-corrected logical qubits that are operated fault-tolerantly, so that reliable computation is possible despite noisy operations. Overcoming imperfections in this way remains a major outstanding challenge for quantum science. Here, we demonstrate fault-tolerant operations on a logical qubit using spin qubits in diamond. Our approach is based on the 5-qubit code with a recently discovered flag protocol that enables fault-tolerance using a total of seven qubits. We encode the logical qubit using a novel protocol based on repeated multi-qubit measurements and show that it outperforms non-fault-tolerant encoding schemes. We then fault-tolerantly manipulate the logical qubit through a complete set of single-qubit Clifford gates. Finally, we demonstrate flagged stabilizer measurements with real-time processing of the outcomes. Such measurements are a primitive for fault-tolerant quantum error correction. While future improvements in fidelity and the number of qubits will be required, our realization of fault-tolerant protocols on the logical-qubit level is a key step towards large-scale quantum information processing based on solid-state spins.

The discrete time crystal (DTC) is a recently discovered phase of matter that spontaneously breaks time-translation symmetry. Disorder-induced many-body-localization is required to stabilize a DTC to arbitrary times, yet an experimental investigation of this localized regime has proven elusive. Here, we observe the hallmark signatures of a many-body-localized DTC using a novel quantum simulation platform based on individually controllable $^{13}$C nuclear spins in diamond. We demonstrate the characteristic long-lived spatiotemporal order and confirm that it is robust for generic initial states. Our results are consistent with the realization of an out-of-equilibrium Floquet phase of matter and establish a programmable quantum simulator based on solid-state spins for exploring many-body physics.

Understanding and protecting the coherence of individual quantum systems is a central challenge in quantum science and technology. Over the last decades, a rich variety of methods to extend coherence have been developed. A complementary approach is to look for naturally occurring systems that are inherently protected against decoherence. Here, we show that pairs of identical nuclear spins in solids form intrinsically long-lived quantum systems. We study three carbon-13 pairs in diamond and realize high-fidelity measurements of their quantum states using a single NV center in their vicinity. We then reveal that the spin pairs are robust to external perturbations due to a unique combination of three phenomena: a clock transition, a decoherence-free subspace, and a variant on motional narrowing. The resulting inhomogeneous dephasing time is $T_2^* = 1.9(3)$ minutes, the longest reported for individually controlled qubits. Finally, we develop complete control and realize an entangled state between two spin-pair qubits through projective parity measurements. These long-lived qubits are abundantly present in diamond and other solids, and provide new opportunities for quantum sensing, quantum information processing, and quantum networks.

A promising approach for multi-qubit quantum registers is to use optically addressable spins to control multiple dark electron-spin defects in the environment. While recent experiments have observed signatures of coherent interactions with such dark spins, it is an open challenge to realize the individual control required for quantum information processing. Here we demonstrate the initialisation, control and entanglement of individual dark spins associated to multiple P1 centers, which are part of a spin bath surrounding a nitrogen-vacancy center in diamond. We realize projective measurements to prepare the multiple degrees of freedom of P1 centers - their Jahn-Teller axis, nuclear spin and charge state - and exploit these to selectively access multiple P1s in the bath. We develop control and single-shot readout of the nuclear and electron spin, and use this to demonstrate an entangled state of two P1 centers. These results provide a proof-of-principle towards using dark electron-nuclear spin defects as qubits for quantum sensing, computation and networks.

Sensing small magnetic fields is relevant for many applications ranging from geology to medical diagnosis. We present a fiber-coupled diamond magnetometer with a sensitivity of (310 $\pm$ 20) pT$/\sqrt{\text{Hz}}$ in the frequency range of 10-150 Hz. This is based on optically detected magnetic resonance of an ensemble of nitrogen vacancy centers in diamond at room temperature. Fiber coupling means the sensor can be conveniently brought within 2 mm of the object under study.

Nuclear magnetic resonance (NMR) is a powerful method for determining the structure of molecules and proteins. While conventional NMR requires averaging over large ensembles, recent progress with single-spin quantum sensors has created the prospect of magnetic imaging of individual molecules. As an initial step towards this goal, isolated nuclear spins and spin pairs have been mapped. However, large clusters of interacting spins - such as found in molecules - result in highly complex spectra. Imaging these complex systems is an outstanding challenge due to the required high spectral resolution and efficient spatial reconstruction with sub-angstrom precision. Here we develop such atomic-scale imaging using a single nitrogen-vacancy (NV) centre as a quantum sensor, and demonstrate it on a model system of $27$ coupled $^{13}$C nuclear spins in a diamond. We present a new multidimensional spectroscopy method that isolates individual nuclear-nuclear spin interactions with high spectral resolution ($< 80\,$mHz) and high accuracy ($2$ mHz). We show that these interactions encode the composition and inter-connectivity of the cluster, and develop methods to extract the 3D structure of the cluster with sub-angstrom resolution. Our results demonstrate a key capability towards magnetic imaging of individual molecules and other complex spin systems.

