Growth and annealing study of hydrogen-doped single diamond crystals under high pressure and high temperature

A series of diamond crystals doped with hydrogen is successfully synthesized using LiH as the hydrogen source in a catalyst-carbon system at a pressure of 6.0 GPa and temperature ranging from 1255℃ to 1350℃. It is shown that the high temperature plays a key role in the incorporation of hydrogen atoms during diamond crystallization. Fourier transform infrared micro-spectroscopy reveals that most of the hydrogen atoms in the synthesized diamond are incorporated into the crystal structure as sp³--CH₂-symmetric (2850 cm^-1) and sp³ CH₂-antisymmetric vibrations (2920 cm^-1). The intensities of these peaks increase gradually with an increase in the content of the hydrogen source in the catalyst. The incorporation of hydrogen impurity leads to a significant shift towards higher frequencies of the Raman peak from 1332.06 cm^-1 to 1333.05 cm^-1 and gives rise to some compressive stress in the diamond crystal lattice. Furthermore, hydrogen to carbon bonds are evident in the annealed diamond, indicating that the bonds that remain throughout the annealing process and the vibration frequencies centred at 2850 and 2920 cm^-1 have no observable shift. Therefore, we suggest that the sp³ C--H bond is rather stable in diamond crystals.