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Dense, near-surface (within 10 nm) ensembles of nitrogen-vacancy (NV) centres in diamond are rapidly moving into prominence as the workhorse of a variety of envisaged applications, ranging from the imaging of fast-fluctuating magnetic signals to the facilitation of nuclear hyperpolarisation. Unlike their bulk counterparts, near-surface ensembles suffer from charge stability issues and reduced NV formation efficiency due to the diamond surface's role as a vacancy sink during annealing and an electron sink afterwards. To this end, work is ongoing to determine the best methods for producing high-quality ensembles in this regime. Here we examine the prospects for creating such ensembles cost-effectively by implanting nitrogen-rich type Ib diamond with electron donors, aiming to exploit the high bulk nitrogen density to combat surface-induced band bending in the process. This approach has previously been successful at creating deeper ensembles, however we find that in the near-surface regime there are fewer benefits over nitrogen implantation into pure diamond substrates. Our results suggest that control over diamond surface termination during annealing is key to successfully creating high-yield near-surface NV ensembles generally, and implantation into type Ib diamond may be worth revisiting once that has been accomplished., Comment: 7 pages, 3 figures

Interest in van der Waals materials often stems from a desire to miniaturise existing technologies by exploiting their intrinsic layered structure to create near atomically-thin components that do not suffer from surface defects. One appealing property is easily-switchable yet robust magnetic order, a quality only sparsely demonstrated in the case of in-plane anisotropy. In this work, we use widefield nitrogen-vacancy (NV) center magnetic imaging to measure the properties of individual flakes of CuCrP$_2$S$_6$, a multiferroic van der Waals magnet known to exhibit weak easy-plane anisotropy in the bulk. We chart the crossover between in-plane ferromagnetism in thin flakes down to the trilayer, and the bulk behaviour dominated by a low-field spin-flop transition. Further, by exploiting the directional dependence of NV center magnetometry, we are able to observe an instance of a predominantly out-of-plane ferromagetic phase near zero field, in contradiction with expectation and previous experiments on the bulk material. We attribute this to the presence of surface anisotropies arising from the sample preparation process or exposure to the ambient environment, which is expected to have more general implications for a broader class of weakly anisotropic van der Waals magnets., Comment: 24 pages, 20 figures (including supplementary information)

Magnetic imaging with nitrogen-vacancy centers in diamond, also known as quantum diamond microscopy, has emerged as a useful technique for the spatial mapping of charge currents in solid-state devices. In this work, we investigate an application to photovoltaic (PV) devices, where the currents are induced by light. We develop a widefield nitrogen-vacancy microscope that allows independent stimulus and measurement of the PV device, and test our system on a range of prototype crystalline silicon PV devices. We first demonstrate micrometer-scale vector magnetic field imaging of custom PV devices illuminated by a focused laser spot, revealing the internal current paths in both short-circuit and open-circuit conditions. We then demonstrate time-resolved imaging of photocurrents in an interdigitated back-contact solar cell, detecting current build-up and subsequent decay near the illumination point with microsecond resolution. This work presents a versatile and accessible analysis platform that may find distinct application in research on emerging PV technologies., Comment: 14 pages, 9 figures

There are two important, and potentially interconnecting, avenues to the realisation of large-scale quantum algorithms: improvement of the hardware, and reduction of resource requirements demanded by algorithm components. In focusing on the latter, one crucial subroutine to many sought-after applications is the quantum adder. A variety of different implementations exist with idiosyncratic pros and cons. One of these, the Draper quantum Fourier adder, offers the lowest qubit count of any adder, but requires a substantial number of gates as well as extremely fine rotations. In this work, we present a modification of the Draper adder which eliminates small-angle rotations to highly coarse levels, matched with some strategic corrections. This reduces hardware requirements without sacrificing the qubit saving. We show that the inherited loss of fidelity is directly given by the rate of carry and borrow bits in the computation. We derive formulae to predict this, complemented by complete gate-level matrix product state simulations of the circuit. Moreover, we analytically describe the effects of possible stochastic control error. We present an in-depth analysis of this approach in the context of Shor's algorithm, focusing on the factoring of RSA-2048. Surprisingly, we find that each of the $7\times 10^7$ quantum Fourier transforms may be truncated down to $\pi/64$, with additive rotations left only slightly finer. This result is much more efficient than previously realised. We quantify savings both in terms of logical resources and raw magic states, demonstrating that phase adders can be competitive with Toffoli-based constructions., Comment: Main text 18 pages, 8 figures. SI 11 pages, 7 figures

The widefield diamond nitrogen-vacancy (NV) microscope is a powerful instrument for imaging magnetic fields. However, a key limitation impeding its wider adoption is its complex operation, in part due to the difficulty of precisely interfacing the sensor and sample to achieve optimum spatial resolution. Here we demonstrate a solution to this interfacing problem that is both practical and reliably minimizes NV-sample standoff. We built a compact widefield NV microscope which incorporates an integrated widefield diamond probe with full position and angular control, and developed a systematic alignment procedure based on optical interference fringes. Using this platform, we imaged an ultrathin (1 nm) magnetic film test sample, and conducted a detailed study of the spatial resolution. We reproducibly achieved an estimated NV-sample standoff (and hence spatial resolution) of at most $\sim2~\mu$m across a $\sim0.5$ mm field of view. Guided by these results, we suggest future improvements for approaching the optical diffraction limit. This work is a step towards realizing a widefield NV microscope suitable for routine high-throughput mapping of magnetic fields.

