Search

Characterising charge transport in a material is central to the understanding of its electrical properties, and can usually only be inferred from bulk measurements of derived quantities such as current flow. Establishing connections between host material impurities and transport properties in emerging electronics materials, such as wide bandgap semiconductors, demands new diagnostic methods tailored to these unique systems, and the presence of optically-active defect centers in these materials offers a non-perturbative, in-situ characterisation system. Here, we combine charge-state sensitive optical microscopy and photoelectric detection of nitrogen-vacancy (NV) centres to directly image the flow of charge carriers inside a diamond optoelectronic device, in 3D and with temporal resolution. We optically control the charge state of background impurities inside the diamond on-demand, resulting in drastically different current flow such as filamentary channels nucleating from specific, defective regions of the device. We then optically engineered conducting channels that control carrier flow, key steps towards optically reconfigurable, wide bandgap designer optoelectronics. We anticipate our approach might be extended to probe other wide-bandgap semiconductors (SiC, GaN) relevant to present and emerging electronic technologies., Comment: 6 pages main text + 11 pages supplement, 3 figures, 8 supplementary figures. Comments welcome

Optically detected magnetic resonance (ODMR) spectroscopy of defect-rich semiconductors is being increasingly exploited for realising a variety of practical quantum sensing devices. A prime example is the on-going development of compact magnetometers based on the nitrogen-vacancy (NV) defect in diamond for the remote sensing of magnetic signals with high accuracy and sensitivity. In these applications, the ODMR-active material is integrated into the overall apparatus to form a self-contained sensor. However, some emerging applications require the sensing material to be in physical contact with an external object of interest, thus requiring an independent readout device. Here we present an ODMR-meter, a compact device specially designed to allow convenient, contactless monitoring of ODMR in a target object, and demonstrate its application to temperature monitoring with NV defects. Our prototype is composed of a handheld readout head (integrating all the necessary optical components and a microwave antenna) and a control box connected to a laptop computer, all made primarily from commercial off-the-shelf components. We test our device using an NV-rich bulk diamond as the object, demonstrate a temperature sensitivity of $10~{\rm mK}/\sqrt{\rm Hz}$ in static conditions, and demonstrate the feasibility of handheld operation. The limitations to measurement speed, sensitivity and accuracy are discussed. The presented device may find immediate use in medical and industrial applications where accurate thermometry is required, and can be extended to magnetic field measurements.

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

Predicting measurement outcomes from an underlying structure often follows directly from fundamental physical principles. However, a fundamental challenge is posed when trying to solve the inverse problem of inferring the underlying source-configuration based on measurement data. A key difficulty arises from the fact that such reconstructions often involve ill-posed transformations and that they are prone to numerical artefacts. Here, we develop a numerically efficient method to tackle this inverse problem for the reconstruction of magnetisation maps from measured magnetic stray field images. Our method is based on neural networks with physically inferred loss functions to efficiently eliminate common numerical artefacts. We report on a significant improvement in reconstruction over traditional methods and we show that our approach is robust to different magnetisation directions, both in- and out-of-plane, and to variations of the magnetic field measurement axis orientation. While we showcase the performance of our method using magnetometry with Nitrogen Vacancy centre spins in diamond, our neural-network-based approach to solving inverse problems is agnostic to the measurement technique and thus is applicable beyond the specific use-case demonstrated in this work., Comment: 11 pages, 6 figures

Widefield quantum microscopy based on nitrogen-vacancy (NV) centres in diamond has emerged as a powerful technique for quantitative mapping of magnetic fields with a sub-micron resolution. However, the accuracy of the technique has not been characterised in detail so far. Here we show that optical aberrations in the imaging system may cause large systematic errors in the measured quantity beyond trivial blurring. We introduce a simple theoretical framework to model these effects, which extends the concept of a point spread function to the domain of spectral imaging. Using this model, the magnetic field imaging of test magnetic samples is simulated under various scenarios, and the resulting errors quantified. We then apply the model to previously published data, show that apparent magnetic anomalies can be explained by the presence of optical aberrations, and demonstrate a post-processing technique to retrieve the source quantity with improved accuracy. This work presents a guide to predict and mitigate aberration induced artefacts in quantitative NV-based widefield imaging and in spectral imaging more generally., Comment: The following article has been submitted to/accepted by AVS Quantum Science. After it is published, it will be found at https://publishing.aip.org/resources/librarians/products/journals/

