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The temperature shifts of the resonances of the NV- center in diamond

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 Added by Marcus Doherty
 Publication date 2013
  fields Physics
and research's language is English




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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.



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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.
The negatively-charged nitrogen-vacancy (NV) center in diamond is at the frontier of quantum nano-metrology and bio-sensing. Recent attention has focused on the application of high-sensitivity thermometry using the spin resonances of NV centers in nano-diamond to sub-cellular biological and biomedical research. Here, we report a comprehensive investigation of the thermal properties of the centers spin resonances and demonstrate an alternate all-optical NV thermometry technique that exploits the temperature dependence of the centers optical Debye-Waller factor.
The negatively charged nitrogen-vacancy (NV-) center in diamond has realized new frontiers in quantum technology. Here, the centers optical and spin resonances are observed under hydrostatic pressures up to 60 GPa. Our observations motivate powerful new techniques to measure pressure and image high pressure magnetic and electric phenomena. Our observations further reveal a fundamental inadequacy of the current model of the center and provide new insight into its electronic structure.
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.
The ground state spin of the negatively charged nitrogen-vacancy center in diamond has many exciting applications in quantum metrology and solid state quantum information processing, including magnetometry, electrometry, quantum memory and quantum optical networks. Each of these applications involve the interaction of the spin with some configuration of electric, magnetic and strain fields, however, to date there does not exist a detailed model of the spins interactions with such fields, nor an understanding of how the fields influence the time-evolution of the spin and its relaxation and inhomogeneous dephasing. In this work, a general solution is obtained for the spin in any given electric-magnetic-strain field configuration for the first time, and the influence of the fields on the evolution of the spin is examined. Thus, this work provides the essential theoretical tools for the precise control and modeling of this remarkable spin in its current and future applications.
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