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Abstract Nitrogen-vacancy (NV) and silicon-vacancy (SiV) color defects in diamond are promising systems for applications in quantum technology. The NV and SiV centers have multiple charge states, and their charge states have different electronic, optical and spin properties. For the NV centers, most investigations for quantum sensing applications are targeted on the negatively charged NV (NV⁻), and it is important for the NV centers to be in the NV⁻state. However, it is known that the NV centers are converted to the neutrally charged state (NV⁰) under laser excitation. An energetically favorable charge state for the NV and SiV centers depends on their local environments. It is essential to understand and control the charge state dynamics for their quantum applications. In this work, we discuss the charge state dynamics of NV and SiV centers under high-voltage nanosecond pulse discharges. The NV and SiV centers coexist in the diamond crystal. The high-voltage pulses enable manipulating the charge states efficiently. These voltage-induced changes in charge states are probed by their photoluminescence spectral analysis. The analysis result from the present experiment shows that the high-voltage nanosecond pulses cause shifts of the chemical potential and can convert the charge states of NV and SiV centers with the transition rates of ∼MHz. This result also indicates that the major population of the SiV centers in the sample is the doubly negatively charged state (SiV²⁻), which is often overlooked because of its non-fluorescent and non-magnetic nature. This demonstration paves a path for a method of rapid manipulation of the NV and SiV charge states in the future. 

Becauseof thehighdielectricstrengthofwater, it isextremelydifficult todischargeplasmainacontrollablewayin the aqueous phase. By using lithographically defined electrodes andmetal/dielectric nanoparticles, we create electric field enhancementthatenablesplasmadischargeinliquidelectrolytesatsignificantlyreducedappliedvoltages.Here,weusehighvoltage (10−30kV)nanosecondpulse(20ns)dischargestogenerateatransientplasmaintheaqueousphase.Anelectrodegeometrywitha radiusofcurvatureofapproximately10μm,agapdistanceof300μm,andanestimatedfieldstrengthof5×106V/cmresultedina reductionintheplasmadischargethresholdfrom28to23kV.Asecondstructurehadaradiusofcurvatureofaround5μmanda gapdistanceof100μmhadanestimatedfieldstrengthof9×106V/cmbutdidnotperformaswellasthelargergapelectrodes. Addinggoldnanoparticles(20nmdiameter) insolutionfurther reducedthethresholdforplasmadischargeto17kVduetothe electricfieldenhancementatthewater/goldinterface,withanestimatedE-fieldenhancementof4×.Addingaluminananoparticles decoratedwithPtreducedtheplasmadischargethresholdto14kV. Inthisscenario, theemergenceofatriplepointatthejuncture ofalumina,Pt,andwaterresultsinthecoexistenceofthreedistinctdielectricconstantsatasingularlocation.Thisleadstoanotable concentrationof electric field, effectively aiding in the initiationof plasma discharge at a reduced voltage. To gain amore comprehensive and detailed understanding of the electric field enhancement mechanism, we performed rigorous numerical simulations.Thesesimulationsprovidevaluableinsights intotheintricateinterplaybetweenthelithographicallydefinedelectrodes, thenanoparticles, andthe resultingelectricfielddistribution, enablingus toextract crucial informationandoptimize thedesign parameters forenhancedperformance. 

Understanding the spatial distribution of the P1 centers is crucial for diamond-based sensors and quantum devices. P1 centers serve as polarization sources for dynamic nuclear polarization (DNP) quantum sensing and play a significant role in the relaxation of nitrogen vacancy (NV) centers. Additionally, the distribution of NV centers correlates with the distribution of P1 centers, as NV centers are formed through the conversion of P1 centers. We utilized DNP and pulsed electron paramagnetic resonance (EPR) techniques that revealed strong clustering of a significant population of P1 centers that exhibit exchange coupling and produce asymmetric line shapes. The 13C DNP frequency profile at a high magnetic field revealed a pattern that requires an asymmetric EPR line shape of the P1 clusters with electron–electron (e–e) coupling strengths exceeding the 13C nuclear Larmor frequency. EPR and DNP characterization at high magnetic fields was necessary to resolve energy contributions from different e–e couplings. We employed a two-frequency pump–probe pulsed electron double resonance technique to show cross-talk between the isolated and clustered P1 centers. This finding implies that the clustered P1 centers affect all of the P1 populations. Direct observation of clustered P1 centers and their asymmetric line shape offers a novel and crucial insight into understanding magnetic noise sources for quantum information applications of diamonds and for designing diamond-based polarizing agents with optimized DNP efficiency for 13C and other nuclear spins of analytes. We propose that room temperature 13C DNP at a high field, achievable through straightforward modifications to existing solution-state NMR systems, is a potent tool for evaluating and controlling diamond defects. 

The nitrogen-vacancy (NV) center in diamond has enabled studies of nanoscale nuclear magnetic resonance (NMR) and electron paramagnetic resonance with high sensitivity in small sample volumes. Most NV-detected NMR (NV-NMR) experiments are performed at low magnetic fields. While low fields are useful in many applications, high-field NV-NMR with fine spectral resolution, high signal sensitivity, and the capability to observe a wider range of nuclei is advantageous for surface detection, microfluidic, and condensed matter studies aimed at probing micro- and nanoscale features. However, only a handful of experiments above 1 T were reported. Herein, we report 13C NV-NMR spectroscopy at 4.2 T, where the NV Larmor frequency is 115 GHz. Using an electron-nuclear double resonance technique, we successfully detect NV-NMR of two diamond samples. The analysis of the NMR linewidth based on the dipolar broadening theory of Van Vleck shows that the observed linewidths from sample 1 are consistent with the intrinsic NMR linewidth of the sample. For sample 2 we find a narrower linewidth of 44 ppm. This work paves the way for new applications of nanoscale NV-NMR.