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

Quantum microscopes based on solid-state spin quantum sensors have recently emerged as powerful tools for probing material properties and physical processes in regimes not accessible to classical sensors, especially on the nanoscale. Such microscopes have already found utility in a variety of problems, from imaging magnetism and charge transport in nanoscale devices, to mapping remanent magnetic fields from ancient rocks and biological organisms. However, applications of quantum microscopes have so far relied on sensors hosted in a rigid, three-dimensional crystal, typically diamond, which limits their ability to closely interact with the sample under study. Here we demonstrate a versatile and robust quantum microscope using quantum sensors embedded within a thin layer of a van der Waals (vdW) material, hexagonal boron nitride (hBN). To showcase the capabilities of this platform, we assemble several active vdW heterostructures, with an hBN layer acting as the quantum sensor. We demonstrate time-resolved, simultaneous temperature and magnetic imaging near the Curie temperature of a vdW ferromagnet as well as apply this unique microscope to map out charge currents and Joule heating in graphene. By enabling intimate proximity between sensor and sample, potentially down to a single atomic layer, the hBN quantum sensor represents a paradigm shift for nanoscale quantum sensing and microscopy. Moreover, given the ubiquitous use of hBN in modern materials and condensed matter physics research, we expect our technique to find rapid and broad adoption in these fields, further motivated by the prospect of performing in-situ chemical analysis and noise spectroscopy using advanced quantum sensing protocols.

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.

A dense layer of nitrogen-vacancy (NV) centers near the surface of a diamond can be interrogated in a widefield optical microscope to produce spatially resolved maps of local quantities such as magnetic field, electric field and lattice strain, providing potentially valuable information about a sample or device placed in proximity. Since the first experimental realization of such a widefield NV microscope in 2010, the technology has seen rapid development and demonstration of applications in various areas across condensed matter physics, geoscience and biology. This Perspective analyzes the strengths and shortcomings of widefield NV microscopy in order to identify the most promising applications and guide future development. We begin with a brief review of quantum sensing with ensembles of NV centers, and the experimental implementation of widefield NV microscopy. We then compare this technology to alternative microscopy techniques commonly employed to probe magnetic materials and charge flow distributions. Current limitations in spatial resolution, measurement accuracy, magnetic sensitivity, operating conditions and ease of use, are discussed. Finally, we identify the technological advances that solve the aforementioned limitations, and argue that their implementation would result in a practical, accessible, high-throughput widefield NV microscope., Comment: 22 pages, 8 figures

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

Studies of individual quantum systems, which have led to considerable progress in our understanding of quantum physics, have traditionally been associated with atomic gases. In the last decades however, the emphasis has shifted towards solid-state systems, which are much more practical for applications. In particular, a new field has recently emerged that is concerned with the study of quantum systems based on single spins localized near point defects in crystalline solids. One such system is the nitrogen-vacancy (NV) defect in diamond. Initially used as an experimental breadboard for testing concepts of quantum physics and quantum computation, the NV defect was soon proposed as a sensitive magnetometer, capable of detecting minute magnetic fields, down to ultimate level of single spins. This atomic-sized magnetometer can be used as a standalone sensor, or integrated into an imaging system providing spatial resolution down to the atomic scale. Diamond-based instruments thus offer new pathways to probe the magnetism of matter from the mesoscale down to the nanoscale. This book chapter gives an overview of the field of diamond-based magnetic sensing and imaging, with an emphasis on already demonstrated applications of this technology. The chapter is divided into three main sections. In Section 2, the underlying physics and methods of diamond-based magnetometry are described. Section 3 is devoted to various experimental implementations that employ this new class of sensors for magnetic sensing and imaging. Finally, some recent applications are presented in Section 4., Comment: 22 pages, 12 figure

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

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

The ability to initialise nuclear spins, which are typically in a mixed state even at low temperature, is a key requirement of many protocols used in quantum computing and simulations as well as in magnetic resonance spectroscopy and imaging. Yet, it remains a challenging task that typically involves complex and inefficient protocols, limiting the fidelity of ensuing operations or the measurement sensitivity. We introduce here a class of dynamical nuclear spin state selective (DNSS) protocols which, when applied to a polarised electron spin such as the nitrogen-vacancy (NV) centre in diamond, permit the addressing of selected nuclear states of the mixture. It works by splitting the underlying eigenstates into two distinct symmetries dependent on the nuclear spin state, and independent of the electron-nuclear coupling strength. As a particular example, we show that DNSS is achievable by simply introducing a detuning in the common Carr-Purcell-Meiboom-Gill (CPMG) protocol, where the state selection is then controlled by the inter-pulse spacing. This approach offers advantages in ultra-high fidelity initialisation of nuclear registers, ensemble polarisation and single-gate manipulation of nuclei.

