Photothermal effects during nanodiamond synthesis from a carbon aerogel in a laser-heated diamond anvil cell

Abstract: Nanodiamonds have emerged as promising materials for quantum computing, biolabeling, and sensing due to their ability to host color centers with remarkable photostability and long spin-coherence times at room temperature. Recently, a bottom-up, high-pressure, high-temperature (HPHT) approach was demonstrated for growing nanodiamonds with color centers from amorphous carbon precursors in a laser-heated diamond anvil cell (LH-DAC) that was supported by a near-hydrostatic noble gas pressure medium. However, a detailed understanding of the photothermal heating and its effect on diamond growth, including the phase conversion conditions and the temperature-dependence of color center formation, has not been reported. In this work, we measure blackbody radiation during LH-DAC synthesis of nanodiamond from carbon aerogel to examine these temperature-dependent effects. Blackbody temperature measurements suggest that nanodiamond growth can occur at 16.3 GPa and 1800 K. We use Mie theory and analytical heat transport to develop a predictive photothermal heating model. This model demonstrates that melting the noble gas pressure medium during laser heating decreases the local thermal conductivity to drive a high spatial resolution of phase conversion to diamond. Finally, we observe a temperature-dependent formation of nitrogen vacancy centers and interpret this phenomenon in the context of HPHT carbon vacancy diffusion using CB{\Omega} theory.