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Single nitrogen vacancy centers in chemical vapor deposited diamond nanocrystals

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 Added by James Rabeau
 Publication date 2007
  fields Physics
and research's language is English




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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.



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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.
Fabrication of single nickel-nitrogen (NE8) defect centers in diamond by chemical vapor deposition is demonstrated. Under continuous-wave 745 nm laser excitation single defects were induced to emit single photon pulses at 797 nm with a linewidth of 1.5 nm at room temperature. Photon antibunching of single centers was demonstrated using a Hanbury-Brown and Twiss interferometer. Confocal images revealed approximately 10^6 optically active sites/cm^2 in the synthesized films. The fabrication of an NE8 based single photon source in synthetic diamond is important for fiber based quantum cryptography. It can also be used as an ideal point-like source for near-field optical microscopy.
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.
Focused MeV ion beams with micrometric resolution are suitable tools for the direct writing of conductive graphitic channels buried in an insulating diamond bulk. Their effectiveness has been shown for the fabrication of multi-electrode ionizing radiation detectors and cellular biosensors. In this work we investigate such fabrication method for the electrical excitation of color centers in diamond. Differently from optically-stimulated light emission from color centers in diamond, electroluminescence (EL) requires a high current flowing in the diamond subgap states between the electrodes. With this purpose, buried graphitic electrode pairs with a spacing of 10 $mu$m were fabricated in the bulk of a single-crystal diamond sample using a 6 MeV C microbeam. The electrical characterization of the structure showed a significant current above an effective voltage threshold of 150V, which was interpreted according to the theory of Space Charge Limited Current. The EL imaging allowed to identify the electroluminescent regions and the residual vacancy distribution associated with the fabrication technique. Measurements evidenced bright electroluminescent emission from native neutrally-charged nitrogen-vacancy centers ($NV^0$); the acquired spectra highlighted the absence of EL associated with radiation damage.
Nitrogen-vacancy (NV-) color centers in diamond were created by implantation of 7 keV 15N (I = 1/2) ions into type IIa diamond. Optically detected magnetic resonance was employed to measure the hyperfine coupling of the NV- centers. The hyperfine spectrum from 15NV- arising from implanted 15N can be distinguished from 14NV- centers created by native 14N (I = 1) sites. Analysis indicates 1 in 40 implanted 15N atoms give rise to an optically observable 15NV- center. This report ultimately demonstrates a mechanism by which the yield of NV- center formation by nitrogen implantation can be measured.
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