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

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)

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

The Dzyaloshinskii-Moriya Interaction (DMI) has recently attracted considerable interest owing to its fundamental role in the stabilization of chiral spin textures in ultrathin ferromagnets, which are interesting candidates for future spintronic technologies. Here we employ a scanning nano-magnetometer based on a single nitrogen-vacancy (NV) defect in diamond to locally probe the strength of the interfacial DMI in CoFeB/MgO ultrathin films grown on different heavy metal underlayers X=Ta,TaN, and W. By measuring the stray field emanating from DWs in micron-long wires of such materials, we observe deviations from the Bloch profile for TaN and W underlayers that are consistent with a positive DMI value favoring right-handed chiral spin structures. Moreover, our measurements suggest that the DMI constant might vary locally within a single sample, illustrating the importance of local probes for the study of magnetic order at the nanoscale., Comment: 9 pages, 4 figures

We analyze the impact of electric field and magnetic field fluctuations in the decoherence of the electronic spin associated with a single nitrogen-vacancy (NV) defect in diamond by engineering spin eigenstates protected either against magnetic noise or against electric noise. The competition between these noise sources is analyzed quantitatively by changing their relative strength through modifications of the environment. This study provides significant insights into the decoherence of the NV electronic spin, which is valuable for quantum metrology and sensing applications., Comment: 8 pages, 4 figures, including supplementary informations

We present a new approach to infer the surface density of magnetic moments $I_s$ in ultrathin ferromagnetic films with perpendicular anisotropy. It relies on quantitative stray field measurements with an atomic-size magnetometer based on the nitrogen-vacancy center in diamond. The method is applied to microstructures patterned in a 1-nm-thick film of CoFeB. We report measurements of $I_s$ with a few percent uncertainty and a spatial resolution in the range of $(100$ nm)$^2$, an improvement by several orders of magnitude over existing methods. As an example of application, we measure the modifications of $I_s$ induced by local irradiation with He$^+$ ions in an ultrathin ferromagnetic wire. This method offers a new route to study variations of magnetic properties at the nanoscale., Comment: 9 pages and 7 figures including main text and Supplemental Information

The recent observation of current-induced domain wall (DW) motion with large velocity in ultrathin magnetic wires has opened new opportunities for spintronic devices. However, there is still no consensus on the underlying mechanisms of DW motion. Key to this debate is the DW structure, which can be of Bloch or N\'eel type, and dramatically affects the efficiency of the different proposed mechanisms. To date, most experiments aiming to address this question have relied on deducing the DW structure and chirality from its motion under additional in-plane applied fields, which is indirect and involves strong assumptions on its dynamics. Here we introduce a general method enabling direct, in situ, determination of the DW structure in ultrathin ferromagnets. It relies on local measurements of the stray field distribution above the DW using a scanning nanomagnetometer based on the Nitrogen-Vacancy defect in diamond. We first apply the method to a Ta/Co40Fe40B20(1 nm)/MgO magnetic wire and find clear signature of pure Bloch DWs. In contrast, we observe left-handed N\'eel DWs in a Pt/Co(0.6 nm)/AlOx wire, providing direct evidence for the presence of a sizable Dzyaloshinskii-Moriya interaction (DMI) at the Pt/Co interface. This method offers a new path for exploring interfacial DMI in ultrathin ferromagnets and elucidating the physics of DW motion under current., Comment: Main text and Supplementary Information, 33 pages and 12 figures

We show that the orientation of nitrogen-vacancy (NV) defects in diamond can be efficiently controlled through chemical vapor deposition (CVD) growth on a (111)-oriented diamond substrate. More precisely, we demonstrate that spontaneously generated NV defects are oriented with a ~ 97 % probability along the [111] axis, corresponding to the most appealing orientation among the four possible crystallographic axes. Such a nearly perfect preferential orientation is explained by analyzing the diamond growth mechanism on a (111)-oriented substrate and could be extended to other types of defects. This work is a significant step towards the design of optimized diamond samples for quantum information and sensing applications., Comment: 6 pages, 4 figures

The isolated electronic spin system of the Nitrogen-Vacancy (NV) centre in diamond offers unique possibilities to be employed as a nanoscale sensor for detection and imaging of weak magnetic fields. Magnetic imaging with nanometric resolution and field detection capabilities in the nanotesla range are enabled by the atomic-size and exceptionally long spin-coherence times of this naturally occurring defect. The exciting perspectives that ensue from these characteristics have triggered vivid experimental activities in the emerging field of "NV magnetometry". It is the purpose of this article to review the recent progress in high-sensitivity nanoscale NV magnetometry, generate an overview of the most pertinent results of the last years and highlight perspectives for future developments. We will present the physical principles that allow for magnetic field detection with NV centres and discuss first applications of NV magnetometers that have been demonstrated in the context of nano magnetism, mesoscopic physics and the life sciences., Comment: Review article, 28 pages, 16 figures

