Electron nuclear interactions in spin-3/2 color centers in silicon carbide: A high-field pulse EPR and ENDOR study

Abstract

High-frequency pulsed electron paramagnetic resonance (EPR) and electron nuclear double resonance (ENDOR) were used to determine electron nuclear interactions on remote ligand shells of silicon and carbon in spin-3/2 color centers with an optically induced high-temperature spin alignment in hexagonal $4H$-, $6H$-, and rhombic $15R$-silicon carbide (SiC) polytypes. The EPR and ENDOR experimental data relate unambiguously to spin-3/2 centers in which the optically induced alignment of the spin-level populations occurs. The identification is based on resolved ligand hyperfine interactions with carbon and silicon nearest, next-nearest, and the more distant neighbors and on the determination of the unpaired electron spin densities. The hyperfine interactions with $^{29}\mathrm{Si}$ and $^{13}\mathrm{C}$ nuclei are unambiguously separated due to the selective population of the fine-structure levels with certain values of ${\mathrm{M}}_{\mathrm{S}}$. The signs of these interactions and, as a result, the signs of oscillating spin density at $^{29}\mathrm{Si}$ and $^{13}\mathrm{C}$ nuclei, are determined. On the basis of the EPR and optically induced ENDOR measurements, signs of the fine-structure splitting for all the centers were demonstrated, which made it possible to establish the character of optically induced spin alignment, including the inverse populations of the spin levels for these centers. The values of hyperfine interaction with $^{29}\mathrm{Si}$ and $^{13}\mathrm{C}$ nuclei, including those remote from the localization of the spin-3/2 center, are tabulated, which can be used by a number of algorithms in quantum information processing as long-term memory.