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Register a new userMicrowave-assisted spectroscopy technique for studying charge state in nitrogen-vacancy ensembles in diamond
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Diana Prado Lopes Aude Craik
Publication date
2018
fields
Physics
and research's language is
English
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We introduce a microwave-assisted spectroscopy technique to determine the relative concentrations of nitrogen vacancy (NV) centers in diamond that are negatively-charged (NV${}^-$) and neutrally-charged (NV${}^0$), and present its application to studying spin-dependent ionization in NV ensembles and enhancing NV-magnetometer sensitivity. Our technique is based on selectively modulating the NV${}^-$ fluorescence with a spin-state-resonant microwave drive to isolate, in-situ, the spectral shape of the NV${}^-$ and NV${}^0$ contributions to an NV-ensemble samples fluorescence. As well as serving as a reliable means to characterize charge state ratio, the method can be used as a tool to study spin-dependent ionization in NV ensembles. As an example, we applied the microwave technique to a high-NV-density diamond sample and found evidence for a new spin-dependent ionization pathway, which we present here alongside a rate-equation model of the data. We further show that our method can be used to enhance the contrast of optically-detected magnetic resonance (ODMR) on NV ensembles and may lead to significant sensitivity gains in NV magnetometers dominated by technical noise sources, especially where the NV${}^0$ population is large. With the high-NV-density diamond sample investigated here, we demonstrate up to a 4.8-fold enhancement in ODMR contrast. The techniques presented here may also be applied to other solid-state defects whose fluorescence can be selectively modulated by means of a microwave drive. We demonstrate this utility by applying our method to isolate room-temperature spectral signatures of the V2-type silicon vacancy from an ensemble of V1 and V2 silicon vacancies in 4H silicon carbide.
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The ability to optically initialize the electronic spin of the nitrogen-vacancy (NV) center in diamond has long been considered a valuable resource to enhance the polarization of neighboring nuclei, but efficient polarization transfer to spin species outside the diamond crystal has proven challenging. Here we demonstrate variable-magnetic-field, microwave-enabled cross-polarization from the NV electronic spin to protons in a model viscous fluid in contact with the diamond surface. Slight changes in the cross-relaxation rate as a function of the wait time between successive repetitions of the transfer protocol suggest slower molecular diffusion near the diamond surface compared to that in bulk, an observation consistent with present models of the microscopic structure of a fluid close to a solid interface.
We present an experimental and theoretical study of electronic spin decoherence in ensembles of nitrogen-vacancy (NV) color centers in bulk high-purity diamond at room temperature. Under appropriate conditions, we find ensemble NV spin coherence times (T_2) comparable to that of single NVs, with T_2 > 600 microseconds for a sample with natural abundance of 13C and paramagnetic impurity density ~10^15 cm^(-3). We also observe a sharp decrease of the coherence time with misalignment of the static magnetic field relative to the NV electronic spin axis, consistent with theoretical modeling of NV coupling to a 13C nuclear spin bath. The long coherence times and increased signal-to-noise provided by room-temperature NV ensembles will aid many applications of NV centers in precision magnetometry and quantum information.
The charge degree of freedom in solid-state defects fundamentally underpins the electronic spin degree of freedom, a workhorse of quantum technologies. Here we study charge state properties of individual near-surface nitrogen-vacancy (NV) centers in diamond, where NV$^{-}$ hosts the metrologically relevant electron spin. We find that NV$^{-}$ initialization fidelity varies between individual centers and over time, and we alleviate the deleterious effects of reduced NV$^{-}$ initialization fidelity via logic-based initialization. We also find that NV$^{-}$ can ionize in the dark, which compromises spin measurements but is mitigated by measurement protocols we present here. We identify tunneling to a single, local electron trap as the mechanism for ionization in the dark and we develop NV-assisted techniques to control and readout the trap charge state. Our understanding and command of the NVs local electrostatic environment will simultaneously guide materials design and provide novel functionalities with NV centers.
We studied the spin depolarization of ensembles of nitrogen-vacancy (NV) centers in nitrogen-rich single crystal diamonds. We found a strong dependence of the evolution of the polarized state in the dark on the concentration of NV centers. At low excitation power, we observed a simple exponential decay profile in the low-density regime and a paradoxical inverted exponential profile in the high-density regime. At higher excitation power, we observed complex behavior, with an initial sharp rise in luminescence signal after the preparation pulse followed by a slower exponential decay. Magnetic field and excitation laser power-dependent measurements suggest that the rapid initial increase of the luminescence signal is related to recharging of the nitrogen-vacancy centers (from neutral to negatively charged) in the dark. The slow relaxing component corresponds to the longitudinal spin relaxation of the NV ensemble. The shape of the decay profile reflects the interplay between two mechanisms: the NV charge state conversion in the dark and the longitudinal spin relaxation. These mechanisms, in turn, are influenced by ionization, recharging and polarization dynamics during excitation. Interestingly, we found that charge dynamics are dominant in NV-dense samples even at very feeble excitation power. These observations may be important for the use of ensembles of NV centers in precession magnetometry and sensing applications.
We use magnetic-field-dependent features in the photoluminescence of negatively charged nitrogen-vacancy centers to measure magnetic fields without the use of microwaves. In particular, we present a magnetometer based on the level anti-crossing in the triplet ground state at 102.4 mT with a demonstrated noise floor of 6 nT/$sqrt{text{Hz}}$, limited by the intensity noise of the laser and the performance of the background-field power supply. The technique presented here can be useful in applications where the sensor is placed closed to conductive materials, e.g. magnetic induction tomography or magnetic field mapping, and in remote-sensing applications since principally no electrical access is needed.
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