Strain is extensively used to controllably tailor the electronic properties of materials. In the context of indirect band-gap semiconductors such as silicon, strain lifts the valley degeneracy of the six conduction band minima, and by extension the valley states of electrons bound to phosphorus donors. Here, single phosphorus atoms are embedded in an engineered thin layer of silicon strained to 0.8% and their wave function imaged using spatially resolved spectroscopy. A prevalence of the out-of-plane valleys is confirmed from the real-space images, and a combination of theoretical modelling tools is used to assess how this valley repopulation effect can yield isotropic exchange and tunnel interactions in the $xy$-plane relevant for atomically precise donor qubit devices. Finally, the residual presence of in-plane valleys is evidenced by a Fourier analysis of both experimental and theoretical images, and atomistic calculations highlight the importance of higher orbital excited states to obtain a precise relationship between valley population and strain. Controlling the valley degree of freedom in engineered strained epilayers provides a new competitive asset for the development of donor-based quantum technologies in silicon.

Tunneling is a fundamental quantum process with no classical equivalent, which can compete with Coulomb interactions to give rise to complex phenomena. Phosphorus dopants in silicon can be placed with atomic precision to address the different regimes arising from this competition. However, they exploit wavefunctions relying on crystal band symmetries, which tunneling interactions are inherently sensitive to. Here we directly image lattice-aperiodic valley interference between coupled atoms in silicon using scanning tunneling microscopy. Our atomistic analysis unveils the role of envelope anisotropy, valley interference and dopant placement on the Heisenberg spin exchange interaction. We find that the exchange can become immune to valley interference by engineering in-plane dopant placement along specific crystallographic directions. A vacuum-like behaviour is recovered, where the exchange is maximised to the overlap between the donor orbitals, and pair-to-pair variations limited to a factor of less than 10 considering the accuracy in dopant positioning. This robustness remains over a large range of distances, from the strongly Coulomb interacting regime relevant for high-fidelity quantum computation to strongly coupled donor arrays of interest for quantum simulation in silicon.

The nitrogen-vacancy (NV) centre in diamond has emerged as a candidate to non-invasively hyperpolarise nuclear spins in molecular systems to improve the sensitivity of nuclear magnetic resonance (NMR) experiments. Several promising proof of principle experiments have demonstrated small-scale polarisation transfer from single NVs to hydrogen spins outside the diamond. However, the scaling up of these results to the use of a dense NV ensemble, which is a necessary prerequisite for achieving realistic NMR sensitivity enhancement, has not yet been demonstrated. In this work, we present evidence for a polarising interaction between a shallow NV ensemble and external nuclear targets over a micrometre scale, and characterise the challenges in achieving useful polarisation enhancement. In the most favourable example of the interaction with hydrogen in a solid state target, a maximum polarisation transfer rate of $\approx 7500$ spins per second per NV is measured, averaged over an area containing order $10^6$ NVs. Reduced levels of polarisation efficiency are found for liquid state targets, where molecular diffusion limits the transfer. Through analysis via a theoretical model, we find that our results suggest implementation of this technique for NMR sensitivity enhancement is feasible following realistic diamond material improvements.

Dynamic nuclear polarisation (DNP) refers to a class of techniques used to increase the signal in nuclear magnetic resonance measurements by transferring spin polarisation from ensembles of highly polarised electrons to target nuclear analytes. These techniques, however, require the application of strong magnetic fields to maximise electron spin polarisation, limiting pathways for electron-nuclear (hyperfine) spin coupling and transfer. In this work we show that, for systems of electronic spin $S\geq1$ possessing an intrinsic zero-field splitting, a separate class of stronger hyperfine interactions based on lab-frame cross relaxation may be utilised to improve DNP efficiency and yield, whilst operating at moderate fields. We analytically review existing methods, and determine that this approach increases the rate of polarisation transfer to the nuclear ensemble by up to an order of magnitude over existing techniques. This result is demonstrated experimentally at room temperature using the optically polarisable $S=1$ electron spin system of the nitrogen vacancy (NV) defect in diamond as the source of electron spin polarisation. Finally we assess the utility of these NV-based approaches for the polarisation of macroscopic quantities of molecular spins external to the diamond for NMR and MRI applications., Comment: 18 pages, 7 figures

After initial proof-of-principle demonstrations, optically pumped nitrogen-vacancy (NV) centres in diamond have been proposed as a non-invasive platform to achieve hyperpolarisation of nuclear spins in molecular samples over macroscopic volumes and enhance the sensitivity in nuclear magnetic resonance (NMR) experiments. In this work, we model the process of polarisation of external samples by NV centres and theoretically evaluate their performance in a range of scenarios. We find that average nuclear spin polarisations exceeding 10% can in principle be generated over macroscopic sample volumes ($\gtrsim\mu$L) with a careful engineering of the system's geometry to maximise the diamond-sample contact area. The fabrication requirements and other practical challenges are discussed. We then explore the possibility of exploiting local polarisation enhancements in nano/micro-NMR experiments based on NV centres. For micro-NMR, we find that modest signal enhancements over thermal polarisation (by 1-2 orders of magnitude) can in essence be achieved with existing technology, with larger enhancements achievable via micro-structuring of the sample/substrate interface. However, there is generally no benefit for nano-NMR where the detection of statistical polarisation provides the largest signal-to-noise ratio. This work will guide future experimental efforts to integrate NV-based hyperpolarisation to NMR systems.

Thin layers of near-surface nitrogen-vacancy (NV) defects in diamond substrates are the workhorse of NV-based widefield magnetic microscopy, which has applications in physics, geology and biology. Several methods exist to create such NV layers, which generally involve incorporating nitrogen atoms (N) and vacancies (V) into the diamond through growth and/or irradiation. While there have been detailed studies of individual methods, a direct side-by-side experimental comparison of the resulting magnetic sensitivities is still missing. Here we characterise, at room and cryogenic temperatures, $\approx100$ nm thick NV layers fabricated via three different methods: 1) low-energy carbon irradiation of N-rich high-pressure high-temperature (HPHT) diamond, 2) carbon irradiation of $\delta$-doped chemical vapour deposition (CVD) diamond, 3) low-energy N$^+$ or CN$^-$ implantation into N-free CVD diamond. Despite significant variability within each method, we find that the best HPHT samples yield similar magnetic sensitivities (within a factor 2 on average) to our $\delta$-doped samples, of $<2$~$\mu$T Hz$^{-1/2}$ for DC magnetic fields and $<100$~nT Hz$^{-1/2}$ for AC fields (for a $400$~nm~$\times~400$~nm pixel), while the N$^+$ and CN$^-$ implanted samples exhibit an inferior sensitivity by a factor 2-5, at both room and low temperature. We also examine the crystal lattice strain caused by the respective methods and discuss the implications this has for widefield NV imaging. The pros and cons of each method, and potential future improvements, are discussed. This study highlights that low-energy irradiation of HPHT diamond, despite its relative simplicity and low cost, is a competitive method to create thin NV layers for widefield magnetic imaging.

