The sharp optical resonances of NV- centers in diamond at cryogenic temperatures offer powerful new capabilities for material characterization, but extracting the most detailed information typically requires careful calibration of individual sensors, limiting scalability. In this work, we use resonant photoluminescence excitation imaging to optically resolve and monitor hundreds of individual NVs across large fields of view, enabling statistical analysis of their spatial distribution with sub-diffraction resolution. This multiplexed, non-destructive approach allows quantum sensors to characterize the material platform they inhabit. Focusing on CVD-grown diamond, we uncover significant deviations from random distributions, including an unexpectedly high occurrence of closely spaced clusters comprising two or more NVs. These findings suggest non-Poissonian formation dynamics and point to spatially correlated defect generation mechanisms. Beyond offering insight into diamond growth and NV center formation, our approach enables the scalable identification of naturally occurring NV clusters - configurations that are promising for entanglement-assisted quantum information protocols and correlated sensing - and establishes a path toward structural and electronic defect analysis in various material hosts at the single-emitter level.
The sharp optical resonances of NV- centers in diamond at cryogenic temperatures offer powerful new capabilities for material characterization, but extracting the most detailed information typically requires careful calibration of individual sensors, limiting scalability. In this work, we use resonant photoluminescence excitation imaging to optically resolve and monitor hundreds of individual NVs across large fields of view, enabling statistical analysis of their spatial distribution with sub-diffraction resolution. This multiplexed, non-destructive approach allows quantum sensors to characterize the material platform they inhabit. Focusing on CVD-grown diamond, we uncover significant deviations from random distributions, including an unexpectedly high occurrence of closely spaced clusters comprising two or more NVs. These findings suggest non-Poissonian formation dynamics and point to spatially correlated defect generation mechanisms. Beyond offering insight into diamond growth and NV center formation, our approach enables the scalable identification of naturally occurring NV clusters - configurations that are promising for entanglement-assisted quantum information protocols and correlated sensing - and establishes a path toward structural and electronic defect analysis in various material hosts at the single-emitter level.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.
The nitrogen-vacancy (NV) center in diamond is a solid-state spin defect that has been widely adopted for quantum sensing and quantum information processing applications. Typically, experiments are performed either with a single isolated NV center or with an unresolved ensemble of many NV centers, resulting in a trade-off between measurement speed and spatial resolution or control over individual defects. In this work, we introduce an experimental platform that bypasses this trade-off by addressing multiple optically resolved NV centers in parallel. We perform charge- and spin-state manipulations selectively on multiple NV centers from within a larger set, and we manipulate and measure the electronic spin states of over 100 NV centers in parallel. We show that the high signal-to-noise ratio of the measurements enables the detection of shot-to-shot pairwise correlations between the spin states of 108 NV centers, corresponding to the simultaneous measurement of 5778 unique correlation coefficients. We discuss how our platform can be scaled to parallel experiments with thousands of individually resolved NV centers. These results enable parallelized high-throughput sensing experiments that retain the spatial resolution of single defects and will, thereby, help to unlock advances in applications such as single-molecule NMR and characterization of integrated circuits. In addition, our approach to multiplexing provides a natural platform for the application of recently developed correlated sensing techniques.
Optically addressable ensembles of solid-state defects, such as nitrogen-vacancy (NV) centers, are a leading modality for imaging-based magnetometry, thermometry, and strain sensing. However, monitoring the fluorescence of individual defects within a sub-diffraction ensemble remains an outstanding challenge that currently limits access to atomic-scale features and dynamics. For compact clusters of NVs, we formulate imaging-based atomic sensing as a low-dimensional multiparameter estimation task in which one seeks to localize each defect and quantify the field strength in its immediate vicinity. In this work, we employ optical spatial mode demultiplexing (SPADE) to enhance localization and brightness estimation accuracy at sub-diffraction scales. Specifically, we develop a two-stage sensing protocol that augments direct imaging by projecting the incoming optical field onto point spread function (PSF)-adapted, i.e., PAD spatial modes and Yuen–Kennedy–Lax (YKL) spatial modes, enabling efficient extraction of emitter positions and brightnesses. The YKL-SPADE measurement used for brightness estimation is shown to be quantum-optimal in the case of two emitters and establishes a new connection between quantum detection and estimation theories. We numerically evaluate the statistical performance of our protocol for sub-diffraction optically detected magnetic resonance (ODMR) and Rabi sensing experiments. Compared to conventional focal plane intensity measurements, our protocol improves emitter localization accuracy by 6× and brightness estimation accuracy by 2× for tightly confined ensembles, residing well below the diffraction limit.
