High growth rate synthesis of diamond film containing perfectly aligned nitrogen-vacancy centers by high-power density plasma CVD

Abstract

Diamond film sensors with large volumes that are synthesized by microwave plasma chemical vapor deposition (MPCVD) and contain perfectly aligned nitrogen-vacancy (NV) ensembles are promising material for achieving highly sensitive quantum magnetometers. The step-flow growth mode of MPCVD on diamond (111) surface is required to realize aligned NV center ensembles. However, it is difficult to control the growth mode on diamond (111) surface due to the presence of twins and the conventional growth rate of aligned NV center ensembles is lower than 0.5 μm/h. In this study, we achieved a high growth rate (6.6 μm/h) of diamond (111) film containing perfectly aligned NV ensembles with high contrast (30%) by applying high power density plasma (103 W/cm3) and precisely controlling the gas flow rate ratios of CH4/H2 and N2/CH4. The growth mode was controlled to realize step flow growth by inducing the hydrogen etching of the nucleation with decreasing the CH4/H2. It was considered that increasing the microwave power density produces a large amount of atomic hydrogen and carbon precursor, leading to a high growth rate of perfectly aligned NV center diamond film. By controlling the N2/CH4 ratio, the nitrogen density in the diamond film could be precisely controlled to obtain a high contrast. Moreover, we measured the quality of the obtained diamond sensor films using the ODMR spectra and Ramsey sequence. We confirmed a high Rabi contrast (approximately 30%) and no significant decrease in T2∗ due to the deterioration of the crystallinity of the diamond film was observed. This result is promising for building material technology for highly sensitive quantum sensors with large sensor volumes.