Stray magnetic fields contain significant information about the electronic and magnetic properties of condensed matter systems. For two-dimensional (2D) systems, stray field measurements can even allow full determination of the source quantity. For instance, a 2D map of the stray magnetic field can be uniquely transformed into the 2D current density that gave rise to the field and, under some conditions, into the equivalent 2D magnetisation. However, implementing these transformations typically requires truncation of the initial data and involves singularities that may introduce errors, artefacts, and amplify noise. Here we investigate the possibility of mitigating these issues through vector measurements. For each scenario (current reconstruction and magnetisation reconstruction) the different possible reconstruction pathways are analysed and their performances compared. In particular, we find that the simultaneous measurement of both in-plane components ($B_x$ and $B_y$) enables near-ideal reconstruction of the current density, without singularity or truncation artefacts, which constitutes a significant improvement over reconstruction based on a single component (e.g. $B_z$). On the other hand, for magnetisation reconstruction, a single measurement of the out-of-plane field ($B_z$) is generally the best choice, regardless of the magnetisation direction. We verify these findings experimentally using nitrogen-vacancy magnetometry in the case of a 2D current density and a 2D magnet with perpendicular magnetisation., Comment: 14 pages, 8 figures

We use a combination of microwave fields and free precession to drive the spin of a nitrogen-vacancy (NV) center in diamond on different trajectories on the Bloch sphere, and investigate the physical significance of the frame-dependent decomposition of the total phase into geometric and dynamic parts. The experiments are performed on a two-level subspace of the spin-1 ground state of the NV, where the Aharonov-Anandan geometric phase manifests itself as a global phase, and we use the third level of the NV ground state triplet to detect it. We show that while the geometric Aharonov-Anandan phase retains its connection to the solid angle swept out by the evolving spin, it is generally accompanied by a dynamic phase that suppresses the geometric dependence of the system dynamics. These results offer insights into the physical significance of frame-dependent geometric phases., Comment: 10 pages, 5 figures

We demonstrate locally coherent heteroepitaxial growth of silicon carbide (SiC) on diamond, a result contrary to current understanding of heterojunctions as the lattice mismatch exceeds $20\%$. High-resolution transmission electron microscopy (HRTEM) confirms the quality and atomic structure near the interface. Guided by molecular dynamics simulations, a theoretical model is proposed for the interface wherein the large lattice strain is alleviated via point dislocations in a two-dimensional plane without forming extended defects in three dimensions. The possibility of realising heterojunctions of technologically important materials such as SiC with diamond offers promising pathways for thermal management of high power electronics. At a fundamental level, the study redefines our understanding of heterostructure formation with large lattice mismatch., Comment: 16 pages, 4 figures

Dynamical decoupling (DD) is a powerful method for controlling arbitrary open quantum systems. In quantum spin control, DD generally involves a sequence of timed spin flips ($\pi$ rotations) arranged to average out or selectively enhance coupling to the environment. Experimentally, errors in the spin flips are inevitably introduced, motivating efforts to optimise error-robust DD. Here we invert this paradigm: by introducing particular control "errors" in standard DD, namely a small constant deviation from perfect $\pi$ rotations (pulse adjustments), we show we obtain protocols that retain the advantages of DD while introducing the capabilities of quantum state readout and polarisation transfer. We exploit this nuclear quantum state selectivity on an ensemble of nitrogen-vacancy centres in diamond to efficiently polarise the $^{13}$C quantum bath. The underlying physical mechanism is generic and paves the way to systematic engineering of pulse-adjusted protocols with nuclear state selectivity for quantum control applications.

Quantum sensors based on optically active defects in diamond such as the nitrogen vacancy (NV) centre represent a promising platform for nanoscale sensing and imaging of magnetic, electric, temperature and strain fields. Enhancing the optical interface to such defects is key to improving the measurement sensitivity of these systems. Photonic nanostructures are often employed in the single emitter regime for this purpose, but their applicability to widefield sensing with NV ensembles remains largely unexplored. Here we fabricate and characterize closely-packed arrays of diamond nanopillars, each hosting its own dense, near-surface ensemble of NV centres. We explore the optimal geometry for diamond nanopillars hosting NV ensembles and realise enhanced spin and photoluminescence properties which lead to increased measurement sensitivities (greater than a factor of 3) when compared to unpatterned surfaces. Utilising the increased measurement sensitivity, we image the mechanical stress tensor in each nanopillar across the arrays and show the fabrication process has negligible impact on in-built stress compared to the unpatterned surface. Our results demonstrate that photonic nanostructuring of the diamond surface is a viable strategy for increasing the sensitivity of ensemble-based widefield sensing and imaging., Comment: 7 pages, 4 figures

