ABSTRACT
Powder diamonds with integrated europium atoms were synthesized at high pressure (7.7 GPa) and temperature (1800 °C) from a mixture of pentaerythritol with pyrolyzate of diphthalocyanine (C64H32N16Eu) being a special precursor. In diamonds prepared by X-ray fluorescence spectroscopy, we have found a concentration of Eu atoms of 51 ± 5 ppm that is by two orders of magnitude greater than that in natural and synthetic diamonds. X-ray diffraction, SEM, X-ray exited optical luminescence, and Raman and IR spectroscopy have confirmed the formation of high-quality diamond monocrystals containing Eu and a substantial amount of nitrogen (~500 ppm). Numerical simulation has allowed us to determine the energy cost of 5.8 eV needed for the incorporation of a single Eu atom with adjacent vacancy into growing diamond crystal (528 carbons).
ABSTRACT
We demonstrate a high-pressure, high-temperature sintering technique to form nitrogen-vacancy-nitrogen centres in nanodiamonds. Polycrystalline diamond nanoparticle precursors, with mean size of 25 nm, are produced by the shock wave from an explosion. These nanoparticles are sintered in the presence of ethanol, at a pressure of 7 GPa and temperature of 1300 °C, to produce substantially larger (3-4 times) diamond crystallites. The recorded spectral properties demonstrate the improved crystalline quality. The types of defects present are also observed to change; the characteristic spectral features of nitrogen-vacancy and silicon-vacancy centres present for the precursor material disappear. Two new characteristic features appear: (1) paramagnetic substitutional nitrogen (P1 centres with spin ½) with an electron paramagnetic resonance characteristic triplet hyperfine structure due to the I = 1 magnetic moment of the nitrogen nuclear spin and (2) the green spectral photoluminescence signature of the nitrogen-vacancy-nitrogen centres. This production method is a strong alternative to conventional high-energy particle beam irradiation. It can be used to easily produce purely green fluorescing nanodiamonds with advantageous properties for optical biolabelling applications.
ABSTRACT
The content of nitrogen-vacancy (NV-) colour centres in the nanodiamonds (DNDs) produced during the detonation of nitrogen-containing explosives was found to be 1.1 ± 0.3 ppm. This value is impressive for nanodiamonds of size < 10 nm with intentionally created NV- centres. The concentration was estimated from the electron paramagnetic resonance as determined from the integrated intensity of the g = 4.27 line. This line is related with "forbidden" ∆ms = 2 transitions between the Zeeman levels of a NV- centre's ground triplet state. Confocal fluorescence microscopy enables detection of the red photoluminescence (PL) of the NV- colour centres in nanoscale DND aggregates formed from the 5-nm nanoparticles. Subwavelength emitters consisting of NV- with sizes a few times smaller than the diffraction-limited spot are clearly distinguished. We have further observed an abrupt drop in the PL intensity when mixing and anti-crossing of the ground and excited states spin levels in NV- occurs under an applied external magnetic field. This effect is a unique quantum feature of NV- centres, which cannot be observed for other visible domain light-emitting colour centres in a diamond lattice.
