Fourier Transform Limited Linewidth of Optical Transitions in Single SiV Centers in “Adamantane” Nanodiamonds

Abstract

Silicon-vacancy (SiV) color centers in diamond offer a promising system for quantum information applications owing to their intense narrowband emission and optically detectable spin states. Here, the fluorescent properties of ensembles and single SiV centers in diamonds obtained by high-pressure high-temperature synthesis from adamantane (below referred to as adamantane diamonds) are investigated at liquid-helium temperatures. Ensembles of SiV centers (~103) are studied in large diamond crystals (1–2 µm in size). Despite the large number of excited centers, the fine structure of the zero-phonon line, corresponding to four allowed optical transitions between the ground- and excited-state doublets of the SiV center, can be observed in the fluorescence spectra of these crystals. The width of individual lines is in the range of 60–80 GHz, which is explained by their inhomogeneous broadening. Single SiV centers are studied in diamond crystallites with sizes of about 200 nm. The width of the narrowest transition lines observed in the fluorescence spectra of single SiV centers under resonant excitation is almost three orders of magnitude smaller than linewidths in the spectra of SiV ensembles and is as small as 94 MHz; i.e., these lines are so narrow that their width is determined by the lifetime of the upper state of the transition. Therefore, adamantane nanodiamond features the narrowest emission line width of a single SiV center at cryogenic temperatures among other types of SiV-con-taining nanodiamonds of similar sizes obtained by the high-pressure high-temperature and chemical vapor deposition techniques.