The precise measurement of mechanical stress at the nanoscale is of fundamental and technological importance. In principle, all six independent variables of the stress tensor, which describe the direction and magnitude of compression/tension and shear stress in a solid, can be exploited to tune or enhance the properties of materials and devices. However, existing techniques to probe the local stress are generally incapable of measuring the entire stress tensor. Here, we make use of an ensemble of atomic-sized in-situ strain sensors in diamond (nitrogen-vacancy defects) to achieve spatial mapping of the full stress tensor, with a sub-micrometer spatial resolution and a sensitivity of the order of 1 MPa (corresponding to a strain of less than $10^{-6}$). To illustrate the effectiveness and versatility of the technique, we apply it to a broad range of experimental situations, including mapping the elastic stress induced by localized implantation damage, nano-indents and scratches. In addition, we observe surprisingly large stress contributions from functional electronic devices fabricated on the diamond, and also demonstrate sensitivity to deformations of materials in contact with the diamond. Our technique could enable in-situ measurements of the mechanical response of diamond nanostructures under various stimuli, with potential applications in strain engineering for diamond-based quantum technologies and in nanomechanical sensing for on-chip mass spectroscopy., Comment: 20 pages including SI

We report on a quantitative analysis of the magnetic field generated by a continuous current running in metallic micro-wires fabricated on an electrically insulating diamond substrate. A layer of nitrogen-vacancy (NV) centres engineered near the diamond surface is employed to obtain spatial maps of the vector magnetic field, by measuring Zeeman shifts through optically-detected magnetic resonance spectroscopy. The in-plane magnetic field (i.e. parallel to the diamond surface) is found to be significantly weaker than predicted, while the out-of-plane field also exhibits an unexpected modulation. We show that the measured magnetic field is incompatible with Ampere's circuital law or Gauss's law for magnetism when we assume that the current is confined to the metal, independent of the details of the current density. This result was reproduced in several diamond samples, with a measured deviation from Ampere's law by as much as 94(6)\%. To resolve this apparent magnetic anomaly, we introduce a generalised description whereby the current is allowed to flow both above the NV sensing layer (including in the metallic wire) and below the NV layer (i.e. in the diamond). Inversion of the Biot-Savart law within this two-channel description leads to a unique solution for the two current densities, which completely explains the data, is consistent with the laws of classical electrodynamics and indicates a total NV-measured current that closely matches the electrically-measured current. However, this description also leads to the surprising conclusion that in certain circumstances the majority of the current appears to flow in the diamond substrate rather than in the metallic wire, and to spread laterally in the diamond by several micrometres away from the wire. No electrical conduction was observed between nearby test wires, ruling out a conventional conductivity effect. [...], Comment: Includes new data and discussions

Band bending is a central concept in solid-state physics that arises from local variations in charge distribution especially near semiconductor interfaces and surfaces. Its precision measurement is vital in a variety of contexts from the optimisation of field effect transistors to the engineering of qubit devices with enhanced stability and coherence. Existing methods are surface sensitive and are unable to probe band bending at depth from surface or bulk charges related to crystal defects. Here we propose an in-situ method for probing band bending in a semiconductor device by imaging an array of atomic-sized quantum sensing defects to report on the local electric field. We implement the concept using the nitrogen-vacancy centre in diamond, and map the electric field at different depths under various surface terminations. We then fabricate a two-terminal device based on the conductive two-dimensional hole gas formed at a hydrogen-terminated diamond surface, and observe an unexpected spatial modulation of the electric field attributed to a complex interplay between charge injection and photo-ionisation effects. Our method opens the way to three-dimensional mapping of band bending in diamond and other semiconductors hosting suitable quantum sensors, combined with simultaneous imaging of charge transport in complex operating devices., Comment: This is a pre-print of an article published in Nature Electronics. The final authenticated version is available online at https://dx.doi.org/10.1038/s41928-018-0130-0

Characteristic dips appear in the coherence traces of a probe qubit when dynamical decoupling (DD) is applied in synchrony with the precession of target nuclear spins, forming the basis for nanoscale nuclear magnetic resonance (NMR). The frequency of the microwave control pulses is chosen to match the qubit transition but this can be detuned from resonance by experimental errors, hyperfine coupling intrinsic to the qubit, or inhomogeneous broadening. The detuning acts as an additional static field which is generally assumed to be completely removed in Hahn echo and DD experiments. Here we demonstrate that this is not the case in the presence of finite pulse-durations, where a detuning can drastically alter the coherence response of the probe qubit, with important implications for sensing applications. Using the electronic spin associated with a nitrogen-vacancy centre in diamond as a test qubit system, we analytically and experimentally study the qubit coherence response under CPMG and XY8 dynamical decoupling control schemes in the presence of finite pulse-durations and static detunings. Most striking is the splitting of the NMR resonance under CPMG, whereas under XY8 the amplitude of the NMR signal is modulated. Our work shows that the detuning error must not be neglected when extracting data from quantum sensor coherence traces.

Sensing techniques based on the negatively charged nitrogen-vacancy (NV) centre in diamond have emerged as promising candidates to characterise ultra-thin and 2D materials. An outstanding challenge to this goal is isolating the contribution of 2D materials from undesired contributions arising from surface contamination, and changes to the diamond surface induced by the sample or transfer process. Here we report on such a scenario, in which the abrasive deposition of trace amounts of materials onto a diamond gives rise to a previously unreported source of magnetic noise. By deliberately scratching the diamond surface with macroscopic blocks of various metals (Fe, Cu, Cr, Au), we are able to form ultra-thin structures (i.e. with thicknesses down to $<1$\,nm), and find that these structures give rise to a broadband source of noise. Explanation for these effects are discussed, including spin and charge noise native to the sample and/or induced by sample-surface interactions, and indirect effects, where the deposited material affects the charge stability and magnetic environment of the sensing layer. This work illustrates the high sensitivity of NV noise spectroscopy to ultra-thin materials down to sub-nm regimes -- a key step towards the study of 2D electronic systems -- and highlights the need to passivate the diamond surface for future sensing applications in ultra-thin and 2D materials., Comment: 12 pages, 11 figures, including Appendix

