The NV-color center in diamond has been demonstrated as a nanoscale sensor for quantum metrology. However, the properties that make it ideal for measuring, e.g., minute electric and magnetic fields, also make it sensitive to imperfections in the diamond host. In this work, we quantify the impact of nearby native defects on the many-body states of NV-. We combine previous quantum embedding results of strain and electric-field susceptibilities of NV-with density functional theory calculations on native defects. The latter are used to parametrize continuum models in order to extrapolate the effects of native defects up to the micrometer scale. We show that under ideal measuring conditions, the optical properties of NV-are measurably affected by the strain caused by single carbon interstitials and vacancies up to 200 nm away; further, the NV-is measurably affected by the electric field of such charged (neutral) native defects within a micron (100 nm). Finally, we show how measuring multiple individual NV-centers in the vicinity of a native defect can be used to determine the nature of the defect and its charge state.

Nitrogen-vacancy (N-V) centers in diamond exhibit long spin-coherence times, optical initialization, and optical-spin readout under ambient conditions, making them excellent quantum sensors. However, the conventional scheme for charge-state initialization based on off-resonant green excitation results in significant state-preparation errors, typically around 30%. One method for improving charge-state initialization fidelity is to use multicolor excitation, which has been demonstrated to achieve a near-unity preparation fidelity for bulk N-V centers by using a few milliseconds of near-infrared (NIR) (5-mW) and green (10-mu W) excitation. The translation of such schemes to N-Vi centers near the diamond surface with higher-efficiency optical pumping would enable new applications in nanoscale sensing. Here, we demonstrate a protocol for efficient charge initialization of shallow N-V centers between 5 nm and 15 nm from the diamond surface. By carefully studying the charge dynamics of shallow N-V centers, we identify a region of parameter space that allows for near-unity (95%) charge initialization within 300 mu s of NIR (905-nm, 1-mW) and green (520-nm, 10-mu W) excitation. The time to 90% charge initialization can be as fast as 10 mu s for 4 mW of NIR and 39 mu W of green illumination. This fast, efficient charge initialization protocol will especially benefit nanoscale sensing applications in which state-preparation errors currently prohibit scaling, such as measuring higher-order multipoint correlators.

As the ability to integrate single-photon emitters into photonic architectures improves, so does the need to characterize and understand their interaction. Here we use a scanning diamond nanocrystal to investigate the interplay between the emission of room-temperature nitrogen-vacancy (NV) centres and a proximal topological waveguide. In our experiments, NVs serve as local, spectrally broad light sources, which we exploit to characterize the waveguide bandwidth as well as the correspondence between the light injection site and the directionality of wave propagation. We find that near-field coupling to the waveguide influences the spectral shape and ellipticity of the NV photoluminescence, revealing nanostructured light fields through polarization and amplitude contrasts exceeding 50%, with a spatial resolution set by the nanoparticle size. Our results expand on the sensing modalities afforded by colour centres, highlighting novel opportunities for on-chip quantum optics devices that leverage topological photonics to optimally manipulate and read out single-photon emitters.

Optically addressable spin impurities in crystals along with device engineering provide an attractive route to realizing quantum technologies in the solid state, but reconciling disparate emitter and host material constraints for a given target application is often challenging. Rare-earth ions in two-dimensional (2D) materials could mitigate this problem given the atomic-like transitions of the emitters and the versatile nature of van der Waals systems. Here we combine ion implantation, confocal microscopy, and ab initio calculations to examine the photon emission of Er-doped WS2 flakes. Optical spectroscopy reveals narrow, long-lived photoluminescence lines in the telecom band, which we activate after low-temperature thermal annealing. Spectroscopic and polarization-selective measurements show a uniform response across the ensemble, while the fluorescence brightness remains mostly unchanged with temperature, suggesting nonradiative relaxation channels are inefficient. Our results create opportunities for novel solid state devices coupling 2D-hosted, telecom-band emitters to photonic heterostructures separately optimized for photon manipulation.

