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Strong interactions between spins in many-body solid-state quantum system is a crucial resource for exploring and applying non-classical states. In particular, electronic spins associated with defects in diamond system are a leading platform for the study of collective quantum phenomena and for quantum technology applications. While such solid-state quantum defect systems have the advantage of scalability and operation under ambient conditions, they face the key challenge of controlling interactions between the defects spins, since the defects are spatially fixed inside the host lattice with relative positions that cannot be well controlled during fabrication. In this work, we present a dressed-state approach to control the effective dipolar coupling between solid-state spins; and then demonstrate this scheme experimentally using two strongly-coupled nitrogen vacancy (NV) centers in diamond. Including Rabi driving terms between the m$_s$ = 0 and $\pm$1 states in the NV spin Hamiltonian allows us to turn on and off or tune the effective dipolar coupling between two NV spins. Through Ramsey spectroscopy, we detect the change of the effective dipolar field generated by the control NV spin prepared in different dressed states. To observe the change of interaction dynamics, we then deploy spin-lock-based polarization transfer measurements via a Hartmann-Hahn matching condition between two NV spins in different dressed states. We perform simulations that indicate the promise for this robust scheme to control the distribution of interaction strengths in strongly-interacting spin systems, including interaction strength homogenization in a spin ensemble, which can be a valuable tool for studying non-equilibrium quantum phases and generating high fidelity multi-spin correlated states for quantum-enhanced sensing.

We introduce a double quantum (DQ) 4-Ramsey measurement protocol that enables wide-field magnetic imaging using nitrogen vacancy (NV) centers in diamond, with enhanced homogeneity of the magnetic sensitivity relative to conventional single quantum (SQ) techniques. The DQ 4-Ramsey protocol employs microwave-phase alternation across four consecutive Ramsey (4-Ramsey) measurements to isolate the desired DQ magnetic signal from any residual SQ signal induced by microwave pulse errors. In a demonstration experiment employing a 1-$\mu$m-thick NV layer in a macroscopic diamond chip, the DQ 4-Ramsey protocol provides volume-normalized DC magnetic sensitivity of $\eta^\text{V}=34\,$nTHz$^{-1/2} \mu$m$^{3/2}$ across a $125\,\mu$m$ \,\times\,125\,\mu $m field of view, with about 5$\times$ less spatial variation in sensitivity across the field of view compared to a SQ measurement. The improved robustness and magnetic sensitivity homogeneity of the DQ 4-Ramsey protocol enable imaging of dynamic, broadband magnetic sources such as integrated circuits and electrically-active cells., Comment: 20 pages, 10 figures

We present a combined theoretical and experimental study of solid-state spin decoherence in an electronic spin bath, focusing specifically on ensembles of nitrogen vacancy (NV) color centers in diamond and the associated substitutional nitrogen spin bath. We perform measurements of NV spin free induction decay times $T_2^*$ and spin-echo coherence times $T_2$ in 25 diamond samples with nitrogen concentrations [N] ranging from 0.01 to 300\,ppm. We introduce a microscopic model and perform numerical simulations to quantitatively explain the degradation of both $T_2^*$ and $T_2$ over four orders of magnitude in [N]. Our results resolve a long-standing discrepancy observed in NV $T_2$ experiments, enabling us to describe NV ensemble spin coherence decay shapes as emerging consistently from the contribution of many individual NV., Comment: 6 pages, 4 figures + supplement

Solid-state spin systems including nitrogen-vacancy (NV) centers in diamond constitute an increasingly favored quantum sensing platform. However, present NV ensemble devices exhibit sensitivities orders of magnitude away from theoretical limits. The sensitivity shortfall both handicaps existing implementations and curtails the envisioned application space. This review analyzes present and proposed approaches to enhance the sensitivity of broadband ensemble-NV-diamond magnetometers. Improvements to the spin dephasing time, the readout fidelity, and the host diamond material properties are identified as the most promising avenues and are investigated extensively. Our analysis of sensitivity optimization establishes a foundation to stimulate development of new techniques for enhancing solid-state sensor performance., Comment: 73 pages, 36 figures, 17 tables

