Much literature is devoted to the applications of optically active point defects, or color centers, in nanodiamond for a wide range of disciplines including biofluorescent imaging of cellular components, quantum information data storage, and temperature, pressure, and magnetic sensing. Among the &gt;100 different color centers in nanodiamond, the negatively charged silicon divacancy (SiV-) is a remarkable single photon emitter whose advantageous optoelectronic properties are utilized in all these applications. Current technologies employ a top down approach of chemical vapor deposition grown (CVD) diamond and ion irradiation and implantation to form the desired color center. CVD grown diamond is very pure, but because of diamond’s small lattice constant and the high energies of the implantation technique, the diamond crystal lattice becomes damaged, requiring post processing techniques to correct. Doping diamond at high temperatures and pressures is also difficult due to diamond’s compact atomic lattice and low atomic diffusivities. In this work, we demonstrate a versatile, bottom-up approach to SiV- fabrication based on molecular doping of amorphous carbonaceous precursors which are converted to diamond at high-pressure, high-temperature (HPHT) conditions (&gt;15 GPa, &gt;1800K) within a laser-heated diamond anvil cell. A molecular dopant, tetraethyl orthosilicate (TEOS), incorporates silicon heteroatoms into the HPHT grown nanodiamond compared to non-doped samples fabricated under similar conditions. Pressure dependent photoluminescence confirms not only the formation of SiV- (lambda ~ 738 nm), it also provides experimental juxtaposition for ab initio quantum cluster calculations modeling the pressure dependence of the center’s zero phonon line (~0.9 meV/GPa). Aberration corrected scanning transmission electron microscopy provides images of the silicon heteroatoms on the surface and the interior of converted diamond material. These results demonstrate the versatility of this approach to doping diamond and that it can be extended to the formation of more complex color centers in diamond.

Bottom up molecular doping approach to synthesizing HPHT color centers in nanostructured diamond

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.