Two-dimentional magnets are of significant interest both as a platform for exploring novel fundamental physics and for their potential in spintronic and optoelectronic devices. Recent bulk magnetometry studies have indicated a weak ferromagnetic response in tungsten disulfide (WS2), and theoretical predictions suggest edge-localized magnetization in flakes with partial hydrogenation. Here, room-temperature wide-field quantum diamond magnetometry to image pristine and Fe-implanted WS2 flakes of varying thicknesses (45-160 nm), exfoliated from bulk crystals and transferred to NV-doped diamond substrates, is used. Direct evidence of edge-localized stray magnetic fields, which scale linearly with applied external magnetic field (4.4-220 mT), reaching up to +/- 4.7 mu T, is observed. The edge signal shows a limited dependence on the flake thickness, consistent with dipolar field decay and sensing geometry. Magnetic simulations using five alternative models favor the presence of edge magnetization aligned along an axis slightly tilted from the normal to the WS2 flake's plane, consistent with spin canting in antiferromagnetically coupled edge states. Thses findings establish WS2 as a promising platform for edge-controlled 2D spintronics.

Understanding the behavior of confined water at liquid-solid interfaces is central to numerous physical, chemical, and biological processes, yet remains experimentally challenging. Here, we utilize shallow nitrogen-vacancy (NV) centers in diamond to investigate the nanoscale dynamics of interfacial water confined between the diamond surface and an overlying fluorinated oil droplet. Using NV-based nuclear magnetic resonance protocols selectively sensitive to 1H and 19F, we independently track water and oil near the interface under ambient conditions. Comparing opposite sides of a doubly-implanted diamond membrane - one exposed to oil, the other not - we uncover a slow, multi-day process in which the interfacial water layer is gradually depleted. This desorption appears to be driven by sustained interactions with the fluorinated oil and is supported by molecular dynamics simulations and surface-sensitive X-ray spectroscopies. Our findings provide molecular-level insight into long-timescale hydration dynamics and underscore the power of NV-NMR for probing liquid-solid heterointerfaces with chemical specificity.

Understanding the generation, transport and capture of charge carriers in semiconductors is of fundamental technological importance. However, the ensemble measurement techniques ubiquitous in electronics offer limited insight into the nanoscale environment that is crucial to the operation of modern quantum-electronic devices. Here, we combine widefield optical microscopy with precision spectroscopy to examine the capture of photogenerated holes by negatively charged nitrogen vacancy (NV-) centers in diamond. Simultaneous single-shot charge readout over hundreds of individual NVs allows us to resolve the roles of ionized impurities, reveal the formation of space charges fields, and monitor the thermalization of hot photo-carriers during diffusion. We measure effective NV- hole capture radii in excess of 0.2 um, a value approaching the Onsager limit and made possible here thanks to the near-complete neutralization of coexisting charge traps. These results establish a new platform for resolving charge dynamics beyond ensemble averages, with direct relevance to nanoscale electronics and quantum devices.

The excited orbitals of color centers often show strong electric dipoles, which can serve as a resource for entanglement, emission tuning, or electric field sensing. Here, we use resonant laser excitation to examine the electric transitions in the excited state (ES) orbitals of the negatively charged nitrogen vacancy center in diamond. By applying microwave electric fields, we perform Rabi driving between ES orbitals, and show that the dressed states can be tuned in frequency and are protected against fluctuations of the transverse electric field. In contrast with previous results, we observe sharp microwave resonances between magnetic states of the ES orbitals, and find that they are broadened due to simultaneous electric dipole driving.

