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The study establishes that the degree of optically induced spin polarization that can be achieved for NV$^- $in 1b diamond is limited by the concentration of single substitutional nitrogen, N$^0$ . The polarization of the individual NV centres in the diamond is dependent on the separation of the NV$^-$ and the nitrogen donor. When the NV$^-$ - N$^+$ pair separation is large the properties of the pair will be as for single sites and a high degree of spin polarization attainable. When the separation decreases the emission is reduced, the lifetime shortened and the spin polarization downgraded. The deterioration occurs as a consequence of electron tunneling in the excited state from NV$^-$ to N$^+$ and results in an optical cycle that includes NV$^0$. The tunneling process is linear in optical excitation and more prevalent the closer the N$^+$ is to the NV$^-$ centre. However, the separation between the NV$^-$ and its donor N$^+$ can be effected by light through the excitation of NV$^-$ and/or ionization of N$^0$. The optical excitation that creates the spin polarization can also modify the sample properties and during excitation creates charge dynamics. The consequence is that the magnitude of spin polarization, the spin relaxation and coherence times T$_1$ and T$_2$ have a dependence on the nitrogen concentration and on the excitation wavelength. The adjacent N$^+$ gives an electric field that Stark shifts the NV$^-$ transitions and for an ensemble results in line broadening. It is observation of changes of these Stark induced effects that allow the variation in NV$^-$ - N$^+$ separation to be monitored. Spectroscopic measurements including that of the varying line widths are central to the study. They are made at low temperatures and include extensive measurements of the NV$^-$ optical transition at 637 nm, the infrared transition at 1042 nm and ODMR at 2.87 GHz.
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The characteristic transition of the NV- centre at 637 nm is between ${}^3mathrm{A}_2$ and ${}^3mathrm{E}$ triplet states. There are also intermediate ${}^1mathrm{A}_1$ and ${}^1mathrm{E}$ singlet states, and the infrared transition at 1042 nm between these singlets is studied here using uniaxial stress. The stress shift and splitting parameters are determined, and the physical interaction giving rise to the parameters is considered within the accepted electronic model of the centre. It is established that this interaction for the infrared transition is due to a modification of electron-electron Coulomb repulsion interaction. This is in contrast to the visible 637 nm transition where shifts and splittings arise from modification to the one-electron Coulomb interaction. It is also established that a dynamic Jahn-Teller interaction is associated with the singlet ${}^1mathrm{E}$ state, which gives rise to a vibronic level 115 $mathrm{cm}^{-1}$ above the ${}^1mathrm{E}$ electronic state. Arguments associated with this level are used to provide experimental confirmation that the ${}^1mathrm{A}_1$ is the upper singlet level and ${}^1mathrm{E}$ is the lower singlet level.
Significant attention has been recently focused on the realization of high precision nano-thermometry using the spin-resonance temperature shift of the negatively charged nitrogen-vacancy (NV-) center in diamond. However, the precise physical origins of the temperature shift is yet to be understood. Here, the shifts of the centers optical and spin resonances are observed and a model is developed that identifies the origin of each shift to be a combination of thermal expansion and electron-phonon interactions. Our results provide new insight into the centers vibronic properties and reveal implications for NV- thermometry.
Creation of nitrogen-vacancy (NV) centers at the nanoscale surface region in diamond, while retaining their excellent spin and optical properties, is essential for applications in quantum technology. Here, we demonstrate the extension of the spin-coherence time ($it{T}$${_2}$), the stabilization of the charge state, and an improvement of the creation yield of NV centers formed by the ion-implantation technique at a depth of $sim$15 nm in phosphorus-doped n-type diamond. The longest $it{T}$${_2}$ of about 580 $mu$s of a shallow NV center approaches the one in bulk diamond limited by the nuclear spins of natural abundant $^{13}$C. The averaged $it{T}$${_2}$ in n-type diamond is over 1.7 times longer than that in pure non-doped diamond. Moreover, the stabilization of the charge state and the more than twofold improvement of the creation yield are confirmed. The enhancements for the shallow NV centers in an n-type diamond-semiconductor are significant for future integrated quantum devices.
The novel aspect of the centre (NV-) in diamond is the high degree of spin polarisation achieved through optical illumination. In this paper it is shown that the spin polarisation occurs as a consequence of an electron-vibration interaction combined with spin-orbit interaction, and an electronic model involving these interactions is developed to account for the observed polarisation.
We studied the parameters to optimize the production of negatively-charged nitrogen-vacancy color centers (NV-) in type~1b single crystal diamond using proton irradiation followed by thermal annealing under vacuum. Several samples were treated under different irradiation and annealing conditions and characterized by slow positron beam Doppler-broadening and photoluminescence (PL) spectroscopies. At high proton fluences another complex vacancy defect appears limiting the formation of NV-. Concentrations as high as 2.3 x 10^18 cm^-3 of NV- have been estimated from PL measurements. Furthermore, we inferred the trapping coefficient of positrons by NV-. This study brings insight into the production of a high concentration of NV- in diamond, which is of utmost importance in ultra-sensitive magnetometry and quantum hybrid systems applications.
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