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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)

Controlling and manipulating individual quantum systems in solids underpins the growing interest in development of scalable quantum technologies1, 2. Recently, hexagonal boron nitride (hBN) has garnered significant attention in quantum photonic applications due to its ability to host optically stable quantum emitters3-7. However, the large band gap of hBN and the lack of efficient doping inhibits electrical triggering and limits opportunities to study electrical control of emitters. Here, we show an approach to electrically modulate quantum emitters in an hBN–graphene van der Waals heterostructure. We show that quantum emitters in hBN can be reversibly activated and modulated by applying a bias across the device. Notably, a significant number of quantum emitters are intrinsically dark, and become optically active at non-zero voltages. To explain the results, we provide a heuristic electrostatic model of this unique behaviour. Finally, employing these devices we demonstrate a nearly-coherent source with linewidths of ~ 160 MHz. Our results enhance the potential of hBN for tunable solid state quantum emitters for the growing field of quantum information science.

Technologies that capture the complex electrical dynamics occurring in biological systems, across fluid membranes and at solid-liquid interfaces drive fundamental understanding and innovation in diverse fields from neuroscience to energy storage. However, the capabilities of existing voltage imaging techniques utilizing micro-electrode arrays, scanning probes, or optical fluorescence methods are respectively limited by resolution, scan speed, and photostability. Here we develop an optoelectronic voltage imaging system which overcomes these limitations by using charge-sensitive fluorescent reporters embedded within a transparent semiconducting diamond device. Electrochemical tuning of the diamond surface termination enables photostable optical voltage imaging with a quantitative linear response at biologically relevant voltages and timescales. This technology represents a major step toward label-free, large-scale, and long-term voltage recording of physical and biological systems with sub-micron resolution.

We demonstrate locally the coherent formation of silicon carbide (SiC) on diamond, a rare example of heteroepitaxy with a lattice mismatch that exceeds 20%. High-resolution transmission electron mi...

Surface micro- and nano-patterning techniques are often employed to enhance the optical interface to single photoluminescent emitters in diamond, but the utility of such surface structuring in applications requiring ensembles of emitters is still open to investigation. Here, we demonstrate scalable and fault-tolerant fabrication of closely packed arrays of fluorescent diamond nanopillars, each hosting its own dense, uniformly bright ensemble of near-surface nitrogen-vacancy centers. We explore the optimal sizes for these structures and realize enhanced spin and photoluminescence properties resulting in a 4.5 times increase in optically detected magnetic resonance sensitivity when compared to unpatterned surfaces. Utilizing the increased measurement sensitivity, we image the mechanical stress tensor in each diamond pillar across the arrays and show that the fabrication process has a negligible impact on in-built stress compared to the unpatterned surface. Our results represent a valuable pathway toward future multimodal and vector-resolved imaging studies, for instance in biological contexts.

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 submicrometer spatial resolution and a sensitivity of the order of 1 MPa (10 MPa) for the shear (axial) stress components. To illustrate the effectiveness and versatility of the technique, we apply it to a broad range of experimental situations, including mapping the stress induced by localized implantation damage, nanoindents, 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.

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., 14 pages, 8 figures

Hydrogenated detonation nanodiamonds are of great interest for emerging applications in areas from biology and medicine to lubrication. Here, we compare the two main hydrogenation techniques&mdash, annealing in hydrogen and plasma-assisted hydrogenation&mdash, for the creation of detonation nanodiamonds with a hydrogen terminated surface from the same starting material. Synchrotron-based soft X-ray spectroscopy, infrared absorption spectroscopy, and electron energy loss spectroscopy were employed to quantify diamond and non-diamond carbon contents and determine the surface chemistries of all samples. Dynamic light scattering was used to study the particles&rsquo, colloidal properties in water. For the first time, steady-state and time-resolved fluorescence spectroscopy analysis at temperatures from room temperature down to 10 K was performed to investigate the particles&rsquo, fluorescence properties. Our results show that both hydrogenation techniques produce hydrogenated detonation nanodiamonds with overall similar physico-chemical and fluorescence properties.