Spins associated to single defects in solids provide promising qubits for quantum information processing and quantum networks. Recent experiments have demonstrated long coherence times, high-fidelity operations and long-range entanglement. However, control has so far been limited to a few qubits, with entangled states of three spins demonstrated. Realizing larger multi-qubit registers is challenging due to the need for quantum gates that avoid crosstalk and protect the coherence of the complete register. In this paper, we present novel decoherence-protected gates that combine dynamical decoupling of an electron spin with selective phase-controlled driving of nuclear spins. We use these gates to realize a 10-qubit quantum register consisting of the electron spin of a nitrogen-vacancy center and 9 nuclear spins in diamond. We show that the register is fully connected by generating entanglement between all 45 possible qubit pairs, and realize genuine multipartite entangled states with up to 7 qubits. Finally, we investigate the register as a multi-qubit memory. We show coherence times up to 63(2) seconds - the longest reported for a single solid-state qubit - and demonstrate that two-qubit entangled states can be stored for over 10 seconds. Our results enable the control of large quantum registers with long coherence times and therefore open the door to advanced quantum algorithms and quantum networks with solid-state spin qubits.

The neutrally-charged silicon vacancy in diamond is a promising system for quantum technologies that combines high-efficiency, broadband optical spin polarization with long spin lifetimes (T2 ~ 1 ms at 4 K) and up to 90% of optical emission into its 946 nm zero-phonon line. However, the electronic structure of SiV0 is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of SiV0 under uniaxial stress, we find the previous excited electronic structure of a single 3A1u state is incorrect, and identify instead a coupled 3Eu - 3A2u system, the lower state of which has forbidden optical emission at zero stress and so efficiently decreases the total emission of the defect: we propose a solution employing finite strain to form the basis of a spin-photon interface. Isotopic enrichment definitively assigns the 976 nm transition associated with the defect to a local mode of the silicon atom.

We demonstrate optical spin polarization of the neutrally-charged silicon-vacancy defect in diamond ($\mathrm{SiV^{0}}$), an $S=1$ defect which emits with a zero-phonon line at 946 nm. The spin polarization is found to be most efficient under resonant excitation, but non-zero at below-resonant energies. We measure an ensemble spin coherence time $T_2>100~\mathrm{\mu s}$ at low-temperature, and a spin relaxation limit of $T_1>25~\mathrm{s}$. Optical spin state initialization around 946 nm allows independent initialization of $\mathrm{SiV^{0}}$ and $\mathrm{NV^{-}}$ within the same optically-addressed volume, and $\mathrm{SiV^{0}}$ emits within the telecoms downconversion band to 1550 nm: when combined with its high Debye-Waller factor, our initial results suggest that $\mathrm{SiV^{0}}$ is a promising candidate for a long-range quantum communication technology.

We present an experimental and theoretical study of the optically detected magnetic resonance signals for ensembles of negatively charged nitrogen-vacancy (NV) centers in 13C isotopically enriched single-crystal diamond. We observe four broad transition peaks with superimposed sharp features at zero magnetic field and study their dependence on applied magnetic field. A theoretical model that reproduces all qualitative features of these spectra is developed. Understanding the magnetic-resonance spectra of NV centers in isotopically enriched diamond is important for emerging applications in nuclear magnetic resonance., Comment: 5 pages, 3 figures

The recently reported violation of a Bell inequality using entangled electronic spins in diamonds (Hensen et al., Nature 526, 682-686) provided the first loophole-free evidence against local-realist theories of nature. Here we report on data from a second Bell experiment using the same experimental setup with minor modifications. We find a violation of the CHSH-Bell inequality of $2.35 \pm 0.18$, in agreement with the first run, yielding an overall value of $S = 2.38 \pm 0.14$. We calculate the resulting $P$-values of the second experiment and of the combined Bell tests. We provide an additional analysis of the distribution of settings choices recorded during the two tests, finding that the observed distributions are consistent with uniform settings for both tests. Finally, we analytically study the effect of particular models of random number generator (RNG) imperfection on our hypothesis test. We find that the winning probability per trial in the CHSH game can be bounded knowing only the mean of the RNG bias, implying that our experimental result is robust for any model underlying the estimated average RNG bias., Comment: Open dataset will be made available online at http://dx.doi.org/10.4121/uuid:53644d31-d862-4f9f-9ad2-0b571874b829