Substitutional donor atoms in silicon are promising qubits for quantum computation with extremely long relaxation and dephasing times demonstrated. One of the critical challenges of scaling these systems is determining inter-donor distances to achieve controllable wavefunction overlap while at the same time performing high fidelity spin readout on each qubit. Here we achieve such a device by means of scanning tunnelling microscopy lithography. We measure anti-correlated spin states between two donor-based spin qubits in silicon separated by 16${\pm}1$ nm. By utilizing an asymmetric system with two phosphorus donors at one qubit site and one on the other (2P-1P), we demonstrate that the exchange interaction can be turned on and off via electrical control of two in-plane phosphorus doped detuning gates. We determine the tunnel coupling between the 2P-1P system to be 200 MHz and provide a roadmap for the observation of two-electron coherent exchange oscillations., Comment: 19 pages, 10 figures - DEV053 - Team Viper

Magnetic imaging with ensembles of nitrogen-vacancy (NV) centres in diamond is a recently developed technique that allows for quantitative vector field mapping. Here we uncover a source of artefacts in the measured magnetic field in situations where the magnetic sample is placed in close proximity (a few tens of nm) to the NV sensing layer. Using magnetic nanoparticles as a test sample, we find that the measured field deviates significantly from the calculated field, in shape, amplitude and even in sign. By modelling the full measurement process, we show that these discrepancies are caused by the limited measurement range of NV sensors combined with the finite spatial resolution of the optical readout. We numerically investigate the role of the stand-off distance to identify an artefact-free regime, and discuss an application to ultrathin materials. This work provides a guide to predict and mitigate proximity-induced artefacts that can arise in NV-based wide-field magnetic imaging, and also demonstrates that the sensitivity of these artefacts to the sample can make them a useful tool for magnetic characterisation., Comment: Submitted to Sensors (Special Issue: Sensors based on Quantum Phenomena)

Diamond-based quantum magnetometers are more sensitive to oscillating (AC) magnetic fields than static (DC) fields because the crystal impurity-induced ensemble dephasing time $T_2^*$, the relevant sensing time for a DC field, is much shorter than the spin coherence time $T_2$, which determines the sensitivity to AC fields. Here we demonstrate measurement of DC magnetic fields using a physically rotating ensemble of nitrogen-vacancy centres at a precision ultimately limited by $T_2$ rather than $T_2^*$. The rotation period of the diamond is comparable to $T_2$ and the angle between the NV axis and the target magnetic field changes as a function of time, thus upconverting the static magnetic field to an oscillating field in the physically rotating frame. Using spin-echo interferometry of the rotating NV centres, we are able to perform measurements for over a hundred times longer compared to a conventional Ramsey experiment. With modifications our scheme could realise DC sensitivities equivalent to demonstrated NV center AC magnetic field sensitivities of order $0.1$\,nT\,Hz$^{-1/2}$., Comment: 7 pages, 4 figures

This work reports the measurement of electron $g$ factor anisotropy ($| \Delta g |$ = $| g_{001} - g_{1 \bar 1 0} |$) for phosphorous donor qubits in strained silicon (sSi = Si/Si$_{1-x}$Ge$_x$) environments. Multi-million-atom tight-binding simulations are performed to understand the measured decrease in $| \Delta g |$ as a function of $x$, which is attributed to a reduction in the interface-related anisotropy. For $x <$7\%, the variation in $| \Delta g |$ is linear and can be described by $\eta_x x$, where $\eta_x \approx$1.62$\times$ 10$^{-3}$. At $x$=20\%, the measured $| \Delta g |$ is 1.2 $\pm$ 0.04 $\times$ 10$^{-3}$, which is in good agreement with the computed value of 1$\times 10^{-3}$. When strain and electric fields are applied simultaneously, the strain effect is predicted to play a dominant role on $| \Delta g |$. Our results provide useful insights on spin properties of sSi:P for spin qubits, and more generally for devices in spintronics and valleytronics areas of research., Comment: 5 pages, 4 figures

Nanoscale quantum probes such as the nitrogen-vacancy centre in diamond have demonstrated remarkable sensing capabilities over the past decade as control over the fabrication and manipulation of these systems has evolved. However, as the size of these nanoscale quantum probes is reduced, the surface termination of the host material begins to play a prominent role as a source of magnetic and electric field noise. In this work, we show that borane-reduced nanodiamond surfaces can on average double the spin relaxation time of individual nitrogen-vacancy centres in nanodiamonds when compared to the thermally oxidised surfaces. Using a combination of infra-red and x-ray absorption spectroscopy techniques, we correlate the changes in quantum relaxation rates with the conversion of sp2 carbon to C-O and C-H bonds on the diamond surface. These findings implicate double-bonded carbon species as a dominant source of spin noise for near surface NV centres and show that through tailored engineering of the surface, we can improve the quantum properties and magnetic sensitivity of these nanoscale probes., Comment: 15 pages, 4 figures

We present a study of the spin properties of dense layers of near-surface nitrogen-vacancy (NV) centres in diamond created by nitrogen ion implantation. The optically detected magnetic resonance contrast and linewidth, spin coherence time, and spin relaxation time, are measured as a function of implantation energy, dose, annealing temperature and surface treatment. To track the presence of damage and surface-related spin defects, we perform in situ electron spin resonance spectroscopy through both double electron-electron resonance and cross-relaxation spectroscopy on the NV centres. We find that, for the energy ($4-30$~keV) and dose ($5\times10^{11}-10^{13}$~ions/cm$^2$) ranges considered, the NV spin properties are mainly governed by the dose via residual implantation-induced paramagnetic defects, but that the resulting magnetic sensitivity is essentially independent of both dose and energy. We then show that the magnetic sensitivity is significantly improved by high-temperature annealing at $\geq1100^\circ$C. Moreover, the spin properties are not significantly affected by oxygen annealing, apart from the spin relaxation time, which is dramatically decreased. Finally, the average NV depth is determined by nuclear magnetic resonance measurements, giving $\approx10$-17~nm at 4-6 keV implantation energy. This study sheds light on the optimal conditions to create dense layers of near-surface NV centres for high-sensitivity sensing and imaging applications., Comment: 12 pages, 7 figures

