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Detecting External Electron Spins Using Nitrogen-Vacancy Centers

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 Publication date 2012
  fields Physics
and research's language is English




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Near-surface nitrogen-vacancy (NV) centers have been created in diamond through low energy implantation of 15N to sense electron spins that are external to the diamond. By performing double resonance experiments, we have verified the presence of g=2 spins on a diamond crystal that was subjected to various surface treatments, including coating with a polymer film containing the free radical 2,2-diphenyl-1-picrylhydrazyl (DPPH). Subsequent acid cleaning eliminated the spin signal without otherwise disrupting the NV center, providing strong evidence that the spins were at the surface. A clear correlation was observed between the size of the detected spin signal and the relaxation time T2 for the six NV centers studied. We have developed a model that takes into account the finite correlation time of the fluctuating magnetic fields generated by the external spins, and used it to infer the signal strength and correlation time of the magnetic fields from these spins. This model also highlights the sensitivity advantage of active manipulation of the longitudinal spin component via double resonance over passive detection schemes that measure the transverse component of spin.

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The nitrogen-vacancy (NV) centre in diamond has emerged as a candidate to non-invasively hyperpolarise nuclear spins in molecular systems to improve the sensitivity of nuclear magnetic resonance (NMR) experiments. Several promising proof of principle experiments have demonstrated small-scale polarisation transfer from single NVs to hydrogen spins outside the diamond. However, the scaling up of these results to the use of a dense NV ensemble, which is a necessary prerequisite for achieving realistic NMR sensitivity enhancement, has not yet been demonstrated. In this work, we present evidence for a polarising interaction between a shallow NV ensemble and external nuclear targets over a micrometre scale, and characterise the challenges in achieving useful polarisation enhancement. In the most favourable example of the interaction with hydrogen in a solid state target, a maximum polarisation transfer rate of $approx 7500$ spins per second per NV is measured, averaged over an area containing order $10^6$ NVs. Reduced levels of polarisation efficiency are found for liquid state targets, where molecular diffusion limits the transfer. Through analysis via a theoretical model, we find that our results suggest implementation of this technique for NMR sensitivity enhancement is feasible following realistic diamond material improvements.
The conversion of neutral nitrogen-vacancy centers to negatively charged nitrogen-vacancy centers is demonstrated for centers created by ion implantation and annealing in high-purity diamond. Conversion occurs with surface exposure to an oxygen atmosphere at 465 C. The spectral properties of the charge-converted centers are investigated. Charge state control of nitrogen-vacancy centers close to the diamond surface is an important step toward the integration of these centers into devices for quantum information and magnetic sensing applications.
We demonstrate preferential orientation of nitrogen-vacancy (NV) color centers along two of four possible crystallographic axes in diamonds grown by chemical vapor deposition on the {100} face. We identify the relevant growth regime and present a possible explanation of this effect. We show that preferential orientation provides increased optical read-out contrast for NV multi-spin measurements, including enhanced AC magnetic field sensitivity, thus providing an important step towards high fidelity multi-spin-qubit quantum information processing, sensing and metrology.
Shallow nitrogen-vacancy (NV) centers in diamond are promising for nano-magnetometry for they can be placed proximate to targets. To study the intrinsic magnetic properties, zero-field magnetometry is desirable. However, for shallow NV centers under zero field, the strain near diamond surfaces would cause level anti-crossing between the spin states, leading to clock transitions whose frequencies are insensitive to magnetic signals. Furthermore, the charge noises from the surfaces would induce extra spin decoherence and hence reduce the magnetic sensitivity. Here we demonstrate that the relatively strong hyperfine coupling (130 MHz) from a first-shell 13C nuclear spin can provide an effective bias field to an NV center spin so that the clock-transition condition is broken and the charge noises are suppressed. The hyperfine bias enhances the dc magnetic sensitivity by a factor of 22 in our setup. With the charge noises suppressed by the strong hyperfine field, the ac magnetometry under zero field also reaches the limit set by decoherence due to the nuclear spin bath. In addition, the 130 MHz splitting of the NV center spin transitions allows relaxometry of magnetic noises simultaneously at two well-separated frequencies (~2.870 +/- 0.065 GHz), providing (low-resolution) spectral information of high-frequency noises under zero field. The hyperfine-bias enhanced zero-field magnetometry can be combined with dynamical decoupling to enhance single-molecule magnetic resonance spectroscopy and to improve the frequency resolution in nanoscale magnetic resonance imaging.
A nitrogen-vacancy (NV) center in diamond is a promising sensor for nanoscale magnetic sensing. Here we report electron spin resonance (ESR) spectroscopy using a single NV center in diamond. First, using a 230 GHz ESR spectrometer, we performed ensemble ESR of a type-Ib sample crystal and identified a substitutional single nitrogen impurity as a major paramagnetic center in the sample crystal. Then, we carried out free-induction decay and spin echo measurements of the single NV center to study static and dynamic properties of nanoscale bath spins surrounding the NV center. We also measured ESR spectrum of the bath spins using double electron-electron resonance spectroscopy with the single NV center. The spectrum analysis of the NV-based ESR measurement identified that the detected spins are the nitrogen impurity spins. The experiment was also performed with several other single NV centers in the diamond sample and demonstrated that the properties of the bath spins are unique to the NV centers indicating the probe of spins in the microscopic volume using NV-based ESR. Finally, we discussed the number of spins detected by the NV-based ESR spectroscopy. By comparing the experimental result with simulation, we estimated the number of the detected spins to be $leq$ 50 spins.
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