Microscopic imaging based on nitrogen-vacancy (NV) centres in diamond, a tool increasingly used for room-temperature studies of condensed matter systems, has recently been extended to cryogenic conditions. However, it remains unclear whether the technique is viable for imaging temperature-sensitive phenomena below 10 K given the inherent laser illumination requirements, especially in a widefield configuration. Here we realise a widefield NV microscope with a field of view of 100 $\mu$m and a base temperature of 4 K, and use it to image Abrikosov vortices and transport currents in a superconducting Nb film. We observe the disappearance of vortices upon increase of laser power and their clustering about hot spots upon decrease, indicating that laser powers as low as 1 mW (4 orders of magnitude below the NV saturation) are sufficient to locally quench the superconductivity of the film ($T_c = 9$ K). This significant local heating is confirmed by resistance measurements, which reveal the presence of large temperature gradients (several K) across the film. We then investigate the effect of such gradients on transport currents, where the current path is seen to correlate with the temperature profile even in the fully superconducting phase. In addition to highlighting the role of temperature inhomogeneities in superconductivity phenomena, this work establishes that, under sufficiently low laser power conditions, widefield NV microscopy enables imaging over mesoscopic scales down to 4 K with a submicrometer spatial resolution, providing a new platform for real-space investigations of a range of systems from topological insulators to van der Waals ferromagnets.

The recent isolation of two-dimensional van der Waals magnetic materials has uncovered rich physics that often differs from the magnetic behaviour of their bulk counterparts. However, the microscopic details of fundamental processes such as the initial magnetization or domain reversal, which govern the magnetic hysteresis, remain largely unknown in the ultrathin limit. Here we employ a widefield nitrogen-vacancy (NV) microscope to directly image these processes in few-layer flakes of magnetic semiconductor vanadium triiodide (VI$_3$). We observe complete and abrupt switching of most flakes at fields $H_c\approx0.5-1$ T (at 5 K) independent of thickness down to two atomic layers, with no intermediate partially-reversed state. The coercive field decreases as the temperature approaches the Curie temperature ($T_c\approx50$ K), however, the switching remains abrupt. We then image the initial magnetization process, which reveals thickness-dependent domain wall depinning fields well below $H_c$. These results point to ultrathin VI$_3$ being a nucleation-type hard ferromagnet, where the coercive field is set by the anisotropy-limited domain wall nucleation field. This work illustrates the power of widefield NV microscopy to investigate magnetization processes in van der Waals ferromagnets, which could be used to elucidate the origin of the hard ferromagnetic properties of other materials and explore field- and current-driven domain wall dynamics., Comment: includes SI

The nitrogen vacancy (NV) center in diamond exhibits spin-dependent fluorescence and long spin coherence times under ambient conditions, enabling applications in quantum information processing and sensing. NV centers near the surface can have strong interactions with external materials and spins, enabling new forms of nanoscale spectroscopy. However, NV spin coherence degrades within 100 nanometers of the surface, suggesting that diamond surfaces are plagued with ubiquitous defects. Prior work on characterizing near-surface noise has primarily relied on using NV centers themselves as probes; while this has the advantage of exquisite sensitivity, it provides only indirect information about the origin of the noise. Here we demonstrate that surface spectroscopy methods and single spin measurements can be used as complementary diagnostics to understand sources of noise. We find that surface morphology is crucial for realizing reproducible chemical termination, and use these insights to achieve a highly ordered, oxygen-terminated surface with suppressed noise. We observe NV centers within 10 nm of the surface with coherence times extended by an order of magnitude.

