Hopping of the Center-of-Mass of Single G Centers in Silicon-on-Insulator

Abstract

Among the wealth of single fluorescent defects recently detected in silicon, the G center catches interest for its telecom single-photon emission that could be coupled to a metastable electron spin triplet. The G center is a unique defect where the standard Born-Oppenheimer approximation used in solid-state physics breaks down as one of its atoms, a silicon atom in interstitial position Si(i), can move between six sites. The impact of its displacement, due either to coherent tunneling or to random jumps from one site to another, on the optical properties of G centers is still largely unknown, especially in silicon-on-insulator (SOI) samples. Here, we investigate the displacement of the center of mass of the G center in silicon. By performing photoluminescence experiments at single-defect scale, we show that individual G defects in SOI exhibit several emission dipoles and zero-phonon line fine structures with splittings up to approximately 1 meV, both indicating a motion of the defect central atom over time. Combining polarization and spectral analysis at the single-photon level, we evidence that the reconfiguration dynamics is drastically different from the one of the unperturbed G center in bulk silicon where the mobile atom is fully delocalized over all six sites through tunneling. The SOI structure freezes the Si(i) delocalization of the G defect and, as a result, enables one to isolate linearly polarized optical lines. Under above-band-gap optical excitation, the central atom of G centers in SOI behaves as if it were in a six-slot roulette wheel, randomly alternating between localized crystal sites at each optical cycle. Comparative measurements in a bulk silicon sample and ab initio calculations highlight that strain is likely the dominant perturbation impacting the G center geometry. These results shed light on the importance of the atomic reconfiguration dynamics to understand and control the photoluminescence properties of the G center in silicon. More generally, these findings emphasize the impact of strain fluctuations inherent to SOI wafers for future quantum integrated photonics applications based on color centers in silicon.