Diamond has been extensively investigated recently due to a wide range of potential applications of nitrogen-vacancy (NV) defect centers existing in a diamond lattice. The applications include magnetometry and quantum information technologies, and long decoherence time (T 2) of NV centers is critical for those applications. Although it has been known that T 2 highly depends on the concentration of paramagnetic impurities in diamond, precise measurement of the impurity concentration remains challenging. In the preset work, we show a method to determine a wide range of the nitrogen concentration (n) in diamond using a wide-band high-frequency electron spin resonance and double electron-electron resonance spectrometer. Moreover, we investigate T 2 of the nitrogen impurities and show the relationship between T 2 and n. The method developed here is applicable for various spin systems in solid and implementable in nanoscale magnetic resonance spectroscopy with NV centers to characterize the concentration of the paramagnetic spins within a microscopic volume.

We present the development of an optically detected magnetic resonance (ODMR) system, which enables us to perform the ODMR measurements of a single defect in solids at high frequencies and high magnetic fields. Using the high-frequency and high-field ODMR system, we demonstrate 115 GHz continuous-wave and pulsed ODMR measurements of a single nitrogen-vacancy (NV) center in a diamond crystal at the magnetic field of 4.2 Tesla as well as investigation of field dependence (0 − 8 Tesla) of the longitudinal relaxation time (T 1 ) of NV centers in nanodiamonds.

Nanodiamonds (NDs) are a new and attractive class of materials for sensing and delivery in biological systems. Methods for functionalizing ND surfaces are highly valuable in these applications, yet reported approaches for covalent modification with biological macromolecules are still limited, and characterizing behaviors of ND-tethered biomolecules is difficult. Here we demonstrated the use of copper-free click chemistry to covalently attach DNA strands at ND surfaces. Using site-directed spin labeling and electron paramagnetic resonance spectroscopy, we demonstrated that the tethered DNA strands maintain the ability to undergo repetitive hybridizations and behave similarly to those in solutions, maintaining a large degree of mobility with respect to the ND. The work established a method to prepare and characterize an easily addressable identity tag for NDs. This will open up future applications such as targeted ND delivery and developing sensors for investigating biomolecules.

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 ≤ 50 spins.