A precessing spin observed in a rotating frame of reference appears frequency-shifted, an effect analogous to the precession of a Foucault pendulum observed on the rotating Earth. This frequency shift can be understood as arising from a magnetic pseudo-field in the rotating frame that nevertheless has physically significant consequences, such as the Barnett effect. Detecting these pseudo-fields is experimentally challenging, as a rotating-frame sensor is required. Previous work has realised classical rotating-frame detectors. Here we use quantum sensors, nitrogen-vacancy (NV) centres, in a rapidly rotating diamond to detect pseudo-fields in the rotating frame. While conventional magnetic fields induce precession at a rate proportional to the gyromagnetic ratio, rotation shifts the precession of all spins equally, and thus primarily affect nearby $^{13}$C nuclear spins. We are thus able to explore these effects via quantum sensing in a rapidly rotating frame, and define a new approach to quantum control using rotationally-induced nuclear spin-selective magnetic fields. This work provides an integral step towards realising precision rotation sensing and quantum spin gyroscopes., Comment: 12 pages including 3 figures

Atomic-scale understanding of phosphorous donor wave functions underpins the design and optimisation of silicon based quantum devices. The accuracy of large-scale theoretical methods to compute donor wave functions is dependent on descriptions of central-cell-corrections, which are empirically fitted to match experimental binding energies, or other quantities associated with the global properties of the wave function. Direct approaches to understanding such effects in donor wave functions are of great interest. Here, we apply a comprehensive atomistic theoretical framework to compute scanning tunnelling microscopy (STM) images of subsurface donor wave functions with two central-cell-correction formalisms previously employed in the literature. The comparison between central-cell models based on real-space image features and the Fourier transform profiles indicate that the central-cell effects are visible in the simulated STM images up to ten monolayers below the silicon surface. Our study motivates a future experimental investigation of the central-cell effects via STM imaging technique with potential of fine tuning theoretical models, which could play a vital role in the design of donor-based quantum systems in scalable quantum computer architectures., Comment: Nanoscale 2017

Exchange coupling is a key ingredient for spin-based quantum technologies since it can be used to entangle spin qubits and create logical spin qubits. However, the influence of the electronic valley degree of freedom in silicon on exchange interactions is presently the subject of important open questions. Here we investigate the influence of valleys on exchange in a coupled donor/quantum dot system, a basic building block of recently proposed schemes for robust quantum information processing. Using a scanning tunneling microscope tip to position the quantum dot with sub-nm precision, we find a near monotonic exchange characteristic where lattice-aperiodic modulations associated with valley degrees of freedom comprise less than 2~\% of exchange. From this we conclude that intravalley tunneling processes that preserve the donor's $\pm x$ and $\pm y$ valley index are filtered out of the interaction with the $\pm z$ valley quantum dot, and that the $\pm x$ and $\pm y$ intervalley processes where the electron valley index changes are weak. Complemented by tight-binding calculations of exchange versus donor depth, the demonstrated electrostatic tunability of donor/QD exchange can be used to compensate the remaining intravalley $\pm z$ oscillations to realise uniform interactions in an array of highly coherent donor spins., Comment: 6 pages, 4 figures, 6 pages Supplemental Material

The s manifold energy levels for phosphorus donors in silicon are important input parameters for the design and modelling of electronic devices on the nanoscale. In this paper we calculate these energy levels from first principles using density functional theory. The wavefunction of the donor electron's ground state is found to have a form that is similar to an atomic s orbital, with an effective Bohr radius of 1.8 nm. The corresponding binding energy of this state is found to be 41 meV, which is in good agreement with the currently accepted value of 45.59 meV. We also calculate the energies of the excited 1s(T) and 1s(E) states, finding them to be 32 and 31 meV respectively. These results constitute the first ab initio confirmation of the s manifold energy levels for phosphorus donors in silicon., Comment: 9 pages, 6 figures

In quantum simulation, many-body phenomena are probed in controllable quantum systems. Recently, simulation of Bose-Hubbard Hamiltonians using cold atoms revealed previously hidden local correlations. However, fermionic many-body Hubbard phenomena such as unconventional superconductivity and spin liquids are more difficult to simulate using cold atoms. To date the required single-site measurements and cooling remain problematic, while only ensemble measurements have been achieved. Here we simulate a two-site Hubbard Hamiltonian at low effective temperatures with single-site resolution using subsurface dopants in silicon. We measure quasiparticle tunneling maps of spin-resolved states with atomic resolution, finding interference processes from which the entanglement entropy and Hubbard interactions are quantified. Entanglement, determined by spin and orbital degrees of freedom, increases with increasing covalent bond length. We find separation-tunable Hubbard interaction strengths that are suitable for simulating strongly correlated phenomena in larger arrays of dopants, establishing dopants as a platform for quantum simulation of the Hubbard model., Comment: 6 pages, 5 figures. Supplementary: 13 pages, 7 figures. New version with some additional discussion, accepted in Nature Communications

Electron Spin Resonance (ESR) describes a suite of techniques for characterising electronic systems, with applications in physics, materials science, chemistry, and biology. However, the requirement for large electron spin ensembles in conventional ESR techniques limits their spatial resolution. Here we present a method for measuring the ESR spectrum of nanoscale electronic environments by measuring the relaxation time ($T_1$) of an optically addressed single-spin probe as it is systematically tuned into resonance with the target electronic system. As a proof of concept we extract the spectral distribution for the P1 electronic spin bath in diamond using an ensemble of nitrogen-vacancy centres, and demonstrate excellent agreement with theoretical expectations. As the response of each NV spin in this experiment is dominated by a single P1 spin at a mean distance of 2.7\,nm, the extension of this all-optical technique to the single NV case will enable nanoscale ESR spectroscopy of atomic and molecular spin systems., Comment: fourteen pages (seven pages associated with main body of work, and seven pages of supplementary information), five figures (four figures associated with main body of work, and one supplementary figure)

