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Direct formation of nitrogen-vacancy centers in nitrogen doped diamond along the trajectories of swift heavy ions

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 Added by Arun Persaud
 Publication date 2020
  fields Physics
and research's language is English




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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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We exposed nitrogen-implanted diamonds to beams of swift uranium and gold ions (~1 GeV) and find that these irradiations lead directly to the formation of nitrogen vacancy (NV) centers, without thermal annealing. We compare the photoluminescence intensities of swift heavy ion activated NV- centers to those formed by irradiation with low-energy electrons and by thermal annealing. NV- yields from irradiations with swift heavy ions are 0.1 of yields from low energy electrons and 0.02 of yields from thermal annealing. We discuss possible mechanisms of NV-center formation by swift heavy ions such as electronic excitations and thermal spikes. While forming NV centers with low efficiency, swift heavy ions enable the formation of three dimensional NV- assemblies over relatively large distances of tens of micrometers. Further, our results show that NV-center formation is a local probe of (partial) lattice damage relaxation induced by electronic excitations from swift heavy ions in diamond.
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size of 50~nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.
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.
201 - A. M. Edmonds 2011
The negatively charged nitrogen-vacancy (NV-) center in diamond is an attractive candidate for applications that range from magnetometry to quantum information processing. Here we show that only a fraction of the nitrogen (typically < 0.5 %) incorporated during homoepitaxial diamond growth by Chemical Vapor Deposition (CVD) is in the form of undecorated NV- centers. Furthermore, studies on CVD diamond grown on (110) oriented substrates show a near 100% preferential orientation of NV- centers along only the [111] and [-1-11] directions, rather than the four possible orientations. The results indicate that NV centers grow in as units, as the diamond is deposited, rather than by migration and association of their components. The NV unit of the NVH- is similarly preferentially oriented, but it is not possible to determine whether this defect was formed by H capture at a preferentially aligned NV center or as a complete unit. Reducing the number of NV orientations from 4 orientations to 2 orientations should lead to increased optically-detected magnetic resonance contrast and thus improved magnetic sensitivity in ensemble-based magnetometry.
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