The application of imaging techniques based on ensembles of nitrogen-vacancy (NV) sensors in diamond to characterise electrical devices has been proposed, but the compatibility of NV sensing with operational gated devices remains largely unexplored. Here we fabricate graphene field-effect transistors (GFETs) directly on the diamond surface and characterise them via NV microscopy. The current density within the gated graphene is reconstructed from NV magnetometry under both mostly p- and n-type doping, but the exact doping level is found to be affected by the measurements. Additionally, we observe a surprisingly large modulation of the electric field at the diamond surface under an applied gate potential, seen in NV photoluminescence and NV electrometry measurements, suggesting a complex electrostatic response of the oxide-graphene-diamond structure. Possible solutions to mitigate these effects are discussed., 13 pages, 9 figures

Surfaces and interfaces can dominate charge carrier transport dynamics in electronic devices, impeding realization of a material's full potential. Here, we investigate transport in a two-terminal diamond device comprising a conductive channel defined by a hydrogen-terminated diamond surface, bridging two TiC contacts. The surface charge distribution was imaged by monitoring the photoluminescence of nitrogen vacancy centers incorporated below the active device layer. A strong charge accumulation near the TiC contact/H-terminated channel interface is observed and is discussed in terms of deviation from Ohmic behavior evident in the DC electrical measurements. Small voltage steps applied to the device result in current transients due to carrier trapping at the contact/diamond interface. This gives rise to dynamic negative capacitance at low AC frequencies and is discussed in detail.

We report the preparation of a silicon terminated (111) diamond surface. Low energy electron diffraction and core level photoemission demonstrate that this surface is highly ordered and homogeneous and possesses a negative electron affinity. Our analysis suggests that the surface reconstruction begins with the formation of silicon trimers that coalesce into a rhombohedral 2D silicon layer reminiscent of rhombohedral silicene.

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

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

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 $, 12 pages, 11 figures, including Appendix

Precise control of the resonant frequency of a spin qubit is of fundamental importance to quantum sensing protocols. We demonstrate a control technique on a single nitrogen-vacancy (NV) centre in diamond where the applied magnetic field is modified by fine-tuning a permanent magnet's magnetisation via temperature control. Through this control mechanism, nanoscale cross-relaxation spectroscopy of both electron and nuclear spins in the vicinity of the NV centre are performed. We then show that through maintaining the magnet at a constant temperature an order of magnitude improvement in the stability of the NV qubit frequency can be achieved. This improved stability is tested in the polarisation of a small ensemble of nearby $^{13}$C spins via resonant cross-relaxation and the lifetime of this polarisation explored. The effectiveness and relative simplicity of this technique may find use in the realisation of portable spectroscopy and/or hyperpolarisation systems., Comment: 8 pages, 6 figures including Supporting Information

We have investigated the growth and atomic interface structures of diamond on aluminum nitride (AlN). The two-step chemical vapor deposition technique is used to control diamond nucleation density, crystal size, and AlN surface orientation and polarity. Highly uniform diamond layers with a nucleation density in the range of 105-1011 cm-2 and a grain size of 0.1-5 μm are fabricated. Crystallographically abrupt interfaces between polycrystalline diamond and single-crystal AlN(0001) layers have been observed via high-resolution transmission electron microscopy and electron energy-loss spectroscopy. A majority of the diamond crystals have been found to have the diamond(111)/AlN(0001) interface relationship. Atomistic models of the bonding mechanism at the heterointerface are used to elucidate experimental observations and the role of hydrogen plasma on the growth of diamond on AlN. Nonpolar and semipolar AlN surfaces have been found to have higher resistance to process plasma and led to better crystallinity of the diamond/AlN heterointerfaces. These results underline the potential of nonpolar and semipolar AlN surfaces for the growth of high-crystal quality diamond/AlN heterointerfaces. © 2013 American Chemical Society.