Building a quantum repeater network for long distance quantum communication requires photons and quantum registers that comprise qubits for interaction with light, good memory capabilities and processing qubits for storage and manipulation of photons. Here we demonstrate a key step, the coherent transfer of a photon in a single solid-state nuclear spin qubit with an average fidelity of 98% and storage over 10 seconds. The storage process is achieved by coherently transferring a photon to an entangled electron-nuclear spin state of a nitrogen vacancy centre in diamond, confirmed by heralding through high fidelity single-shot readout of the electronic spin states. Stored photon states are robust against repetitive optical writing operations, required for repeater nodes. The photon-electron spin interface and the nuclear spin memory demonstrated here constitutes a major step towards practical quantum networks, and surprisingly also paves the way towards a novel entangled photon source for photonic quantum computing.

For more than 80 years, the counterintuitive predictions of quantum theory have stimulated debate about the nature of reality. In his seminal work, John Bell proved that no theory of nature that obeys locality and realism can reproduce all the predictions of quantum theory. Bell showed that in any local realist theory the correlations between distant measurements satisfy an inequality and, moreover, that this inequality can be violated according to quantum theory. This provided a recipe for experimental tests of the fundamental principles underlying the laws of nature. In the past decades, numerous ingenious Bell inequality tests have been reported. However, because of experimental limitations, all experiments to date required additional assumptions to obtain a contradiction with local realism, resulting in loopholes. Here we report on a Bell experiment that is free of any such additional assumption and thus directly tests the principles underlying Bell's inequality. We employ an event-ready scheme that enables the generation of high-fidelity entanglement between distant electron spins. Efficient spin readout avoids the fair sampling assumption (detection loophole), while the use of fast random basis selection and readout combined with a spatial separation of 1.3 km ensure the required locality conditions. We perform 245 trials testing the CHSH-Bell inequality $S \leq 2$ and find $S = 2.42 \pm 0.20$. A null hypothesis test yields a probability of $p = 0.039$ that a local-realist model for space-like separated sites produces data with a violation at least as large as observed, even when allowing for memory in the devices. This result rules out large classes of local realist theories, and paves the way for implementing device-independent quantum-secure communication and randomness certification., Comment: Raw data will be made available after publication

We report direct measurement of population dynamics in the excited state manifold of a nitrogen-vacancy (NV) center in diamond. We quantify the phonon-induced mixing rate and demonstrate that it can be completely suppressed at low temperatures. Further, we measure the intersystem crossing (ISC) rate for different excited states and develop a theoretical model that unifies the phonon-induced mixing and ISC mechanisms. We find that our model is in excellent agreement with experiment and that it can be used to predict unknown elements of the NV center's electronic structure. We discuss the model's implications for enhancing the NV center's performance as a room-temperature sensor.

Nitrogen impurities help to stabilize the negatively-charged-state of NV$^-$ in diamond, whereas magnetic fluctuations from nitrogen spins lead to decoherence of NV$^-$ qubits. It is not known what donor concentration optimizes these conflicting requirements. Here we used 10-MeV $^{15}$N$^{3+}$ ion implantation to create NV$^-$ in ultrapure diamond. Optically detected magnetic resonance of single centers revealed a high creation yield of $40\pm3$% from $^{15}$N$^{3+}$ ions and an additional yield of $56\pm3$% from $^{14}$N impurities. High-temperature anneal was used to reduce residual defects, and charge stable NV$^-$, even in a dilute $^{14}$N impurity concentration of 0.06 ppb were created with long coherence times.

Quantum measurements not only extract information from a system but also alter its state. Although the outcome of the measurement is probabilistic, the backaction imparted on the measured system is accurately described by quantum theory. Therefore, quantum measurements can be exploited for manipulating quantum systems without the need for control fields. We demonstrate measurement-only state manipulation on a nuclear spin qubit in diamond by adaptive partial measurements. We implement the partial measurement via tunable correlation with an electron ancilla qubit and subsequent ancilla readout. We vary the measurement strength to observe controlled wavefunction collapse and find post-selected quantum weak values. By combining a novel quantum non-demolition readout on the ancilla with real-time adaption of the measurement strength we realize steering of the nuclear spin to a target state by measurements alone. Besides being of fundamental interest, adaptive measurements can improve metrology applications and are key to measurement-based quantum computing., Comment: 6 pages, 4 figures