Electron and nuclear spins of donor ensembles in isotopically pure silicon experience a vacuum-like environment, giving them extraordinary coherence. However, in contrast to a real vacuum, electrons in silicon occupy quantum superpositions of valleys in momentum space. Addressable single-qubit and two-qubit operations in silicon require that qubits are placed near interfaces, modifying the valley degrees of freedom associated with these quantum superpositions and strongly influencing qubit relaxation and exchange processes. Yet to date, spectroscopic measurements only indirectly probe wavefunctions, preventing direct experimental access to valley population, donor position, and environment. Here we directly probe the probability density of single quantum states of individual subsurface donors, in real space and reciprocal space, using scanning tunneling spectroscopy. We directly observe quantum mechanical valley interference patterns associated with linear superpositions of valleys in the donor ground state. The valley population is found to be within $5 \%$ of a bulk donor when $2.85\pm0.45$ nm from the interface, indicating that valley perturbation-induced enhancement of spin relaxation will be negligible for depths $>3$ nm. The observed valley interference will render two-qubit exchange gates sensitive to atomic-scale variations in positions of subsurface donors. Moreover, these results will also be of interest to emerging schemes proposing to encode information directly in valley polarization., Comment: 5 pages, 4 figures. Supplementary Information: 10 pages, 8 figures

Magnetic resonance detection is one of the most important tools used in life-sciences today. However, as the technique detects the magnetization of large ensembles of spins it is fundamentally limited in spatial resolution to mesoscopic scales. Here we detect the natural fluctuations of nanoscale spin ensembles at ambient temperatures by measuring the decoherence rate of a single quantum spin in response to introduced extrinsic target spins. In our experiments 45 nm nanodiamonds with single nitrogen-vacancy (NV) spins were immersed in solution containing spin 5/2 Mn^2+ ions and the NV decoherence rate measured though optically detected magnetic resonance. The presence of both freely moving and accreted Mn spins in solution were detected via significant changes in measured NV decoherence rates. Analysis of the data using a quantum cluster expansion treatment of the NV-target system found the measurements to be consistent with the detection of ~2,500 motionally diffusing Mn spins over an effective volume of (16 nm)^3 in 4.2 s, representing a reduction in target ensemble size and acquisition time of several orders of magnitude over state-of-the-art electron spin resonance detection. These measurements provide the basis for the detection of nanoscale magnetic field fluctuations with unprecedented sensitivity and resolution in ambient conditions., Comment: 9 pages, 5 figures

The confluence of quantum physics and biology is driving a new generation of quantum-based sensing and imaging technology capable of harnessing the power of quantum effects to provide tools to understand the fundamental processes of life. One of the most promising systems in this area is the nitrogen-vacancy centre in diamond - a natural spin qubit which remarkably has all the right attributes for nanoscale sensing in ambient biological conditions. Typically the nitrogen-vacancy qubits are fixed in tightly controlled/isolated experimental conditions. In this work quantum control principles of nitrogen-vacancy magnetometry are developed for a randomly diffusing diamond nanocrystal. We find that the accumulation of geometric phases, due to the rotation of the nanodiamond plays a crucial role in the application of a diffusing nanodiamond as a bio-label and magnetometer. Specifically, we show that a freely diffusing nanodiamond can offer real-time information about local magnetic fields and its own rotational behaviour, beyond continuous optically detected magnetic resonance monitoring, in parallel with operation as a fluorescent biomarker., Comment: 9 pages, with 5 figures

We demonstrate that the internal magnetic states of a single nitrogen-vacancy defect, within a rotating diamond crystal, acquire geometric phases. The geometric phase shift is manifest as a relative phase between components of a superposition of magnetic substates. We demonstrate that under reasonable experimental conditions a phase shift of up to four radians could be measured. Such a measurement of the accumulation of a geometric phase, due to macroscopic rotation, would be the first for a single atom-scale quantum system., Comment: 5 pages, 2 figures: Accepted for publication in Physical Review Letters

Optically active defect centers in diamond are of considerable interest, and ab initio calculations have provided valuable insight into the physics of these systems. Candidate structures for the Xe center in diamond, for which little structural information is known, are modeled using density functional theory. The relative thermodynamic stabilities were calculated for two likely structural arrangements. The split-vacancy structure is found to be the most stable for all temperatures up to 1500 K. A vibrational analysis was also carried out, predicting Raman- and IR-active modes which may aid in distinguishing between center structures.

The ground state spin of the negatively charged nitrogen-vacancy center in diamond has many exciting applications in quantum metrology and solid state quantum information processing, including magnetometry, electrometry, quantum memory and quantum optical networks. Each of these applications involve the interaction of the spin with some configuration of electric, magnetic and strain fields, however, to date there does not exist a detailed model of the spin's interactions with such fields, nor an understanding of how the fields influence the time-evolution of the spin and its relaxation and inhomogeneous dephasing. In this work, a general solution is obtained for the spin in any given electric-magnetic-strain field configuration for the first time, and the influence of the fields on the evolution of the spin is examined. Thus, this work provides the essential theoretical tools for the precise control and modeling of this remarkable spin in its current and future applications., Comment: 14 pages, 8 figures

Ultra-scaled FinFET transistors bear unique fingerprint-like device-to-device differences attributed to random single impurities. This paper describes how, through correlation of experimental data with multimillion atom tight-binding simulations using the NEMO 3-D code, it is possible to identify the impurity's chemical species and determine their concentration, local electric field and depth below the Si/SiO$_{\mathrm{2}}$ interface. The ability to model the excited states rather than just the ground state is the critical component of the analysis and allows the demonstration of a new approach to atomistic impurity metrology., Comment: 6 pages, 3 figures

We present atomistic simulations of the D0 to D- charging energies of a gated donor in silicon as a function of applied fields and donor depths and find good agreement with experimental measure- ments. A self-consistent field large-scale tight-binding method is used to compute the D- binding energies with a domain of over 1.4 million atoms, taking into account the full bandstructure of the host, applied fields, and interfaces. An applied field pulls the loosely bound D- electron towards the interface and reduces the charging energy significantly below the bulk values. This enables formation of bound excited D-states in these gated donors, in contrast to bulk donors. A detailed quantitative comparison of the charging energies with transport spectroscopy measurements with multiple samples of arsenic donors in ultra-scaled FinFETs validates the model results and provides physical insights. We also report measured D-data showing for the first time the presence of bound D-excited states under applied fields.

