Single neutral silicon-vacancy (SiV 0 ) color centers under H-, O-, or N-terminated diamond (001) surfaces were investigated using density functional theory. The formation energy calculation indicated that it is generally easier for SiV 0 to be embedded in an O-terminated diamond (001) surface as compared with H-and N-terminated surfaces, which were effected above the fifth C layer. The effects of the surface termination species on inner diamond atoms decay to be negligible below the fifth C layer. The binding energy results indicated that SiV centers exhibited rather high energetic stability once formed. Additionally, it was revealed that these three surface-terminating species had contracting or expanding effects on inner surface atoms. The calculation for density of states showed that the N-terminated diamond (001) surface served as a suitable medium for single SiV 0 to function as a single-photon source.Appl. Sci. 2019, 9, 5471 2 of 15 nanodiamonds (NDs), which fail to meet the key requirements [10] for ideal single-photon sources. In contrast, negatively charged silicon-vacancy (SiV − ) centers exhibit a sharp ZPL at 738 nm (1.681 eV) at room temperature, with a large DW factor of 0.7 [23] and a short luminescence lifetime of 1 to 4 ns [24]. Similar to SiV − , the SiV center in a neutral charge state (SiV 0 ) also possesses a high DW factor (~0.9), with most of its emitted light concentrated into the ZPL at 946 nm (1.31 eV) [25], rendering SiV 0 a promising candidate for serving as single-photon emitters.The SiV 0 has a ground state electron spin of S = 1. Single SiV defects in diamond are composed of a silicon substituting a C atom (Si) and a vacancy (V) in the nearest neighboring C site. Unlike the NV center, where the nitrogen atom is covalently bonded to its three nearest C atoms, and thus exhibiting C 3V structural symmetry, the SiV center theoretically forms a split-vacancy structure (i.e., a silicon atom located at a bond-center site) in bulk diamond (Figure 1), thus, exhibiting D 3d symmetry.Appl. Sci. 2020, 10, x FOR PEER REVIEW 2 of 15 fluorescence lifetime of up to ~24 ns [20][21][22] in nanodiamonds (NDs), which fail to meet the key requirements [10] for ideal single-photon sources. In contrast, negatively charged silicon-vacancy (SiV − ) centers exhibit a sharp ZPL at 738 nm (1.681 eV) at room temperature, with a large DW factor of 0.7 [23] and a short luminescence lifetime of 1 to 4 ns [24]. Similar to SiV − , the SiV center in a neutral charge state (SiV 0 ) also possesses a high DW factor (~0.9), with most of its emitted light concentrated into the ZPL at 946 nm (1.31 eV) [25], rendering SiV 0 a promising candidate for serving as single-photon emitters.The SiV 0 has a ground state electron spin of S = 1. Single SiV defects in diamond are composed of a silicon substituting a C atom (Si) and a vacancy (V) in the nearest neighboring C site. Unlike the NV center, where the nitrogen atom is covalently bonded to its three nearest C atoms, and thus exhibiting 3 structural symmetry, the SiV center th...