Nanoscale confinement of liquids can result in enhanced viscosity, local fluidic order, or collective motion. Studying these effects, however, is notoriously difficult, mainly due to the lack of experimental methods with the required sensitivity and spatial or time resolution. Here we leverage shallow nitrogen-vacancy (NV) centers in diamond to probe the dynamics of room-temperature water molecules entrapped within ∼5 nm-tall channels formed between the diamond crystal and a suspended hexagonal boron nitride (hBN) flake. NV-enabled nuclear magnetic resonance measurements of confined water protons reveal a much reduced H2O self-diffusivity, orders of magnitude lower than that in bulk water. We posit the slow dynamics stem from the accumulation of photogenerated carriers at the interface and trapped fluid, a notion we support with the help of molecular dynamics modeling. Our results expose the importance of space charge fields in theories describing interfacial water and lay out a route for investigating other fluids under confinement.

The NV$^{-}$ color center in diamond has been demonstrated as a powerful nanosensor for quantum metrology due to the sensitivity of its optical and spin properties to external electric, magnetic, and strain fields. In view of these applications, we use quantum embedding to derive a many-body description of strain and charge induced Stark effects on the NV$^{-}$ center. We quantify how strain longitudinal to the axis of NV$^{-}$ shifts the excited states in energy, while strain with a component transverse to the NV$^{-}$ axis splits the degeneracies of the $^{3}E$ and $^{1}E$ states. The largest effects are for the optically relevant $^{3}E$ manifold, which splits into $E_{x}$ and $E_{y}$ with transverse strain. From these responses we extract strain susceptibilities for the $E_{x/y}$ states within the quasi-linear regime. Additionally, we study the many-body dipole matrix elements of the NV$^{-}$ and find a permanent dipole 1.64 D at zero strain, which is somewhat smaller than that obtained from recent density functional theory calculations. We also determine the transition dipole between the $E_{x}$ and $E_{y}$ and how it evolves with strain.

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.

Dynamic critical fluctuations in magnetic materials encode important information about magnetic ordering in the associated critical exponents. Using nitrogen-vacancy centers in diamond, we implement T_2 (spin-decoherence) noise magnetometry to study critical dynamics in a 2D Van der Waals magnet CrSBr. By analyzing NV decoherence on time scales approaching the characteristic correlation time τ_c of critical fluctuations, we extract the critical exponent ν for the correlation length. Our result deviates from the Ising prediction and highlights the role of long-range dipolar interactions in 2D CrSBr. Furthermore, analyzing the divergence of the correlation length suggests the possibility of 2D-XY criticality in CrSBr in a temperature window near T_C where static magnetic domains are absent. Our work provides a first demonstration of T_2 noise magnetometry to quantitatively analyze critical scaling behavior in 2D materials.

Optically-active spin qubits in wide-bandgap semiconductors exist in several charge states, though typically only specific charge states exhibit desirable spin or photonic properties. An understanding of how interconversion between different charge states occurs is important for most applications seeking to employ such defects in quantum sensing and information processing, and additionally serves as a means of testing and verifying models of the defect electronic structure. Here, we use charge-sensitive confocal imaging to study the wavelength dependence of optical carrier generation in diamonds hosting nitrogen-vacancy (NV) centers, silicon vacancy (SiV) centers and substitutional nitrogen (N). We study the generation of distinctive charge-capture patterns formed when photogenerated charge carriers are captured by photoluminescent defects, using light spanning 405-633\,nm (1.96-3.06\,eV). We observe distinct regimes where one- or two-photon ionization or recombination processes dominate, and a third regime where anti-Stokes mediated recombination drives weak NV charge cycling with red light. We then compare red-induced charge cycling to fast charge carrier transport between isolated single NV centers driven with green and blue light. This work reports new optically-mediated charge cycling processes of the NV centers, and has consequences for schemes using charge transfer to identify non-luminescent defects and photoelectric detection, where ambiguity exists as to the source of photocurrent.