Spins of negatively charged nitrogen-vacancy (NV$^-$) defects in diamond are among the most promising candidates for solid-state qubits. The fabrication of quantum devices containing these spin-carrying defects requires position-controlled introduction of NV$^-$ defects having excellent properties such as spectral stability, long spin coherence time, and stable negative charge state. Nitrogen ion implantation and annealing enable the positioning of NV$^-$ spin qubits with high precision, but to date, the coherence times of qubits produced this way are short, presumably because of the presence of residual radiation damage. In the present work, we demonstrate that a high temperature annealing at 1000$^\circ$C allows 2 millisecond coherence times to be achieved at room temperature. These results were obtained for implantation-produced NV$^-$ defects in a high-purity, 99.99% $^{12}$C enriched single crystal chemical vapor deposited diamond. We discuss these remarkably long coherence times in the context of the thermal behavior of residual defect spins. [Published in Physical Review B {\bf{88}}, 075206 (2013)]

Quantum entanglement between spatially separated objects is one of the most intriguing phenomena in physics. The outcomes of independent measurements on entangled objects show correlations that cannot be explained by classical physics. Besides being of fundamental interest, entanglement is a unique resource for quantum information processing and communication. Entangled qubits can be used to establish private information or implement quantum logical gates. Such capabilities are particularly useful when the entangled qubits are spatially separated, opening the opportunity to create highly connected quantum networks or extend quantum cryptography to long distances. Here we present a key experiment towards the realization of long-distance quantum networks with solid-state quantum registers. We have entangled two electron spin qubits in diamond that are separated by a three-meter distance. We establish this entanglement using a robust protocol based on local creation of spin-photon entanglement and a subsequent joint measurement of the photons. Detection of the photons heralds the projection of the spin qubits onto an entangled state. We verify the resulting non-local quantum correlations by performing single-shot readout on the qubits in different bases. The long-distance entanglement reported here can be combined with recently achieved initialization, readout and entanglement operations on local long-lived nuclear spin registers, enabling deterministic long-distance teleportation, quantum repeaters and extended quantum networks.

We demonstrate preferential orientation of nitrogen-vacancy (NV) color centers along two of four possible crystallographic axes in diamonds grown by chemical vapor deposition on the {100} face. We identify the relevant growth regime and present a possible explanation of this effect. We show that preferential orientation provides increased optical read-out contrast for NV multi-spin measurements, including enhanced AC magnetic field sensitivity, thus providing an important step towards high fidelity multi-spin-qubit quantum information processing, sensing and metrology., Comment: 5 pages, 3 figures

The negatively charged nitrogen-vacancy (NV-) center in diamond is an attractive candidate for applications that range from magnetometry to quantum information processing. Here we show that only a fraction of the nitrogen (typically < 0.5 %) incorporated during homoepitaxial diamond growth by Chemical Vapor Deposition (CVD) is in the form of undecorated NV- centers. Furthermore, studies on CVD diamond grown on (110) oriented substrates show a near 100% preferential orientation of NV- centers along only the [111] and [-1-11] directions, rather than the four possible orientations. The results indicate that NV centers grow in as units, as the diamond is deposited, rather than by migration and association of their components. The NV unit of the NVH- is similarly preferentially oriented, but it is not possible to determine whether this defect was formed by H capture at a preferentially aligned NV center or as a complete unit. Reducing the number of NV orientations from 4 orientations to 2 orientations should lead to increased optically-detected magnetic resonance contrast and thus improved magnetic sensitivity in ensemble-based magnetometry., Comment: 13 Pages (inlcuding suplementary information), 4 figures

Realization of devices based on quantum laws might lead to building processors that outperform their classical analogues and establishing unconditionally secure communication protocols. Solids do usually present a serious challenge to quantum coherence. However, owing to their spin-free lattice and low spin orbit coupling, carbon materials and particularly diamond are suitable for hosting robust solid state quantum registers. We show that scalable quantum logic elements can be realized by exploring long range magnetic dipolar coupling between individually addressable single electron spins associated with separate color centers in diamond. Strong distance dependence of coupling was used to characterize the separation of single qubits 98 A with unprecedented accuracy (3 A) close to a crystal lattice spacing. Our demonstration of coherent control over both electron spins, conditional dynamics, selective readout as well as switchable interaction, opens the way towards a room temperature solid state scalable quantum register. Since both electron spins are optically addressable, this solid state quantum device operating at ambient conditions provides a degree of control that is currently available only for atomic systems., Comment: original submitted version of the manuscript