Since its first isolation in 2004, graphene has been found to host a plethora of unusual electronic transport phenomena, making it a fascinating system for fundamental studies in condensed-matter physics as well as offering tremendous opportunities for future electronic and sensing devices. However, to fully realise these goals a major challenge is the ability to non-invasively image charge currents in monolayer graphene structures and devices. Typically, electronic transport in graphene has been investigated via resistivity measurements, however, such measurements are generally blind to spatial information critical to observing and studying landmark transport phenomena such as electron guiding and focusing, topological currents and viscous electron backflow in real space, and in realistic imperfect devices. Here we bring quantum imaging to bear on the problem and demonstrate high-resolution imaging of current flow in graphene structures. Our method utilises an engineered array of near-surface, atomic-sized quantum sensors in diamond, to map the vector magnetic field and reconstruct the vector current density over graphene geometries of varying complexity, from mono-ribbons to junctions, with spatial resolution at the diffraction limit and a projected sensitivity to currents as small as 1 {\mu}A. The measured current maps reveal strong spatial variations corresponding to physical defects at the sub-{\mu}m scale. The demonstrated method opens up an important new avenue to investigate fundamental electronic and spin transport in graphene structures and devices, and more generally in emerging two-dimensional materials and thin film systems., Comment: 10 pages, 4 figures; SI: 15 pages, 8 figures

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., Submitted to Sensors (Special Issue: Sensors based on Quantum Phenomena)

Fast and reliable DNA sequencing is a long-standing target in biomedical research. Recent advances in graphene-based electrical sensors have demonstrated their unprecedented sensitivity to adsorbed molecules, which holds great promise for label-free DNA sequencing technology. To date, the proposed sequencing approaches rely on the ability of graphene electric devices to probe molecular-specific interactions with a graphene surface. Here we experimentally demonstrate the use of graphene field-effect transistors (GFETs) as probes of the presence of a layer of individual DNA nucleobases adsorbed on the graphene surface. We show that GFETs are able to measure distinct coverage-dependent conductance signatures upon adsorption of the four different DNA nucleobases; a result that can be attributed to the formation of an interface dipole field. Comparison between experimental GFET results and synchrotron-based material analysis allowed prediction of the ultimate device sensitivity, and assessment of the feasibility of single nucleobase sensing with graphene.

Diamond surface termination with substitutional nitrogen is reported, leading to the formation of a stable surface which is essentially clear of sub-band surface states and has a positive electron affinity. This is predicted to be an ideal environment for near-surface nitrogen-vacancy centers in diamond and may enable magnetic and quantum sensing breakthroughs with these devices.

Synthetic diamond/AlN composite materials have been fabricated by a combination of microwave plasma-assisted chemical vapor deposition and molecular beam epitaxy. These wide band gap semiconductor heterojunctions show promises for many applications, including thermal management, deep ultraviolet light emitting devices, and high power and high temperature electronics. Here, we report results of an interface study of polycrystalline diamond layers grown on single crystal AlN(0001). High resolution transmission microscopy revealed atomically sharp interfaces between diamond and AlN. Temperature dependent Raman spectroscopy measurements showed reduced thermal resistance on diamond-coated AlN substrates compared to uncoated AlN at temperatures above 330 K.

Many advanced applications of diamond materials are now being limited by unknown surface defects, including in the fields of high power/frequency electronics and quantum computing and quantum sensing. Of acute interest to diamond researchers worldwide is the loss of quantum coherence in near-surface nitrogen-vacancy (NV) centers and the generation of associated magnetic noise at the diamond surface. Here for the first time is presented the observation of a family of primal diamond surface defects, which is suggested as the leading cause of band-bending and Fermi-pinning phenomena in diamond devices. A combination of density functional theory and synchrotron-based X-ray absorption spectroscopy is used to show that these defects introduce low-lying electronic trap states. The effect of these states is modeled on band-bending into the diamond bulk and it is shown that the properties of the important NV defect centers are affected by these defects. Due to the paramount importance of near-surface NV center properties in a growing number of fields, the density of these defects is further quantified at the surface of a variety of differently-treated device surfaces, consistent with best-practice processing techniques in the literature. The identification and characterization of these defects has wide-ranging implications for diamond devices across many fields.