The silicon vacancy (SiV) center in diamond is drawing much attention due to its optical and spin properties, attractive for quantum information processing and sensing. Comparatively little is known, however, about the dynamics governing SiV charge state interconversion mainly due to challenges associated with generating, stabilizing, and characterizing all possible charge states, particularly at room temperature. Here, multi-color confocal microscopy and density functional theory are used to examine photo-induced SiV recombination - from neutral, to single-, to double-negatively charged - over a broad spectral window in chemical-vapor-deposition (CVD) diamond under ambient conditions. For the SiV0 to SiV- transition, a linear growth of the photo-recombination rate with laser power at all observed wavelengths is found, a hallmark of single photon dynamics. Laser excitation of SiV‒, on the other hand, yields only fractional recombination into SiV2‒, a finding that is interpreted in terms of a photo-activated electron tunneling process from proximal nitrogen atoms.

Thanks to its low or negative surface electron affinity and chemical inertness, diamond is attracting broad attention as a source material of solvated electrons produced by optical excitation of the solid-liquid interface. Unfortunately, its wide bandgap typically imposes the use of wavelengths in the ultraviolet range, hence complicating practical applications. Here, we probe the photocurrent response of water surrounded by single-crystal diamond surfaces engineered to host shallow nitrogen-vacancy (NV) centers. We observe clear signatures of diamond-induced photocurrent generation throughout the visible range and for wavelengths reaching up to 594 nm. Experiments as a function of laser power suggest that NV centers and other coexisting defects─likely in the form of surface traps─contribute to carrier injection, though we find that NVs dominate the system response in the limit of high illumination intensities. Given our growing understanding of near-surface NV centers and adjacent point defects, these results open new perspectives in the application of diamond-liquid interfaces to photocarrier-initiated chemical and spin processes in fluids.

A significant hurdle in developing high-performance semiconductor quantum technologies utilizing deep defects is related to charge dynamics. Unfortunately, progress in modeling their charge dynamics has been hindered over recent decades due to the absence of appropriate multiscale models capable of accurately representing the atomic properties of these defects and their impact on device performance. Here, we present a semi-\textit{ab initio} method for modeling the bound states of deep defects in semiconductor quantum technologies, applied to the negatively charged nitrogen vacancy (NV$^-$) center in diamond. We employ density functional theory calculations to construct accurate potentials for an effective mass model, which allow us to unveil the structure of the bound hole states. We develop a model to calculate the nonradiative capture cross sections, which agrees with experiment within one order of magnitude. Finally, we present our attempt at constructing the photoionization spectrum of NV$^0\rightarrow$ NV$^-$ + bound hole, showing that the electronic transitions of the bound holes can be distinguished from phonon sidebands. This paper offers a practical and efficient solution to a long-standing challenge in understanding the charge dynamics of deep defects.

Color centers in wide-bandgap semiconductors feature metastable charge states that can be interconverted with the help of optical excitation at select wavelengths. The distinct fluorescence and spin properties in each of these states have been exploited to show storage of classical information in three dimensions, but the memory capacity of these platforms has been thus far limited by optical diffraction. Here, we leverage local heterogeneity in the optical transitions of color centers in diamond to demonstrate selective charge state control of individual point defects sharing the same diffraction-limited volume. Further, we apply this approach to dense color center ensembles, and show rewritable, multiplexed data storage with large areal density. These results portend alternative approaches to information processing in the form of devices with enhanced optical storage capacity.

Establishing connections between material impurities and charge transport properties in emerging electronic and quantum materials, such as wide-bandgap semiconductors, demands new diagnostic methods tailored to these unique systems. Many such materials host optically-active defect centers which offer a powerful in situ characterization system, but one that typically relies on the weak spin-electric field coupling to measure electronic phenomena. In this work, charge-state sensitive optical microscopy is combined with photoelectric detection of an array of nitrogen-vacancy (NV) centers to directly image the flow of charge carriers inside a diamond optoelectronic device, in 3D and with temporal resolution. Optical control is used to change 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. Conducting channels that control carrier flow, key steps toward optically reconfigurable, wide-bandgap optoelectronics are then engineered using light. This work might be extended to probe other wide-bandgap semiconductors (SiC, GaN) relevant to present and emerging electronic and quantum technologies.