An important challenge in silicon quantum electronics in the few electron regime is the potentially small energy gap between the ground and excited orbital states in 3D quantum confined nanostructures due to the multiple valley degeneracies of the conduction band present in silicon. Understanding the "valley-orbit" (VO) gap is essential for silicon qubits, as a large VO gap prevents leakage of the qubit states into a higher dimensional Hilbert space. The VO gap varies considerably depending on quantum confinement, and can be engineered by external electric fields. In this work we investigate VO splitting experimentally and theoretically in a range of confinement regimes. We report measurements of the VO splitting in silicon quantum dot and donor devices through excited state transport spectroscopy. These results are underpinned by large-scale atomistic tight-binding calculations involving over 1 million atoms to compute VO splittings as functions of electric fields, donor depths, and surface disorder. The results provide a comprehensive picture of the range of VO splittings that can be achieved through quantum engineering., Comment: 4 pages, 4 figures

We report the observation of Lifetime Enhanced Transport (LET) based on perpendicular valleys in silicon by transport spectroscopy measurements of a two-electron system in a silicon transistor. The LET is manifested as a peculiar current step in the stability diagram due to a forbidden transition between an excited state and any of the lower energy states due perpendicular valley (and spin) configurations, offering an additional current path. By employing a detailed temperature dependence study in combination with a rate equation model, we estimate the lifetime of this particular state to exceed 48 ns. The two-electron spin-valley configurations of all relevant confined quantum states in our device were obtained by a large-scale atomistic tight-binding simulation. The LET acts as a signature of the complicated valley physics in silicon; a feature that becomes increasingly important in silicon quantum devices., Comment: 4 pages, 4 figures. (The current version (v3) is the result of splitting up the previous version (v2), and has been completely rewritten)

In drug discovery research there is a clear and urgent need for non-invasive detection of cell membrane ion channel operation with wide-field capability. Existing techniques are generally invasive, require specialized nano structures, or are only applicable to certain ion channel species. We show that quantum nanotechnology has enormous potential to provide a novel solution to this problem. The nitrogen-vacancy (NV) centre in nano-diamond is currently of great interest as a novel single atom quantum probe for nanoscale processes. However, until now, beyond the use of diamond nanocrystals as fluorescence markers, nothing was known about the quantum behaviour of a NV probe in the complex room temperature extra-cellular environment. For the first time we explore in detail the quantum dynamics of a NV probe in proximity to the ion channel, lipid bilayer and surrounding aqueous environment. Our theoretical results indicate that real-time detection of ion channel operation at millisecond resolution is possible by directly monitoring the quantum decoherence of the NV probe. With the potential to scan and scale-up to an array-based system this conclusion may have wide ranging implications for nanoscale biology and drug discovery., Comment: 7 pages, 6 figures

We propose an experiment that would produce and measure a large Aharonov-Casher (A-C) phase in a solid-state system under macroscopic motion. A diamond crystal is mounted on a spinning disk in the presence of a uniform electric field. Internal magnetic states of a single NV defect, replacing interferometer trajectories, are coherently controlled by microwave pulses. The A-C phase shift is manifested as a relative phase, of up to 17 radians, between components of a superposition of magnetic substates, which is two orders of magnitude larger than that measured in any other atom-scale quantum system., Comment: 5 pages, 2 figures

We present a systematic study of quasi-one-dimensional density of states (DOS) in electron accumulation layers near a Si-SiO2 interface. In the experiments we have employed two conceptually different objects to probe DOS, namely, a phosphorus donor and a quantum dot, both operating in the single-electron tunneling regime. We demonstrate how the peaks in DOS can be moved in the transport window independently of the other device properties, and in agreement with the theoretical analysis. This method introduces a fast and convenient way of identifying excited states in these emerging nanostructures., Comment: 4 pages, 4 figures

Recent work on fault-tolerant quantum computation making use of topological error correction shows great potential, with the 2d surface code possessing a threshold error rate approaching 1% (NJoP 9:199, 2007), (arXiv:0905.0531). However, the 2d surface code requires the use of a complex state distillation procedure to achieve universal quantum computation. The colour code of (PRL 97:180501, 2006) is a related scheme partially solving the problem, providing a means to perform all Clifford group gates transversally. We review the colour code and its error correcting methodology, discussing one approximate technique based on graph matching. We derive an analytic lower bound to the threshold error rate of 6.25% under error-free syndrome extraction, while numerical simulations indicate it may be as high as 13.3%. Inclusion of faulty syndrome extraction circuits drops the threshold to approximately 0.1%., Comment: 20 pages, 19 figures

The ability to manipulate nano-particles at the nano-scale is critical for the development of active quantum systems. This paper presents a new technique to manipulate diamond nano-crystals at the nano-scale using a scanning electron microscope, nano-manipulator and custom tapered optical fibre probes. The manipulation of a ~ 300 nm diamond crystal, containing a single nitrogen-vacancy centre, onto the endface of an optical fibre is demonstrated. The emission properties of the single photon source post manipulation are in excellent agreement with those observed on the original substrate., Comment: 6 pages, 4 figures