In order to improve the performance of existing technologies based on single crystal diamond grown by chemical vapour deposition (CVD), and to open up new technologies in fields such as quantum computing or solid state and semiconductor disc lasers, control over surface and bulk crystalline quality is of great importance. Inductively coupled plasma (ICP) etching using an Ar/Cl gas mixture is demonstrated to remove sub-surface damage of mechanically processed surfaces, whilst maintaining macroscopic planarity and low roughness on a microscopic scale. Dislocations in high quality single crystal CVD diamond are shown to be reduced by using substrates with a combination of low surface damage and low densities of extended defects. Substrates engineered such that only a minority of defects intersect the epitaxial surface are also shown to lead to a reduction in dislocation density. Anisotropy in the birefringence of single crystal CVD diamond due to the preferential direction of dislocation propagation is reported. Ultra low birefringence plates (< 10-5) are now available for intra-cavity heat spreaders in solid state disc lasers, and the application is no longer limited by depolarisation losses. Birefringence of less than 5*10-7 along a direction perpendicular to the CVD growth direction has been demonstrated in exceptionally high quality samples., Comment: 25 pages, 12 figures

Homoepitaxial chemical vapour deposition (CVD) on high pressure high temperature (HPHT) synthetic diamond substrates allows production of diamond material with controlled point defect content. In order to minimize the extended defect content, however, it is necessary to minimize the number of substrate extended defects that reach the initial growth surface and the nucleation of dislocations at the interface between the CVD layer and its substrate. X-ray topography has indicated that when type IIa HPHT synthetic substrates are used the density of dislocations nucleating at the interface can be less than 400 cm-2. X-ray topography, photoluminescence imaging and birefringence microscopy of HPHT grown synthetic type IIa diamond clearly show that the extended defect content is growth sector dependent. <111> sectors contain the highest concentration of both stacking faults and dislocations but <100> sectors are relatively free of both. It has been shown that HPHT treatment of such material can significantly reduce the area of stacking faults and cause dislocations to move. This knowledge, coupled with an understanding of how growth sectors develop during HPHT synthesis, has been used to guide selection and processing of substrates suitable for CVD synthesis of material with high crystalline perfection and controlled point defect content., Comment: 11 pages, 8 figures

We report on the effects of thermal treatment and ultraviolet irradiation on the point defect concentrations and optical absorption profiles of single crystal CVD synthetic diamond. All thermal treatments were below 850 K, which is lower than the growth temperature and unlikely to result in any structural change. UV-visible absorption spectroscopy measurements showed that upon thermal treatment (823 K), various broad absorption features diminished: an absorption band at 270 nm (used to deduce neutral single substitutional nitrogen (NS 0) concentrations), and also two broad features centred at approximately 360 and 520 nm. Point defect centre concentrations as a function of temperature were also deduced using electron paramagnetic resonance (EPR) spectroscopy. Above ~500 K, we observed a decrease in the concentration of NS 0 centres and a concomitant increase in the negatively charged nitrogen-vacancy-hydrogen complex (NVH \bar) concentration. Both transitions exhibited an activation energy between 0.6 and 1.2 eV, which is lower than that for the NS 0 donor (~1.7 eV). Finally, it was found that illuminating samples with intense short-wave ultraviolet light recovered the NS 0 concentration and also the 270, 360 and 520 nm absorption features. From these results, we postulate a valence-band mediated charge-transfer process between NVH and single nitrogen centres with an acceptor trap depth for NVH of 0.6- 1.2 eV. Because the loss of NS 0 concentration is greater than the increase in NVH \bar concentration we also suggest the presence of another unknown acceptor existing at a similar energy as NVH. The extent to which the colour in CVD synthetic diamond is dependent on prior history is discussed., Comment: 15 pages, 7 figures

Substantial developments have been achieved in the synthesis of chemical vapour deposition (CVD) diamond in recent years, providing engineers and designers with access to a large range of new diamond materials. CVD diamond has a number of outstanding material properties that can enable exceptional performance in applications as diverse as medical diagnostics, water treatment, radiation detection, high power electronics, consumer audio, magnetometry and novel lasers. Often the material is synthesized in planar form, however non-planar geometries are also possible and enable a number of key applications. This article reviews the material properties and characteristics of single crystal and polycrystalline CVD diamond, and how these can be utilized, focusing particularly on optics, electronics and electrochemistry. It also summarizes how CVD diamond can be tailored for specific applications, based on the ability to synthesize a consistent and engineered high performance product., Comment: 51 pages, 16 figures