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Register a new userCoupled charge and spin dynamics in high-density ensembles of nitrogen-vacancy centers in diamond
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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.
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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.
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.
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size of 50~nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.
We investigate the strain-induced coupling between a nitrogen-vacancy impurity and a resonant vibrational mode of a diamond nanoresonator. We show that under near-resonant laser excitation of the electronic states of the impurity, this coupling can modify the state of the resonator and either cool the resonator close to the vibrational ground state or drive it into a large amplitude coherent state. We derive a semi-classical model to describe both effects and evaluate the stationary state of the resonator mode under various driving conditions. In particular, we find that by exploiting resonant single and multi-phonon transitions between near-degenerate electronic states, the coupling to high-frequency vibrational modes can be significantly enhanced and dominate over the intrinsic mechanical dissipation. Our results show that a single nitrogen-vacancy impurity can provide a versatile tool to manipulate and probe individual phonon modes in nanoscale diamond structures.
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