We employ a scanning NV-center microscope to perform stray field imaging of bubble magnetic domains in a perpendicularly magnetized Pt/Co/AlOx trilayer with 6 {\AA} of Co. The stray field created by the domain walls is quantitatively mapped with few-nanometer spatial resolution, with a probe-sample distance of about 100 nm. As an example of application, we show that it should be possible to determine the Bloch or N\'eel nature of the domain walls, which is of crucial importance to the understanding of current-controlled domain wall motion., Comment: Proceedings of the 58th Annual Magnetism and Magnetic Materials (MMM) Conference

Thin-film ferromagnetic disks present a vortex spin structure whose dynamics, added to the small size (~10 nm) of their core, earned them intensive study. Here we use a scanning nitrogen-vacancy (NV) center microscope to quantitatively map the stray magnetic field above a 1 micron-diameter disk of permalloy, unambiguously revealing the vortex core. Analysis of both probe-to-sample distance and tip motion effects through stroboscopic measurements, allows us to compare directly our quantitative images to micromagnetic simulations of an ideal structure. Slight perturbations with respect to the perfect vortex structure are clearly detected either due to an applied in-plane magnetic field or imperfections of the magnetic structures. This work demonstrates the potential of scanning NV microscopy to map tiny stray field variations from nanostructures, providing a nanoscale, non-perturbative detection of their magnetic texture., Comment: 5 pages, 4 figures

We report an experimental study of the longitudinal relaxation time ($T_1$) of the electron spin associated with single nitrogen-vacancy (NV) defects hosted in nanodiamonds (ND). We first show that $T_1$ decreases over three orders of magnitude when the ND size is reduced from 100 to 10 nm owing to the interaction of the NV electron spin with a bath of paramagnetic centers lying on the ND surface. We next tune the magnetic environment by decorating the ND surface with Gd$^{3+}$ ions and observe an efficient $T_{1}$-quenching, which demonstrates magnetic noise sensing with a single electron spin. We estimate a sensitivity down to $\approx 14$ electron spins detected within 10 s, using a single NV defect hosted in a 10-nm-size ND. These results pave the way towards $T_1$-based nanoscale imaging of the spin density in biological samples., Comment: Main text with 4 figures together with supplemental information

Despite decades of advances in magnetic imaging, obtaining direct, quantitative information with nanometer scale spatial resolution remains an outstanding challenge. Recently, a new technique has emerged that employs a single nitrogen-vacancy (NV) defect in diamond as an atomic-size magnetometer. Although NV magnetometry promises significant advances in magnetic imaging, the effectiveness of the technique, when applied to realistic magnetic nanostructures, remains to be demonstrated. Here we use a scanning NV magnetometer to image a magnetic vortex, which is one of the most iconic object of nanomagnetism, owing to the small size (~10 nm) of the vortex core. We report three-dimensional, vectorial, and quantitative measurements of the stray magnetic field emitted by a vortex in a ferromagnetic square dot, including the detection of the vortex core. We find excellent agreement with micromagnetic simulations, both for regular vortex structures and for higher-order magnetization states. These experiments establish scanning NV magnetometry as a practical and unique tool for fundamental studies in nanomagnetism.

Magnetometry and magnetic imaging with nitrogen-vacancy (NV) defects in diamond rely on the optical detection of electron spin resonance (ESR). However, this technique is inherently limited to magnetic fields that are weak enough to avoid electron spin mixing. Here we focus on the high off-axis magnetic field regime for which spin mixing alters the NV defect spin dynamics. We first study in a quantitative manner the dependence of the NV defect optical properties on the magnetic field vector B. Magnetic-field-dependent time-resolved photoluminescence (PL) measurements are compared to a seven-level model of the NV defect that accounts for field-induced spin mixing. The model reproduces the decreases in (i) ESR contrast, (ii) PL intensity and (iii) excited level lifetime with an increasing off-axis magnetic field. We next demonstrate that those effects can be used to perform all-optical magnetic imaging in the high off-axis magnetic field regime. Using a scanning NV defect microscope, we map the stray field of a magnetic hard disk through both PL and fluorescence lifetime imaging. This all-optical method for high magnetic field imaging at the nanoscale might be of interest in the field of nanomagnetism, where samples producing fields in excess of several tens of milliteslas are typical.

We demonstrate quantitative magnetic field mapping with nanoscale resolution, by applying a lock-in technique on the electron spin resonance frequency of a single nitrogen-vacancy defect placed at the apex of an atomic force microscope tip. In addition, we report an all-optical magnetic imaging technique which is sensitive to large off-axis magnetic fields, thus extending the operation range of diamond-based magnetometry. Both techniques are illustrated by using a magnetic hard disk as a test sample. Owing to the non-perturbing and quantitative nature of the magnetic probe, this work should open up numerous perspectives in nanomagnetism and spintronics.