Individual, luminescent point defects in solids, so-called color centers, are atomic-sized quantum systems enabling sensing and imaging with nanoscale spatial resolution. In this overview, we introduce nanoscale sensing based on individual nitrogen vacancy (NV) centers in diamond. We discuss two central challenges of the field: first, the creation of highly-coherent, shallow NV centers less than 10 nm below the surface of a single-crystal diamond; second, the fabrication of tip-like photonic nanostructures that enable efficient fluorescence collection and can be used for scanning probe imaging based on color centers with nanoscale resolution.
The NV defect center in diamond forms a pseudo-atomic quantum system with discreet optically excitable transitions between ground and excited states in the gap between valence and conduction bands, making the NV center a deep-level defect center in diamond. For the negatively charged NV center (NV-), both the ground and excited states are spin triplets (S=1) and coupling between optical and spin states provides unique opportunities for optical detection of magnetic resonance (ODMR) and quantum metrology under ambient conditions. As an atomically sized point defect that is stable in single nanodiamonds as small as a few nanometers, the NV center enables spin based imaging of temperature, electric fields, magnetic fields and mechanical strain with nanoscale spatial resolution. Made of carbon, nanodiamonds are also ideal nanoparticles for use in biological systems, exhibiting extremely low cytotoxicity, no photo bleaching and exceptional contrast in transmission electron and light microscopy. With the ability to act as both a passive, non perturbing sensor (e.g. a diamagnetic material used for sensing magnetic fields) and a connection point for two way, direct coupling of far field optics to NV− spins and indirectly to the highly localized neighborhood of atoms, electronic states and phonon modes in the local vicinity, NV diamond provides a route to nanoscale field sensing and spin based optical microscopy. These sensors are also stable in nanodiamonds. For nanoparticles, the reduction in particle diameter dramatically enhances the proportion of the material that is surface exposed, enhancing any surface related properties. Nitrogen Vacancy centers in nanodiamonds provide another example of material properties that vary with particle size. In chapter 5, evidence that modulation of nanodiamonds fluorescent emissions by electrical perturbations in their surrouding environment allows transduction of local electrodynamics into a far field optical signal capable of mapping action potentials in cardiomyocytes in presented. The unifying theme for all of the work presented in this dissertation is to enable the use of magnetic resonance signals and interactions for imaging and sensing in previously inaccessible regimes. The specific focus is on methods and techniques to enable nanoscale physical sensing and functional imaging in live tissues, with the ultimate aim to lay the predicate for the combination of both without compromise.
Single nitrogen vacancy (NV) centers in diamond have been used extensively for high-sensitivity nanoscale sensing, but conventional approaches use confocal microscopy to measure individual centers sequentially, limiting throughput and access to nonlocal physical properties, where simultaneous, high-fidelity measurement of multiple centers is required. Here, we design and implement a multiplexed NV sensing platform that allows us to read out many single NV centers simultaneously using a low-noise camera. Using this platform, we coherently manipulate and read out the spin states of hundreds of individual NV centers in parallel, achieving comparable magnetic field sensitivity to confocal measurements. We also implement a parallelized version of spin-to-charge-conversion readout for low NV center spin state readout noise and use it to demonstrate multiplexed covariance magnetometry, in which we measure ten two-point magnetic field correlators from five NV centers simultaneously. From these measurements, we demonstrate the quantitative reconstruction of spatially varying magnetic correlations arising from a current-carrying wire. The number of correlators we can measure is limited only by the available laser power, opening the door to massively multiplexed covariance magnetometry. In contrast to scanning probes for imaging spatially varying magnetic fields, our approach measures the temporal dynamics of the magnetic field at many precisely defined positions simultaneously, from which the local noise spectrum and nonlocal properties such as correlation functions can be computed. This high-fidelity readout platform will find immediate applications in studying condensed matter phenomena that are characterized by the noise spectrum or correlation functions, including quantum phase transitions, dynamics far from equilibrium, magnetic order, and correlated electron phenomena.