Identification of native defects (vacancies and antisites) in CdSiP2 crystals

Abstract

Electron paramagnetic resonance (EPR) is used to identify four native defects in single crystals of CdSiP2. This nonlinear optical material is used in optical parametric oscillators to generate tunable output in the mid-infrared. The performance of these frequency-conversion devices is limited when infrared absorption bands associated with native defects overlap a pump wavelength. Cadmium, silicon, and phosphorus vacancies and also silicon-on-cadmium antisites are present in the as-grown undoped CdSiP2 crystals. Using near-band-edge 632.8 nm light from a He-Ne laser, a paramagnetic charge state, and thus an EPR spectrum, is formed at liquid-helium temperatures for three of the four defects. The EPR spectrum from the singly ionized silicon vacancy (VSi−) is present without light and has five hyperfine lines due to equal interactions with the four neighboring 31P nuclei. In contrast, the photoinduced EPR spectrum from the singly ionized cadmium vacancy (VCd−) has a three-line hyperfine pattern due to equal interactions with only two of its four neighboring 31P nuclei. The light-induced spectrum from the singly ionized silicon-on-cadmium antisite (Si Cd+) also has a three-line hyperfine pattern, thus indicating that the unpaired spin interacts primarily with only two 31P neighbors. For the neutral phosphorus vacancy (VP 0), the unpaired spin is primarily localized on the nearest-neighbor silicon ions and the photoinduced EPR spectrum has no resolved 31P hyperfine interactions. The silicon and cadmium vacancies are acceptors, and the silicon-on-cadmium antisite and the phosphorus vacancy are donors.