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Register a new userObservation of the dynamic Jahn-Teller effect in the excited states of nitrogen-vacancy centers in diamond
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The optical transition linewidth and emission polarization of single nitrogen-vacancy (NV) centers are measured from 5 K to room temperature. Inter-excited state population relaxation is shown to broaden the zero-phonon line and both the relaxation and linewidth are found to follow a T^5 dependence for T up to 100 K. This dependence indicates that the dynamic Jahn-Teller effect is the dominant dephasing mechanism for the NV optical transitions at low temperatures.
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We show a marked reduction in the emission from nitrogen-vacancy (NV) color centers in single crystal diamond due to exposure of the diamond to hydrogen plasmas ranging from 700{deg}C to 1000{deg}C. Significant fluorescence reduction was observed beneath the exposed surface to at least 80mm depth after ~10 minutes, and did not recover after post-annealing in vacuum for seven hours at 1100{deg}C. We attribute the fluorescence reduction to the formation of NVH centers by the plasma induced diffusion of hydrogen. These results have important implications for the formation of nitrogen-vacancy centers for quantum applications, and inform our understanding of the conversion of nitrogen-vacancy to NVH, whilst also providing the first experimental evidence of long range hydrogen diffusion through intrinsic high-purity diamond material.
Nanodiamond crystals containing single color centers have been grown by chemical vapor deposition (CVD). The fluorescence from individual crystallites was directly correlated with crystallite size using a combined atomic force and scanning confocal fluorescence microscope. Under the conditions employed, the optimal size for single optically active nitrogen-vacancy (NV) center incorporation was measured to be 60 to 70 nm. The findings highlight a strong dependence of NV incorporation on crystal size, particularly with crystals less than 50 nm in size.
Optical and microwave double resonance techniques are used to obtain the excited state structure of single nitrogen-vacancy centers in diamond. The excited state is an orbital doublet and it is shown that it can be split and associated transition strengths varied by external electric fields and by strain. A group theoretical model is developed. It gives a good account of the observations and contributes to an improved understanding of the electronic structure of the center. The findings are important for quantum information processing and other applications of the center.
First-principles density functional theory methods are used to investigate the structure, energetics, and vibrational motions of the neutral vacancy defect in diamond. The measured optical absorption spectrum demonstrates that the tetrahedral $T_d$ point group symmetry of pristine diamond is maintained when a vacancy defect is present. This is shown to arise from the presence of a dynamic Jahn-Teller distortion that is stabilised by large vibrational anharmonicity. Our calculations further demonstrate that the dynamic Jahn-Teller-distorted structure of $T_d$ symmetry is lower in energy than the static Jahn-Teller distorted tetragonal $D_{2d}$ vacancy defect, in agreement with experimental observations. The tetrahedral vacancy structure becomes more stable with respect to the tetragonal structure by increasing temperature. The large anharmonicity arises mainly from quartic vibrations, and is associated with a saddle point of the Born-Oppenheimer surface and a minimum in the free energy. This study demonstrates that the behaviour of Jahn-Teller distortions of point defects can be calculated accurately using anharmonic vibrational methods. Our work will open the way for first-principles treatments of dynamic Jahn-Teller systems in condensed matter.
We report depth-resolved photoluminescence measurements of nitrogen-vacancy (NV$^-$) centers formed along the tracks of swift heavy ions (SHIs) in type Ib synthetic single crystal diamonds that had been doped with 100 ppm nitrogen during crystal growth. Analysis of the spectra shows that NV$^-$ centers are formed preferentially within regions where electronic stopping processes dominate and not at the end of the ion range where elastic collisions lead to formation of vacancies and defects. Thermal annealing further increases NV yields after irradiation with SHIs preferentially in regions with high vacancy densities. NV centers formed along the tracks of single swift heavy ions can be isolated with lift-out techniques for explorations of color center qubits in quasi-1D registers with an average qubit spacing of a few nanometers and of order 100 color centers per micrometer along 10 to 30 micrometer long percolation chains.
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