Quantum spin dephasing is caused by inhomogeneous coupling to the environment, with resulting limits to the measurement time and precision of spin-based sensors. The effects of spin dephasing can be especially pernicious for dense ensembles of electronic spins in the solid-state, such as for nitrogen-vacancy (NV) color centers in diamond. We report the use of two complementary techniques, spin bath control and double quantum coherence, to enhance the inhomogeneous spin dephasing time ($T_2^*$) for NV ensembles by more than an order of magnitude. In combination, these quantum control techniques (i) eliminate the effects of the dominant NV spin ensemble dephasing mechanisms, including crystal strain gradients and dipolar interactions with paramagnetic bath spins, and (ii) increase the effective NV gyromagnetic ratio by a factor of two. Applied independently, spin bath control and double quantum coherence elucidate the sources of spin dephasing over a wide range of NV and spin bath concentrations. These results demonstrate the longest reported $T_2^*$ in a solid-state electronic spin ensemble at room temperature, and outline a path towards NV-diamond magnetometers with broadband femtotesla sensitivity., Comment: PRX version

Efficient optical readout of a single, solid-state electronic spin at room temperature is a key challenge for nanoscale quantum sensing. Here we apply the technique of spin-to-charge conversion to enhance the optical spin-state readout of a single Nitrogen-Vacancy (NV) color center in room temperature diamond, with no degradation in the NV spin coherence time. We demonstrate an order-of-magnitude improvement in spin readout noise per shot and about a factor of five improvement in AC magnetometry sensitivity, compared to the conventional NV spin-state optical readout method. This improvement is realized in a widely-applicable bulk diamond system. We show that selecting for successful charge state initialization leads to possible further improvement in sensitivity. This technique is well suited to sensing applications involving low duty cycle pulsed signals, e.g., in biomagnetometry, where long deadtimes demand optimized sensitivity per shot., Comment: 11 pages

Nitrogen vacancy (NV) color centers in diamond are a leading modality for both superresolution optical imaging and nanoscale magnetic field sensing. In this work, we solve the remaining key challenge of performing optical magnetic imaging and spectroscopy selectively on multiple NV centers that are located within a diffraction-limited field-of-view. We use spin-RESOLFT microscopy to enable precision nanoscale mapping of magnetic field patterns with resolution down to ~20 nm, while employing a low power optical depletion beam. Moreover, we use a shallow NV to demonstrate the detection of proton nuclear magnetic resonance (NMR) signals exterior to the diamond, with 50 nm lateral imaging resolution and without degrading the proton NMR linewidth., Comment: main text: 5 pages, 4 figures. Supplementary Material: 5 pages, 8 figures

A high-nitrogen-concentration diamond sample was subject to 200-keV electron irradiation using a transmission electron microscope. The optical and spin-resonance properties of the nitrogen-vacancy (NV) color centers were investigated as a function of the irradiation dose up to 6.4\times1021 e-/cm2. The microwave transition frequency of the NV- center was found to shift by up to 0.6% (17.1 MHz) and the linewidth broadened with increasing electron-irradiation dose. Unexpectedly, the measured magnetic sensitivity is best at the lowest irradiation dose, even though the NV concentration increases monotonically with increasing dose. This is in large part due to a sharp reduction in optically-detected spin contrast at higher doses., Comment: 14 pages, 4 figures

We examine the possibility of probing superconductivity effects in metal nanoclusters via diamond magnetometry. Metal nanoclusters have been proposed as constitutive elements of high T$_c$ superconducting nanostructured materials. Magnetometry based on the detection of spin-selective fluorescence of nitrogen-vacancy (NV) centers in diamond is capable of nanoscale spatial resolution and could be used as a tool for investigating the properties of single or multiple clusters interacting among each other or with a surface. We have carried out sensitivity estimates and experiments to understand how these magnetometers could be used in such a situation. We studied the behavior of the sensor as a function of temperature and detected the flux exclusion effect in a superconductor by monitoring the [111]-orientation fine structure spectrum in high-NV density diamond. Our results show that phase transitions can be ascertained in a bulk superconductor with this technique while the principal zero field splitting parameter ($D$) demonstrates a temperature dependence that may require compensation schemes.